Ngokubhekiselele kwiinkxalabo zokusingqongileyo kunye nokutshintsha kwamandla, ukuncipha kwe-electrochemical CO2 (ECR) kwixabiso elongeziweyo le-multicarbon (C2 +) amafutha kunye neekhemikhali, kusetyenziswa umbane ohlaziyekayo, kunika isisombululo esihle sexesha elide sokuvala umjikelo wekhabhoni kunye neenzuzo zoqoqosho ezongezelelweyo.Nangona kunjalo, ukudibanisa i-electrocatalytic C─C kwi-electrolyte yamanzi kusengumngeni ovulekileyo ngenxa yokukhetha okuphantsi, umsebenzi kunye nokuzinza.Uyilo lwee-catalysts kunye ne-reactors lubambe isitshixo sokujongana naloo mingeni.Sishwankathela inkqubela-phambili yamva nje malunga nendlela yokufezekisa ukudibanisa kwe-C─C ngokufanelekileyo nge-ECR, ngokugxininiswa kwizicwangciso ze-electrocatalysts kunye ne-electrocatalytic electrode / i-reactor design, kunye neendlela zabo ezihambelanayo.Ukongeza, iibhotile zangoku kunye namathuba exesha elizayo kwimveliso yeC2 + kuxoxwa ngayo.Sijonge ukubonelela ngophononongo oluneenkcukacha lwezicwangciso zokudibanisa i-C─C zanamhlanje kuluntu ukuze kuphuhliswe ngakumbi kunye nenkuthazo ekuqondeni okusisiseko kunye nokusetyenziswa kwethekhinoloji.

Ukukhutshwa okugqithisileyo kwe-carbon dioxide (CO2) kwi-atmosfera kubangele iziphumo ezinzulu zokusingqongileyo kwaye kukwabonisa isoyikiso esingxamisekileyo nesingenakuguqulwa kuluntu lwabantu (1, 2).Njengoko i-atmospheric CO2 i-concentration inyuke ngokukhawuleza ukusuka kwi-270 ppm (iinxalenye ngesigidi) ekuqaleni kwe-1800 ukuya kwi-401.3 ppm ngoJulayi 2015, ukuvumelana kwehlabathi lonke malunga nokuphinda kusetyenziswe i-carbon footprint ekhutshwe yimisebenzi yabantu ifikeleleke (3, 4).Ukuqonda i-loop esondeleyo ye-carbon footprint, enye indlela enokubakho kukutshintsha ukuxhomekeka kwamandla akhoyo kunye nemizi-mveliso yeekhemikhali kude kumafutha efosili ukuya kwimithombo ehlaziyekayo efana nelanga kunye nomoya (5–8).Nangona kunjalo, iqhezu lamandla avela kuloo mithombo ehlaziyekayo lilinganiselwe kuphela kwi-30% ngenxa yendalo yabo ephakathi, ngaphandle kokuba iindlela zokugcina amandla amakhulu ziyafumaneka (9).Yiyo loo nto, njengenye indlela, ukubanjwa kwe-CO2 ukusuka kwimithombo yeendawo efana nezityalo zamandla, kulandele ukuguqulwa kwi-feedstocks yeekhemikhali kunye namafutha, kusebenza ngakumbi (9-12).Ukunciphisa i-Electrocatalytic CO2 (ECR) usebenzisa umbane ohlaziyiweyo imele isisombululo esihle sexesha elide ngenxa yeemeko zokusebenza ezithambileyo ezifunekayo ekuguquleni, apho iimveliso ezongezelelweyo zexabiso zinokuveliswa ngokukhethiweyo (13).Njengoko kuboniswe ngokucwangcisiweyo kwi-Fig. 1, kule nkqubo, i-electrochemical electrolyzer iguqula i-CO2 kunye namanzi kwiikhemikhali kunye namafutha anikwe amandla ombane ohlaziyiweyo.I-fuel ebangelwayo iyakwazi ukugcina ixesha elide kwaye ingasasazwa okanye idliwe, ikhuphe i-CO2 njengeyona nkunkuma iphambili, eya kuthi ibanjwe kwaye ifakwe kwi-reactor ukuvala i-loop.Ngaphezu koko, isiphumo se-molekyuli encinci yokutya kweekhemikhali [umzekelo, i-carbon monoxide (CO) kunye ne-formate] evela kwi-ECR inokusetyenziswa njengezinto ezikrwada zokudibanisa imichiza entsonkothileyo.

Amafutha kunye neekhemikhali zinokufezekiswa kwi-ECR kunye nomjikelezo wekhabhoni ovaliweyo onikwe amandla yimithombo yamandla ahlaziyekayo njengelanga, umoya, kunye ne-hydro.Ubunjineli beeseli kunye nobunjineli be-catalyst budlala indima ebalulekileyo ekukhuthazeni ukukhetha, umsebenzi, kunye nokusebenza kakuhle kokuguqulwa kwe-CO2 kwiimveliso ze-C2 + ezinexabiso eliphezulu.

Nangona kunjalo, i-CO2 yimolekyuli yomgca ezinzileyo ene-C═O bond eyomeleleyo (750 kJ mol-1) (14), eyenza kube nzima ukuguqulwa kwe-electrochemical.Ngaloo ndlela, idinga umqobo ophezulu wokusebenza, othi, emva koko, ukhokelela kwizinto ezingaphezulu (15).Ngapha koko, i-ECR kwi-electrolyte enamanzi ibandakanya iinkqubo ezininzi zokudlulisa i-electron/proton kunye nenani lee-intermediates ezinokwenzeka ezahlukeneyo zokusabela kunye neemveliso (16-18), okwenza kube nzima kakhulu.Itheyibhile 1 ishwankathela isiqingatha electrochemical reactions thermodynamic yeemveliso eziphambili ECR, kuquka CO, methane (CH4), methanol (CH3OH), formic acid (HCOOH), ethylene (C2H4), ethanol (CH3CH2OH), njalo njalo, kunye zabo ezihambelanayo umgangatho redox amathuba (19).Ngokubanzi, ngexesha lenkqubo ye-ECR, iimolekyuli ze-CO2 kuqala zingena kwi-adsorption kunye nokusebenzisana neeathom kumphezulu we-catalyst ukuze zenze i-*CO2-, zilandelwa kukudluliselwa okuhamba ngamanyathelo okugqithisela kweeproton kunye/okanye ii-electron ukuya kwiimveliso ezahlukeneyo zokugqibela.Umzekelo, i-CH4 kukholelwa ukuba yenziwa ngezi ndlela zilandelayo: CO2 → *COOH → *CO → *CHO → *CH2O → *CH3O → CH4 + *O → CH4 + *OH → CH4 + H2O (20).

Umzobo we-2A ushwankathela ukusebenza kweFaradaic (FE) phantsi kwamazinga ahlukeneyo okuvelisa (uxinzelelo lwangoku) kwi-electrocatalysts ye-ECR exeliweyo, emele ukukhethwa kwemveliso yokusabela (21-43).Ngokucacileyo, ngelixa i-electrocatalysts yaseburhulumenteni inokuguqula i-CO2 ibe yimveliso ye-C1 (CO okanye i-formate) ngaphezu kwe-95% ye-FE phantsi kwezinga eliphezulu lemveliso (> 20 mA cm−2 yohlobo lweseli ye-H kunye > 100 mA cm− I-2 ye-flow cell) (9, 21, 22, 25, 28, 44, 45), i-highly selective (> 90%) kunye nokuveliswa ngokufanelekileyo kweekhemikhali ezininzi ze-multicarbon (C2 +) ezifumanekayo ngoku.Oku kungenxa yokuba ukudityaniswa kweemveliso ze-C2+ kufuna ukufika kunye nokubhengezwa kweemolekyuli ezininzi ze-CO2 kumphezulu, ukuguqulwa kwenyathelo, kunye nokumiswa kwendawo (13).Ukuchaneka, njengoko kuboniswe kwi-Fig. 2B, ukuphendula okulandelayo kwe-* CO intermediates kugqiba iimveliso zeC2 + zokugqibela ze-ECR.Ngokubanzi, i-C2H6 kunye ne-CH3COO− zabelana ngokufanayo *CH2 ephakathi, eveliswa kumanyathelo okudlulisa i-electron-proton edibeneyo ye-*CO.Iprotonation eyongezelelweyo ye-*CH2 inika *CH3 ephakathi, ekhokelela ekubunjweni kwe-C2H6 nge-*CH3 dimerization.Ngokungafaniyo nesizukulwana se-C2H6, i-CH3COO− yenziwe ngokufakela i-CO kwi-*CH2.I-*CO dimerization linyathelo lokumisela izinga le-C2H4, CH3CH2OH, kunye ne-n-propanol (n-C3H7OH) yokwakheka.Emva koluhlu lwamanyathelo okudluliselwa kwe-electron kunye ne-protonation, i-*CO─CO dimer yenza i-*CH2CHO ephakathi, esebenza njengenyathelo lokukhetha i-C2H4 kunye ne-C2H5OH.Ukongezelela, kwafunyaniswa ukuba ukunciphisa * I-CH2CHO ukuya kwi-C2H4 inesithintelo samandla esisezantsi kunokuguqula * CH3CHO ukuya kwi-C2H5OH (46), enokuthi ichaze i-FE ephezulu ye-C2H4 ngaphezu kwe-C2H5OH kuninzi lwe-catalysts zethusi.Ngaphezu koko, i-C2 intermediates ezinzileyo inokudluliselwa kwi-n-C3H7OH ngokufaka i-CO.Iindlela zokuphendula eziyinkimbinkimbi kunye nezingalawulekiyo ngexesha le-C2 + ukubunjwa kweekhemikhali zibangelwa ubukhulu becala ngenxa yeemvume ezininzi ezininzi kwiindawo ze-protonation, kunye nokubandakanyeka okunokwenzeka kwesinyathelo se-nonelectrochemical (19, 47).Ngaloo ndlela, uyilo lwee-electrocatalysts ezikhethiweyo kakhulu ziyimfuneko yokwenziwa kwemveliso ethile yeC2 + kwisivuno esiphezulu.Kolu hlaziyo, sijonge ukugqamisa inkqubela phambili yamva nje kwizicwangciso zoyilo lwe-electrocatalyst ekukhetheni ukuveliswa kwemveliso yeC2 + nge-ECR.Sikwabonelela ngesishwankathelo sokuqondwa kweendlela ezinxulumeneyo.I-Electrode kunye noyilo lwe-reactor luya kugxininiswa kwakhona ukubonisa indlela yokufezekisa ngokufanelekileyo, okuzinzileyo, kunye nokusebenza okukhulu kwe-ECR.Ngaphezu koko, siza kuxubusha imingeni eseleyo kunye namathuba azayo okuguqulwa kwe-electrochemical ye-CO2 kwiikhemikhali ze-C2 + zexabiso elongeziweyo.

(A) I-FE phantsi kwamazinga ahlukeneyo okuvelisa (uxinzelelo lwangoku) kwi-electrocatalysts ye-ECR exeliweyo (21-43, 130).(B) Uninzi lweendlela zeC2 + ezinokwenzeka ngexesha le-ECR.Iveliswe kwakhona ngemvume evela kwi-American Chemical Society (47).

Ukuguqulwa kwe-Electrocatalytic ye-CO2 kwi-fuel fuels kunye ne-feedstocks iteknoloji enokuthi iphumelele umjikelezo wamandla we-carbon-neutral (11).Nangona kunjalo, i-FE yeemveliso ze-C2 + isekude nesicelo esisebenzayo, apho i-state-of-the-art catalysts ivumela ukuveliswa kweemveliso ze-C2 kunye ne-60% FE (13, 33), ngelixa imveliso ye-C3 ilinganiselwe ngaphantsi kwe-10% I-FE (48, 49).Ukudityaniswa kokunciphisa i-CO2 kwiimveliso ze-C2 + kufuna i-catalysts engafaniyo eneempawu ezilungelelanisiweyo ze-morphological kunye ne-elektroniki (50, 51).Umphezulu we-catalytic ufuna ukwaphula ubudlelwane bokulinganisa phakathi kwabaphakathi (47, 52, 53).Ngaphezu koko, ukufezekisa ukubunjwa kwebhondi ye-C─C, i-reaction intermediates efunliweyo kwindawo ye-catalyst kufuneka ibe kufuphi enye kwenye.Ngaphaya koko, indlela esuka kwi-adsorbed yokuqala ephakathi ukuya kwimveliso ethile ye-C2+ kufuneka ilawulwe kakuhle ngenxa yamanyathelo okudlulisa i-electron amaninzi ancediswa yiproton.Ukuqwalasela ubunzima obuphezulu bokunciphisa i-CO2 ngokubhekiselele kwiimveliso ze-C2 +, i-electrocatalysts kufuneka ilungiswe ngononophelo ukunyusa ukukhetha.Ngokweentlobo eziphakathi kunye nokwakhiwa kweekhemikhali, sihlula imveliso ye-C2 + kwi-multicarbon hydrocarbons kunye ne-oxygen (4, 54).Ukusondela kwi-electrocatalysts efanelekileyo kakhulu yokuveliswa kwe-molecule ye-C2 +, izicwangciso ezininzi zokuyila, ezifana ne-heteroatom doping, i-crystal facet regulation, i-alloy / i-dealloying, i-oxidation state tuning, kunye nokulawulwa kwe-ligand yomhlaba, kubonisiwe (35, 41, 55-61) .Uyilo olulolona lufanelekileyo kufuneka luthathele ingqalelo le mpembelelo ikhankanywe ngasentla kwaye yandise inzuzo.Kungenjalo, ukuqonda ukuba yeyiphi i-motifs esebenzayo yesiza ekhokelela kwindlela enje yokuziphatha ekhuthazayo kunokukhanyisela ngakumbi uyilo oluchanekileyo lwe-catalyst yokudibanisa i-C─C.Ke, indlela yokuyila i-ECR i-catalyst ukuya kwiimveliso ezithile (i-multicarbon hydrocarbons kunye ne-oksijeni) kunye nendlela ehambelana nayo iya kuxoxwa kule nxalenye.

