Ngenxa yokukhathazeka kwemvelo nokushintsha kwamandla, ukwehla kwe-electrochemical CO2 (ECR) kumafutha namakhemikhali e-value-added multicarbon (C2+), kusetshenziswa ugesi ovuselelekayo, kuletha isisombululo esihle sesikhathi eside sokuvala umjikelezo wekhabhoni ngezinzuzo zezomnotho ezengeziwe.Kodwa-ke, ukuhlangana kwe-electrocatalytic C─C kuma-electrolyte anamanzi kuseyinselelo evulekile ngenxa yokukhetha okuphansi, umsebenzi, nokuzinza.Idizayini yama-catalyst nama-reactors inokhiye wokubhekana nalezo zinselele.Sifingqa inqubekelaphambili yakamuva yokuthi ungafinyelela kanjani ukuhlangana kwe-C─C okuphumelelayo nge-ECR, sigcizelela amasu kuma-electrocatalyst kanye ne-electrocatalytic electrode/reactor design, kanye nezindlela zabo ezihambisanayo.Ngaphezu kwalokho, kuxoxwa ngamabhodlela amanje kanye namathuba esikhathi esizayo okukhiqizwa komkhiqizo we-C2+.Sihlose ukuhlinzeka ngokubuyekezwa okuningiliziwe kwamasu okuhlanganisa e-C─C asezingeni eliphezulu emphakathini ukuze uthole intuthuko eyengeziwe kanye nogqozi kukho kokubili ukuqonda okuyisisekelo kanye nezinhlelo zokusebenza zobuchwepheshe.

Ukukhishwa ngokweqile kwe-carbon dioxide (CO2) emkhathini kubangele imiphumela emibi yemvelo futhi kuveza usongo oluphuthumayo nolungenakulungiseka emiphakathini yabantu (1, 2).Njengoba ukugxila emkhathini we-CO2 kukhuphuke kakhulu kusuka ku-270 ppm (izingxenye ngesigidi) ekuqaleni kweminyaka yawo-1800 kuya ku-401.3 ppm ngoJulayi 2015, kufinyelelwe ukuvumelana emhlabeni wonke mayelana nokugaywa kabusha kwe-carbon footprint ekhishwa imisebenzi yabantu (3, 4).Ukubona iluphu eseduze ye-carbon footprint, enye indlela engaba khona ukususa ukuncika kwamandla amanje nezimboni zamakhemikhali kude nezibaseli ezimbiwa phansi kuyise emithonjeni evuselelekayo efana nelanga nomoya (5–8).Kodwa-ke, ingxenye yamandla evela kuleyo mithombo evuselelekayo ikhawulelwe kuphela ku-30% ngenxa yesimo sayo esishintshashintshayo, ngaphandle uma izindlela zokugcina amandla amakhulu zitholakala (9).Ngakho-ke, njengenye indlela, ukuthwebula i-CO2 emithonjeni yamaphuzu efana nezitshalo zikagesi, okulandelwa ukuguqulwa kube yizinto eziphakelayo zamakhemikhali kanye nezibaseli, kungenzeka kakhulu (9-12).Ukuncishiswa kwe-Electrocatalytic CO2 (ECR) kusetshenziswa ugesi ovuselelekayo kumelela isixazululo esihle sesikhathi eside ngenxa yezimo zokusebenza ezithambile ezidingekayo ekuguquleni, lapho imikhiqizo engeziwe ingakhiqizwa ngokukhetha (13).Njengoba kuboniswe ngohlelo ku-Fig. 1, kule nqubo, i-electrolyzer ye-electrochemical iguqula i-CO2 namanzi abe amakhemikhali namafutha anikwa amandla kagesi ovuselelekayo.Uphethiloli ovelayo uyakwazi ukugcina isikhathi eside futhi ungasatshalaliswa noma udliwe, ukhiphe i-CO2 njengodoti oyinhloko, ozobanjwa futhi ubuyiselwe ku-reactor ukuze kuvalwe iluphu.Ngaphezu kwalokho, okuwumphumela wokuphakelayo kwamakhemikhali e-molecule encane [isb, i-carbon monoxide (CO) kanye ne-formate] evela ku-ECR ingasetshenziswa njengezinto zokusetshenziswa ukuze kuhlanganiswe amakhemikhali ayinkimbinkimbi.

Amafutha namakhemikhali kungafinyelelwa ku-ECR ngomjikelezo wekhabhoni ovaliwe onikwa amandla yimithombo yamandla avuselelekayo njengelanga, umoya, kanye namanzi.Ubunjiniyela bamaselula nobunjiniyela be-catalyst budlala indima ebalulekile ukuze kuthuthukiswe ukukhetha, umsebenzi, nokusebenza kahle kokuguqulwa kwe-CO2 ibe imikhiqizo ye-C2+ ene-value enokuminyana okuphezulu kwamandla.

Nokho, i-CO2 iyi-molecule yomugqa ezinzile enesibopho esiqinile se-C═O (750 kJ mol−1) (14), okwenza kube nzima ukuguqulwa kwe-electrochemical.Ngakho-ke, idinga umgoqo wokwenza kusebenze okuphezulu, okubuye kuholele ekusetshenzisweni okubalulekile (15).Ngaphezu kwalokho, i-ECR ku-electrolyte enamanzi ihilela izinqubo zokudlulisa ama-electron/proton amaningi kanye nenani lezithako ezihlukene zokusabela ezingaba khona kanye nemikhiqizo (16-18), okwenza kube yinkimbinkimbi kakhulu.Ithebula 1 lifingqa ukusabela kwengxenye ye-electrochemical thermodynamic yemikhiqizo eyinhloko ye-ECR, okuhlanganisa i-CO, i-methane (CH4), i-methanol (CH3OH), i-formic acid (HCOOH), i-ethylene (C2H4), i-ethanol (CH3CH2OH), njalonjalo, amandla ahambisanayo ajwayelekile e-redox (19).Ngokuvamile, phakathi nenqubo ye-ECR, ama-molecule e-CO2 aqale adsorption futhi asebenzisane nama-athomu endaweni ye-catalyst ukuze akhe i-*CO2−, okulandelwa ukudluliswa okuhlukahlukene okulandelanayo kwama-proton kanye/noma ama-electron emikhiqizweni ehlukene yokugcina.Isibonelo, i-CH4 kukholakala ukuthi yakheka ngalezi zindlela ezilandelayo: CO2 → *COOH → *CO → *CHO → *CH2O → *CH3O → CH4 + *O → CH4 + *OH → CH4 + H2O (20).

Umfanekiso we-2A ufingqa ukusebenza kahle kwe-Faradaic (FE) ngaphansi kwamazinga ahlukene okukhiqiza (ukuminyana kwamanje) kuma-electrocatalysts e-ECR abikiwe, amele ukukhetha komkhiqizo kokusabela (21-43).Ngokuphawulekayo, nakuba ama-electrocatalyst asezingeni eliphezulu angaguqula i-CO2 ibe yimikhiqizo ye-C1 (CO noma ifomathi) ene-FE engaphezu kuka-95% ngaphansi kwezinga eliphezulu lokukhiqiza (>20 mA cm−2 kuseli lohlobo lwe-H kanye > no-100 mA cm− 2 yeseli eligelezayo) (9, 21, 22, 25, 28, 44, 45), ukukhetha okuphezulu (>90%) nokukhiqizwa okuphumelelayo kwamakhemikhali e-multicarbon (C2+) atholakalayo kakhulu kuze kube manje.Lokhu kungenxa yokuthi ukuhlangana nemikhiqizo ye-C2+ kudinga ukufika kanye nokukhangiswa kwama-molecule e-CO2 ambalwa phezulu, ukuguqulwa kwesinyathelo ngesinyathelo, kanye nokuma kwendawo (13).Ukucacisa, njengoba kuboniswe ku-Fig. 2B, ukusabela okulandelayo kwe-*CO intermediates kunquma imikhiqizo yokugcina ye-C2+ ye-ECR.Ngokuvamile, i-C2H6 ne-CH3COO− yabelana ngokulinganayo *CH2 okumaphakathi, okukhiqizwa ezinyathelweni zokudlulisa ama-electron ahlanganiswe ne-proton ze-*CO.I-protonation eyengeziwe ye-*CH2 inikeza *CH3 okumaphakathi, okuholela ekwakhekeni kwe-C2H6 nge-*CH3 dimerization.Ngokungafani nesizukulwane se-C2H6, i-CH3COO− yenziwa ngokufakwa kwe-CO ku-*CH2.I-*CO dimerization isinyathelo esinquma isilinganiso sokwakheka kwe-C2H4, CH3CH2OH, kanye ne-n-propanol (n-C3H7OH).Ngemva kochungechunge lwezinyathelo zokudlulisa ama-electron kanye ne-protonation, i-*CO─CO dimer yenza *CH2CHO intermediate, esebenza njengesinyathelo sokunquma ukukhetha ku-C2H4 kanye ne-C2H5OH.Ukwengeza, kutholwe ukuthi ukwehlisa *CH2CHO ukuya ku-C2H4 kunomkhawulo ophansi wamandla kunokuguqula *CH3CHO iye ku-C2H5OH (46), okungase kuchaze i-FE ephakeme ye-C2H4 ngaphezu kwe-C2H5OH kuma-catalyst amaningi ethusi.Ngaphezu kwalokho, izimaphakathi ze-C2 ezizinzile zingadlulisela ku-n-C3H7OH ngokufaka i-CO.Izindlela zokusabela eziyinkimbinkimbi nezingalawuleki ngesikhathi sokwakheka kwamakhemikhali e-C2+ ngokuyinhloko kungenxa yezimvume eziningi ezengeziwe kumasayithi e-protonation, kanye nokubandakanyeka okungenzeka kwesinyathelo esingenawo ugesi (19, 47).Kanjalo, ukuklanywa kwama-electrocatalyst akhethwa kakhulu kuyimfuneko yokwakhiwa komkhiqizo othize we-C2+ ngesivuno esikhulu.Kulesi sibuyekezo, sihlose ukugqamisa inqubekelaphambili yakamuva yamasu ekwakhiweni kwe-electrocatalyst yokukhiqiza umkhiqizo okhethiwe we-C2+ nge-ECR.Siphinde sinikeze isifinyezo sokuqondwa kwezinqubo ezihlobene.Idizayini ye-Electrode ne-reactor izophinde igcizelelwe ukuze kuboniswe indlela yokufinyelela ukusebenza kahle, okuzinzile, nokukhulu kwe-ECR.Ngaphezu kwalokho, sizoxoxa ngezinselele ezisele kanye namathuba esikhathi esizayo okuguqulwa kwe-electrochemical ye-CO2 ibe amakhemikhali e-value-added C2+.

(A) I-FE ngaphansi kwamazinga ahlukene okukhiqiza (ukuminyana kwamanje) kuma-electrocatalyst e-ECR abikiwe (21–43, 130).(B) Izindlela eziningi ezingenzeka ze-C2+ phakathi ne-ECR.Ikhiqizwe kabusha ngemvume evela ku-American Chemical Society (47).

Ukuguqulwa kwe-Electrocatalytic ye-CO2 ibe izinto zokubasa zamakhemikhali kanye nezimpahla zokudla kuwubuchwepheshe obungaba khona ukuze kuzuzwe umjikelezo wamandla we-carbon-neutral (11).Kodwa-ke, i-FE yemikhiqizo ye-C2+ isekude ekusebenziseni okungokoqobo, lapho ama-catalysts asezingeni eliphezulu avumela ukukhiqizwa kwemikhiqizo ye-C2 cishe nge-60% FE (13, 33), kuyilapho ukukhiqizwa kwe-C3 kunqunyelwe ngaphansi kuka-10% I-FE (48, 49).Ukuhlanganiswa okuncishisiwe kwe-CO2 kumikhiqizo ye-C2+ kudinga ama-catalysts ahlukahlukene anezakhiwo ezididiyelwe kakhulu ze-morphological and electronic (50, 51).Indawo ye-catalytic idinga ukunqamula ubudlelwano bokukala phakathi kwabamaphakathi (47, 52, 53).Ngaphezu kwalokho, ukuze kuzuzwe ukwakheka kwebhondi ye-C─C, ukusabela okumuncwe okuphakathi endaweni ye-catalyst kumele kube seduze komunye nomunye.Ngaphezu kwalokho, indlela esuka endaweni emaphakathi ekhangisiwe eya kumkhiqizo othize we-C2+ idinga ukulawulwa kahle ngenxa yezinyathelo eziningi zokudlulisa ama-electron asizwa yi-proton.Uma kucatshangelwa ubunkimbinkimbi obuphezulu bokwehliswa kwe-CO2 kumikhiqizo ye-C2+, ama-electrocatalyst kufanele enziwe ngokucophelela ukuze kwandiswe ukukhetha.Ngokuya ngezinhlobo ezimaphakathi kanye nokwakheka kwamakhemikhali, sihlukanisa imikhiqizo ye-C2+ kuma-multicarbon hydrocarbons nama-oxygeates (4, 54).Ukuze usondele kuma-electrocatalysts asebenza kahle kakhulu ekukhiqizweni kwe-molecule ye-C2+, kukhonjisiwe amasu amaningi okuklama i-catalyst, njenge-heteroatom doping, i-crystal facet regulation, i-alloy/dealloying, i-oxidation state tuning, nokulawulwa kwe-ligand ebusweni, kukhonjisiwe (35, 41, 55-61) .Idizayini efanelekile kufanele icabangele imiphumela eshiwo ngenhla futhi yandise izinzuzo.Uma kungenjalo, ukuqonda ukuthi yiziphi izisusa ezisebenzayo zesayithi eziholela ekuziphatheni okuyingqayizivele okunjalo kungase kukhanyise nakakhulu idizayini ye-catalyst enembile yokuhlanganisa i-C─C.Ngakho-ke, indlela yokuklama i-ECR catalyst emikhiqizweni ethile (ama-multicarbon hydrocarbon nama-oxygenates) kanye nendlela ehlobene nayo kuzoxoxwa ngayo kule ngxenye.

