Selective and High Current CO2 Electro-Reduction to Multicarbon Products in Near-Neutral KCl Electrolytes

Zhang, Xiao1,2; Li, Jiachen1,2; Li, Yuan-Yao1,2,3; Jung, Yunha1,2; Kuang, Yun1,2; Zhu, Guanzhou1,2; Liang, Yongye4; Dai, Hongjie1,2

2021-03-03

10.1021/jacs.0c13427

Journal of the American Chemical Society   影响因子和分区

0002-7863

1520-5126

Reducing CO2 to value-added multicarbon (C2+) fuels and chemicals using renewable energy is a viable way to circumvent CO2 buildup in the atmosphere and facilitate closing the carbon cycle. To date it remains a challenge to achieve high product selectivity and long-term stability of electrocatalytic carbon dioxide reduction reaction (CO2RR) especially at practically relevant high current levels >100 mA cm(-2). Here, we report a simple electrodeposited Cu electrocatalyst on a hydrophobic porous gas-diffusion layer (GDL) electrode affording stable and selective CO2RR to C2+ products in nearneutral KCI electrolytes. By directing the CO, stream to fully submerged hydrophobic GDLs in a H-cell, high C2+ partial current densities near 100 mA cm(-2) were achieved. In a flow-cell setup, the Cu/GDL cathode in 2 M KCl afforded stable CO2RR superior to that in widely used KOH electrolytes. We found that Cu etching/corrosion associated with trace oxygen played a role in the catalyst instability in alkaline media under cathodic CO2 RR conditions, a problem largely suppressed in near-neutral electrolyte. A two-electrode CO2 electrolyzer was constructed with a Cu/GDL cathode in KCI catholyte and an anode comprised of nickel-iron hydroxide on nickel foam (NiFe/NF) in a KOH anolyte separated by Nafion membrane. By periodically adding HCl to the KCl catholyte to compensate the increasing pH and remove accumulated (bi)carbonates, we observed little decay over similar to 30 h in flow-cell CO2RR activity and selectivity at 150 mA cm(-2) with a high Faradaic efficiency (FE) of similar to 75% and energy efficiency of 40% for C2+ products.

SCI ; EI

英语

NI论文 ; ESI高被引

其他

Shenzhen fundamental research funding[JCYJ20160608140827794] ; Guangdong Provincial Key Laboratory[2018B030322001]

Chemistry

Chemistry, Multidisciplinary

WOS:000626325000027

AMER CHEMICAL SOC

20211010025064

Alkalinity ; Carbon dioxide ; Cathodes ; Copper ; Diffusion in gases ; Electrocatalysts ; Electrolytes ; Energy efficiency ; Etching ; Hydrophobicity ; Iron compounds ; Nickel compounds ; Pollution control ; Potassium hydroxide

Energy Conservation:525.2 ; Copper:544.1 ; Chemistry, General:801.1 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Inorganic Compounds:804.2 ; Physical Properties of Gases, Liquids and Solids:931.2

Web of Science

1.Stanford Univ, Dept Chem, Stanford, CA 94305 USA
2.Stanford Univ, BioX, Stanford, CA 94305 USA
3.Natl Chung Cheng Univ, Dept Chem Engn, Chiayi 62102, Taiwan
4.Southern Univ Sci & Technol, Dept Mat Sci & Engn, Shenzhen 518055, Peoples R China

Zhang, Xiao,Li, Jiachen,Li, Yuan-Yao,et al. Selective and High Current CO2 Electro-Reduction to Multicarbon Products in Near-Neutral KCl Electrolytes[J]. Journal of the American Chemical Society,2021,143(8):3245-3255.

Zhang, Xiao.,Li, Jiachen.,Li, Yuan-Yao.,Jung, Yunha.,Kuang, Yun.,...&Dai, Hongjie.(2021).Selective and High Current CO2 Electro-Reduction to Multicarbon Products in Near-Neutral KCl Electrolytes.Journal of the American Chemical Society,143(8),3245-3255.

Zhang, Xiao,et al."Selective and High Current CO2 Electro-Reduction to Multicarbon Products in Near-Neutral KCl Electrolytes".Journal of the American Chemical Society 143.8(2021):3245-3255.