I-C2 + hydrocarbons, njenge-C2H4, iikhemikhali ze-nexus kwiindidi zamashishini amachiza, njengemveliso ye-polyethylene (62, 63).Ngaphandle koko, inokusetyenziswa ngokuthe ngqo njengesibaso se-welding okanye icandelo elixutywe kwigesi yendalo (12).I-Hydrogenation ye-CO (i-Fischer-Tropsch synthesis) kunye ne-CO2 isetyenziselwe ukuvelisa i-C2 + i-hydrocarbons ixesha elide kwi-industrial scale kodwa icela umngeni ngokusetyenziswa kwamandla aphezulu kunye nefuthe lokusingqongileyo (64).Ngokwahlukileyo, ukunciphisa i-electrochemical CO2 usebenzisa amandla ahlaziyekayo kunika indlela ecocekileyo kunye nezinzileyo.Umzamo omkhulu uye wenziwa ukuphuhlisa i-electrocatalysts esebenzayo ngokubhekiselele kwi-C2 + hydrocarbons (32, 33, 65-70).

I-Bimetallic electrocatalysts iphandwe ngokubanzi ukuphula ubudlelwane bokulinganisa ngexesha lokuguqulwa kwe-electrochemical CO2, enokuzinzisa i-key intermediate kunye nokunciphisa i-overpotential kwaye, ngoko ke, ukwandisa ukukhetha (71-74).Ngelixa uchungechunge lwezixhobo ze-alloy ezibandakanya i-Au-Cu, i-Ag-Cu, i-Au-Pd, kunye ne-Cu-Pt ibonakaliswe ngokusebenza okuphezulu kwemveliso ye-C1 ngokuzinzisa i-intermediate ebalulekileyo (73, 75), umphumo we-alloy ngokubhekiselele kwi-C2 + i-hydrocarbon formation ibonakala. ukuba nzima ngakumbi (76).Ngokomzekelo, kwinkqubo ye-bimetallic ye-Cu-Ag, ukuhanjiswa kwemveliso kunokulawulwa lula ngokulungelelanisa umlinganiselo we-athomu ye-athomu ye-Ag kunye ne-Cu (77).I-surface Cu-rich sample ikhethwa kwimveliso ye-hydrocarbon, ngelixa iimveliso zomphezulu we-Ag-rich zilawulwa yi-CO, igxininisa ukubaluleka komlinganiselo we-athomu kwi-electrocatalysts ye-ECR edibeneyo.Umphumo wejometri obangelwa ukulungiswa kwe-athomu yendawo inokuchaphazela kakhulu amandla okubopha abaphakathi.I-Gewirth kunye nabasebenzi abasebenzisana nabo (36) babonise ukuba i-Cu-Ag alloys evela kwi-electrodeposition eyongeziweyo elawulwayo ibonakaliswe ~ 60% FE ye-C2H4 kwi-alkaline flow electrolyzer (Umfanekiso 3, A kunye no-B).Kule meko, ukhetho oluphuculweyo lwe-C2H4 lunokuphunyezwa nge-morphology kunye ne-Ag-loading tuning.Iindawo ze-Ag zazikholelwa ukuba zidlala indima yokukhuthaza ukwakhiwa kwe-CO ngexesha le-ECR.Emva koko, ukufumaneka okugqibeleleyo kwe-CO ephakathi kunokunceda ukudibanisa kwe-C─C kwiCu engummelwane.Ngaphandle koko, i-Ag inokukhuthaza ukubunjwa kwe-Cu2O ngexesha le-Cu-Ag catalyst synthesis (Umfanekiso 3C), okukhokelela ekuphuculweni kwemveliso yeC2H4.Le synergy ivula amathuba amatsha okuphuhlisa iC─C coupling catalysts.Ngaphaya koko, ipateni yokuxuba yeentsimbi ezahlukeneyo kwinkqubo yealloyi inokumisela ukuhanjiswa kweemveliso ze-ECR.Ukusebenzisa i-Pd-Cu i-alloy njengomzekelo (umfanekiso we-3D), i-Kenis kunye nabasebenzi abasebenzisana nabo (71) babonise ukuba i-Pd-Cu i-catalyst eyahlulwe ngesigaba inokunika ukhetho oluphezulu (~ 50%) lwe-C2H4 xa kuthelekiswa nomyalelo kunye nokuphazamiseka. abalingane.Ngokwethiyori ye-d-band, ngokwesiqhelo, isinyithi soguqulo esineziko le-d-band elisezantsi libonisa ukubophelela okubuthathaka kwe-in situ eyenziweyo ephakathi kumphezulu wesinyithi (78).Ngelixa i-Pd-Cu i-alloy eyahlulwe ngesigaba ibonise ukukhethwa okufanayo kwe-catalytic kunye nomsebenzi we-CO kunye ne-Cu nanoparticles (NPs), inikeze amandla okubopha ahluke ngokupheleleyo kuma-intermediates nge-Pd tuning.Njengoko kubonisiwe kwi-Fig. 3E, i-Cu-Pd i-alloy eyahlulwe ngesigaba ibonise i-d-band centre, ngelixa i-Cu NP iphezulu.Iphakamisa ukuba i-alloy ye-Cu-Pd eyahlulwe ngesigaba yayinamandla aphantsi okubopha kwi-CO ephakathi.Olu qwalaselo luthetha ukuba i-geometric kunye ne-structure effect inokudlala indima enkulu kunempembelelo ye-elektroniki yokuphucula ukukhethwa kwe-hydrocarbon kwimeko ye-Cu-Pd ye-alloy ehlukeneyo yesigaba.Ukuza kuthi ga ngoku, kuphela ubhedu olucocekileyo okanye i-alloy-based alloy-based alloy ibonisa ukhetho oluphezulu kunye nomsebenzi wokunciphisa i-electrochemical ye-CO2 ukuya kwi-C2 + hydrocarbons.Ke, kubaluleke kakhulu ukuphuhlisa i-electrocatalyst yenoveli yeC2 + yemveliso ye-hydrocarbon evela kwi-ECR.Iphefumlelwe yi-CO2 hydrogenation, uphando lokuqala lubonise ukuba i-alloy ye-Ni-Ga enezigaba ezahlukeneyo ingasetyenziselwa isizukulwana se-C2H4 (79).Kubonise ukuba ifilimu ye-Ni5Ga3 inokunciphisa i-CO2 kwi-C2H4 kunye ne-ethane (C2H6).Nangona i-FE ebhekiselele kwi-C2+ hydrocarbons ingaphantsi kwe-5%, inokuvula imigca emitsha yokuhlolwa kwe-electrocatalyst ukuya kwi-C─C coupling ngokusekelwe kwisiphumo se-alloy.

(A ukuya ku-C) I-Cu-Ag i-bimetallic catalysts eyenziwe nge-electrodeposition elawulwayo eyongeziweyo: (A) i-electron microscopy yokuskena (SEM) ye-Cu wire, i-Cu-Ag ye-poly, kunye ne-Cu-Ag yocingo kunye (B) ehambelana ne-C2H4 FE.(C) I-EXAFS ibonise ukuba ucingo lwe-Cu-Ag lwaluxutywe ngokulinganayo kwaye i-Cu(I) oxide yaboniswa.(A) ukuya ku (C) ziveliswa kwakhona ngemvume evela kwi-American Chemical Society (36).(D kunye no-E) I-Cu-Pd catalysts eneendlela ezahlukeneyo zokuxuba: (D) Umzobo, imifanekiso ye-electron microscopy (TEM) yothumelo, kunye ne-energy-dispersive spectroscopy element iimephu ze-odolo, ukuphazamiseka, kunye nesigaba esahlulwe i-Cu-Pd alloys kunye (E ) i-surface valence band photoemission spectra kunye ne-d-band centre (umgca othe nkqo) we-Cu-Pd i-alloys enxulumene nenqanaba leFermi.(D) kunye (E) ziveliswa kwakhona ngemvume evela kwi-American Chemical Society (71).okanye, iiyunithi ezingafanelekanga.

Ngaphandle kwesiphumo se-alloy, ukuxhaphaza amazwe e-oxidation ngomnye umgaqo-siseko omkhulu wokulungelelanisa ukusebenza kwee-electrocatalysts, ezinokuchaphazela isakhiwo se-elektroniki sendawo.Umzekelo wokuqala wokulungelelaniswa kwemeko ye-oxidation ye-catalyst kukusebenzisa izinto ezenziwe nge-oxide.Iintlobo ze-oksijini ezishiyekileyo kumphezulu okanye ngaphantsi kwe-catalyst emva kokunciphisa i-situ inokulawula imeko ye-oxidation yeziko lesinyithi.Ngokomzekelo, i-plasma-oxidized Cu ibonise ngaphezu kwe-60% ukhetho olubhekiselele kwi-C2H4, echazwe kwi-Cu + (37) enganyangekiyo.Ukuqinisekisa ukuba i-Cu + iyipharamitha ephambili yokukhethwa kwe-ethylene ephezulu, senze iimvavanyo zokulawula usebenzisa i-plasma eyahlukileyo (umzobo 4A).Kwisitu enzima x-reyi ukufunxa ispectroscopy kwakhona yabonisa ukuba intsalela oxides kumphezulu (ngaphantsi) umaleko uzinzile ngokuchasene nemeko yokunciphisa, kunye nesixa esibalulekileyo seentlobo ze-Cu+ eziseleyo emva kweyure e-1 yokunciphisa kumandla aphezulu -1.2 V xa kuthelekiswa nokubuyiselwa umva. i-hydrogen electrode (RHE).Ngaphezu koko, i-electroredeposition yobhedu evela kwi-sol-gel yethusi i-oxychloride iphinde yaqinisekisa kwakhona ukuba i-surface ezinzileyo ye-Cu + iintlobo inokuphucula ukukhethwa kwe-C2H4 (61).Imeko ye-oxidation ye-catalyst yobhedu phantsi kweendlela ezahlukeneyo ezisetyenzisiweyo zalandelelwa kusetyenziswa ixesha elisonjululwe kwi-situ ethambileyo ye-x-reyi yokufunxa ispectroscopy.Inyathelo lokuqala lokutshintsha ukusuka kwiCu2 + ukuya kwiCu + likhawuleza kakhulu;nangona kunjalo, ukucutha ngakumbi kwe-electrochemical ye-Cu + iintlobo ukuya kwi-Cu0 icotha kakhulu.Malunga ne-23% yeentlobo ze-Cu+ zihlala nasemva kweyure enye yokuncipha rhoqo phantsi kwe-−1.2 V xa kuthelekiswa ne-RHE (Fig. 4B).Izifundo zoomatshini zibonise ukuba ujongano phakathi kwe-Cu+ kunye ne-Cu0 lukhokelela kumtsalane we-electrostatic phakathi kwabaphakathi ekubeni i-athomu ye-C ye-*CO @ Cu+ ichajiwe kakuhle, ngelixa leyo ye-*CO @ Cu0 ihlawuliswa kakubi (80), yona, iphakamisa Ukwakhiwa kwebhondi ye-C─C kwaye ngaloo ndlela ivelisa i-C2 + hydrocarbons.Ukongeza kwizinto ezenziwe nge-oxide, i-nitride yobhedu (Cu3N) nayo yasetyenziselwa ukuphumeza (i-sub)surface yeentlobo ze-Cu+ ukunciphisa umqobo we-dimerization wamandla we-*CO (81).Ukongezelela, xa kuthelekiswa ne-oxyde-derived Cu, iintlobo zeCu3-derived Cu + zizinzile ngakumbi (umzobo 4C).Ngenxa yoko, i-nitride-derived copper catalyst ibonisa i-FE ye-39 ± 2% ye-C2H4, idlula i-Cu ecocekileyo (~ 23%) kunye ne-Cu (~ 28%).Ngokufana nale ikhankanywe ngasentla yeCu+/Cu catalytic system, iboron isetyenziswe njenge heteroatom dopant ukwazisa nokuzinzisa iCuδ+ (41).Umyinge wemeko ye-oxidation yobhedu inokulawulwa ukusuka +0.25 ukuya +0.78 ngokuguqula ukuxinwa kwe-boron dopant.Uxinaniso lwamazwe oluqikelelweyo lubonise ukuba ii-electron zikhutshelwe ukusuka kwikopolo ukuya kwi-boron, okukhokelela kwiziza zobhedu ezifakwe kwi-dopant.Ubhedu lwe-boron-doped lubonise ukonyuka kwamandla okwenziwa kwe-*CHO phakathi kwaye, ngoko, yacinezela indlela yokusabela kwiimveliso ze-C1.Ukongeza, inokonyusa ukhetho oluya kwi-multicarbon hydrocarbons ngokunciphisa *CO dimerization reaction energy (Fig. 4D).Ngokulungisa umyinge wemeko ye-oxidation ye-copper, i-C2 FE ephezulu ye-~80% kunye ne- ~ 53% ye-C2H4 inokufezekiswa phantsi komgangatho we-oxidation yethusi ye-0.35 (Fig. 4E).Ukuza kuthi ga ngoku, iindawo ezisebenzayo kubhedu ziye zachongwa njengeCu0, Cuδ+, kunye / okanye i-interface yazo ye-ECR kwizifundo ezahlukeneyo (39, 41, 42, 81, 82).Nangona kunjalo, yintoni isayithi esebenzayo kusaxoxwa ngayo.Ngelixa i-heteroatom doping-induced Cuδ+ catalysts ibonakaliswe isebenza kakhulu kwi-ECR ngokubhekiselele kwiimveliso ze-C2+, isiphumo se-synergistic esivela kwiziphene ezenziwe ngaxeshanye kunye nojongano kufuneka ziqwalaselwe.Yiyo loo nto, ukucwangciswa kweempawu ze-operando kufuneka kuphuhliswe ukuchonga iziko elisebenzayo kumphezulu wobhedu kunye nokubeka iliso kwinguqu enokubakho kwimeko yeendawo ezisebenzayo phantsi kweemeko zokusabela.Ngaphandle koko, ukuzinza kobhedu oluhlanjululweyo ngenye inkxalabo phantsi kweemeko zokunciphisa i-electrochemical.Indlela yokwenza ii-catalysts ngeziza ezizinzileyo ze-Cuδ+ zihlala zingumceli mngeni.