I-C2+ hydrocarbons, njenge-C2H4, ingamakhemikhali e-nexus ezimboni zamakhemikhali ezihlukahlukene, njengokukhiqizwa kwe-polyethylene (62, 63).Ngaphandle kwalokho, ingasetshenziswa ngokuqondile njengesibaseli sokushisela noma into exutshwe negesi yemvelo (12).I-Hydrogenation ye-CO (i-Fischer-Tropsch synthesis) ne-CO2 isetshenziselwe ukukhiqiza ama-hydrocarbon e-C2+ isikhathi eside esikalini sezimboni kodwa inselelo yokusetshenziswa kwamandla okuphezulu nomthelela wemvelo (64).Ngokuphambene kakhulu, ukuncishiswa kwe-electrochemical CO2 kusetshenziswa amandla avuselelekayo kunikeza umzila ohlanzekile futhi ozinzile.Umzamo omkhulu wenziwe ukuze kuthuthukiswe ama-electrocatalyst asebenza kahle abheke ku-C2+ hydrocarbons (32, 33, 65–70).

Ama-electrocatalysts e-Bimetallic aphenywe kabanzi ukuze aphule ubudlelwano bokulinganisa ngesikhathi sokuguqulwa kwe-electrochemical CO2, okungakwazi ukuzinzisa ukhiye ophakathi futhi wehlise i-overpotential futhi, ngaleyo ndlela, ukwandisa ukukhetha (71-74).Ngenkathi uchungechunge lwezinto ze-alloy ezihlanganisa i-Au-Cu, i-Ag-Cu, i-Au-Pd, ne-Cu-Pt ziboniswe ukusebenza kahle okuphezulu kwe-C1 ngokuzinzisa okuphakathi okubalulekile (73, 75), umphumela we-alloy ekubunjweni kwe-C2+ hydrocarbon kubonakala sengathi. kube nzima kakhulu (76).Isibonelo, kusistimu ye-Cu-Ag bimetallic, ukusatshalaliswa komkhiqizo kungalawulwa kalula ngokulungisa isilinganiso se-athomu engaphezulu ye-Ag ne-Cu (77).Isampula elingaphezulu kwe-Cu-rich lincanyelwa ukukhiqizwa kwe-hydrocarbon, kuyilapho imikhiqizo yendawo engaphezulu kwe-Ag-rich ibuswa yi-CO, egqamisa ukubaluleka kwesilinganiso se-athomu kuma-electrocatalyst e-ECR ahlanganisiwe.Umthelela wejiyomethri obangelwa ukuhlelwa kwe-athomu yendawo ungathinta kakhulu amandla okubopha okuphakathi.U-Gewirth kanye nozakwabo (36) babonise ukuthi ama-alloys e-Cu-Ag avela ku-electrodeposition elawulwa yi-additive abonise ~ 60% FE ye-C2H4 ku-alkaline flow electrolyzer (Fig. 3, A no-B).Kulesi simo, ukukhetha okuthuthukisiwe kwe-C2H4 kungafinyelelwa nge-morphology nokushuna kokulayisha kwe-Ag.Izingosi ze-Ag kukholakala ukuthi zidlala indima yomgqugquzeli wokwakhiwa kwe-CO ngesikhathi se-ECR.Bese, ukutholakala okuphelele kwe-CO ephakathi nendawo kungasiza ukuhlangana kwe-C─C ku-Cu engumakhelwane.Ngaphandle kwalokho, i-Ag ingase futhi ikhuthaze ukwakheka kwe-Cu2O ngesikhathi se-Cu-Ag catalyst synthesis (Fig. 3C), okuholela ekuthuthukiseni ukusebenza kahle kokukhiqiza kwe-C2H4.Lokhu kusebenzisana kuvula amathuba amasha okuthuthukisa ama-C─C coupling catalysts.Ngaphezu kwalokho, iphethini yokuxuba yezinsimbi ezihlukene ohlelweni lwe-alloy ingase futhi inqume ukusatshalaliswa kwemikhiqizo ye-ECR.Kusetshenziswa ingxubevange ye-Pd-Cu njengesibonelo (I-Fig. 3D), u-Kenis kanye nozakwabo (71) babonise ukuthi i-catalyst ehlukaniswe ngesigaba ye-Pd-Cu inganikeza ukukhetha okuphezulu kakhulu (~50%) kwe-C2H4 uma kuqhathaniswa nokuhlelekile nokungahlelekile. ozakwabo.Ngokuvumelana nethiyori ye-d-band, ngokuvamile, insimbi eguquguqukayo enesikhungo se-d-band ephansi ibonisa ukubophezela okubuthakathaka kwe-in situ ekhiqizwe okumaphakathi endaweni yensimbi (78).Ngenkathi ingxubevange ye-Pd-Cu ehlukaniswe ngesigaba ibonise ukukhetha okufanayo kwe-catalytic kanye nomsebenzi we-CO nge-Cu nanoparticles (NPs), inikeze amandla okubopha ahluke ngokuphelele kuma-intermediates ngokushuna kwe-Pd.Njengoba kuboniswe ku-Fig. 3E, i-Cu-Pd alloy ehlukaniswe ngesigaba ibonise isikhungo se-d-band esiphansi kunazo zonke, kanti leso se-Cu NP siphezulu kakhulu.Iphakamisa ukuthi ingxubevange ye-Cu-Pd ehlukaniswe ngesigaba inamandla aphansi okubopha okuphakathi kwe-CO.Lokhu kubheka kusho ukuthi umphumela wejiyomethri kanye nesakhiwo ungase udlale indima enkulu kunomphumela we-elekthronikhi wokuthuthukisa ukukhetha kwe-hydrocarbon kukesi yengxubevange ye-Cu-Pd ehlukaniswe ngesigaba.Kuze kube manje, kuphela ithusi elimsulwa noma i-alloy-based alloy ebonisa ukukhetha okuphakeme nomsebenzi wokunciphisa i-electrochemical ye-CO2 ukuya ku-C2+ hydrocarbons.Ngakho-ke, kudingekile kakhulu ukuthuthukisa i-electrocatalyst yenoveli yokukhiqizwa kwe-C2+ hydrocarbon evela ku-ECR.Ikhuthazwe yi-CO2 hydrogenation, ucwaningo lokuqala lubonise ukuthi ingxubevange ye-Ni-Ga enezigaba ezihlukene ingasetshenziselwa isizukulwane se-C2H4 (79).Kubonise ukuthi ifilimu ye-Ni5Ga3 inganciphisa i-CO2 ku-C2H4 kanye ne-ethane (C2H6).Nakuba i-FE ebheke ku-C2+ hydrocarbons ingaphansi kuka-5%, ingase ivule imigqa emisha yokuhlolwa kwe-electrocatalyst ngasekuhlanganiseni kwe-C─C ngokusekelwe kumphumela we-alloy.

(A kuya ku-C) Ama-Cu-Ag bimetallic catalysts akhiwe nge-electrodeposition elawulwa ngokungeziwe: (A) i-electron microscopy (SEM) yokuskena ye-Cu wire, i-Cu-Ag poly, ne-Cu-Ag wire kanye (B) ehambisana ne-C2H4 FE.(C) I-EXAFS ibonise ukuthi intambo ye-Cu-Ag yayixutshwe ngendlela efanayo futhi i-Cu(I) oxide yethulwa.(A) kuya ku-(C) akhiqizwa kabusha ngemvume evela ku-American Chemical Society (36).(D no-E) Ama-Cu-Pd ama-catalyst anamaphethini ahlukene okuxutshwa: (D) Umdwebo, izithombe ze-electron microscopy (TEM) yokudlulisela, namamephu wesici se-spectroscopy esihlakazeka amandla wama-alloys e-Cu-Pd a-odiwe, angahlelekile, futhi ahlukaniswe ngezigaba kanye (E ) i-surface valence band photoemission spectra kanye nesikhungo se-d-band (umugqa oqondile) wama-alloys e-Cu-Pd ahlobene nezinga le-Fermi.(D) kanye no-(E) akhiqizwe kabusha ngemvume evela ku-American Chemical Society (71).noma, amayunithi angenasizathu.

Ngaphandle komphumela we-alloy, ukukhohlisa izifunda ze-oxidation kungomunye umgomo omkhulu wokushuna ukusebenza kwama-electrocatalyst, okungathinta ukwakheka kwe-elekthronikhi yendawo.Isibonelo sokuqala se-oxidation state tuning ye-catalyst ukusebenzisa izinto eziphuma ku-oxide.Izinhlobo ze-oksijini ezisele endaweni noma ngaphansi kwe-catalyst ngemva kokunciphisa in situ zingalawula isimo se-oxidation sesikhungo sensimbi.Isibonelo, i-Cu ye-plasma-oxidized ibonise ukukhetha okungaphezu kuka-60% ku-C2H4, okuphawulwe ku-Cu+ (37) engazweli ekunciphiseni.Ukuqinisekisa ukuthi i-Cu + iyipharamitha eyinhloko yokukhetha okuphezulu kwe-ethylene, senze ukuhlolwa kokulawula sisebenzisa i-plasma ehlukile (Fig. 4A).I-spectroscopy yokumuncwa kwe-x-ray eqinile ye-in situ yaphinde yabonisa ukuthi ama-oxide ayinsalela kungqimba (olungaphansi) olungaphezulu azinzile uma kuqhathaniswa nesimo sokuncipha, nenani elibalulekile lezinhlobo ze-Cu+ ezisele ngemva kwehora elingu-1 lokuncishiswa ngamandla amakhulu uma kuqhathaniswa angu-−1.2 V uma kuqhathaniswa nokuhlehlakeleka. i-hydrogen electrode (RHE).Ngaphezu kwalokho, i-electroredeposition of copper kusukela ku-sol-gel yethusi oxychloride kuphinde kwaqinisekisa ukuthi izinhlobo ezizinzile ze-Cu+ zingathuthukisa ukukhetha kwe-C2H4 (61).Isimo se-oxidation se-catalyst yethusi ngaphansi kwamandla ahlukene asetshenzisiwe salandelelwa kusetshenziswa i-spectroscopy yokumuncwa kwe-x-ray exazululwe ngesikhathi.Isinyathelo sokuqala soshintsho ukusuka ku-Cu2+ ukuya ku-Cu+ siyashesha kakhulu;nokho, ukuncishiswa okwengeziwe kwe-electrochemical kwezinhlobo ze-Cu+ kuya ku-Cu0 kuhamba kancane kakhulu.Cishe u-23% wezinhlobo ze-Cu+ zisala ngisho nangemva kokuncishiswa njalo kwehora eli-1 ngaphansi kuka-−1.2 V uma kuqhathaniswa ne-RHE (Fig. 4B).Ucwaningo lwezemishini lwembule ukuthi ukuxhumana phakathi kwe-Cu+ ne-Cu0 kuholela ekukhangekeni kwe-electrostatic phakathi kweziphakathi njengoba i-athomu engu-C ye-*CO@Cu+ ishajwe kahle, kanti leyo ye-*CO@Cu0 ishajwe kabi (80), yona, ekhuthaza ukushajwa. Ukwakheka kwebhondi ye-C─C futhi ngaleyo ndlela kukhiqiza ama-hydrocarbon e-C2+.Ngokungeziwe ezintweni ezisuselwe ku-oxide, i-copper nitride (Cu3N) nayo yasetshenziswa ukuze kuzuzwe (sub)surface izinhlobo ze-Cu+ ukuze kwehliswe umgoqo wamandla we-dimerization we-*CO (81).Ngaphezu kwalokho, uma kuqhathaniswa ne-Cu + etholakala nge-oxide, izinhlobo ze-Cu + ezitholakala ku-Cu3N zizinzile nakakhulu (Fig. 4C).Ngenxa yalokho, i-catalyst yethusi etholakala ku-nitride ibonisa i-FE ye-39 ± 2% ye-C2H4, idlula i-Cu ehlanzekile (~ 23%) kanye ne-Cu etholakala nge-oxide (~ 28%).Ngokufana nohlelo olushiwo ngenhla lwe-Cu+/Cu, i-boron iye yasetshenziswa njenge-heteroatom dopant ukwethula kanye nokuzinzisa i-Cuδ+ (41).Isimo se-oxidation esimaphakathi sethusi singalawulwa ukusuka ku-+0.25 kuya ku-+0.78 ngokushintsha ukugcwala kwe-boron dopant.Ukuminyana okucatshangelwayo kwezifunda kubonise ukuthi ama-electron adluliswa esuka ethusi aye ku-boron, okuholela kumasayithi ethusi afakwe nge-dopant.Ikhopha ye-boron-doped ibonise amandla okwakheka anyukile e-*CHO emaphakathi futhi, ngaleyo ndlela, yacindezela indlela yokusabela emikhiqizweni ye-C1.Ngaphezu kwalokho, ingakhuphula ukukhetha kuma-multicarbon hydrocarbon ngokunciphisa *CO dimerization reaction energy (Fig. 4D).Ngokuthuthukisa isilinganiso sesimo se-oxidation ebusweni bethusi, i-C2 FE ephezulu engu-~80% ene-~53% C2H4 ingafinyelelwa ngaphansi kwesilinganiso sesimo se-copper oxidation esingu-+0.35 (Fig. 4E).Kuze kube manje, amasayithi asebenzayo ekhopha akhonjwe njenge-Cu0, Cuδ+, kanye/noma i-interface yawo ye-ECR ezifundweni ezihlukene (39, 41, 42, 81, 82).Kodwa-ke, iyiphi indawo esebenzayo okusaxoxwa ngayo.Nakuba i-heteroatom doping–induced Cuδ+ catalysts ikhonjiswe ukuthi iyasebenza kakhulu ku-ECR kumikhiqizo ye-C2+, umthelela we-synergistic osuka ekulimaleni okukhiqizwa ngesikhathi esisodwa nokuxhumana kufanele kucatshangelwe.Ngakho-ke, ukulinganisa okuhlelekile kwezinhlamvu ze-operando kufanele kuthuthukiswe ukuze kuhlonzwe isikhungo esisebenzayo endaweni yethusi futhi kuqashwe ukuguqulwa okungaba khona kwezindawo ezisebenzayo ngaphansi kwezimo zokusabela.Ngaphandle kwalokho, ukuzinza kwethusi elifakwe kahle kungenye into ekhathazayo ngaphansi kwezimo zokunciphisa i-electrochemical.Indlela yokwenza ama-catalyst ngeziza ezizinzile ze-Cuδ+ kuseyinselele.

