Selective Electrochemical Production of Formate from Carbon Dioxide with Bismuth-Based Catalysts in an Aqueous Electrolyte,ACS Catalysis

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Selective Electrochemical Production of Formate from Carbon Dioxide with Bismuth-Based Catalysts in an Aqueous Electrolyte
ACS Catalysis ( IF 11.3 ) Pub Date : 2018-01-05 00:00:00 , DOI: 10.1021/acscatal.7b03242
Chan Woo Lee _{1,

2} , Jung Sug Hong ₁ , Ki Dong Yang ₁ , Kyoungsuk Jin ₁ , Jun Ho Lee ₁ , Hyo-Yong Ahn ₁ , Hongmin Seo ₁ , Nark-Eon Sung ₃ , Ki Tae Nam ₁

Affiliation

For the efficient electroconversion of CO₂ to formate, CO and H₂ evolution must be suppressed. Herein, carbon-supported BiO_x nanoparticles (BiO_x/C) were investigated as a potential candidate for CO₂ reduction. In bicarbonate solutions, the BiO_x/C catalysts exhibited a high Faradaic efficiency of 93.4% for formate from −1.37 to −1.70 V versus Ag/AgCl with a negligible amount of CO and H₂. Stable partial current densities and high Faradaic efficiencies were also achieved in 0.5 M NaCl (12.5 mA cm^–2 and 96.0%, respectively). The possible reaction pathways and kinetic parameters of formate formation were examined using systematic electrochemical methods, including Tafel, pH dependence, and in situ X-ray absorption near-edge structure analyses. From the results of these mechanistic studies, we propose that dual mechanisms are functional on the BiO_x/C catalysts. Specifically, a two-electron and one-proton transfer reaction to adsorbed CO₂ or a chemical proton transfer reaction to CO₂^– anion are the possible rate-determining steps (RDSs) at low potentials, whereas a one-electron transfer reaction to CO₂ is the RDS at high potentials.

中文翻译：

电解质中铋基催化剂从二氧化碳中选择性地生成甲酸盐

为了将CO ₂有效电转化为甲酸，必须抑制CO和H _2的逸出。在此，研究了碳负载的BiO _x纳米颗粒（BiO _x / C）作为CO ₂还原的潜在候选者。在碳酸氢盐溶液中，相对于Ag / AgCl和少量的CO和H ₂，BiO _x / C催化剂对-1.37至-1.70 V的甲酸有93.4％的高法拉第效率。在0.5 M NaCl（12.5 mA cm ^–2）中也实现了稳定的部分电流密度和高法拉第效率和96.0％）。使用系统的电化学方法，包括Tafel，pH依赖性和原位X射线吸收近边缘结构分析，检查了甲酸形成的可能反应途径和动力学参数。从这些机理研究的结果，我们提出双重机理在BiO _x / C催化剂上起作用。具体地，为了吸附在两电子和一个质子转移反应的CO ₂，或CO的化学质子转移反应₂^-阴离子是可能的速率决定步骤（RDS中）在低电势，而对CO的单电子转移反应₂是高电位的RDS。

更新日期：2018-01-05

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