(A) Isishwankathelo sokukhethwa kwe-C2H4 yee-catalysts zobhedu ezahlukeneyo ze-plasma.Iveliswe kwakhona ngemvume evela kwiQela loPapasho lweNdalo (37).Imivalo yokulinganisa, i-500 nm.(B) Umlinganiselo we-Cu oxidation uthi xa kuthelekiswa nexesha lokusabela kwi- -1.2 V xa kuthelekiswa ne-RHE kwi-electroredeposited copper.Iveliswe kwakhona ngemvume evela kwiQela loPapasho lweNdalo (61).(C) Umlinganiselo weentlobo ze-Cu + kunye nomsebenzi wexesha lokuphendula kwi-−0.95 V ngokuchasene ne-RHE kwi-Cu-on-Cu3N okanye i-Cu-on-Cu2O.Iveliswe kwakhona ngemvume evela kwiQela loPapasho lweNdalo (81).(D) I-Boron doping yakwazi ukutshintsha i-avareji ye-adsorption energy ye-CO kwindawo yobhedu kwaye yehlisa amandla e-CO─CO dimerization.I-1[B], i-2[B], i-3[B], i-4[B], kunye ne-8[B] ibhekisela kuxinzelelo lwe-doping engaphantsi komhlaba kwi-catalysts yobhedu, eyayiyi-1/16, 1/8, 3/ 16, 1/4, kunye ne-1/2 ngokulandelelanayo.(E) Ubudlelwane phakathi kwemeko ye-oxidation kunye ne-FE ye-C2 okanye i-C1 yeemveliso kwi-boron-doped catalysts zethusi.(D) kunye no (E) ziphinde zenziwe kwakhona ngemvume evela kwiQela loPapasho lweNdalo (41).(F) Imifanekiso ye-SEM yeefoyile zobhedu ezinobunzima obuhlukeneyo beefilimu ze-Cu2O ngaphambi (phezulu) nasemva (ezantsi) kwe-ECR.Iveliswe kwakhona ngemvume evela kwi-American Chemical Society (83).

Ngaphandle kwesakhiwo se-elektroniki, izinto eziphuma kwi-oxide zinokukhokelela kwi-morphology okanye kwi-structure evolution ngexesha lenkqubo yokunciphisa indawo.Ukususela kumbono we-morphology okanye isakhiwo, ukuphuculwa kwentsebenzo ye-electrochemical ye-electrocatalysts ephuma kwi-oxide iye yabangelwa ukubunjwa kwemida yengqolowa esebenzayo, imiphetho, kunye namanyathelo (83-85).U-Yeo kunye nabasebenzi abasebenzisana nabo (i-83) bachaze ukudibanisa kwe-C─C ekhethiweyo kwiifilimu ze-Cu2O ze-electrodeposited ezinobunzima obuhlukeneyo (Umfanekiso we-4F).I-In situ Raman spectroscopy ibonise ukuba umphezulu weefilimu ze-Cu2O wancitshiswa waba yi-Cu0 yentsimbi ezinzileyo ngexesha le-ECR (83).Ngenxa yoko, i-metallic Cu0 iye yaqinisekiswa njengeziko elisebenzayo le-catalytic endaweni yeentlobo ze-Cu + okanye i-Cu +/Cu0 interface.Kwinkqubo yokunciphisa i-Cu2O ukuya kwi-Metallic Cu0, umphezulu we-catalyst unokwenzeka ukuba ube kwi-situ form amanyathelo, imiphetho, kunye neeterras.Kwacaciswa ukuba amanyathelo abunjiweyo kunye namaphethelo asebenzayo ngakumbi kuneendawo zokuhlala, ezisuka ekuzibopheni kwazo ezomeleleyo kunye ne-*CO, enokuthi iqhube i-hydrogenate * CO ukuya * Cho okanye * CH2O.Ngaphandle koko, ii-athomu ze-edge Cu zingumgqugquzeli wokunyusa i-*CHO kunye ne-*CH2O yokwakheka.Umsebenzi wangaphambili ucebise ukuba * I-CHO kunye ne-*CH2O abaphakathi balungele ngakumbi ukudibanisa kwe-C─C kune-CO kwi-kinetics (86).Ngokulawula i-morphology ye-surface, amandla e-chemisorption e-*CHO kunye ne-*CH2O intermediates anokuphuculwa.Kulo cwaningo, ababhali bafumanisa ukuba i-FE ye-C2H4 yehla ukusuka kwi-40 ukuya kwi-22% xa inyusa ubukhulu befilimu ye-Cu2O encinci ukusuka kwi-0.9 ukuya kwi-8.8 μm.Oku kungenxa yokuxinana kweCu elungelelanisiweyo ephantsi eye yanda ngokunyuka kweCu2O ubukhulu.Ezi athom zingalungelelaniswanga kakhulu zinokubopha ngamandla kunye ne-H kwaye, ngenxa yoko, zikhethwa ngakumbi kwi-hydrogen evolution kunokudibanisa i-C─C.Lo msebenzi ubonise ukuba i-oxyde-derived copper catalyst inokunyusa kakhulu ukukhetha kwe-C2H4 ngokwakhiwa ngokutsha kwe-morphology endaweni yokwazisa iindidi ze-Cuδ+ ezihlawuliweyo.Ukusebenzisa i-catalysts ephuma kwi-oxide, i-ethane (C2H6) iphinde iveliswe ngokukhethiweyo ngoncedo lwe-palladium (II) i-chloride (PdCl2) eyongeziweyo kwi-electrolyte (34).Ibonise ukuba i-adsorbed PdClx kumphezulu weCu2O-derived Cu idlale indima ebalulekileyo kwi-C2H6 evolution.Ngokukodwa, i-CO2 yaqala yancitshiswa yaba yi-C2H4 kwiindawo ze-Cu2O-derived active Cu, kwaye emva koko i-C2H4 eyenziwe iya kuba yi-hydrogenated ngoncedo lwe-adsorbed PdClx ukuvelisa i-C2H6.I-FE ye-C2H6 inyuke ukusuka ku-<1 ukuya kwi-30.1% ngoncedo lwe-PdCl2.Lo msebenzi ucebisa ukuba ukudibanisa kwe-ECR catalyst echazwe kakuhle kunye ne-electrolyte additive inokuvula amathuba amatsha kwimveliso ethile yeC2 +.

I-Morphology kunye / okanye ukulawulwa kwesakhiwo kubonisa esinye isicwangciso sokulungelelanisa ukhetho kunye nomsebenzi.Ukulawula ubungakanani, imilo, kunye neenkalo eziveziweyo ze-catalyst zibonakaliswe ngokubanzi ekuphuculeni ukusebenza kwe-ECR (58, 87, 88).Umzekelo, i-Cu(100) i-facet ikhethwa ngokunyanisekileyo kwisizukulwana se-C2H4, ngelixa imveliso elawulwayo evela kwi-Cu (111) catalyst yi-methane (CH4) (87).Kuphononongo lwe-Cu nanocrystals eneemilo ezahlukeneyo kunye nobukhulu, i-Buonsanti kunye nabasebenzi abasebenzisana nabo (i-58) ibonise ukuxhomekeka kobungakanani be-nonmonotonic ye-C2H4 yokukhetha kwi-cube-shaped copper nanocrystals (Fig. 5A).Ngokwemvelo, i-cubic Cu nanocrystals ibonise umsebenzi ophezulu we-C2H4 kunye nokukhetha kune-spherical Cu nanocrystals ngenxa ye-predominance ye-facet (100).Ubungakanani obuncinci bekristale beCubic Cu bunokubonelela ngomsebenzi ophezulu ngenxa yokunyuka koxinzelelo lweendawo ezisezantsi ezilungelelanisiweyo, ezinje ngeekona, amanyathelo, kunye neekinks.Nangona kunjalo, i-chemisorption eyomeleleyo yeendawo ezilungelelanisiweyo eziphantsi zihamba kunye nokukhethwa okuphezulu kwe-H2 kunye ne-CO, okukhokelela kwi-FE ye-hydrocarbon ephantsi.Ngakolunye uhlangothi, umlinganiselo weendawo ezinqamlekileyo kwiindawo zendiza ziye zancipha ngokunyuka kobukhulu beengqungquthela, ezichaphazela nokusebenza kwemveliso yeC2H4.Ababhali babonise ukuba i-nanocubes yobhedu ephakathi kunye ne-44-nm edge ubude ibonise ukhetho oluphezulu lwe-C2H4 ngenxa yebhalansi ephuculweyo phakathi kobukhulu be-particle kunye nobuninzi beendawo ezinqamlekileyo.Ngapha koko, i-morphology inokuchaphazela i-pH yendawo kunye nokuthuthwa kobuninzi ngexesha le-ECR.Kubonisiwe ukuba i-pH ephezulu yendawo kwindawo ekufutshane ne-catalyst surface, ebangelwa yi-in situ eyenziwe yi-OH−, icinezela indlela yokusabela ebandakanyekayo kwiproton.Ngenxa yoko, ukwenziwa kwe-C2+ hydrocarbon ngokusebenzisa *CO dimerization kunokuphuculwa, kwaye i-CH4 eyenziwe nge-*COH ephakathi inokuthintelwa.I-Copper nanowire arrays (Umfanekiso we-5B) ibonakaliswe ukuphumeza ukunyuka kwe-pH yendawo (68).Njenge-electrolyte esetyenziswa ngokuqhelekileyo, isisombululo se-CO2 saturated potassium bicarbonate (KHCO3) siya kunciphisa ngokukhawuleza i-OH-(HCO3- + OH- = CO32- + H2O) kunye nokunciphisa i-pH yendawo.Nge-microstructure emide, i-diffusion yeHCO3- kwi-Cu nanowire arrays ingathotywa ngandlela-thile ukwenzela ukuba i-neutralization effect ye-OH-yasekhaya iya kunyanzeliswa kwinqanaba elithile.Ngokwesiseko somgaqo ofanayo, i-meshes yobhedu ene-mesopores elawulwa ngokuchanekileyo (Umfanekiso we-5C) ubonise i-FE ephuculweyo ye-C2H4 okanye i-C2H6 yemveliso (32).Ibonise ukuba i-pH yendawo kwindawo ye-electrode inokunyuswa ngokunciphisa ububanzi be-pore, okukhokelela ekunciphiseni kwe-C1 imveliso ye-FE kunye nokuphucula imveliso ye-C2 ye-FE.Ngaphandle koko, ngokwandisa ubunzulu bepore, imveliso enkulu yokunciphisa inokulungiswa ukusuka kwiC2H4 ukuya kwiC2H6.I-FE ye-C2H6 yayiphezulu njenge-46%.Ekubeni iikhemikhali zivalelwe ngaphakathi kwee-pores ngexesha le-ECR, ixesha elide lokugcinwa kwezinto eziphambili ezibangelwa yi-pores ezinzulu zichazwe njengesona sizathu sokukhethwa okuphezulu kwi-C2 hydrocarbon egcweleyo.I-CuI-derived Cu nanofibers nayo ibonise ukukhetha okuphezulu ngokubhekiselele kwi-C2H6 (FE = 30% kwi- -0.735 V ngokuchasene ne-RHE) (89).I-anisotropic morphology kunye ne-high surface roughness ye-CuI-derived Cu nanofibers inokuphucula ukusebenza kakuhle kwe-H2 efunyenweyo kwaye ngoko yandise i-FE ye-C2H6.