(A) Isifinyezo sokukhethwa kwe-C2H4 kwama-catalyst ethusi asetshenziswe nge-plasma ahlukene.Ikhiqizwe kabusha ngemvume evela ku-Nature Publishing Group (37).Amabha esikali, 500 nm.(B) Isilinganiso sezimo ze-Cu oxidation ezihlobene nesikhathi sokusabela kokuthi −1.2 V uma kuqhathaniswa ne-RHE ku-electroredeposited copper.Ikhiqizwe kabusha ngemvume evela ku-Nature Publishing Group (61).(C) Isilinganiso sohlobo lwe-Cu+ olunomsebenzi wesikhathi sokusabela kokuthi −0.95 V uma kuqhathaniswa ne-RHE kokuthi Cu-on-Cu3N noma Cu-on-Cu2O.Ikhiqizwe kabusha ngemvume evela ku-Nature Publishing Group (81).(D) I-Boron doping ikwazile ukushintsha isilinganiso samandla okukhangisa we-CO endaweni yethusi futhi yehlisa amandla e-CO─CO we-dimerization.I-1[B], 2[B], 3[B], 4[B], kanye no-8[B] ibhekisela ekuhlanganiseni kwe-boron doping engaphansi komhlaba kuma-catalysts ethusi, okwakungu-1/16, 1/8, 3/ 16, 1/4, no-1/2, ngokulandelana.(E) Ubudlelwano phakathi kwesimo se-oxidation kanye ne-FE yemikhiqizo ye-C2 noma ye-C1 kuma-catalyst ethusi e-boron-doped.(D) kanye no-(E) akhiqizwa kabusha ngemvume evela ku-Nature Publishing Group (41).(F) Izithombe ze-SEM zamafoyili ethusi anobukhulu obuhlukahlukene bamafilimu e-Cu2O ngaphambi (phezulu) nangemuva (phansi) kwe-ECR.Ikhiqizwe kabusha ngemvume evela ku-American Chemical Society (83).

Ngaphandle kwesakhiwo se-elekthronikhi, izinto ezitholakala nge-oxide nazo zingaholela ekuguqukeni kwe-morphology noma kwesakhiwo ngesikhathi senqubo yokunciphisa i-in situ.Ngokombono we-morphology noma ukwakheka, ukusebenza okuthuthukisiwe kwe-electrochemical kwama-electrocatalyst asuselwa ku-oxide kuye kwathiwa kudalwe ukwakhiwa kwemingcele esebenzayo yokusanhlamvu, imiphetho, nezinyathelo (83-85).U-Yeo kanye nozakwabo (83) babike ukuhlangana kwe-C─C okukhethiwe kumafilimu e-Cu2O ane-electrodeposited enobukhulu obuhlukahlukene (Fig. 4F).I-spectroscopy ye-in situ Raman iveze ukuthi ingaphezulu lamafilimu e-Cu2O lehlisiwe laba yi-Cu0 eyinsimbi ezinzile ngesikhathi se-ECR (83).Ngenxa yalokho, i-Metallic Cu0 iqinisekisiwe njengesikhungo esisebenzayo esikhundleni sezinhlobo ze-Cu+ noma isixhumi esibonakalayo se-Cu+/Cu0.Enqubweni yokunciphisa i-Cu2O ibe yi-Metallic Cu0, indawo ye-catalyst cishe yenza izinyathelo, imiphetho, kanye namasimu.Kwavezwa ukuthi izinyathelo ezakhiwe namaphethelo asebenza kakhulu kunamasimu, asuka ekubopheni kwawo okuqinile nge-*CO, engaqhubekisela phambili i-hydrogenate *CO ukuya ku-*CHO noma *CH2O.Ngaphandle kwalokho, ama-athomu e-Cu onqenqemeni angumgqugquzeli wokuthuthukisa ukwakheka kwe-*CHO kanye ne-*CH2O.Umsebenzi wangaphambilini uphakamise ukuthi *CHO kanye *CH2O intermediate zivuna C─C coupling kune-CO in kinetics (86).Ngokulawula i-surface morphology, amandla e-chemisorption we-*CHO kanye ne-*CH2O intermediate angathuthukiswa.Kulolu cwaningo, ababhali bathole ukuthi i-FE ye-C2H4 yehle isuka ku-40 yaya ku-22% lapho benyusa ukushuba kwefilimu elincanyana le-Cu2O lisuka ku-0.9 laya ku-8.8 μm.Lokhu kungenxa yokugxila kwe-Cu edidiyelwe ephansi ekhuphuke ngokunyuka kogqinsi lwe-Cu2O.Lawa ma-athomu angaxhumene kahle angabopha ngokuqinile no-H futhi, ngalokho, akhethwa kakhulu ekuguqukeni kwe-hydrogen kunokuhlangana kwe-C─C.Lo msebenzi ubonise ukuthi i-catalyst yethusi etholakala nge-oxide ingathuthukisa kakhulu ukukhetha kwe-C2H4 ngokwakhiwa kabusha kwe-surface morphology esikhundleni sokwethula izinhlobo ze-Cuδ+ ezikhokhiswayo.Kusetshenziswa ama-catalysts atholakala ku-oxide, i-ethane (C2H6) nayo iye yakhiqizwa ngokukhetha ngosizo lwe-palladium(II) chloride (PdCl2) additive in electrolyte (34).Kubonise ukuthi i-PdClx ekhangisiwe ebusweni be-Cu2O-derived Cu idlale indima ebalulekile ekuziphendukeleni kwemvelo kwe-C2H6.Ngokucacile, i-CO2 yehliswe okokuqala yaba yi-C2H4 kumasayithi e-Cu2O-derived asebenzayo e-Cu, kwase kuthi i-C2H4 eyakhiwe izokwenziwa i-hydrogenated ngosizo lwe-adsorbed PdClx ukukhiqiza i-C2H6.I-FE ye-C2H6 inyuke isuka ku-<1 yaya ku-30.1% ngosizo lwe-PdCl2.Lo msebenzi uphakamisa ukuthi inhlanganisela ye-ECR catalyst echazwe kahle kanye nesengezo se-electrolyte ingase ivule amathuba amasha okukhiqiza umkhiqizo othize we-C2+.

I-morphology kanye/noma ukulawulwa kwesakhiwo kumele elinye isu lokushintsha ukukhetha kanye nomsebenzi.Ukulawula usayizi, umumo, nezici eziveziwe ze-catalyst kukhonjiswe kabanzi ukuze kuthuthukiswe ukusebenza kwe-ECR (58, 87, 88).Isibonelo, i-Cu(100) facet ithandwa kakhulu esizukulwaneni se-C2H4, kuyilapho umkhiqizo obuswa kakhulu ovela ku-Cu(111) catalyst i-methane (CH4) (87).Ocwaningweni lwe-Cu nanocrystals enobumo nobukhulu obuhlukahlukene, i-Buonsanti kanye nabasebenza nabo (58) baveze ukuncika kosayizi we-nonmonotonic we-C2H4 ukukhetha ku-nanocrystals yethusi emise okwe-cube (Fig. 5A).Ngaphakathi, ama-cubic Cu nanocrystals abonise umsebenzi ophezulu we-C2H4 nokukhetha kunama-Cu nanocrystals ayindilinga ngenxa yobukhulu be-facet (100).Usayizi omncane wekristalu we-cubic Cu unganikeza umsebenzi ophezulu ngenxa yokwanda kokugxila kwezindawo ezisezingeni eliphansi ezixhumene, njengamakhona, izinyathelo, nama-kinks.Kodwa-ke, i-chemisorption enamandla yezindawo ezixhumene kancane yayihambisana nokukhethwa okuphezulu kwe-H2 kanye ne-CO, okuholele ekwehleni kwayo yonke i-hydrocarbon FE.Ngakolunye uhlangothi, isilinganiso sezindawo ezisemaphethelweni nezindawo zendiza sehle ngokunyuka kosayizi bezinhlayiyana, okuphinde kuthinte ukusebenza kokukhiqizwa kwe-C2H4.Ababhali babonise ukuthi ama-nanocubes ethusi anosayizi omaphakathi anobude obuyi-44-nm onqenqemeni abonise ukukhetha okuphezulu kwe-C2H4 ngenxa yebhalansi elungiselelwe phakathi kosayizi wezinhlayiyana kanye nokuminyana kwezingosi ezisemaphethelweni.Ngaphezu kwalokho, i-morphology ingaphinda ithinte i-pH yendawo kanye nokuhamba ngobuningi ngesikhathi se-ECR.Kubonisiwe ukuthi i-pH yendawo ephezulu eduze nendawo ye-catalyst, ebangelwa i-in situ ekhiqizwe i-OH−, icindezela indlela yokusabela ebandakanyekayo ye-proton.Ngenxa yalokho, ukwakheka kwe-C2+ hydrocarbon *nge-CO dimerization kungathuthukiswa, futhi i-CH4 eyenziwe *nge-COH emaphakathi ingase ivinjwe.Ama-array e-copper nanowire (Fig. 5B) aboniswe ukuze afinyelele i-pH yendawo ekhuphukile (68).Njenge-electrolyte evame ukusetshenziswa, isixazululo se-CO2 saturated potassium bicarbonate (KHCO3) sizonciphisa ngokushesha i-OH− (HCO3− + OH− = CO32− + H2O) futhi yehlise i-pH yendawo.Nge-microstructure emide, ukuhlukaniswa kwe-HCO3− ku-Cu nanowire arrays kungase kuncishiswe ngandlela thize ukuze umphumela wokungathathi hlangothi we-OH- yendawo uzocindezelwa ngezinga elithile.Ngokwesisekelo sesimiso esifanayo, amameshi ethusi anama-mesopores alawulwa ngokunembile (Umfanekiso 5C) abonise i-FE ethuthukisiwe yokukhiqizwa kwe-C2H4 noma i-C2H6 (32).Kubonise ukuthi i-pH yendawo endaweni ye-electrode inganyuswa ngokunciphisa ububanzi bembotshana, okuholela ekwehleni komkhiqizo we-C1 we-FE kanye nomkhiqizo we-C2 othuthukisiwe we-FE.Ngaphandle kwalokho, ngokwandisa ukujula kwembotshana, umkhiqizo omkhulu wokunciphisa ungashunwa usuka ku-C2H4 uye ku-C2H6.I-FE ye-C2H6 yayiphezulu ngokufinyelela ku-46%.Njengoba amakhemikhali evalelwe ngaphakathi kwezimbotshana ngesikhathi se-ECR, isikhathi eside sokugcinwa kwezixhumi eziyinhloko ezibangelwa ama-pores ajulile siye sachazwa njengesizathu esiyinhloko sokukhetha okuphezulu ku-hydrocarbon ye-C2 egcwele.Ama-Cu nanofibers asuselwa ku-CuI nawo abonise ukukhetha okuphezulu ku-C2H6 (FE = 30% ku-−0.735 V uma kuqhathaniswa ne-RHE) (89).I-anisotropic morphology kanye nobulukhuni obuphezulu be-CuI-derived Cu nanofibers kungathuthukisa ukusebenza kahle kokucupha kwe-H2 emuncwe futhi ngaleyo ndlela kwandise i-FE ye-C2H6.

