Electrochemical reduction of CO_(2) to formic acid(HCOOH)is an important route for storing renewable energy and achieving carbon neutrality.Herein,we propose the continuous production of HCOOH solution from electrocat...Electrochemical reduction of CO_(2) to formic acid(HCOOH)is an important route for storing renewable energy and achieving carbon neutrality.Herein,we propose the continuous production of HCOOH solution from electrocatalytic CO_(2) reduction using highly mesoporous bismuth oxide(Bi_(2)O_(3))nanosheets as an electrocatalyst and membrane electrode assembly with solid-state electrolyte as an electrolyzer.Precisely,0.1 M of HCOOH solution could be produced continuously at a current density of -56 mA cm^(-2) for at least 43 h.The underlying mechanism for the high performance of the electrocatalytic system was investigated by experimental studies and theoretical calculations.展开更多
To improve the electrocatalytic conversion of carbon dioxide(CO_(2))into C_(2+)products(such as ethylene(C_(2)H_(4))and ethanol(CH_(3)CH_(2)OH),etc.)is of great importance,but remains challenging.Herein,we proposed a ...To improve the electrocatalytic conversion of carbon dioxide(CO_(2))into C_(2+)products(such as ethylene(C_(2)H_(4))and ethanol(CH_(3)CH_(2)OH),etc.)is of great importance,but remains challenging.Herein,we proposed a strategy that directs the C–C coupling pathway through enriching and confining the carbon monoxide(CO)intermediate to internal pores of Cu nanocubes,for electrocatalytic reduction of CO_(2)into C_(2+)chemicals.In H-type cell,the Faraday efficiency(FE)for ethylene and ethanol reaches 70.3%at−1.28 V versus the reversible hydrogen electrode(vs.RHE),with a current density of 47.9 mA·cm^(−2).In flow cell,the total current density is up to 340.3 mA·cm^(−2)at^(−2).38 V(vs.RHE)and the FE for C_(2+)products is 67.4%.Experimental and theoretical studies reveal that both the CO intermediate adsorption and C–C coupling reaction on such an internal porous catalyst are facilitated,thus improving CO_(2)-to-C_(2+)conversion efficiency.展开更多
To enhance the activity and selectivity of electrocatalytic CO_(2)reduction to formate is of great importance from both environmental and economical viewpoints.Herein,the BiO_(2-x)nanosheets with surface electron loca...To enhance the activity and selectivity of electrocatalytic CO_(2)reduction to formate is of great importance from both environmental and economical viewpoints.Herein,the BiO_(2-x)nanosheets with surface electron localizations were constructed and utilized for the efficient CO_(2)-to-formate conversion.The formate Faraday efficiency reaches 99.1%with current density of 12 mA cm^(−2)at^(−1).1 V versus the reversible hydrogen electrode(RHE)in an H-type cell while those in the flow cell are 91.3%and 319 mA cm^(−2)at^(−1).0 V versus RHE,respectively.Theoretical calculations indicate that the electron localization presenting in the BiO_(2-x)nanosheet favors OCHO*intermediate stabilization and suppresses H*intermediate adsorption,thus improving the CO_(2)-to-formate efficiency.The BiO_(2-x)electrocatalyst is nondopant,easily prepared,low-cost,highly active and selective for CO_(2)RR to formate,which has demonstrated potential for application in the Zn-CO_(2)battery.The maximum power density can reach 2.33 mW cm^(−2),and the charge/discharge cycling stability is>100 h(300 cycles)at 4.5 mA cm^(−2).展开更多
基金supported by the National Natural Science Foundation of China(grant nos.22033009,22121002,and 22238011).
文摘Electrochemical reduction of CO_(2) to formic acid(HCOOH)is an important route for storing renewable energy and achieving carbon neutrality.Herein,we propose the continuous production of HCOOH solution from electrocatalytic CO_(2) reduction using highly mesoporous bismuth oxide(Bi_(2)O_(3))nanosheets as an electrocatalyst and membrane electrode assembly with solid-state electrolyte as an electrolyzer.Precisely,0.1 M of HCOOH solution could be produced continuously at a current density of -56 mA cm^(-2) for at least 43 h.The underlying mechanism for the high performance of the electrocatalytic system was investigated by experimental studies and theoretical calculations.
基金supported by the National Natural Science Foundation of China(Nos.22033009 and 22121002).
文摘To improve the electrocatalytic conversion of carbon dioxide(CO_(2))into C_(2+)products(such as ethylene(C_(2)H_(4))and ethanol(CH_(3)CH_(2)OH),etc.)is of great importance,but remains challenging.Herein,we proposed a strategy that directs the C–C coupling pathway through enriching and confining the carbon monoxide(CO)intermediate to internal pores of Cu nanocubes,for electrocatalytic reduction of CO_(2)into C_(2+)chemicals.In H-type cell,the Faraday efficiency(FE)for ethylene and ethanol reaches 70.3%at−1.28 V versus the reversible hydrogen electrode(vs.RHE),with a current density of 47.9 mA·cm^(−2).In flow cell,the total current density is up to 340.3 mA·cm^(−2)at^(−2).38 V(vs.RHE)and the FE for C_(2+)products is 67.4%.Experimental and theoretical studies reveal that both the CO intermediate adsorption and C–C coupling reaction on such an internal porous catalyst are facilitated,thus improving CO_(2)-to-C_(2+)conversion efficiency.
基金This work was financially supported by the National Natural Science Foundation of China(grant nos.22033009 and 22121002)the Ministry of Science and Technology of China(grant no.2017YFA0403003).
文摘To enhance the activity and selectivity of electrocatalytic CO_(2)reduction to formate is of great importance from both environmental and economical viewpoints.Herein,the BiO_(2-x)nanosheets with surface electron localizations were constructed and utilized for the efficient CO_(2)-to-formate conversion.The formate Faraday efficiency reaches 99.1%with current density of 12 mA cm^(−2)at^(−1).1 V versus the reversible hydrogen electrode(RHE)in an H-type cell while those in the flow cell are 91.3%and 319 mA cm^(−2)at^(−1).0 V versus RHE,respectively.Theoretical calculations indicate that the electron localization presenting in the BiO_(2-x)nanosheet favors OCHO*intermediate stabilization and suppresses H*intermediate adsorption,thus improving the CO_(2)-to-formate efficiency.The BiO_(2-x)electrocatalyst is nondopant,easily prepared,low-cost,highly active and selective for CO_(2)RR to formate,which has demonstrated potential for application in the Zn-CO_(2)battery.The maximum power density can reach 2.33 mW cm^(−2),and the charge/discharge cycling stability is>100 h(300 cycles)at 4.5 mA cm^(−2).