(A ukuya ku-C) I-Morphology okanye iziphumo zesakhiwo.(A) Ubuninzi bee-athom (umgca ohamba ngasekhohlo) kunye nomlinganiselo weeathom kwiindawo ezisekupheleni (i-Nedge) ukuya kwii-athom ezikwi-(100) kwinqwelo-moya (N100) (i-axis yasekunene) ngokunxulumene nobude bodini (d).Iveliswe kwakhona ngemvume evela kuJohn Wiley kunye noonyana (58).(B) Inkqubo ye-morphology ibangele ukutshintsha kwe-pH.Iveliswe kwakhona ngemvume evela kuJohn Wiley kunye noonyana (68).(C) Ukukhethwa kwemveliso yobhedu lwe-mesopore kunye nobukhulu obuhlukeneyo kunye nobunzulu.Iveliswe kwakhona ngemvume evela kuJohn Wiley kunye noonyana (32).(D ukuya kuH) Iziphumo zeLigand.(D kunye no-E) I-ECR kwi-copper nanowire (Cu NW) eneentlobo ezahlukeneyo zee-amino acids (D) okanye izilungisi (E) e- -1.9 V. Iveliswe kwakhona ngemvume evela kwiRoyal Society of Chemistry (35).(F) Amazinga okuvelisa i-C2H4 kwii-electrolyte ezahlukeneyo ze-halide kunye ne-adsorption ehlukeneyo ye-adsorption kwi-Cu (35).Iveliswe kwakhona ngemvume evela kwi-American Chemical Society (91).I-NHE, i-electrode ye-hydrogen eqhelekileyo.(G) I-FE ye-C2H4 kunye ne-CO kwiindawo ezahlukeneyo ze-KOH electrolytes kunye (H) i-Tafel slope ye-C2H4 kwiimpawu ezahlukeneyo ze-KOH electrolytes.(G) kunye (H) ziveliswa kwakhona kwi-American Association for the Advancement of Science (AAAS) (33).

Ukuguqulwa komphezulu we-Catalyst usebenzisa iimolekyuli ezincinci sesinye isicwangciso esaziwayo sokuphucula ukusebenza kwe-electrochemical ye-ECR.Esi sicwangciso sinokuchaphazela i-microenvironment kufuphi ne-catalyst surface, enokuzinzisa i-intermediates eziphambili ngenxa yokusebenzisana phakathi kwe-surface ligand kunye ne-intermediate.I-Amine iye yabikwa njenge-modifier yokukhuthaza i-ECR (35).Iintlobo ezahlukeneyo ze-amino acids, kuquka i-glycine (Gly), i-dl-alanine (i-Ala), i-dl-leucine (i-Leu), i-dl-tryptophan (iTyr), i-dl-arginine (i-Arg), kunye ne-dl-tryptophan (Trp), ziye zaphandwa ukuze funda iziphumo zazo kwiinanowires zethusi (35).Njengoko kuboniswe kwi-Fig. 5D, zonke ii-amino acid-based ligands zikwazi ukuphucula ukukhethwa kwe-C2 + hydrocarbons.Uphuculo olunjalo lucebisa ukuba i-─COOH kunye ne-─NH2 amaqela asebenzayo kwi-amino acid mhlawumbi anoxanduva lokukhetha okuphuculweyo kwe-ECR.Iingxelo zangaphambili zibonise ukuba i-adsorption ye-amino acids kwi-Cu surface iphunyezwe ngokusebenzisa zombini i-─COOH kunye ne-─NH2 amaqela (35, 90).I-Stearic acid (C17H35COOH, RCO2H), equlethe kuphela iqela le-─COOH, likhethwe ukuchonga indima ye-─COOH.Ezinye izilungisi, ezifana ne-a-anthraquinone diazonium salt (AQ), i-o-nitrobenzene diazonium salt (PhNO2), kunye ne-dodecyl mercaptan (C12H25SH, RSH), ezingaqulathanga ─COOH okanye ─NH2 amaqela, nazo ziye zaphandwa.Nangona kunjalo, zonke azizange zilungele ukuphuculwa kwe-C2 + hydrocarbon FE (Umfanekiso 5E).Ubalo lwethiyori lubonise ukuba amaqela e-─NH3+ kwi-adsorbed zwitterionic glycine anokuzinzisa *CHO phakathi ngenxa yokusebenzisana okunamandla, okufana neebhondi ze-hydrogen.Ukuqaliswa kweeoni ze-halide kwi-electrolyte enye indlela yokuguqula i-catalysts (91, 92).Njengoko kuboniswe kwi-Fig. 5F, izinga lokuvelisa i-C2H4 kwi-plasma-activated Cu inokwandiswa kakhulu ngoncedo lwezongezo ze-halide.Kwaboniswa ukuba i-I− ion isebenza ngakumbi kune-Br− ne-Cl-, ngokuvumelana namandla ahambelanayo e-adsorption ye-I-, Br-, kunye ne-Cl-kwi-Cu(100) facet (91).Ngaphandle kwe-halides, i-ion ye-hydroxide nayo ibonise umphumo omuhle kwi-C2H4 yokukhetha.Kungekudala, i-Sargent kunye nabasebenzi abasebenzisana nabo (33) babika ukuguqulwa kwe-CO2-to-C2H4 kunye ~ 70% FE usebenzisa i-electrolyte ye-potassium hydroxide (KOH) edibeneyo (ukuya kwi-10 M) kwiseli yokuhamba.Njengoko kuboniswe kwi-Fig. 5G, amandla okuqala e-CO kunye ne-C2H4 kwi-electrolyte ye-10 M KOH yayiphantsi kakhulu xa kuthelekiswa naleyo kwi-1 M KOH.Ngaphaya koko, amathambeka eTafel (Umfanekiso 5H) weC2H4 ukwakheka kwehle ngokunyuka koxinzelelo lwehydroxide (135 mV decade−1 kwi-1 M KOH kunye ne-65 mV decade−1 kwi-10 M KOH), ecebisa ukutshintshwa kwereyithi iyonke- inyathelo lokumisela.Iziphumo zethiyori esebenzayo yoxinaniso (DFT) zibonise ukuba ubukho beehydroxides ezigxininisiweyo zinokuthoba amandla okubopha kwi-CO ephakathi kwaye konyuse ukungalingani kwentlawulo phakathi kweeathom zekhabhoni ezimbini kwi-adsorbed OCCO intermediates.Ngenxa yoko, i-OCCO ephakathi iya kuzinziswa ngakumbi ngomtsalane we-dipole enamandla, ekhokelela ekuvuleni okusezantsi komqobo we-CO dimerization, eya kuthi emva koko iphucule ukusebenza ngokubanzi.

I-C2+ oxygenates efana ne-ethanol (CH3CH2OH) lolunye udidi oluphambili lweemveliso ze-ECR ezibaluleke kakhulu.I-industrial synthesis ye-ethanol yinkqubo enamandla kakhulu, ekwasebenzisa isixa esikhulu se-ethylene okanye i-feedstocks yezolimo (40).Ngaloo ndlela, imveliso ye-electrocatalytic ye-ethanol okanye enye i-C2 + oxygenates esuka kwi-CO2 yenza ubuninzi bezoqoqosho kunye nokusingqongileyo.Ekubeni isizukulwana se-ethanol esivela kwi-ECR sabelana nge-penultimate intermediate kunye ne-C2H4 oko kukuthi * C2H3O (43), i-hydrogenation ekhethiweyo yale ndawo iphakathi inokutshintsha iindlela ze-ECR ukusuka kwi-C2H4 ukuya kwi-alcohols (64).Nangona kunjalo, kwiinkqubo ezininzi, ukhetho olubhekiselele kwi-C2 + oxygenates luphantsi kakhulu kune-hydrocarbons (31, 37, 39, 41, 42, 67).Ngaloo ndlela, kweli candelo, siya kugxininisa izicwangciso zoyilo ze-electrocatalyst ezinokufikelela kwi-C2 + oxygenate FE ekhangayo ngaphezu kwe-25%.

Njengoko kuxoxwe ngasentla, i-bimetallic catalysts eyilwe kakuhle inokuphucula ukhetho kunye nomsebenzi weC2 + hydrocarbon production.Isicwangciso esifanayo kodwa esingafaniyo sisetyenziselwe ukuphucula ukusebenza kwe-electrocatalytic ye-C2 + oxygenates (38, 93, 94).Ngokomzekelo, i-Ag-incorporated Cu-Cu2O catalysts ibonise ukukhethwa kwe-ethanol enokutyibilika, kwaye eyona FE iphezulu ye-ethanol yayiyi-34.15% (95).Umda we-biphasic kwi-alloy ye-Ag-Cu edibeneyo yesigaba, endaweni ye-Ag / Cu ye-atomic ratio, ichongiwe njengento ephambili yokuvelisa okukhethiweyo kwe-ethanol.Ekubeni indawo ye-Cu isondele kakhulu kwindawo ye-Ag kwipatheni edibeneyo yesigaba (i-Ag-Cu2OPB), izinga lokubunjwa kwe-ethanol intermediates kwisampula edibeneyo yesigaba inokukhuthazwa xa kuthelekiswa nesigaba esahlukileyo (Ag-Cu2OPS). ), ekhokelela ekusebenzeni ngcono kwesizukulwana se-ethanol.Ngaphandle kwe-ethanol, i-Cu-Ag ye-bimetallic NPs nayo ibonakaliswe ukuguqula i-CO2 kwi-acetate kunye nokongezwa kwe-benzotriazole (93).Kwi- -1.33 V ngokuchasene ne-RHE, i-FE ye-acetate yayiyi-21.2%.Iindlela ezimbini zokusabela ezinokwenzeka zacetywa kule meko: Enye isekelwe kwi-CO dimerization, kwaye enye iphezu kokufaka i-CO, igxininisa indima ebalulekileyo yokwenziwa kwe-CO ephakathi kwiindawo ezisebenzayo ze-Ag.Ukuqwalaselwa okufanayo kuchazwe kwi-Cu-Zn catalysts (umzobo 6, A kunye no-B) wemveliso ye-ethanol (38).Ngokulungelelanisa umxholo we-Zn kwi-Zn-Cu i-catalysts edibeneyo, umlinganiselo we-ethanol ngokumelene ne-C2H4 FE unokulawulwa kakuhle kwi-0.48 ukuya kwi-6, ebonisa ukubaluleka kweendawo ze-CO-evolving for C2 + oxygenate formation.Ukwenziwa kweecatalysts ezidityanisiweyo kunokubangela uxinzelelo kwimathiriyeli yematrix, esenokunganqweneleki ngamanye amaxesha.Ke ngoko, indlela ethe ngqo eya kwi-bimetallic catalysts inokufaneleka ngakumbi kwiimveliso ezithile ekujoliswe kuzo.UJaramillo kunye nabasebenzi abasebenzisana nabo (i-96) bakha inkqubo ye-bimetallic ye-Au-Cu eyenziwe lula, ehlanganiswe ngokuthe ngqo kwi-NP yegolide kwi-polycrystalline Cu foil, ukuphanda i-tandem catalysis effect.I-bimetallic i-Au-Cu ibonise ukukhethwa kwe-synergistic kunye nomsebenzi obhekiselele kwi-C2+ alcohols, ukugqithisa ubhedu olusulungekileyo kunye negolide, kunye ne-Au-Cu ialloy.Xa kuthelekiswa ne-Cu foil, inkqubo ye-Au-Cu ye-bimetallic ibonise ukunyuka kwe-CO yoxinaniso lwendawo ngenxa yobukho be-Au NPs (Umfanekiso we-6C) owawusebenza kwi-CO sizukulwana.Kuba igolide ingasebenzi kunciphiso lweCO, iqondo eliphuculweyo le-C2+ lemveliso yotywala kwi-Au-Cu bimetallic catalysts ibalelwe kwindlela ye-tandem catalysis.Ngokukodwa, i-NP yegolide inokuvelisa i-CO yoxinaniso lwendawo ephezulu kufuphi ne-Cu surface.Okulandelayo, iimolekyuli ezininzi ze-CO zendawo zingancitshiswa ngakumbi kwi-C2 + alcohols yiCu.