(A kuya ku-C) I-morphology noma imiphumela yesakhiwo.(A) Ukuminyana kwama-athomu (i-eksisi yesokunxele) kanye nesilinganiso sama-athomu ezindaweni ezisemaphethelweni (i-Nedge) kuma-athomu endizeni engu-(100) (N100) (i-eksisi yesokudla) ngokuhambisana nobude bonqenqema (d).Ikhiqizwe kabusha ngemvume evela kuJohn Wiley and Sons (58).(B) Uhlelo lwe-morphology lubangele ukushintsha kwe-pH.Ikhiqizwe kabusha ngemvume evela ku-John Wiley and Sons (68).(C) Ukukhethwa komkhiqizo we-mesopore yethusi enobukhulu obuhlukahlukene bembotshana nokujula.Ikhiqizwe kabusha ngemvume evela kuJohn Wiley and Sons (32).(D kuya ku-H) Imiphumela ye-Ligand.(D no-E) I-ECR ku-copper nanowire (Cu NW) enezinhlobo ezahlukene zama-amino acid (D) noma izishintshi (E) kokuthi −1.9 V. Ikhiqizwe kabusha ngemvume evela ku-Royal Society of Chemistry (35).(F) Amazinga okukhiqiza e-C2H4 kuma-electrolyte e-halide ahlukene anamandla ahlukene e-adsorption ku-Cu(35).Ikhiqizwe kabusha ngemvume evela ku-American Chemical Society (91).I-NHE, i-hydrogen electrode evamile.(G) I-FE ye-C2H4 ne-CO ekugxilweni okuhlukile kwama-electrolyte e-KOH kanye (H) ne-Tafel slope ye-C2H4 ekugxilweni okuhlukile kwama-electrolyte e-KOH.(G) kanye no-(H) kukhiqizwe kabusha kusukela ku-American Association for the Advancement of Science (AAAS) (33).

Ukuguqulwa kwendawo ye-Catalyst kusetshenziswa ama-molecule amancane kungenye isu elaziwayo lokuthuthukisa ukusebenza kwe-electrochemical kwe-ECR.Leli su lingathonya imvelo encane eduze nendawo ye-catalyst, engase izinze iziphakathi eziyinhloko ngenxa yokusebenzisana phakathi kwe-surface ligand kanye ne-intermediate.I-Amine ibikwe njenge-modifier yokukhuthaza i-ECR (35).Ama-amino acid ahlukahlukene, okuhlanganisa i-glycine (Gly), i-dl-alanine (Ala), i-dl-leucine (Leu), i-dl-tryptophan (Tyr), i-dl-arginine (Arg), ne-dl-tryptophan (Trp), iye yaphenywa ukuze funda imiphumela yazo kuma-nanowires ethusi (35).Njengoba kuboniswe ku-Fig. 5D, wonke ama-ligands asekelwe ku-amino acid akwazi ukuthuthukisa ukukhethwa kwe-C2 + hydrocarbons.Ukuthuthukiswa okunjalo kuphakamisa ukuthi amaqembu asebenzayo e-─COOH kanye ─NH2 ku-amino acid cishe anesibopho sokukhetha okuthuthukisiwe kwe-ECR.Imibiko yangaphambilini ibonise ukuthi ukufakwa kwama-amino acid endaweni ye-Cu kwafinyelelwa ngawo womabili amaqembu ─COOH kanye ─NH2 (35, 90).I-Stearic acid (C17H35COOH, RCO2H), equkethe kuphela iqembu le-─COOH, ikhethiwe ukuze kuhlonzwe indima ye-─COOH.Ezinye izilungisi, ezifana ne-a-anthraquinone diazonium salt (AQ), i-o-nitrobenzene diazonium salt (PhNO2), ne-dodecyl mercaptan (C12H25SH, RSH), ezingaqukethe amaqembu e-─COOH noma ─NH2, nazo ziye zaphenywa.Kodwa-ke, zonke bezingekho ezinhle ekuthuthukisweni kwe-C2 + hydrocarbon FE (Fig. 5E).Izibalo zetiyori zibonise ukuthi amaqembu angu-─NH3+ ku-zwitterionic glycine ekhangisiwe akwazi ukuzinza *CHO phakathi nendawo ngenxa yokusebenzisana kwawo okuqinile, njengamabhondi e-hydrogen.Ukwethulwa kwe-halide ion ku-electrolyte kungenye indlela yokuguqula ama-catalysts (91, 92).Njengoba kuboniswe ku-Fig. 5F, izinga lokukhiqiza le-C2H4 ku-Cu ecushwe yi-plasma linganyuswa kakhulu ngosizo lwezithako ze-halide.Kwaboniswa ukuthi i-I− ion isebenza kakhulu kune-Br− ne-Cl−, ngokuvumelana namandla e-adsorption ahambisanayo e-I-, Br-, kanye ne-Cl− ku-Cu(100) facet (91).Ngaphandle kwama-halides, i-hydroxide ion iphinde yabonisa umphumela omuhle ekukhetheni kwe-C2H4.Muva nje, i-Sargent kanye nozakwabo (33) babike ukuguqulwa kwe-CO2-to-C2H4 nge-~70% FE kusetshenziswa i-concentrated potassium hydroxide (KOH) electrolyte (kufika ku-10 M) kuseli lokugeleza.Njengoba kuboniswe ku-Fig. 5G, amandla okuqala e-CO ne-C2H4 ku-electrolyte engu-10 M KOH ayephansi kakhulu uma kuqhathaniswa nalawo aku-1 M KOH.Ngaphezu kwalokho, imithambeka ye-Tafel (Umdwebo 5H) wokwakheka kwe-C2H4 yehla ngokunyuka kokugxiliswa kwe-hydroxide (135 mV decade−1 ku-1 M KOH kanye ne-65 mV ishumi leshumi−1 ku-10 M KOH), okuphakamisa ukuguqulwa kwenani eliphelele- isinyathelo esinqumayo.Imiphumela ye-Density functional theory (DFT) ifakazele ukuthi ukuba khona kwama-hydroxides agxilile kungehlisa amandla okubopha we-CO ephakathi nendawo futhi kukhuphule ukungalingani kweshaji phakathi kwama-athomu ekhabhoni amabili kumaphakathi we-OCCO adsorbed.Ngenxa yalokho, i-OCCO emaphakathi izophinde iqiniswe ngokukhanga kwe-dipole enamandla, okuholela ekwehliseni umkhawulo wamandla wokwenza kusebenze we-CO dimerization, okuzobe sekuthuthukise ukusebenza kukonke.

I-C2+ oxygenates efana ne-ethanol (CH3CH2OH) ingesinye isigaba esikhulu semikhiqizo ye-ECR ebaluleke kakhulu.Ukuhlanganiswa kwezimboni kwe-ethanol kuyinqubo edla amandla, ephinde idle inani elikhulu le-ethylene noma i-feedstocks yezolimo (40).Ngakho, ukukhiqizwa kwe-electrocatalytic ye-ethanol noma enye i-C2 + oxygenates evela ku-CO2 yenza umqondo omningi wezomnotho nemvelo.Njengoba isizukulwane se-ethanol esivela ku-ECR sabelane ngokumaphakathi ne-C2H4 okungukuthi *C2H3O (43), i-hydrogenation ekhethiwe yalokhu okumaphakathi ingase ishintshe izindlela ze-ECR zisuka ku-C2H4 ziye ezitshwaleni (64).Kodwa-ke, kumasistimu amaningi, ukukhetha okuya ku-C2+ oxygenates kuphansi kakhulu kunama-hydrocarbons (31, 37, 39, 41, 42, 67).Ngakho, kulesi sigaba, sizogqamisa amasu okuklama kwe-electrocatalyst angafinyelela i-C2+ oxygenate FE ehlaba umxhwele engaphezu kuka-25%.

Njengoba kuxoxwe ngenhla, ama-bimetallic catalysts aklanywe kahle angathuthukisa ukukhetha kanye nomsebenzi wokukhiqiza i-C2 + hydrocarbon.Isu elifanayo kodwa elingafani nalo liye lasetshenziswa ukuthuthukisa ukusebenza kwe-electrocatalytic ye-C2+ oxygenates (38, 93, 94).Isibonelo, ama-catalyst e-Cu-Cu2O e-Ag-incorporated abonise ukukhetha kwe-ethanol eguqulekayo, futhi i-ethanol FE ephakeme kakhulu yayingu-34.15% (95).Umngcele we-biphasic ku-alloy ye-Ag-Cu exutshwe ngesigaba, esikhundleni se-athomu ye-Ag/Cu, ukhonjwe njengento eyinhloko yokukhiqiza okukhethiwe kwe-ethanol.Njengoba isayithi le-Cu liseduze kakhulu nesayithi le-Ag kuphethini ehlanganisiwe yesigaba (Ag-Cu2OPB), izinga lokwakheka kwe-ethanol eliphakathi kwesampula elihlanganisiwe lesigaba lingathuthukiswa uma kuqhathaniswa nehlukaniswe ngesigaba (Ag-Cu2OPS ), okuholela ekusebenzeni okungcono kwesizukulwane se-ethanol.Ngaphandle kwe-ethanol, i-Cu-Ag bimetallic NPs nayo iye yaboniswa ukuguqula i-CO2 ku-acetate ngokungezwa kwe-benzotriazole (93).Ku-−1.33 V uma kuqhathaniswa ne-RHE, i-FE ye-acetate yayingu-21.2%.Kuhlongozwa izindlela ezimbili zokusabela ezingenzeka kulesi simo: Eyodwa isekelwe ku-CO dimerization, kanti enye iphezu kokufaka i-CO, egqamisa indima ebalulekile yokwakheka okuphakathi kwe-CO kumasayithi e-Ag asebenzayo.Ukubhekwa okufanayo kubikwe kuma-catalysts e-Cu-Zn (Umfanekiso 6, A no-B) wokukhiqizwa kwe-ethanol (38).Ngokulungisa okuqukethwe kwe-Zn kuma-catalyst alloyed e-Zn-Cu, isilinganiso se-ethanol uma kuqhathaniswa ne-C2H4 FE singalawulwa kahle kububanzi obungu-0.48 ukuya ku-6, okuphakamisa ukubaluleka kwezindawo eziguqukayo ze-CO zokwakheka kwe-C2+ oxygenate.Ukwakhiwa kwama-catalyst ane-alloyed kungase kubangele umphumela wokucindezeleka kokubalulekile kwe-matrix, okungenzeka kungafiseki ngezinye izikhathi.Ngakho, umzila oqondile obheke kuma-bimetallic catalyst ungase ulungele eminye imikhiqizo eqondiwe.U-Jaramillo kanye nozakwabo (96) bakhe isistimu ye-bimetallic ye-Au-Cu eyenziwe lula, ehlanganiswe ngokufakwa okuqondile kwama-NP egolide kucwecwe lwe-polycrystalline Cu, ukuze kuphenywe umphumela we-catalysis we-tandem.I-bimetallic Au-Cu ibonise ukukhetha okuvumelanayo nomsebenzi obheke ku-C2+ alcohols, osebenza kahle kakhulu kunethusi elimsulwa negolide, kanye ne-Au-Cu alloy.Uma kuqhathaniswa ne-Cu foil, uhlelo lwe-bimetallic Au-Cu lubonise ukwanda kwe-CO yendawo ngenxa yokuba khona kwe-Au NPs (I-Fig. 6C) eyayisebenza esizukulwaneni se-CO.Njengoba igolide lingasebenzi ekwehliseni i-CO, izinga lokukhiqiza utshwala elithuthukisiwe le-C2+ kuma-Au-Cu bimetallic catalysts liphawulwe kumshini we-catalysis we-tandem.Ngokukhethekile, ama-NP egolide angakhiqiza ukugxiliswa okuphezulu kwendawo ye-CO eduze kwendawo ye-Cu.Okulandelayo, ama-molecule amaningi e-CO endawo angancishiswa nakakhulu abe yi-C2+ alcohols nge-Cu.