(A ukuya ku-C) Iziphumo ze-alloy.(A) Ubuninzi be-FE ye-ethanol kunye ne-C2H4 kunye ne-FE ratio ye-ethanol kunye ne-ethylene kwii-alloys ezahlukeneyo ze-Cu-Zn.(B) Uxinaniso lwangoku lwe-ethanol kwii-alloys ezahlukeneyo ze-Cu-Zn.(A) kunye (B) ziveliswa kwakhona ngemvume evela kwi-American Chemical Society (38).(C) Ukunciphisa i-CO2 kunye namazinga e-CO evolution kwigolide, ubhedu, kunye ne-Au-Cu bimetallic system.Iveliswe kwakhona ngemvume evela kwiQela loPapasho lweNdalo (96).(D ukuya ku-L) I-Morphology okanye iziphumo zesakhiwo.(D) Umzobo weskimu wendlela yokukhwela ibhayisekile ye-ion yensimbi.(E kunye noF) Imifanekiso ye-SEM ye-100-cycle Cu ngaphambi (E) nasemva (F) ukuncitshiswa kwangaphambili phantsi kweemeko ze-ECR.(G) I-TEM kunye ne-elektroni yendawo ekhethiweyo ye-diffraction iphakamise ukuba i-Cu (100) ibonakaliswe kunye (H) amandla amahhala kwi-*OCCO kunye nokwakheka kwe-OCCHO kwi-Cu (100), i-Cu (111), kunye ne-Cu (211) facets.(D) ukuya ku (G) ziyaveliswa kwakhona ngemvume evela kwiQela loPapasho lweNdalo (42).(I) Umlinganiselo we-oksijeni kunye ne-hydrocarbons njengomsebenzi onokwenzeka kwi-Cu (111), i-Cu (751), kunye ne-Cu (100).(J) Amanani olungelelaniso ka-Cu(111), Cu(100), kunye noCu(751).(I) kunye no-(J) zenziwe kwakhona ngemvume evela kwi-National Academy of Sciences (97).(K) ISkimu senkqubo yenguqu ukusuka kwi-Cu NPs ukuya kwi-cubic-like copper.Iveliswe kwakhona ngemvume evela kwiNational Academy of Sciences (98).(L) Imifanekiso ye-SEM yobhedu lwe-nanodendritic ngaphambi nangemva kwe-ECR.Iveliswe kwakhona ngemvume evela kwi-American Chemical Society (99).

Ukuvezwa okukhethiweyo kweempawu zekristale kwii-electrocatalysts kubonakaliswe njengendlela esebenzayo nethe ngqo yokuphumeza i-FE eyongeziweyo kwiimveliso ezithile ze-ECR kunye nendlela ebalulekileyo yokuqonda okusisiseko.Ukudityaniswa okulula kodwa okunokwehla kwee-catalysts zekristale enye kulucelomngeni.Iphefumlelwe yinkqubo ye-galvanostatic charging-discharging (GCD) yeebhetri, iqela lethu liphuhlise indlela ye-ion ion cycling yensimbi (Umfanekiso we-6D) ngokukhetha ukuveza i-crystal facet ye-Cu catalyst (42).Emva kwemijikelezo ye-GCD eyi-100, i-Cu nanocube i-dense i-array ye-Cu nanocube yenziwe kwi-Cu foil kunye neenkalo eziveziweyo (i-100) (umzobo 6, u-E ukuya ku-G).I-catalyst ye-100-cycle catalyst ibonise i-C2+ yotywala i-FE engaphezulu kwe-30% kunye ne-C2 + ehambelanayo yoxinaniso lotywala olungaphezulu kwe-20 mA cm−2.Nangona kunjalo, i-10-cycle Cu kunye nomlinganiselo ophantsi we-facet (100) inikezela kuphela i-C2 + alcohol FE ye ~ 10%.Ukulinganisa kwe-DFT kuqinisekisile ukuba i-Cu (100) kunye ne-steped (211) facets yayithandeka ngakumbi kwi-C─C yokudibanisa phezu kwe-Cu (111), njengoko kubonisiwe kwi-Fig. 6H.Imodeli ye-catalyst, ifilimu ye-epitaxial Cu eneenkalo ezahlukeneyo eziveziweyo, isetyenziselwe ukumisela i-motifs esebenzayo-site ngokubhekiselele kwimveliso ye-C2 + ye-oxygen (Umfanekiso 6I) (97).Kuba kunqabile ngokwezibalo ukuba i-CO* dimer ikufuphi ne-athomu ye-H* kumphezulu onabamelwane abambalwa, iziza ze-Cu ezilungelelanisiweyo eziphantsi zinokucinezela ukwenziwa kwee-hydrocarbons kwaye zikhokelele ekuphuculweni kwe-C2+ oxygenate FE kuba kunzima kakhulu ukwenza i-hydrogenate. I-C─C idityaniswe ne-ECR ephakathi kumphezulu wayo (97).Kwisifundo sefilimu ye-epitaxial Cu, ababhali baqinisekisa ukuba i-ECR kwi-Cu (751) facet ibonise ukuphuculwa kwe-oxygen / hydrocarbon ratio.Olu lwando lunokubalelwa kumphezulu we-Cu athom yejometri yeenkalo ezahlukeneyo ze-Cu kunye nenani eliphantsi elihambelanayo elisezantsi elilungelelanisiweyo (umzobo 6J), apho i-Cu atom ilungelelaniswa, ngokulandelelanayo, kunye nesibini, isine, kunye nabamelwane abasondeleyo abathandathu kwiCu(751), Cu(100), kunye Cu(111) facets.I-in situ morphology reconstruction iye yasetyenziselwa ukuphucula i-C2 + oxygenate FE.I-Cube esebenzayo efana ne-Cu catalyst yaphuhliswa nguYang kunye nabasebenzi abasebenzisana nabo (98), ebonisa ukuphuculwa kokusebenza kokudibanisa kwe-C─C.Ngokweenkcukacha, i-monodisperse Cu NPs (i-6.7 nm) enokulayishwa okuhlukeneyo yafakwa kwinkxaso yephepha lekhabhoni njenge-catalyst ye-ECR.Ngokucacileyo, ukunyuka kwe-FE ye-C2 + i-oksijeni yabonwa ngokunyuka kwe-Cu NP yokulayisha.Kwaboniswa ukuba i-Cu NPs epakishwe ngokuxineneyo phantsi kweemeko zokulayisha eziphezulu zenziwa kwi-situ morphological transformation ngexesha le-ECR, apho i-cube-like morphologies yagqitywa ekugqibeleni (Fig. 6K).Esi sakhiwo esitsha safunyanwa sisebenza ngakumbi nge-electrocatalytically.Uhlalutyo lwe-Tafel lucebise ukuba i-CO dimerization yayiyinyathelo lokumisela izinga lokwenziwa kwemveliso ye-C2, ngelixa i-n-propanol ibonisa indlela ecacileyo kule nkqubo ye-catalytic.Ubhedu lwe-Nanodendritic ngomnye umzekelo obonisa ukubaluleka kokulawulwa kwe-morphology kwi-C2 + ukuveliswa kwe-oxygen (99).Ngokufutshane, i-FE iyonke ye-nanodendrite yethusi echazwe kakuhle (Fig. 6L) ye-C2 + yotywala yayimalunga ne-25% kwi- -1.0 V ngokubhekiselele kwi-RHE.I-n-propanol FE echukumisayo ye-13% inokufezekiswa kwi-−0.9 V. Ukuqwalasela umsebenzi ophezulu we-Cu atom, ii-catalysts ezisekelwe kwi-copper zihlala zihlupheka ngenxa yokuthotywa kwesakhiwo ngexesha le-ECR, ngakumbi kumandla aphezulu, okukhokelela ekuhluphekeni. uzinzo.Nangona kunjalo, ubhedu olunjalo lwe-nanodendritic lubonise ukuzinza okulungileyo kwimveliso yotywala, ebonisa i-FE yotywala ye-~24% ngaphezu kweeyure ze-6.

Iziphene ze-electrocatalysts, ezifana nezithuba ze-athomu kunye ne-dopants, zibonisa ukuba kunokwenzeka ukubhengeza i-ECR intermediates engavumelekanga kwaye, ngoko ke, ngokukhetha ukunyusa indlela ehambelanayo ye-oxygen (29, 43, 100).Ukuthatha * i-C2H3O njengomzekelo, eyona nto inokuba yi-penultimate intermediate ye-ethylene kunye nemveliso ye-ethanol, i-Sargent kunye nabasebenzi abasebenzisana nabo (43) bafunde indima yeziphene kwi-core-shell Cu electrocatalyst ngokweenkcukacha.Babonisa ngokwethiyori ukuba izithintelo zamandla okusabela kwi-ethylene kunye nokwakheka kwe-ethanol zazifana nenqanaba lokuqala lokudibanisa C─C (0.5-V overpotential) (Fig. 7A).Phantsi kwesimo esinjalo, ukuqaliswa kwesithuba sobhedu kuya kwandisa kancinane umqobo wamandla ekubunjweni kwe-ethylene, kodwa ayizange ibonise impembelelo kwisizukulwana se-ethanol (Fig. 7B).Nangona kunjalo, njengoko kubonisiwe kumfanekiso we-7C, ii-catalyst zobhedu ezinesithuba kunye ne-subsurface sulfur dopant zinokunyusa kakhulu umqobo wamandla wendlela ye-ethylene, iyenza ingathandekiyo kwi-thermodynamically.Nangona kunjalo, ukuguqulwa okunjalo kubonise umphumo ongathandekiyo kwindlela ye-ethanol.Lo mcimbi waqinisekiswa ngakumbi ngomfuniselo.I-core-shell eyakhiwe i-Cu2S-Cu enezithuba ezininzi zomhlaba (Cu2S-Cu-V; Fig. 7D) yenziwe.Umlinganiselo wotywala kwi-ethylene unyuke ukusuka ku-0.18 kwi-Cu NPs ukuya kwi-0.34 kwi-Cu2S-Cu ye-vacancy-free kwaye emva koko ukuya kwi-1.21 kwi-Cu2S-Cu-V, nangona i-FE iyonke yeemveliso ze-C2 + kuzo zonke ii-catalysts zahlala zifana (Fig. 7E) .Olu qwalaselo lubonise ukuba ukunyuswa kokukhethwa kotywala kwakunxulumene nokunyanzeliswa kwemveliso ye-ethylene, ehambelana nesiphumo se-DFT.Ukongeza, ubunjineli besiphene budlala indima ebaluleke ngakumbi kwi-catalyst yekhabhoni engenazintsimbi kuba izinto ezicocekileyo zekhabhoni zingasebenzi kwi-ECR.I-Dopants efana ne-nitrogen kunye ne-boron isetyenziselwe ukuguqula isakhiwo se-elektroniki se-carbon-based catalyst (31, 43, 100).Ngokomzekelo, ifilimu ye-nitrogen-doped nanodiamond (NDD) kwi-silicon substrate yachithwa nguQuan et al.(29) kwimveliso ye-acetate ekhethiweyo evela kwi-ECR (Umfanekiso 7F).I-acetate iqala amandla yayiphantsi njenge--0.36 V ngokuchasene ne-RHE isebenzisa i-NDD catalyst, kwaye i-FE ye-acetate yayingaphezulu kwe-75% kwinqanaba elinokubakho ukusuka -0.8 ukuya -1.0 V ngokuchasene ne-RHE.Ukuqonda imvelaphi yophuculo olumangalisayo olunjalo, i-NDD / i-electrodes enee-nitrogen ezahlukeneyo okanye iintlobo ze-nitrogen zalungiswa kwaye zaphandwa (Umfanekiso we-7G).Ababhali baphetha ngokuthi ukusebenza okuphezulu kwe-NDD / Si i-catalyst ye-ECR inokuthi ifakwe kwi-overpotential ephezulu ye-hydrogen evolution kunye ne-N doping, apho iintlobo ze-N-sp3C zazisebenza kakhulu kwimveliso ye-acetate.Idatha ye-Electrokinetic kunye ne-situ infrared spectrum ibonise ukuba indlela engundoqo yokwenziwa kwe-acetate ingaba yi-CO2 → *CO2− → *(COO)2 → CH3COO−.Ngaphandle kwenitrogen, iboron yenye iheteroatom ephononongwe kakuhle ukulawula ubume be-elektroniki benanodiamond.Nangona kunjalo, i-boron-doped nanodiamond (BDD) ikhetha ukunciphisa i-CO2 kwi-formaldehyde okanye i-formal (101).Ngaphaya koko, i-Quan kunye nabasebenzisana nabo (102) babonise ukuba i-boron kunye ne-nitrogen co-doped nanodiamond (BND) ibonise i-synergistic effect kwi-ECR, enokoyisa umda we-BDD kwaye emva koko ivelise i-ethanol ngokukhethayo.I-BND1, i-BND2, kunye ne-BND3 i-catalysts enemixholo ye-nitrogen eyahlukeneyo kunye namanqanaba afana ne-boron doping alungiselelwe.Njengoko kuboniswe kwi-Fig. 7H, ukhetho oluphezulu lwe-ethanol ukuya kwi-93% lunokufezekiswa kwi-BND3 catalyst kwi -1.0 V ngokubhekiselele kwi-RHE, eneyona doping ephezulu ye-nitrogen.Ubalo lwethiyori lubonise ukuba inkqubo yokudityaniswa kwe-C─C kwi-BND yayithandeka kwi-thermodynamically, apho i-athomu ye-boron yakhuthaza ukubanjwa kwe-CO2 kunye ne-nitrogen dopant iququzelele i-hydrogenation ephakathi ukuya kwi-ethanol.Nangona i-heteroatom-doped nanodiamond yayikwazi ukuguqula i-CO2 ibe yi-oksijeni ye-multicarbon ene-selectivity ephezulu, umsebenzi wayo we-ECR ulinganiselwe kakhulu ngenxa yenkqubo yokudlulisa intlawulo ecothayo (uxinzelelo lwangoku lungaphantsi kwe-2 mA cm−2).Imathiriyeli esekwe kwigraphene inokuba sisisombululo esinokubakho ukoyisa iziphene zedayimani esekelwe kwi-catalysts.Ngokwethiyori, iindawo ezisekupheleni kwe-pyridinic N kumqolo wegraphene zithathwe njengeziza ezisebenzayo zokudityaniswa kwe-C─C (103).Oku kungenxa yokuba ubukho be-pyridinic N kwiindawo ezinqamlekileyo kunokuguqula i-CO2 ibe yi-CO, enokuthi idibaniswe ngakumbi kwi-molecule ye-C2 + (umzobo 7I).Umzekelo, i-*C2O2 ephakathi inokuzinziswa kwi-nitrogen-doped carbon apho iiathom ezimbini ze-C zidityaniswe ne-pyridinic N kunye ne-athomu ye-C ekufutshane, ngokulandelelana (103).Ukuqikelelwa kwethiyori emva koko kwaqinisekiswa kusetyenziswa i-nitrogen-doped graphene quantum dot (NGQD) catalysts (31).Emva kwe-pulverization ye-nitrogen-doped graphene sheets (1 ukuya kwi-3 μm) (Fig. 7J), i-1- ukuya kwi-3-nm NGQDs yafunyanwa apho ubuninzi be-pyridinic N kwiindawo ezisemaphethelweni zanda ngemiyalelo emithathu yobukhulu.Kwi- -0.78 V ngokubhekiselele kwi-RHE, i-FE ephezulu ye-C2 + i-oxygenates inokufikelela kwi-26%.Ukongeza, njengoko kubonisiwe kumfanekiso we-7K, uxinano lwangoku lwe-C2 + i-oksijeni isondele kwi-40 mA cm-2 kwi- -0.86 V ngokuchasene ne-RHE, ephezulu kakhulu kune-nanodiamond eguquliweyo.Xa kuthelekiswa, i-N-free graphene quantum dots kunye ne-N-doped graphene oxide, ebonisa isiza esisezantsi kakhulu se-pyridinic N, ivelise i-H2, i-CO, kunye nefomati.

(A ukuya kuC) Gibbs amandla asimahla ukusuka *C2H3O ukuya kwi-ethylene kunye ne-ethanol yobhedu, ubhedu olunesithuba, kunye nobhedu olunesithuba sobhedu kunye nesulfure engaphantsi komhlaba.(D) Umzobo weskimu weCu2S-Cu-V catalyst.(E) I-FE ye-C2 + i-alcohol kunye ne-ethylene, kunye ne-FE ratio ye-alcohols kwi-alkenes.(A) ukuya ku (E) ziyaveliswa kwakhona ngemvume evela kwiQela loPapasho lweNdalo (43).(F) umfanekiso we-SEM we-NDD.(G) Amazinga emveliso ye-acetate kunye nefomati kwi-NDD enemixholo yenitrogen eyahlukeneyo.kwi%, atom%.(F) kunye no (G) ziveliswa kwakhona ngemvume evela kwi-American Chemical Society (29).(H) IiFEs ze-NDD, BDD, kunye nee-BND e-−1.0 V. Iveliswe kwakhona ngemvume evela ku-John Wiley kunye noNyana (102).(I) Umzobo weskim weendawo ezisebenzayo zokudibanisa i-C─C kwii-NGQD.(I) iveliswa kwakhona ngemvume evela kwi-American Chemical Society (103).(J) Umfanekiso we-TEM wee-NGQDs.Imivalo yokulinganisa, i-1 nm.(K) Uxinaniso lwangoku lwenxalenye yeemveliso ezahlukeneyo zisebenzisa ii-NGQDs.(J) kunye no-(K) zenziwe kwakhona ngemvume evela kwiQela loPapasho lweNdalo (31).

Ngaphaya kwee-electrocatalysts, i-electrode kunye noyilo lwe-catalytic reactor architecture lubonisa enye indlela esebenzayo yokunyusa ukusebenza kwe-ECR, ngakumbi izinga lemveliso kunye nokusebenza kakuhle kwamandla.Uphuculo olubalulekileyo lwenziwe kuyilo kunye nokwenziwa kweendlela ezintsha zokunciphisa i-electroreduction ukuze kuphunyezwe imveliso yeC2+ esebenza kakhulu.Kweli candelo, siza kuxubusha i-ECR electrode / i-reactor design ngokubanzi.

Iiseli zohlobo lwe-H zisetyenziswa kakhulu kuvavanyo lwesikali selebhu, kuthathelwa ingqalelo ukudityaniswa kwazo ngokulula, ukusebenza ngokulula, kunye neendleko eziphantsi.Iiseli zixhotyiswe nge-cathode ezimeleyo kunye namagumbi e-anode adibaniswe yi-ion-exchange membrane (104, 105).Ukungalungi okuphambili kolu hlobo lweseli ye-H yi-solubility ephantsi ye-CO2 kwi-electrolyte yamanzi, eyi-0.034 M kuphela phantsi kweemeko ze-ambient, ekhokelela ekunciphiseni kwe-CO2 yokunciphisa uxinano lwangoku lwe-j <100 mA cm-2 (64).Ngaphezu koko, ezinye izithintelo zangaphakathi, kubandakanywa indawo eqingqiweyo ye-electrode kunye nomgama omkhulu we-interelectrode, ayiphumelelanga ukuhlangabezana neemfuno zophando ezikhulayo (105, 106).Ukuveliswa kwemveliso ye-C2 +, iiseli zohlobo lwe-H zihlala zibonisa ukukhetha okuphantsi phantsi kwee-overpotentials eziphezulu, umzekelo, i-32% ye-ethylene kwi--0.98 V ngokubhekiselele kwi-RHE (107), i-13.1% ye-n-propanol kwi--0.9 V ngokubhekiselele kwi-RHE (99), kunye I-20.4% ye-ethanol ku--0.46 V ngokuchasene ne-RHE (108), ngenxa yokhuphiswano olunzulu lwe-hydrogen evolution.

Ukujongana nale miba ingentla, i-flow reactor yaphakanyiswa (15, 109).Kwiiseli ezihambayo, umlambo we-CO2 wegesi unokusetyenziswa ngokuthe ngqo njenge-feedstock kwi-cathode, ngaloo ndlela ikhokelela ekuphuculeni kakhulu ukusasazwa kobuninzi kunye nezinga lokuvelisa (104, 110).Umzobo we-8A ubonisa i-architecture eqhelekileyo ye-flow cell, apho i-polymer electrolyte membrane (PEM) isebenza njenge-electrode separator ehlanganiswe phakathi kweendlela ezimbini zokuhamba.I-catalyst immobilized kwi-gas diffusion electrode (GDE) ukuze isebenze njenge-electrode ye-cathode, apho i-CO2 yegesi yondliwe ngokuthe ngqo.I-catholyte, efana ne-0.5 M KHCO3, ihamba ngokuqhubekayo ngaphakathi kwinqanaba elincinci phakathi kwe-catalyst electrode kunye ne-PEM.Ukongeza, icala le-anode lijikeleziswa nge-electrolyte enamanzi ye-oxygen evolution reaction (43, 110).Xa kuthelekiswa nohlobo lweeseli ze-H, ezi seli ze-membrane-based flow flow zibonisa ukusebenza okuphezulu kwe-ECR.Ngokomzekelo, i-Sargent kunye nabasebenzi abasebenzisana nabo (43) bavavanya ukusebenza kwe-ECR ye-Cu2S-Cu-V catalyst kuzo zombini i-H-type cell kunye ne-flow cell cell, njengoko kuboniswe kwi-Fig. 8 (B ukuya ku-E).Ukusebenzisa iiseli zohlobo lwe-H, i-FE ephezulu yeemveliso ze-C2 + yayiyi-41% kunye ne-total density yangoku ye-~30 mA cm-2 phantsi kwe--0.95 V ngokuchasene ne-RHE.Nangona kunjalo, i-FE yeemveliso ze-C2+ inyuke yaya kutsho kuma-53% ngoxinano lulonke lwangoku ngokulula oludlula i-400 mA cm−2 phantsi -0.92 V xa kuthelekiswa ne-RHE kwinkqubo yokuhamba.Olo phuculo lubalulekileyo lokwenziwa komsebenzi kusetyenziswa i-reactor yokuqukuqela inokunxulunyaniswa ne-CO2 eyandisiweyo yokusasazwa kunye nokucinezelwa kweempendulo ezisecaleni, ikakhulu ezisuka kwi-gas-electrolyte-catalyst triple-interface architecture.

(A) Umzobo we-electrolyzer ehamba kunye ne-zoomed-in schematic ye-electrolyte interface ye-electrolyte.(A) iveliswa kwakhona ngemvume evela kuJohn Wiley kunye noonyana (30).(B ukuya ku-E) Ukuthelekiswa kokusebenza kwe-ECR usebenzisa i-H-type cell kunye ne-flow cell.(B) ukuya ku (E) ziyaveliswa kwakhona ngemvume evela kwiNature Publishing Group (43).(F ukuya ku-H) Ii-electrolyte ezahlukeneyo ezisetyenzisiweyo kwiiseli ezihambayo ngokubhekiselele ekusebenzeni kwe-ECR.(F) ukuya (H) ziyaveliswa ngemvume evela kuJohn Wiley kunye noonyana (30).(I ukuya ku-K) Ulwakhiwo kunye nokusebenza kozinzo lwe-electrode ye-polymer-based gas diffusion electrode.(I) ukuya ku (K) ziyaveliswa kwakhona ngemvume evela kwi-AAAS (33).

Iseli ye-gap engu-zero yenye iklasi evelayo ye-electrolyzers, ethi iphinde isuse imijelo yokuhamba kwiiseli zokuhamba kwaye icinezele i-electrode ezimbini kunye ne-ion-exchange membrane phakathi.Olu lungelelwaniso lunokunciphisa kakhulu ukuhanjiswa kobuninzi kunye nokuchasana nokugqithiswa kwe-electron kwaye ngaloo ndlela kuphuculwe ukusebenza kakuhle kwamandla, okwenza kube nokwenzeka ngakumbi kwizicelo eziphathekayo (110).I-reactants ezondliwa kwi-cathode ingaba yi-CO2-saturated catholyte okanye umjelo we-CO2 ofumileyo.Umphunga wamanzi okanye i-electrolyte enamanzi ngokugunyazisiweyo yondliwe kwi-anode yokukhutshwa kweproton ukubuyisela intlawulo yeentlobo zokunciphisa i-CO2 (111).UGutiérrez-Guerra et al.(109) ivavanye ukusebenza kweCu-AC hybrid catalyst kwi-zero gap cell kwaye yabika ukuba i-acetaldehyde iyona mveliso ephambili kunye nokukhetha okuphezulu kwe-60%.Njengenye inzuzo yesi sixhobo, kulula kakhulu ukucinezela ukuhamba kwe-reactant kunye nokuphucula kakhulu i-CO2 yoxinaniso lwendawo, oko kubangele ukuxinana okukhulu kwangoku kunye namazinga aphezulu okuphendula (110).Nangona kunjalo, isantya sokutshintshiselana nge-ion ekhawulezileyo kwiiseli ze-gap zero ithande ukwenza i-catholyte, itshintshe indlela yokusabela kwi-H2 endaweni yokunciphisa i-CO2 (112).Ukujongana nale ngxaki, uZhou kunye nabasebenzi abasebenzisana nabo (112, 113) bafake i-buffer layer kunye ne-electrolyte yamanzi ejikelezayo phakathi kwe-cathode kunye ne-membrane ukuze kugcinwe i-pH efanelekileyo kufuphi ne-cathode ye-CO2 yokuphendula ukunciphisa.Nangona iimveliso ezahlukeneyo ze-C2 + zifunyenwe ngesiseko seeseli ze-gap zero, ezibandakanya i-acetone, i-ethanol, kunye ne-n-propanol, ii-FE zisephantsi.Uninzi lwezifundo ezixeliweyo zihlala zijolise kwiimveliso zeC1 ezibandakanya amanani ambalwa eproton kunye nokudluliselwa kwe-electron ngexesha lokunciphisa ukusabela.Ngoko ke, ukuba nokwenzeka kweseli ye-gap ye-zero kwiimveliso ze-C2 + kusephantsi kwengxoxo (110).