(A kuya ku-C) Imiphumela ye-alloy.(A) I-FE Ephezulu ye-ethanol ne-C2H4 kanye nesilinganiso se-FE se-ethanol ne-ethylene kuma-alloy ahlukahlukene e-Cu-Zn.(B) Ukuminyana kwamanje kwe-ethanol kuma-alloys ahlukahlukene e-Cu-Zn.(A) kanye no-(B) akhiqizwe kabusha ngemvume evela ku-American Chemical Society (38).(C) Ukwehliswa kwe-CO2 namazinga e-CO kugolide, ithusi, nohlelo lwe-Au-Cu bimetallic.Ikhiqizwe kabusha ngemvume evela ku-Nature Publishing Group (96).(D kuya ku-L) I-morphology noma imiphumela yesakhiwo.(D) Umdwebo wohlelo lwendlela yebhayisikili ye-ion yensimbi.(E no-F) Izithombe ze-SEM ze-100-umjikelezo we-Cu ngaphambi kuka-(E) nangemuva (F) ukuncishiswa ngaphambi kwemibandela ye-ECR.(G) I-TEM kanye ne-electron diffraction yendawo ekhethiwe iphakamise ukuthi i-Cu(100) idaluliwe kanye (H) namandla amahhala *e-OCCO kanye nokwakheka kwe-*OCCHO kuma-Cu(100), Cu(111), kanye ne-Cu(211) facets.(D) kuya ku-(G) akhiqizwa kabusha ngemvume evela ku-Nature Publishing Group (42).(I) Isilinganiso sama-oxygen nama-hydrocarbons njengomsebenzi wamandla ku-Cu(111), Cu(751), kanye ne-Cu(100).(J) Izinombolo zokuxhumanisa ze-Cu(111), Cu(100), kanye ne-Cu(751).(I) kanye no-(J) akhiqizwe kabusha ngemvume evela ku-National Academy of Sciences (97).(K) Uhlelo lwenqubo yoguquko ukusuka kuma-Cu NP ukuya ethusi elifana ne-cubic.Ikhiqizwe kabusha ngemvume evela ku-National Academy of Sciences (98).(L) Izithombe ze-SEM zethusi le-nanodendritic ngaphambi nangemuva kwe-ECR.Ikhiqizwe kabusha ngemvume evela ku-American Chemical Society (99).

Ukuvezwa okukhethekile kwama-crystal facets ama-electrocatalyst kuboniswe njengendlela ephumelelayo neqondile yokuzuza i-FE ethuthukisiwe emikhiqizweni ethile ye-ECR kanye nendlela ebalulekile yokuqonda okuyisisekelo.Ukuhlanganiswa okulula kodwa okuhlaziywayo kwe-single-crystal catalysts kuyinselele.Ligqugquzelwe inqubo ye-galvanostatic charging-discharging (GCD) yamabhethri, iqembu lethu lenze indlela ye-ion yensimbi yamabhayisikili (Fig. 6D) ukuze iveze ngokukhethayo i-crystal facet ye-Cu catalyst (42).Ngemuva kwemijikelezo ye-GCD eyi-100, kwakheka umugqa ominyene we-Cu nanocube ku-Cu foil enezingxenye eziveziwe (100) (Fig. 6, E kuya ku-G).I-catalyst yemijikelezo engu-100 yethule i-C2+ alcohol FE iyonke engaphezu kuka-30% kanye nokuminyana kwamanje kotshwala kwe-C2+ okungaphezu kuka-20 mA cm−2.Nokho, i-Cu yomjikelezo oyi-10 enesilinganiso esiphansi se-facet (100) inikeze kuphela i-C2+ alcohol FE engu-~10%.Ukulingisa kwe-DFT kuqinisekise ukuthi i-Cu(100) kanye ne-steped (211) facets yayivuna kakhulu ekuhlanganisweni kwe-C─C ne-Cu(111), njengoba kuboniswe ku-Fig. 6H.Imodeli ye-catalyst, ifilimu ye-epitaxial Cu enezici ezihlukahlukene eziveziwe, isetshenziselwe ukunquma i-motifs yesayithi esebenzayo ekukhiqizweni kwe-C2+ oxygenate (Fig. 6I) (97).Njengoba ngokwezibalo mancane amathuba okuthi i-CO* dimer isondele kuma-athomu e-H* endaweni enomakhelwane abambalwa, amasayithi e-Cu ahlanganiswe kancane angacindezela ukwakheka kwama-hydrocarbons futhi aholele ekuthuthukisweni kwe-C2+ oxygenate FE ngoba kunzima kakhulu ukwenza i-hydrogenate. I-C─C ihlanganise i-ECR intermediates endaweni yayo (97).Ocwaningweni lwefilimu ye-epitaxial Cu, ababhali baqinisekisile ukuthi i-ECR ku-Cu(751) facet ikhombise isilinganiso esithuthukisiwe se-oxygenate/hydrocarbon.Lesi sithuthukisi singahlotshaniswa ne-Cu athomu yejometri yezingxenye ezihlukene ze-Cu kanye nenani elilinganiselwe eliphansi elihambisanayo elididiyelwe (Fig. 6J), lapho i-Cu athomu ididiyelwa khona, ngokulandelana, nomakhelwane abaseduze ababili, abane, nabayisithupha ku-Cu(751), I-Cu(100), kanye ne-Cu(111) izici.Ukwakhiwa kabusha kwe-in situ morphology kuphinde kwasetshenziswa ukuthuthukisa i-C2+ oxygenate FE.I-Cube esebenzayo efana ne-cube catalyst yasungulwa ngu-Yang kanye nozakwabo (98), ebonise ukusebenza okuthuthukisiwe kokuhlanganisa kwe-C─C.Ngokuningiliziwe, i-monodisperse Cu NPs (6.7 nm) enokulayisha okuhlukile yafakwa ekusekelweni kwephepha lekhabhoni njenge-catalyst ye-ECR.Ngokusobala, i-FE eyengeziwe ye-C2+ oxygenates yabonwa ngokunyuka kokulayisha kwe-Cu NP.Kwaboniswa ukuthi ama-Cu NP aminyene agcwele ngaphansi kwezimo eziphakeme zokulayisha abhekana nokuguqulwa kwe-situ morphological ngesikhathi se-ECR, lapho i-morphology efana ne-cube yagcina kwakhiwa (Fig. 6K).Lesi sakhiwo esisha sitholakale sisebenza kakhulu nge-electrocatalytically.Ukuhlaziywa kwe-Tafel kuphakamise ukuthi i-CO dimerization kwakuyisinyathelo sokunquma izinga lokwakheka komkhiqizo we-C2, kuyilapho lokho kwe-n-propanol kubonise indlela eqondile kulolu hlelo lwe-catalytic.Ithusi le-Nanodendritic ngesinye isibonelo esibonisa ukubaluleka kokulawulwa kwe-morphology yokukhiqizwa kwe-C2 + oxygenate (99).Kafushane, isamba se-FE se-nanodendrite yethusi echazwe kahle (I-Fig. 6L) ye-C2+ yotshwala yayicishe ibe ngu-25% ku-−1.0 V uma kuqhathaniswa ne-RHE.I-n-propanol FE ehlaba umxhwele ka-13% ingafinyelelwa ku-−0.9 V. Ngokucabangela umsebenzi ophezulu we-Cu athomu, ama-catalyst asekelwe ethusi ahlala ehlushwa ukuwohloka kwesakhiwo ngesikhathi se-ECR, ikakhulukazi lapho kunamandla amakhulu, okuholela ebumpofu. ukuzinza.Nokho, ithusi elinjalo le-nanodendritic libonise ukuzinza okuhle ekukhiqizweni kotshwala, libonisa i-FE yotshwala engu-~24% ngaphezu kwamahora angu-6.

Amaphutha ama-electrocatalyst, njengezikhala ze-athomu nama-dopants, akhombisa ukuthi kungenzeka yini ukukhangisa ama-ECR angajwayelekile futhi, ngaleyo ndlela, ngokukhetha athuthukise indlela ehambisanayo ebheke kuma-oxygen (29, 43, 100).Ukuthatha *C2H3O njengesibonelo, okuyinto engase ibe phakathi kwe-penultimate ephakathi kokukhiqizwa kwe-ethylene ne-ethanol, u-Sargent kanye nabasebenza nabo (43) bafunde indima yeziphambeko ku-core-shell Cu electrocatalyst ngokuningiliziwe.Bathi theory wabonisa ukuthi ukusabela amandla izithiyo for ethylene kanye ethanol ukwakheka ayefana ekuqaleni C─C coupling isigaba (0.5-V overpotential) (Fig. 7A).Ngaphansi kwesimo esinjalo, ukwethulwa kwesikhala sethusi bekuzokwandisa kancane umgoqo wamandla wokwakheka kwe-ethylene, nokho akubonisi ithonya esizukulwaneni se-ethanol (Fig. 7B).Kodwa-ke, njengoba kubonisiwe ku-Fig. 7C, ama-copper catalysts anesikhala kanye ne-subsurface sulphur dopant angase akhulise kakhulu umgoqo wamandla womzila we-ethylene, awenze ungabi mnandi ngokwe-thermodynamically.Kodwa-ke, ukuguqulwa okunjalo kubonise umphumela ongabalulekile endleleni ye-ethanol.Lesi simo sabuye saqinisekiswa ngokuhlolwa.I-core-shell eyakheke kahle i-Cu2S-Cu enezikhala zomsebenzi eziningi (Cu2S-Cu-V; Fig. 7D) yahlanganiswa.Isilinganiso sotshwala ne-ethylene sikhuphuke sisuka ku-0.18 kuma-Cu NPs angenalutho saya ku-0.34 ku-Cu2S-Cu engenazikhala futhi safinyelela ku-1.21 ku-Cu2S-Cu-V, nakuba isamba se-FE semikhiqizo ye-C2+ yazo zonke izisusa zahlala zifana (Fig. 7E) .Lokhu kubheka kubonise ukuthi ukukhuthazwa kokukhethwa kotshwala kwakuhlotshaniswa nokucindezelwa kokukhiqizwa kwe-ethylene, okuhambisana nomphumela we-DFT.Ngaphezu kwalokho, ubunjiniyela obunamaphutha budlala indima ebaluleke kakhulu ye-carbon catalyst engenansimbi njengoba izinto zekhabhoni emsulwa zingasebenzi ku-ECR.Ama-Dopants afana ne-nitrogen ne-boron asetshenziselwe ukuguqula isakhiwo se-electronic se-catalyst esekelwe ku-carbon (31, 43, 100).Isibonelo, ifilimu ye-nitrogen-doped nanodiamond (NDD) ku-silicon substrate yasetshenziswa ngu-Quan et al.(29) ngokukhiqiza okukhethiwe kwe-acetate kusuka ku-ECR (Fig. 7F).Amandla okuqala e-acetate ayephansi njengokuthi -0.36 V uma kuqhathaniswa ne-RHE esebenzisa i-NDD catalyst, futhi i-FE ye-acetate yayingaphezu kuka-75% ebangeni elingase libe khona ukusuka ku-−0.8 kuya ku-−1.0 V uma kuqhathaniswa ne-RHE.Ukuze uqonde umsuka wokuthuthukiswa okumangalisayo okunjalo, ama-electrode e-NDD/Si ​​ane-nitrogen ehlukene noma izinhlobo ze-nitrogen alungiswa futhi aphenywa (Fig. 7G).Ababhali baphethe ngokuthi ukusebenza okuphezulu kwe-NDD/Si ​​catalyst ye-ECR kungase kubangelwe amandla ayo aphezulu e-hydrogen evolution kanye ne-N doping, lapho izinhlobo ze-N-sp3C zazisebenza kakhulu ekukhiqizeni i-acetate.Idatha ye-Electrokinetic kanye ne-in situ infrared spectrum yembula ukuthi indlela eyinhloko yokwakheka kwe-acetate ingase ibe yi-CO2 → *CO2− → *(COO)2 → CH3COO−.Ngaphandle kwe-nitrogen, i-boron ingenye i-heteroatom ehlolisiswe kahle yokulawula ukwakheka kwe-elektroniki kwe-nanodiamond.Kodwa-ke, i-boron-doped nanodiamond (BDD) ikhetha ukunciphisa i-CO2 ibe yi-formaldehyde noma i-formate (101).Ngaphezu kwalokho, u-Quan kanye nozakwabo (102) babonise ukuthi i-boron ne-nitrogen co-doped nanodiamond (BND) ibonise umphumela wokusebenzisana ku-ECR, onganqoba ukukhawulelwa kwe-BDD bese ukhiqiza i-ethanol ngokukhetha.Ama-catalyst e-BND1, BND2, kanye ne-BND3 anokuqukethwe kwe-nitrogen okuhlukile kanye namazinga afanayo e-boron doping alungiswa.Njengoba kuboniswe ku-Fig. 7H, ukukhetha okuphezulu kakhulu kwe-ethanol kufika ku-93% kungafinyelelwa ku-BND3 catalyst ku-−1.0 V ngokumelene ne-RHE, ene-doping ye-nitrogen ephakeme kakhulu.Ukubala okungokwetiyori kubonise ukuthi inqubo yokuhlanganisa i-C─C ku-BND yayivuna i-thermodynamically, lapho i-athomu ye-boron ikhuthaze ukuthunjwa kwe-CO2 kanye ne-nitrogen dopant yenza kube lula ukwenziwa kwe-hydrogenation okumaphakathi kuya ku-ethanol.Nakuba i-nanodiamond ye-heteroatom-doped ikwazile ukuguqula i-CO2 ibe ama-oksijeni e-multicarbon ngokukhetha okuphezulu, umsebenzi wayo we-ECR unomkhawulo kakhulu ngenxa yenqubo yokudlulisa ukushaja okuhamba kancane (ukuminyana kwamanje kungaphansi kuka-2 mA cm−2).Izinto ezisuselwa ku-graphene zingase zibe yisixazululo esingaba khona sokunqoba ukushiyeka kwama-catalyst asuselwa kwidayimane.Ngokwethiyori, amasayithi e-pyridinic N asemaphethelweni kusendlalelo se-graphene athathwe njengamasayithi asebenzayo wokuhlanganisa i-C─C (103).Lokhu kungenxa yokuthi ukuba khona kwe-pyridinic N ezindaweni ezisemaphethelweni kungaguqula i-CO2 ibe yi-CO, engahlanganiswa futhi ibe yi-molecule ye-C2 + (Fig. 7I).Isibonelo, *i-C2O2 emaphakathi ingase iqiniswe kukhabhoni ene-nitrogen-doped lapho ama-athomu amabili e-C ahlanganiswa khona ne-pyridinic N kanye ne-athomu yayo engu-C eseduze, ngokulandelana (103).Isibikezelo setiyetha sabe sesiqinisekiswa kusetshenziswa i-nitrogen-doped graphene quantum dot (NGQD) catalysts (31).Ngemva kokuphonswa kwamashidi e-nitrogen-doped graphene sheets (1 kuya ku-3 μm) (Fig. 7J), 1- kuya ku-3-nm NGQDs atholwe lapho ukuminyana kwe-pyridinic N ezindaweni ezisemaphethelweni kwanda ngama-oda amathathu wobukhulu.Ku-−0.78 V uma kuqhathaniswa ne-RHE, i-FE ephezulu ye-C2+ oxygenates ingafinyelela ku-26%.Ngaphezu kwalokho, njengoba kuboniswe ku-Fig. 7K, ukuminyana kwamanje okuyingxenye ye-C2 + oxygenates kuseduze ne-40 mA cm−2 ku- -0.86 V ngokumelene ne-RHE, ephakeme kakhulu kune-nanodiamond eguquliwe.Uma kuqhathaniswa, amachashazi e-graphene quantum e-N-free kanye ne-N-doped graphene oxide, abonisa indawo ephansi kakhulu yonqenqema lwesayithi i-pyridinic N, ekhiqiza i-H2, CO, kanye nefomethi.

(A kuya ku-C) Ama-Gibbs amahhala asuka ku-*C2H3O aye ku-ethylene kanye ne-ethanol yethusi, ikhopha enesikhala, kanye nekhopha enezikhala zethusi nesibabule esingaphansi komhlaba.(D) Umfanekiso wohlelo lwe-Cu2S-Cu-V catalyst.(E) I-FE ye-C2+ utshwala ne-ethylene, kanye nesilinganiso se-FE sotshwala kuma-alkenes.(A) kuya ku-(E) akhiqizwa kabusha ngemvume evela ku-Nature Publishing Group (43).(F) Isithombe se-SEM se-NDD.(G) Amazinga okukhiqiza e-acetate kanye ne-formate ku-NDD enokuqukethwe okuhlukile kwe-nitrogen.ku-%, i-athomu %.(F) kanye no-(G) akhiqizwe kabusha ngemvume evela ku-American Chemical Society (29).(H) Ama-FE we-NDD, BDD, kanye nama-BND kokuthi −1.0 V. Akhiqizwe kabusha ngemvume evela ku-John Wiley and Sons (102).(I) Umfanekiso wohlelo wamasayithi asebenzayo okuhlanganiswa kwe-C─C kuma-NGQD.(I) ikhiqizwe kabusha ngemvume evela ku-American Chemical Society (103).(J) Isithombe se-TEM sama-NGQD.Amabha esikali, 1 nm.(K) Ukuminyana kwamanje ngokwengxenye yemikhiqizo ehlukahlukene esebenzisa ama-NGQD.(J) kanye no-(K) akhiqizwa kabusha ngemvume evela ku-Nature Publishing Group (31).

Ngale kwama-electrocatalyst, idizayini ye-electrode ne-catalytic reactor architecture iveza omunye umzila osebenzayo wokuthuthukisa ukusebenza kwe-ECR, ikakhulukazi ngezinga lokukhiqiza nokusebenza kahle kwamandla.Intuthuko enkulu yenziwe ekwakhiweni nasekukhiqizeni amanoveli amasistimu e-electroreduction ukuze kuzuzwe ukukhiqizwa kwe-C2+ esebenza kahle kakhulu.Kulesi sigaba, sizoxoxa nge-ECR electrode/reactor design ngokuningiliziwe.

Amaseli ohlobo lwe-H asetshenziswa kakhulu ekuhlolweni kwesilinganiso selebhu, kucatshangelwa ukuhlangana kwawo okulula, ukusebenza okulula, kanye nezindleko eziphansi.Amaseli afakwe ama-cathode azimele kanye namakamelo e-anode axhunywe ulwelwesi lwe-ion-exchange (104, 105).Ububi obuyinhloko baleli seli lohlobo lwe-H ukuncibilika okuphansi kwe-CO2 ku-electrolyte enamanzi, okuyi-0.034 M kuphela ngaphansi kwezimo ze-ambient, okuholela ekunciphiseni kwe-CO2 ukuminyana kwamanje okungu-j <100 mA cm−2 (64).Ngaphezu kwalokho, ezinye izithiyo zangaphakathi, okuhlanganisa indawo engaphezulu ye-electrode elinganiselwe kanye nebanga elikhulu le-interelectrode, yehlulekile ukuhlangabezana nezidingo zocwaningo ezikhulayo (105, 106).Ngokukhiqizwa komkhiqizo we-C2+, amaseli ohlobo lwe-H ngokuvamile abonisa ukukhetha okuphansi ngaphansi kwamandla aphezulu, isb, 32% we-ethylene ku-−0.98 V ngokumelene ne-RHE (107), 13.1% ye-n-propanol ku-−0.9 V ngokumelene ne-RHE (99), futhi U-20.4% we-ethanol kokuthi −0.46 V uma kuqhathaniswa ne-RHE (108), ngenxa yokuvela kwe-hydrogen enokuncintisana kakhulu.

Ukuze kubhekwane nalezi zinkinga ezingenhla, kwahlongozwa i-reactor flow (15, 109).Kumaseli okugeleza, umfudlana wegesi we-CO2 ungasetshenziswa ngokuqondile njenge-feedstock ku-cathode, ngaleyo ndlela kuholele ekuthuthukisweni kokusatshalaliswa kwenqwaba kanye nezinga lokukhiqiza (104, 110).Umfanekiso 8A ubonisa ukwakheka okujwayelekile kweseli eligelezayo, lapho i-polymer electrolyte membrane (PEM) isebenze njengesihlukanisi se-electrode esihlukaniswa phakathi kwamashaneli amabili okugeleza.I-catalyst ivalwa ku-electrode ye-gas diffusion (GDE) ukuze isebenze njenge-cathode electrode, lapho i-CO2 enegesi iphakelwa khona ngokuqondile.I-catholyte, efana ne-0.5 M KHCO3, igeleza ngokuqhubekayo ngaphakathi kongqimba oluncane phakathi kwe-catalyst electrode ne-PEM.Ngaphezu kwalokho, uhlangothi lwe-anode luvamise ukuzuzwa nge-electrolyte enamanzi yokusabela kokuvela komoyampilo (43, 110).Uma kuqhathaniswa namaseli ohlobo lwe-H, lawa maseli okugeleza asekelwe kulwelwesi abonisa ukusebenza kwe-ECR ephakeme kakhulu.Isibonelo, u-Sargent kanye nozakwabo (43) bahlole ukusebenza kwe-ECR kwe-Cu2S-Cu-V catalyst kukho kokubili iseli yohlobo lwe-H neseli eligelezayo, njengoba kuboniswe ku-Fig. 8 (B kuya ku-E).Kusetshenziswa amaseli ohlobo lwe-H, i-FE ephezulu yemikhiqizo ye-C2+ ibingu-41% enengqikithi yamanje yokuminyana engu-~30 mA cm−2 ngaphansi kuka-−0.95 V uma iqhathaniswa ne-RHE.Nokho, i-FE yemikhiqizo ye-C2+ ikhuphuke yafinyelela ku-53% ngenani eliphelele lamanje elidlula kalula ku-400 mA cm−2 ngaphansi kuka-−0.92 V uma kuqhathaniswa ne-RHE ohlelweni lokugeleza.Ukuthuthukiswa kokusebenza okuphawulekayo okunjalo kusetshenziswa i-reactor egelezayo kungase kubalulwe ekusakazweni okuthuthukisiwe kwe-CO2 kanye nokusabela okuseceleni okucindezelwe, ikakhulukazi okuvela kusakhiwo sendawo segesi-electrolyte-catalyst triple-interface architecture.

(A) Umdwebo we-electrolyzer egelezayo onohlelo olusondeziwe lwesixhumi esibonakalayo se-electrolyte.(A) kukhiqizwa kabusha ngemvume evela ku-John Wiley and Sons (30).(B kuya ku-E) Ukuqhathaniswa kokusebenza kwe-ECR kusetshenziswa iseli yohlobo lwe-H kanye neseli eligelezayo.(B) kuye ku-(E) akhiqizwa kabusha ngemvume evela ku-Nature Publishing Group (43).(F ukuya ku-H) Ama-electrolyte ahlukene asetshenziswa kumaseli okugeleza ngokuqhathaniswa nokusebenza kwe-ECR.(F) kuye ku-(H) akhiqizwa kabusha ngemvume evela ku-John Wiley and Sons (30).(I kuya ku-K) Ukwakheka nokusebenza kokuqina kwe-electrode yokusabalalisa igesi esekelwe ku-polymer.(I) kuye ku-(K) akhiqizwa kabusha ngemvume evela ku-AAAS (33).

Iseli yegebe elinguziro ingelinye ikilasi elikhulayo lama-electrolyzer, eliqhubeka lisusa iziteshi zokugeleza kumaseli okugeleza bese licindezela ama-electrode amabili kanye nolwelwesi lwe-ion-exchange phakathi.Lokhu kumisa kunganciphisa kakhulu ukudluliswa kwenqwaba kanye nokumelana nokudluliswa kwama-electron futhi ngaleyo ndlela kuthuthukise ukusebenza kahle kwamandla, kukwenze kube nokwenzeka kakhulu ezisetshenziswayo ezingokoqobo (110).Ama-reactants aphakelwa ku-cathode angaba i-CO2-saturated catholyte noma umfudlana we-CO2 omswakama.Umhwamuko wamanzi noma i-electrolyte enamanzi inikezwa ngokuyisibopho ku-anode ukuze kukhishwe i-proton ukuze kunxeshezelwe inkokhiso yezinhlobo zokunciphisa i-CO2 (111).UGutiérrez-Guerra et al.(109) ihlole ukusebenza kwe-Cu-AC hybrid catalyst kuseli gap eyiziro futhi yabika ukuthi i-acetaldehyde iwumkhiqizo oyinhloko onokukhetha okuphezulu okungu-60%.Njengenye inzuzo yale divayisi, kulula kakhulu ukucindezela ukugeleza kwe-reactant futhi kuthuthukise kakhulu ukugxiliswa kwendawo ye-CO2, ngaleyo ndlela kubangele ukuminyana okukhulu kwamanje kanye namazinga aphezulu okusabela (110).Kodwa-ke, izinga lokushintshaniswa kwe-ion elisheshayo kumaseli we-zero gap livame ukwenza i-catholyte i-asidi, iguqule ukusabela ekuziphendukeleni kwe-H2 esikhundleni sokunciphisa i-CO2 (112).Ukuze kubhekwane nale nkinga, u-Zhou kanye nozakwabo (112, 113) bafake isendlalelo se-buffer esine-electrolyte enamanzi ezungezayo phakathi kwe-cathode ne-membrane ukuze kugcinwe i-pH efanele eduze kwe-cathode yokusabela kokunciphisa i-CO2.Nakuba imikhiqizo ehlukahlukene ye-C2+ itholwe ngesisekelo samaseli egebe elinguziro, okuhlanganisa i-acetone, i-ethanol, ne-n-propanol, ama-FE asephansi kakhulu.Ucwaningo oluningi olubikiwe luhlala lugxile emikhiqizweni ye-C1 ebandakanya izinombolo ezimbalwa ze-proton kanye nokudluliselwa kwama-electron phakathi nokusabela kokunciphisa.Ngakho-ke, ukuba nokwenzeka kweseli yegebe elinguziro lemikhiqizo ye-C2+ kusengaphansi kwenkulumompikiswano (110).