Ngaphezu koko, iiseli ze-electrolytic microfluidic (MECs) luhlobo lokucwangciswa kwe-electrolyzer enomtsalane kakhulu ephuhliswe nguKenis kunye nabasebenzi abasebenzisana nabo (39, 114).Kule fowuni, i-membrane ithathelwa indawo yindawo encinci (<1 mm ubukhulu) ezaliswe ngumjelo ojikelezayo we-electrolyte ukwahlula i-anode kunye ne-cathode.Iimolekyuli ze-CO2 zinokusasazeka ngokukhawuleza kwi-electrode-electrolyte interface kufuphi ne-cathode, kwaye ezimbini ezisisigxina ze-GDE zigungxulwa yi-electrolyte ehambayo.Xa kuthelekiswa neeseli zokuhamba ezisekwe kwi-membrane, ii-MEC aziphepheli kuphela iindleko eziphezulu ze-membrane kodwa zikwanciphisa nolawulo lwamanzi, olubhekisa ngakumbi kwi-anode dry-out kunye nezandyondyo ze-cathode xa zisebenza kuxinzelelo oluphezulu lwangoku ngenxa yokutsalwa kwe-osmotic yeemolekyuli zamanzi uthutho lweproton ukusuka kwi-anode ukuya kwi-cathode ngapha kwe-membrane (115).Ngokokwazi kwethu, ngaphandle kokuncomeka okubonakalayo kunye nempumelelo, lincinci inani lezifundo ezifumene iimveliso ze-C2+ kwii-MEC zokuqala.Oku mhlawumbi kubangelwa yimpembelelo "ejikelezayo" yokuba iiprotoni ezenziwe kwi-anode zikhutshwe ngokulula ukusuka kwindawo ye-cathode okanye zihlanjwe yi-electrolyte ehambayo, kunokuba ithathe inxaxheba kwiiproton ezininzi ezifunekayo ukusabela kwe-C2 +.Uqikelelo lunokuqinisekiswa ngokulandelayo.Kwi-2016, i-Kenis kunye nabasebenzi abasebenzisana nabo (31) babika ukunciphisa ngempumelelo kwe-CO2 kwiimveliso ze-C2 + kwi-MEC eguqulweyo kunye ne-membrane, apho i-NGQD inokunciphisa i-CO2 i-molecule ukuya kwi-C2 + kunye ne-55% FE (31% ye-ethylene, i-14% i-ethanol, i-6% ye-acetate, kunye ne-4% ye-n-propanol) kwi-application potential of -0.75 V ngokuchasene ne-RHE kwi-1 M KOH isisombululo.Kubalulekile ukubonisa ukuba indawo ye-electrolyte inokuchaphazela kakhulu ukukhethwa kwemveliso ngokunjalo.Ngokomzekelo, i-Jiao kunye nabasebenzi abasebenzisana nabo (30) badibanisa i-nanoporous Cu catalyst kwaye emva koko bavavanya ukusebenza kwayo kwe-ECR ngokusebenzisa i-electrolytes eyahlukeneyo (KHCO3, KOH, K2SO4, kunye ne-KCl) kwi-MEC esekelwe kwi-membrane.Baye babonisa ukuba i-CO2 yokunciphisa i-alkaline electrolyte (KOH) ibonisa ukhetho oluphezulu lwe-C2 + kunye nokuxinana kwangoku, njengoko kuboniswe kwi-Fig. 8 (F kunye ne-G).Ku-−0.67 V xa kuthelekiswa ne-RHE kwi-electrolyte ye-1 M KOH, i-FE efunyenweyo ye-C2+ ifikelela kuma-62% ngoxinano lwangoku oluyi-653 mA cm−2, oluphakathi kwezona ngxinano ziphezulu ezikhe zaxelwa kunciphiso lwe-electrochemical CO2. malunga neemveliso zeC2+.I-Ethylene (38.6%), i-ethanol (i-16.6%), kunye ne-n-propanol (4.5%) yizona mveliso eziphambili ze-C2 + ezinomlinganiselo omncinci we-acetate.Baye babonisa ukuba kukho ulungelelwaniso oluqinileyo phakathi kobuso obubaliweyo pH kunye ne-FE kwiimveliso ze-C2 +: Ukuphakama kwendawo ye-pH, ukuxinana okuphezulu kwangoku kunye nemveliso ye-C2 + yemveliso, njengoko kuboniswe kwi-Fig. 8H.Ubalo lwethiyori lucebise ukuba i-OH− ions ekufutshane nomphezulu ingaququzelela ngamandla ukudityaniswa kwe-C─C (31).

Ukongeza kulungiselelo lwe-electrolyzer, i-electrolyte esetyenziswa kwii-electrolyzers ezahlukeneyo inokutshintsha kakhulu iimveliso ze-ECR zokugqibela.Njengoko sele sikhankanyile ngasentla, izisombululo ze-alkaline ze-KOH zihlala zisetyenziswa kwiiseli ezihambayo kunye nokusebenza okugqwesileyo kunokuba kwiiseli zohlobo lwe-H.Oku kubalelwa kwinto yokuba i-electrolyte ye-KOH inokubonelela nge-electrolyte ephezulu kakhulu, yehlise ukuxhathisa kwe-ohmic phakathi kotyatyazo lwe-electrolyte ebhityileyo kwi-catalyst kunye ne-electrolyte enkulu, kwaye inciphise ngakumbi amandla angaphezulu afunekayo okwenziwa kwe-C2+ (31).Iziphumo ze-DFT ziqinisekisa ngakumbi ukuba ubukho bee-OH− ion bunokunciphisa umqobo wamandla kwi-CO dimerization, ngaloo ndlela ikhulise ukubunjwa kwe-C2 + kunye nokucinezela ukhuphiswano kwi-C1 kunye nokwakheka kwe-H2 (30, 33).Nangona kunjalo, i-alkaline KOH ayinakusetyenziswa njenge-electrolyte kwiiseli zohlobo lwe-H.Oku kungenxa yokuba imilambo ye-CO2 iya kusabela ngokukhawuleza kunye nezisombululo ze-KOH kwaye ekugqibeleni idale isisombululo se-bicarbonate kunye ne-pH engathathi hlangothi kwiiseli ze-H (30).Kwiiseli ezihambayo, nangona kunjalo, xa i-CO2 isasazeka nge-GDE, i-molecule ze-CO2 ziya kusetyenziswa kwinqanaba lomda we-triple (CO2-catalyst-electrolyte) ukwenza iimveliso ezincitshisiweyo ngokukhawuleza.Ngaphandle koko, umthamo ombi we-electrolyte uyakwazi ukunyusa ngokukhawuleza i-pH ejikeleze i-electrode kuhlengahlengiso lwe-electrolyzer emileyo, ngelixa i-electrolyte ehambayo iya kuwuhlaziya umphezulu kwaye icuthe ukuguquguquka kwe-pH kwi-electrolyte (33, 116).

Njengoko kukhankanyiwe ngasentla ukuba i-ECR yimpendulo elawulwa lusasazo, uxinzelelo oluphezulu lokusabela lunokwandisa kakhulu ubuninzi kunye nojongano lwe-CO2 yoxinaniso.Iimpawu eziqhelekileyo zoxinzelelo oluphezulu zifana ne-autoclave yensimbi engenasici, apho i-CO2 ephezulu (ukuya kwi-60 atm) ingangeniswa kwiseli, ekhokelela ekunyuseni okuphawulekayo kwi-FE kunye nokuxinana kwangoku kweC2 + (117). , 118).I-Sakata kunye nabasebenzi abasebenzisana nabo (119) babonise ukuba ukuxinana kwangoku kungaphuculwa ukuya kwi-163 mA cm−2 phantsi kwe-30 atm kwi-Cu electrode ene-ethylene njengemveliso enkulu.Uninzi lwee-catalysts zetsimbi (umzekelo, i-Fe, i-Co, kunye ne-Ni), ngaphandle komsebenzi we-C2 + wemveliso kuxinzelelo lwe-ambient, inokunciphisa i-CO2 kwi-ethylene, i-ethane, i-propane, kunye nezinye iimveliso ze-C2 + eziphezulu kwiingcinezelo eziphakamileyo.Kuye kwaboniswa ukuba ukukhethwa kweemveliso ngokuphawulekayo kuxhomekeke kuxinzelelo lwe-CO2 ngendlela yokuguqula ukufumaneka kwe-CO2 kwindawo ye-electrode (117, 120).Iimveliso eziphambili ezincitshisiweyo zitshintshwa ukusuka kwi-H2 ukuya kwi-hydrocarbons (i-C2 + ifakiwe) kwaye ekugqibeleni i-CO / HCOOH ngokunyuka kwe-CO2 uxinzelelo.Ngokucacileyo, uxinzelelo lwe-CO2 kufuneka lubekwe esweni ngononophelo kuba uxinzelelo oluphezulu okanye oluphantsi lwe-CO2 lunokubangela umbane ogqithisileyo okanye olinganiselweyo we-CO2, othanda ukuthanda ukuveliswa kwe-CO/HCOOH okanye i-H2.Kuphela isixa esihambelanayo se-CO ephakathi kunye noxinaniso lwangoku oluveliswe kumphezulu we-electrode lunokwenza lula ukusabela kokudibanisa kwe-C─C kunye nokuphucula ukukhethwa kwemveliso yeC2 + (119).

Ukuyila i-electrode yenoveli enezakhiwo eziphambili lolunye ulwalathiso olubalulekileyo lokuphucula imveliso yeC2 + ekhethiweyo.Kwinqanaba lokuqala, ii-electrode ezisebenzayo azikho iifoyile zetsimbi ezingasebenziyo kwaye zithwaxwa bubuvila bokudluliswa kobunzima (26, 105).Ngenxa yoko, i-GDE yacetywayo yokunciphisa ukusebenza kakubi kweeseli ngokubonelela ngeeshaneli ze-hydrophobic eziququzelela ukusabalalisa kwe-CO2 kwiincinci ze-catalyst (121).I-GDE eqhelekileyo idla ngokubandakanya i-catalyst layer (CL) kunye ne-gas diffusion layer (GDL), njengoko kuboniswe kwindawo engezantsi ye-Fig. 8A (30, 33).I-gas-liquid-catalyst interface eyenziwe kwi-GDE ibalulekile ekuphuculeni ukusebenza kweeseli.I-GDL idityaniswe kunye nezinto ezixubileyo (ngokuqhelekileyo i-carbon paper) inokubonelela ngeendlela ezininzi ze-CO2 kwaye iqinisekise izinga lokusasazwa kwe-electrolyte ngokukhawuleza.Ikwasebenza njengendlela yokuthutha ephantsi yokumelana neeproton, ii-electron, kunye neemveliso zokunciphisa ukusuka kwi-CL ukuya kwi-electrolyte (121).I-drop casting, i-airbrush, kunye ne-electrodeposition yitekhnoloji eqhelekileyo yokulungiselela ii-GDEs (122).Ii-Catalysts ezihlanganiswe kunye ne-GDE ziphandwe kakhulu kwi-CO2 electroreduction kwiimveliso ze-C2 +.Ngokucacileyo, iiseli ezihambayo ezikhankanywe ngasentla ezinentsebenzo encomekayo zonke zidityaniswa nee-GDE.Kwangoko ngo-1990, i-Sammells kunye nabasebenzi abasebenzisana nabo (123) baxela ukuba i-Cu-coated GDEs ifumene i-FE ephezulu ye-53% ye-ethylene ene-high density ye-667 mA cm−2.Ukuphucula ukukhethwa kwe-ethylene kunye ne-ethanol ngumceli mngeni omkhulu osoloko uveliswa kwi-Cu-based catalysts ngenxa yeendlela zabo zokusabela ngoomatshini ezifanayo.Ngaphezu koko, kubalulekile ukubonisa ukuba imveliso ephakamileyo kunye nokukhetha kwe-ethylene xa kuthelekiswa ne-ethanol kuye kwabonwa kwi-Cu-based GDE (25, 36).I-Gewirth kunye nabasebenzisana nabo (36) babonise i-FE egqwesileyo ye-60% ye-ethylene kunye ne-FE ecinezelweyo ye-ethanol ye-25% kwi-electrodeposited Cu-Ag GDE, xa ubuninzi bangoku bubonke bufikelele kwi- ~ 300 mA cm−2 ku -0.7 V xa kuthelekiswa ne- RHE.Ngumsebenzi onqabileyo ofumene ukhetho oluphezulu kubuninzi bangoku.Oku kufunyanisiweyo kucebisa ukuba i-electrode efakwe kwi-GDE ibonelela ngendlela ethembisayo yokulungisa iindlela zokusabela, apho ukukhethwa kweemveliso ezincitshisiweyo kunokufunyanwa kuxinzelelo oluphezulu lwangoku.