Ngaphezu kwalokho, amaseli e-microfluidic electrolytic (MECs) awuhlobo lokucushwa kwe-electrolyzer okukhanga kakhulu okuthuthukiswe nguKenis kanye nozakwabo (39, 114).Kulo mshini, ulwelwesi luthathelwa indawo isikhala esincane (<1 mm ubukhulu) esigcwele umfudlana we-electrolyte ogelezayo ukuhlukanisa i-anode ne-cathode.Ama-molecule e-CO2 angasakazeka ngokushesha kusixhumi esibonakalayo se-electrode-electrolyte eduze ne-cathode, futhi ama-GDE amabili angaguquki athululelwa i-electrolyte egelezayo.Uma kuqhathaniswa namaseli okugeleza asekelwe kulwelwesi, ama-MEC awagwemi nje kuphela izindleko eziphakeme zolwelwesi kodwa futhi anciphisa nokuphathwa kwamanzi, okubhekisela ikakhulukazi ekomisweni kwe-anode kanye nezikhukhula ze-cathode lapho zisebenza ngokuminyanisa okukhulu kwamanje ngenxa yokudonsa kwe-osmotic yama-molecule amanzi ukuthuthwa kwe-proton ukusuka ku-anode kuye ku-cathode ngaphesheya kolwelwesi (115).Ngokwazi kwethu, ngaphandle kokufaneleka okuphawulekayo kanye nezimpumelelo, inani elincane locwaningo lizuze imikhiqizo ye-C2+ kuma-MEC okuqala.Lokhu cishe kubangelwa umphumela "ontantayo" wokuthi ama-protons akheke ku-anode adonswa kalula endaweni ye-cathode noma ashaywe yi-electrolyte egelezayo, kunokuba abambe iqhaza ku-proton eminingi edingekayo yokusabela kokwakheka kwe-C2+.Ukuqagela kungaqinisekiswa yisibonelo esilandelayo.Ku-2016, u-Kenis kanye nabasebenza nabo (31) babike ukuncishiswa okuphumelelayo kwe-CO2 kumikhiqizo ye-C2 + ku-MEC eguquliwe futhi ene-membrane, lapho i-NGQDs inganciphisa khona ama-molecule e-CO2 ku-C2 + nge-55% FE (31% ye-ethylene, i-14% nge-ethanol, u-6% we-acetate, no-4% we-n-propanol) ngamandla asetshenziswayo angu-−0.75 V uma kuqhathaniswa ne-RHE kusixazululo esingu-1 M KOH.Kubalulekile ukuveza ukuthi indawo ye-electrolyte ingathinta kakhulu ukukhetha komkhiqizo.Isibonelo, i-Jiao kanye nozakwabo (30) bahlanganise i-Cu catalyst e-nanoporous base behlola ukusebenza kwayo kwe-ECR kusetshenziswa ama-electrolyte ahlukene (KHCO3, KOH, K2SO4, ne-KCl) ku-MEC esekwe kulwelwesi.Baveze ukuthi ukuncishiswa kwe-CO2 ku-alkaline electrolyte (KOH) kukhombisa ukukhetha okuphezulu kwe-C2+ nokuminyana kwamanje, njengoba kuboniswe ku-Fig. 8 (F no-G).Ku-−0.67 V uma kuqhathaniswa ne-RHE ku-electrolyte engu-1 M KOH, i-FE etholiwe ye-C2+ ifinyelela ku-62% nengxenye yamanje yokuminyana engu-653 mA cm−2, okuphakathi kokuminyana okuphezulu kakhulu okwake kwabikwa ekuncishisweni kwe-electrochemical CO2. kumikhiqizo ye-C2+.I-Ethylene (38.6%), i-ethanol (16.6%), ne-n-propanol (4.5%) yimikhiqizo eyinhloko ye-C2+ enenani elincane le-acetate.Baphinde baveza ukuthi kunokuhlobana okuqinile phakathi kwendawo ebaliwe ye-pH ne-FE yemikhiqizo ye-C2+: Lapho iphezulu i-pH engaphezulu, ukuminyana okuphezulu kwamanje kanye nesivuno semikhiqizo ye-C2+, njengoba kuboniswe ku-Fig. 8H.Isibalo setiyetha siphakamise ukuthi ama-ion aseduze nendawo ye-OH− angakwazi kakhulu ukuhlanganisa i-C─C (31).

Ngokungeziwe ekucushweni kwe-electrolyzer, i-electrolyte esetshenziswa kuma-electrolyzer ahlukene ingase futhi iguqule kakhulu imikhiqizo yokugcina ye-ECR.Njengoba sishilo ngenhla, izixazululo ze-KOH ezine-alkaline kakhulu zihlala zisetshenziswa kumaseli agelezayo asebenza kahle kakhulu kunakumaseli ohlobo lwe-H.Kuchazwa iqiniso lokuthi i-KOH electrolyte inganikeza ukuqhutshwa kwe-electrolyte ephakeme, yehlise ukumelana ne-ohmic phakathi kwento ecolekile ye-electrolyte ku-catalyst ne-electrolyte yobuningi, futhi yehlise nakakhulu amandla angaphezu kwamandla adingekayo okwakheka kwe-C2+ (31).Imiphumela ye-DFT iphinde iqinisekise ukuthi ukuba khona kwama-OH− ion kungase kwehlise umgoqo wamandla we-CO dimerization, ngaleyo ndlela kukhuphule ukwakheka kwe-C2+ futhi kucindezele umncintiswano ekubunjweni kwe-C1 ne-H2 (30, 33).Nokho, i-alkaline KOH ayikwazanga ukusetshenziswa njenge-electrolyte kumaseli ohlobo lwe-H.Lokhu kungenxa yokuthi ukusakaza kwe-CO2 kuzosabela ngokushesha ngezixazululo ze-KOH futhi ekugcineni kudale isisombululo se-bicarbonate esine-pH engathathi hlangothi kumaseli ohlobo lwe-H (30).Kumaseli okugeleza, nokho, uma i-CO2 isisakazeka nge-GDE, ama-molecule e-CO2 azosetshenziswa esigabeni semingcele emithathu (CO2-catalyst-electrolyte) ukuze akhe imikhiqizo encishisiwe ngokushesha.Ngaphandle kwalokho, umthamo ongemuhle wokubhafa we-electrolyte uyakwazi ukukhulisa ngokushesha i-pH ezungeze i-electrode ekucushweni kwe-electrolyzer emile, kuyilapho i-electrolyte egelezayo izovuselela indawo engaphezulu futhi inciphise ukushintshashintsha kwe-pH ku-electrolyte (33, 116).

Njengoba kushiwo ngenhla ukuthi i-ECR iwukusabela okulawulwa ukusabalalisa, ingcindezi ephezulu yokusabela ingase futhi ithuthukise ngokuphawulekayo ukugxiliswa kwenqwaba kanye nesixhumi esibonakalayo se-CO2.Ama-reactors avamile okucindezela okuphezulu afana ne-autoclave yensimbi engagqwali, lapho umfutho ophezulu we-CO2 (ofika ku-60 atm) ungethulwa kuseli, okuholela ekwenyukeni okumangalisayo kukho kokubili i-FE kanye nokuminyana kwamanje kwe-C2+ (117). , 118).I-Sakata kanye nozakwabo (119) babonise ukuthi ukuminyana kwamanje kungathuthukiswa kube ngu-163 mA cm−2 ngaphansi kuka-30 atm ku-Cu electrode ene-ethylene njengomkhiqizo omkhulu.Ama-catalyst amaningi ensimbi (isb., i-Fe, i-Co, ne-Ni), ngaphandle komsebenzi wokukhiqizwa kwe-C2+ ngengcindezi yendawo, anganciphisa i-CO2 ibe i-ethylene, i-ethane, i-propane, neminye imikhiqizo ye-C2+ ephezulu ekucindezelweni okuphezulu.Kuye kwaboniswa ukuthi ukukhethwa kwemikhiqizo ngokuphawulekayo kuncike ekucindezelweni kwe-CO2 ngendlela yokuguqula ukutholakala kwe-CO2 endaweni ye-electrode (117, 120).Imikhiqizo eyinhloko encishisiwe iguqulwa isuka ku-H2 iye kuma-hydrocarbons (i-C2+ ifakiwe) futhi ekugcineni ibe yi-CO/HCOOH ngokunyuka kwengcindezi ye-CO2.Ngokuphawulekayo, ingcindezi ye-CO2 kufanele iqashwe ngokucophelela ngoba izingcindezi eziphezulu kakhulu noma eziphansi ze-CO2 zingadala izinga lokusatshalaliswa kwe-CO2 elingaphezu kwamandla noma elilinganiselwe, elivame ukuvumela ukukhiqizwa kwe-CO/HCOOH noma i-H2.Inani elihambisanayo kuphela le-CO ephakathi nendawo kanye nokuminyana kwamanje okukhiqizwe endaweni ye-electrode engasiza ukusabela kokuhlangana kwe-C─C futhi kuthuthukise ukukhetha komkhiqizo we-C2+ (119).

Ukuklama i-electrode yenoveli enezakhiwo ezithuthukile kungenye indlela ebalulekile yokuthuthukisa ukukhiqizwa kwe-C2+ okukhethiwe.Ekuqaleni, ama-electrode asebenzayo ayizinsalela zensimbi ezingenazimbobo futhi zihlushwa ukudluliswa kwenqwaba okuvilaphayo (26, 105).Ngenxa yalokho, i-GDE yahlongozwa ukunciphisa ukusebenza kabi kwamaseli ngokuhlinzeka ngeziteshi ze-hydrophobic ezenza kube lula ukusakazeka kwe-CO2 ezinhlayiyeni ze-catalyst (121).I-GDE evamile ngokuvamile ihlanganisa isendlalelo se-catalyst (CL) kanye nesendlalelo se-gas diffusion (GDL), njengoba kuboniswe engxenyeni engezansi ye-Fig. 8A (30, 33).I-interface ye-gas-liquid-catalyst eyakhelwe ku-GDE ibalulekile ukuze kuthuthukiswe ukusebenza kweseli.I-GDL ehlanganiswe nezinto ezimbotshana (imvamisa iphepha lekhabhoni) inganikeza izindlela eziningi ze-CO2 futhi iqinisekise izinga lokusabalalisa i-electrolyte ngokushesha.Iphinde isebenze njengendawo yokuthutha ekwazi ukumelana nokuphansi yama-proton, ama-electron, nemikhiqizo yokunciphisa isuka ku-CL iye ku-electrolyte (121).I-drop casting, i-airbrushing, kanye ne-electrodeposition ubuchwepheshe obuvamile bokulungiselela ama-GDEs (122).Ama-Catalyst ahlanganiswe nama-GDE aphenywe kakhulu ekuncishisweni kogesi kwe-CO2 emikhiqizweni ye-C2+.Ngokuphawulekayo, amaseli okugeleza okukhulunywe ngawo ngenhla asebenza kahle wonke ahlanganiswe nama-GDE.Kusukela ngo-1990, abakwaSammells kanye nabasebenza nabo (123) babike ukuthi ama-GDE e-Cu-coated athole i-FE ephezulu engu-53% ye-ethylene ene-high density engu-667 mA cm−2.Ukuthuthukisa ukukhethwa kwe-ethylene ne-ethanol kuyinselelo enkulu ehlala ikhiqizwa ngokuhlanganyela kuma-Cu-based catalysts ngenxa yezindlela zawo zokusabela zemishini ezifanayo kakhulu.Ngaphezu kwalokho, kubalulekile ukuveza ukuthi ukukhiqiza okuphezulu nokukhetha kwe-ethylene uma kuqhathaniswa ne-ethanol kuye kwabonwa ku-Cu-based GDE (25, 36).U-Gewirth kanye nozakwabo (36) babonise i-FE enhle kakhulu engu-60% ye-ethylene kanye ne-FE ecindezelwe ye-ethanol engu-25% ku-electrodeposited Cu-Ag GDE, lapho isamba sokuminyana samanje sifinyelela ku-~300 mA cm−2 kokuthi −0.7 V uma kuqhathaniswa ne RHE.Kungumsebenzi ongavamile ozuze ukukhetha okuphezulu kangaka endaweni enkulu yamanje.Lokhu okutholakele kuphakamisa ukuthi i-electrode ehlanganiswe ne-GDE inikeza indlela ethembisayo yokulungisa izindlela zokusabela, lapho ukukhethwa kwemikhiqizo encishisiwe kungatholwa lapho kuminyene khona manje.

Ukuzinza kwama-GDE nakho kuyindaba ebalulekile okufanele kubhekwane nayo ngoba ukusebenza okuzinzile kwesikhathi eside kubalulekile ukuze kuqashwe ukusetshenziswa okungokoqobo kwamaseli agelezayo.Naphezu kokusebenza okuvelele kwe-CO2-to-C2+ okuzuzwe ngama-GDE, ukuzinza kusekubi ngenxa yokunamathela okubuthakathaka komshini kwe-catalyst, GDL, kanye nezingqimba ze-binder (77, 124).Indawo yekhabhoni ye-GDL ingase ishintshe isuke ku-hydrophobic iye ku-hydrophilic ngesikhathi sokusabela kwe-electrochemical ngenxa yokusabela kwe-oxidation okwenzeka ezindaweni eziphakeme kakhulu, okuholela ezikhukhuleni ku-GDL nezindlela ezivimbekile ze-CO2 (33).Ukuxazulula le nkinga, abacwaningi bahlanganisa i-hydrophobic scaffold ye-polytetrafluoroethylene (PTFE) kuma-GDE.Uma kuqhathaniswa ne-hydrophilic Nafion, isendlalelo se-PTFE se-hydrophobic sinikeza ukuzinza okuphakeme kwesikhathi eside (33).I-Sargent kanye nabasebenza nabo (33) bahlanganisa i-Cu catalyst phakathi kwe-PTFE ehlukanisiwe ne-carbon NPs, lapho ungqimba lwe-hydrophobic PTFE lungakwazi ukuvimbela ama-NPs kanye nezingqimba ze-graphite, ngaleyo ndlela yakhe i-electrode interface ezinzile (Fig. 8, I no-J).Ngenxa yalokho, i-FE yokukhiqizwa kwe-ethylene yanda yaba ngu-70% kusisombululo se-7 M KOH ekuminyaniseni kwamanje kuka-75 kuya ku-100 mA cm−2.Ubude besikhathi sempilo yalesi senzo sokugeleza sandiswa saba ngaphezu kwamahora angu-150 ngokulahleka okunganakwa ekukhetheni kwe-ethylene, okuphindwe izikhathi ezingu-300 kune-GDE evamile, njengoba kuboniswe ku-Fig. 8K.Isakhiwo sesemishi esinjalo siboniswe ukuthi siwumklamo omuhle kakhulu we-GDE.Isibonelo, u-Cui kanye nozakwabo (124) baklame isakhiwo se-trilayer enesendlalelo se-electrode esebenzayo esisikwe amafilimu amabili e-hydrophobic nanoporous polyethylene.Izendlalelo zangaphandle ze-hydrophobic zingabambezela ukugeleza kwe-electrolyte kusuka kusixazululo senqwaba, okuholela ku-pH yendawo ezinzile, ephezulu ezungeze i-electrode esebenzayo.Ukwenziwa ngcono kwesikhala se-interlayer, esingathuthukisa ezokuthutha ze-CO2 nokukhangisa, nakho kubalulekile kumklamo onjalo (124).Muva nje, ama-carbon nanotubes nawo ahlanganiswe kuma-GDE ngenxa ye-porosity yawo ephezulu, ukuhamba kahle kwawo, kanye ne-hydrophobicity, engenza lula ukuthuthwa kwama-electron nokuhamba ngobuningi (77).

Naphezu kwenqubekelaphambili ethokozisayo ku-ECR, amasu okukhiqiza umkhiqizo oshibhile, omkhulu we-C2+ awavamile ukuba khona (125).Kulesi sigaba, izinselelo namathuba kuyahambisana ukuqonda izindlela zokusabela ze-ECR nokwenza lobu buchwepheshe obuthembisayo buhwebe.

Njengesixazululo esihle sokuvala i-carbon loop nokugcina amandla avuselelekayo ngezikhathi ezithile, njengomoya nelanga, inqubekelaphambili enkulu yenziwe ukuze kuzuzwe ukuguqulwa okuphumelelayo kwe-CO2 emashumini eminyaka adlule.Nakuba ukuqonda kwezinqubo ezihlotshaniswa ne-ECR sekuhambe ibanga elide kusukela ezinsukwini zayo zakuqala (126), ukuhlangana kwe-C─C nge-ECR kubheke kumikhiqizo ye-C2+ kusekude ukuthi ilungele ukusetshenziswa okungokoqobo.Kulesi sibuyekezo, sibheke kabanzi amasu amanje angakhuthaza ukukhethwa nezinga lokukhiqiza lemikhiqizo ye-C2+ nge-ECR, okuhlanganisa ukushuna okuhle kwe-catalyst, imiphumela ye-electrolyte, izimo ze-electrochemical, kanye nomklamo we-electrochemical electrode/reactor.

Naphezu kwawo wonke umzamo owenziwe ku-ECR, kusenezinkinga eziningi nge-catalysts yamanje kanye nohlelo lwe-ECR okufanele kubhekwane nalo ngaphambi kokuthengisa i-ECR.Okokuqala, njenge-catalyst ebusayo yokuthola ukuhlangana kwe-C─C okuphumelelayo, i-Cu ihlushwa izinkinga ezingathi sína zokuzinza, ikakhulukazi ku-electrolyte emanzi, futhi ayivamisile ukuphila amahora angu-100 ngenxa yokuhamba kwayo okuphezulu kwe-athomu, ukuhlanganisa izinhlayiyana, kanye nokuwohloka kwesakhiwo ngaphansi kwezimo ze-ECR.Ngakho-ke, indlela yokuthola ukuzinza kwesikhathi eside usebenzisa i-Cu-based catalyst kuseyinselelo evulekile.Ukugxilisa i-catalyst esekelwe ku-Cu ekusekelweni okuqondile nokusebenzisana okuqinile kungase kube isu elithembekile lokulondoloza isakhiwo/i-morphology ye-catalyst futhi ngaleyo ndlela kunikeze ubude bempilo obuthuthukisiwe.Ngaphezu kwalokho, ukusebenzisa i-electrolyte ye-polymer membrane esikhundleni sesisombululo samanzi ngesikhathi se-ECR cishe kungase kuthuthukise ukuzinza kwe-catalyst esekelwe ku-Cu.Ukwengeza, ngokombono wama-catalysts, amasu okulinganisa i-in situ/in operando kanye nokumodela kwetiyetha kufanele futhi kusetshenziselwe ukuqapha nokuqonda ukuwohloka kokusebenza kwe-catalyst, ngaleyo ndlela, ukucindezela ukuwohloka nobuthi be-catalyst kumazinga aphansi kakhulu.Olunye udaba olubalulekile lwama-catalysts e-ECR okufanele kubhekwane nawo ukwenza i-synthesis protocol isebenze ekukhiqizeni ngobuningi.Kuze kube manje, kunconyelwa ukuhlehlisa izinqubo zokwenziwa kusetshenziswa ama-feedstocks atholakala kabanzi.

Okwesibili, i-C2+ ekhiqizwe umoya-mpilo evela ku-ECR ivamise ukuxutshwa nezinyibiliki (isb, i-KHCO3 ne-KOH) ku-electrolyte yama-H- noma ama-flow-cell reactors, okuthi, nokho, adinga ukuhlukaniswa okwengeziwe nezinqubo zokugxilisa ingqondo ukuze kubuyiselwe izixazululo zamafutha oketshezi olumsulwa izicelo ezingokoqobo.Ngesikhathi esifanayo, ama-hydrocarbon e-C2+ athuthukisiwe nawo axutshwe ne-H2 kanye ne-CO2 esele.Ngakho, inqubo yokuhlukanisa ebizayo ibalulekile kubuchwepheshe bamanje be-ECR, obuphinde buvimbele i-ECR ekusebenziseni okungokoqobo.Ngakho-ke, ukukhiqiza kanjani ngokuqondile nangokuqhubekayo izixazululo zamafutha oketshezi oluhlanzekile nama-hydrocarbon egesi ahlanzekile, ikakhulukazi anokugxila okuphezulu kwemikhiqizo, kufiseleka kakhulu ekusetshenzisweni kwe-ECR ngendlela engokoqobo.Ngakho sibikezela ukubaluleka okukhulayo kokukhiqizwa okuqondile kwemikhiqizo ehlanzekile nge-ECR maduze nje, okungase kuthathe ubuchwepheshe be-ECR busondele kakhulu emakethe (127).

Okwesithathu, ngenkathi ukwakheka kwezibopho ze-C─O ne-C─H, njenge-ethanol, i-acetic acid, ne-ethylene, kubuchwepheshe be-ECR kufundwe kakhulu, ukuhlola ezinye izinhlobo zemikhiqizo nakho kubalulekile kubuchwepheshe be-ECR futhi kubonisa isithakazelo somnotho.Isibonelo, muva nje, u-Han kanye nozakwabo (128) babike ukukhiqizwa kwe-2-bromoethnol yi-ECR.Ukwakheka kwe-in situ kwebhondi ye-C─Br kuguqula umkhiqizo usuka ku-ethanol uye ku-2-bromoethnol, okuyisakhiwo esibalulekile ekuhlanganiseni kwamakhemikhali nokwemithi futhi ebonisa inani eliphakeme elingeziwe.Ngakho-ke, ngale kwemikhiqizo yamanje ye-C2+ efundwe kahle, sikholelwa ukuthi ukukhonjwa kweminye imikhiqizo engavamile ukuhlola njenge-oxalic acid (129) kanye nokuhlanganiswa kwama-molecule e-C2+ ayinkimbinkimbi njengama-cyclic compounds kungenye indlela ethembisayo yocwaningo lwe-ECR lwesikhathi esizayo.

Okokugcina, imiklamo yenoveli kagesi kanye ne-reactor efana ne-GDE engangeni manzi, amaseli okugeleza koketshezi, neseli ye-PEM kufanele yamukelwe kabanzi ukuze kukhuliswe izinga lokukhiqiza le-ECR libe sezingeni lezentengiso (>200 mA cm−2).Kodwa-ke, umehluko omkhulu emsebenzini we-electrocatalytic uhlale ubonwa lapho ama-electrocatalyst esetshenziswa ekuhlolweni kweseli eligcwele.Ngakho-ke, ucwaningo oluhlelekile kakhulu kufanele lwenziwe ukuze kuncishiswe igebe phakathi kocwaningo lweseli elinguhhafu kanye nokusetshenziswa kwedivayisi yeseli egcwele ukuletha i-ECR kusukela ekuhlolweni kwesilinganiso selebhu iye ekusetshenzisweni okungokoqobo.

Kafushane, ukuncishiswa kwe-electrochemical CO2 kunikeza ithuba elihle lokubhekana nenkinga yemvelo evela kumagesi abamba ukushisa akhishwa imisebenzi yabantu.Iphinde ibonise ukuthi kungenzeka ukuzuza amafutha ahlanzekile namakhemikhali usebenzisa amandla avuselelekayo.Nakuba kusele izinselelo eziningi kubuchwepheshe be-ECR kulesi sigaba samanje, ikakhulukazi inqubo yokuhlanganisa i-C─C, kukholakala ukuthi ngocwaningo oluqhubekayo nokuthuthukiswa kukho kokubili ukuthuthukiswa kwe-catalyst kanye nokuphelela kwamaseli, umbono we-electrolysis ye-CO2 yomhlaba wangempela kaphethiloli ohlanzekile. futhi amakhemikhali azobonakala esikhathini esizayo esiseduze.

Lena indatshana yokufinyelela evulekile esatshalaliswa ngaphansi kwemigomo yelayisensi ye-Creative Commons Attribution-NonCommerce, evumela ukusetshenziswa, ukusatshalaliswa, nokukhiqizwa kabusha kunoma iyiphi imidiya, inqobo nje uma ukusetshenziswa okuwumphumela kungekona okokuhweba futhi inqobo nje uma umsebenzi wokuqala ufanelekile. ikhonjiwe.

QAPHELA: Sicela ikheli lakho le-imeyili kuphela ukuze umuntu omncomayo ikhasi azi ukuthi ubufuna alibone, nokuthi aliyona i-imeyili eyimfucuza.Asithathi noma yiliphi ikheli le-imeyili.

© 2020 Inhlangano YaseMelika Yokuthuthukiswa Kwesayensi.Wonke Amalungelo Agodliwe.I-AAAS inguzakwethu we-HINARI, AGORA, OARE, CHORUS, CLOCKSS, CrossRef kanye ne-COUNTER.Science Advances ISSN 2375-2548.