Uzinzo lwe-GDEs lukwangumba obalulekileyo ekufuneka kujongwane nawo kuba umsebenzi ozinzileyo wexesha elide ubalulekile ukuze kuphunyezwe ukusetyenziswa okusebenzayo kweeseli zokuhamba.Ngaphandle kokugqwesa kwe-CO2-to-C2 + ukusebenza okuphunyeziweyo kunye ne-GDE, ukuzinza kusenzima ngenxa yobuthakathaka bokubambelela komatshini we-catalyst, i-GDL, kunye ne-binder layers (77, 124).Umphezulu wekhabhoni ye-GDL unokutshintsha ukusuka kwi-hydrophobic ukuya kwi-hydrophilic ngexesha le-electrochemical reaction ngenxa ye-oxidation reaction eyenzeke kwindawo ephezulu, ekhokelela kwizikhukula kwi-GDL kunye ne-CO2 ethintele iindlela zokusasazwa (33).Ukusombulula le ngxaki, abaphandi badibanisa i-hydrophobic scaffold ye-polytetrafluoroethylene (PTFE) kwi-GDEs.Xa kuthelekiswa ne-hydrophilic Nafion, i-hydrophobic PTFE layer inika uzinzo oluphezulu lwexesha elide (33).I-Sargent kunye nabasebenzi abasebenzisana nabo (i-33) bahlanganise i-Cu catalyst phakathi kwe-PTFE ehlukeneyo kunye ne-carbon NPs, apho i-hydrophobic PTFE layer ingakwazi ukuphazamisa i-NPs kunye ne-graphite layers, ngaloo ndlela yakha i-electrode interface ezinzileyo (Umfanekiso 8, I kunye no-J).Ngenxa yoko, i-FE yemveliso ye-ethylene yanda ukuya kwi-70% kwisisombululo se-7 M KOH kwi-inxinano yangoku ye-75 ukuya kwi-100 mA cm-2.Ubude bexesha lokuphila kwesi sixhobo sokuhamba sandiswa ukuya kwiiyure ezingaphezu kwe-150 kunye nelahleko engabalulekanga kwi-ethylene selectivity, eyi-300-ixesha elide kune-GDE yendabuko, njengoko kuboniswe kwi-Fig. 8K.Ulwakhiwo lwesandwich olunjalo lubonakaliswe ukuba luyilo olugqwesileyo lwe-GDE.Ngokomzekelo, i-Cui kunye nabasebenzi abasebenzisana nabo (i-124) baqulunqa isakhiwo se-trilayer kunye ne-electrode layer esebenzayo ekhutshwe ngeefilimu ezimbini ze-hydrophobic nanoporous polyethylene.Iingqimba zangaphandle ze-hydrophobic zingacotha i-electrolyte flux kwisisombululo sobuninzi, ekhokelela kwi-stable, i-pH yendawo ephakamileyo malunga ne-electrode esebenzayo.Ukulungiswa kwendawo ye-interlayer, enokuphucula ukuthuthwa kwe-CO2 kunye ne-adsorption, nayo ibalulekile kuyilo olunjalo (124).Kungekudala, i-carbon nanotubes nayo idibaniswe kwi-GDEs ngenxa ye-porosity ephezulu, ukuqhuba kakuhle, kunye ne-hydrophobicity, enokuthi iququzelele i-electron kunye nokuhamba ngobuninzi (77).

Nangona inkqubela phambili enomdla kwi-ECR, izicwangciso zexabiso eliphantsi, imveliso enkulu yeC2 + yokuvelisa imveliso ayifane ibekho (125).Kweli nqanaba, imingeni kunye namathuba ahambelanayo ukuqonda iindlela zokuphendula ze-ECR kunye nokuthengisa obu buchwepheshe buthembisayo.

Njengesisombululo esihle sokuvala iluphu yekhabhoni kunye nokugcina amandla ahlaziyekayo ngamaxesha athile, afana nomoya kunye nelanga, inkqubela phambili enkulu yenziwe ukuphumeza uguqulo olusebenzayo lweCO2 kumashumi eminyaka adlulileyo.Ngelixa ukuqonda kweenkqubo ezinxulumene ne-ECR kuhambe umgama omde ukususela kwiintsuku zayo zokuqala (126), ukudityaniswa kwe-C─C nge-ECR ukuya kwiimveliso ze-C2+ kusekude ukuba ilungele ukusetyenziswa.Kolu hlaziyo, sijonge ngokweenkcukacha izicwangciso zangoku ezinokukhuthaza ukukhethwa kunye nezinga lokuvelisa iimveliso ze-C2 + nge-ECR, kubandakanywa ukulungiswa kwe-fine-catalyst, iziphumo ze-electrolyte, iimeko ze-electrochemical, kunye ne-electrochemical electrode / i-reactor design.

Naphezu kwayo yonke inzame eyenziwe kwi-ECR, kusekho iingxaki ezininzi kunye ne-catalysts yangoku kunye nenkqubo ye-ECR ekufuneka iqwalaselwe ngaphambi kokuthengisa i-ECR.Okokuqala, njenge-catalyst elawulayo yokuqonda ukudibanisa okusebenzayo kwe-C─C, i-Cu inengxaki yozinzo olunzima, ngakumbi kwi-electrolyte yamanzi, kwaye ayinakuphila iiyure ezili-100 ngenxa yokuhamba kwazo okuphezulu kwe-athomu, ukuhlanganiswa kwamasuntswana, kunye nokuwohloka kwesakhiwo phantsi kweemeko ze-ECR.Ngaloo ndlela, indlela yokufezekisa ukuzinza kwexesha elide usebenzisa i-Cu-based catalyst isengumngeni ovulekileyo.Ukumilisela i-Cu-based catalyst kwinkxaso ethile ngonxibelelwano oluluqilima inokuba sisicwangciso esithembekileyo sokulondoloza ubume becatalyst/morphology kwaye ngaloo ndlela ibonelele ubomi obongezelelweyo.Ngaphezu koko, ukusebenzisa i-polymer membrane electrolyte ukutshintsha isisombululo samanzi ngexesha le-ECR mhlawumbi kunokuphucula ngakumbi ukuzinza kwe-Cu-based catalyst.Ukongezelela, ngokwembono yee-catalysts, kwi-situ/in operando characterization techniques kunye ne-theoretical modeling kufuneka kwakhona isetyenziswe ukubeka iliso nokuqonda ukubola kwentsebenzo ye-catalyst, ngoko ke, ukucinezela ukuthotywa kunye netyhefu ye-catalyst ukuya kumanqanaba aphantsi.Omnye umba obalulekileyo wee-catalysts ze-ECR ekufuneka zijongwe kukwenza iprotocol ye-synthesis isebenze kwimveliso yobuninzi.Ukuza kuthi ga ngoku, ukulungelelanisa iinkqubo zokwenziwa kusetyenziswa i-feedstocks efumaneka ngokubanzi kuyakhethwa.

Okwesibini, i-C2+ eyenziwe nge-oksijini esuka kwi-ECR idla ngokuxutywa kunye ne-solutes (umzekelo, i-KHCO3 kunye ne-KOH) kwi-electrolyte ye-H- okanye i-flow-cell reactors, leyo, nangona kunjalo, idinga ulwahlulo olongezelelweyo kunye neenkqubo zokuxilisa ukubuyisela izisombululo zamafutha olwelo olusulungekileyo. izicelo eziphathekayo.Ngexesha elifanayo, i-C2 + i-hydrocarbons eguqukileyo nayo ixutywe kunye ne-H2 kunye ne-CO2 eseleyo.Ke ngoko, inkqubo yokwahlula ebiza imali eninzi iyimfuneko kwitekhnoloji ye-ECR yangoku, ethintela ngakumbi i-ECR ekusebenziseni okusebenzayo.Ke ngoko, indlela yokuvelisa ngokuthe ngqo nangokuqhubekayo izisombululo zamafutha olwelo olusulungekileyo kunye neehydrocarbons zerhasi esulungekileyo, ngakumbi ezinogxininiso lwemveliso ephezulu, inqweneleka kakhulu ukusasazwa okusebenzayo kwe-ECR.Ke ngoko siqikelela ukubaluleka kokunyuka kokuveliswa ngokuthe ngqo kweemveliso ezicocekileyo nge-ECR kungekudala, enokuthi ithathe itekhnoloji ye-ECR isondele kakhulu kwintengiso (127).

Okwesithathu, ngelixa ukubunjwa kweebhondi ze-C─O kunye ne-C─H, ezifana ne-ethanol, i-acetic acid, kunye ne-ethylene, kwi-teknoloji ye-ECR ifundwe kakhulu, ukuhlola ezinye iintlobo zeemveliso nazo zibalulekile kwi-teknoloji ye-ECR kwaye ibonisa umdla wezoqoqosho.Ngokomzekelo, kutshanje, uHan kunye nabasebenzi abasebenzisana nabo (128) babike ukuveliswa kwe-2-bromoethnol yi-ECR.Ukwakhiwa kwe-in situ ye-C─Br bond iguqula imveliso ukusuka kwi-ethanol ukuya kwi-2-bromoethnol, eyona nto ibalulekileyo kwisakhiwo sekhemikhali kunye ne-pharmaceutical synthesis kwaye ibonisa ixabiso elongezelelweyo eliphezulu.Ngaloo ndlela, ngaphaya kweemveliso ze-C2 + ezifundwe kakuhle ngoku, sikholelwa ukuba ukujoliswa kwezinye iimveliso eziphononongwa ngokungaqhelekanga ezifana ne-oxalic acid (129) kunye nokuhlanganiswa kwee-molecule ze-C2 + eziyinkimbinkimbi ezifana ne-cyclic compounds yenye indlela ethembisayo yophando lwe-ECR oluzayo.

Okokugqibela kodwa kuncinci, i-electrode yenoveli kunye noyilo lwe-reactor olufana ne-GDE yokungangeni manzi, iiseli zokuqukuqela ulwelo, kunye neseli yePEM kufuneka yamkelwe ngokubanzi ukunyusa izinga lemveliso ye-ECR ukuya kwinqanaba lezorhwebo (>200 mA cm−2).Nangona kunjalo, umahluko omkhulu kumsebenzi we-electrocatalytic uhlala ubonwa xa i-electrocatalysts isetyenziswa kuvavanyo olupheleleyo lweeseli.Ke ngoko, izifundo ezicwangcisiweyo ngakumbi kufuneka zenziwe ukunciphisa umsantsa phakathi kwezifundo zeeseli ezinesiqingatha kunye nesicelo sesixhobo esigcweleyo ukuzisa i-ECR kuvavanyo lwesikali selebhu ukuya kusetyenziso olusebenzayo.

Isishwankathelo, ukunciphisa i-electrochemical CO2 kunika ithuba elihle lokuba sijongane nomcimbi wokusingqongileyo kwi-greenhouse gases ekhutshwa yimisebenzi yabantu.Ikwabonisa ukuba nokwenzeka kokufikelela kumafutha acocekileyo kunye neekhemikhali kusetyenziswa amandla ahlaziyekayo.Ngelixa imiceli mngeni emininzi isele kwitekhnoloji ye-ECR kwinqanaba langoku, ngakumbi kwinkqubo yokudibanisa i-C─C, kukholelwa ukuba ngokuqhubeka kophando kunye nophuhliso kuzo zombini i-catalyst optimization kunye nokugqibelela kweeseli, umbono wehlabathi lokwenyani le-CO2 electrolysis ye-fuel ecocekileyo. kwaye imichiza iya kuphunyezwa kungekudala.

Eli linqaku elivulekileyo lokufikelela lisasazwe phantsi kwemiqathango yelayisensi ye-Creative Commons Attribution-NonCommercial, evumela ukusetyenziswa, ukuhanjiswa, kunye nokuveliswa kwakhona kuyo nayiphi na indlela, okoko nje ukusetyenziswa okubangelwayo kungeyonzuzo yorhwebo kwaye ibonelele umsebenzi wokuqala ngokufanelekileyo. icatshulwe.

QAPHELA: Sicela idilesi yakho ye-imeyile kuphela ukuze umntu omcebisayo eli phepha azi ukuba ubufuna alibone, kwaye asiyoimeyile eyinkunkuma.Asithathi nayiphi na idilesi ye-imeyile.

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