Effect of halides on catalytic activity and selectivity of silver electrodes for CO2 electroreduction

doi:10.11949/j.issn.0438-1157.20160976

Abstract

Abstract:

Silver (Ag) is an excellent electrocatalyst for carbon dioxide (CO₂) to carbon monoxide (CO) conversion in aqueous or nonaqueous electrolytes. However, polycrystalline silver needs significant overpotentials to achieve ideal selectivity and reaction rate, thus new methods are required to increase catalytic performance of polycrystalline silver. Effects of halides on silver foil for CO₂ electrochemical reduction were studied by Faradaic efficiency and current density of carbon monoxide (CO) as a function of working potential with presence of Cl^-, Br^-, and I^- in KHCO3 solution. The results showed that all of these halides increased CO selectivity and reaction rate with CO enhancement in the order of Cl^- < Br^- < I^-. CO selectivity of I^- added electrolyte was 28 times that of halide-free electrolyte at 590 mV overpotential. Besides enhancement of CO reaction rate, Cl^- and Br^- also improved hydrogen evolution reaction at the same time, which was not observed in I^-. The remarkable catalytic performance of I^- could be attributed to its strong adsorption, which might form nanoparticles on Ag surface and increase number of activity sites for CO, and its easy charge donation to Ag surface, which might enhance interaction with partially positive-charged carbon atom of CO₂. In conclusion, I^- was more suitable for CO₂ reduction than Cl^- and Br^-, which could benefit industrialized CO production and maximize economic output.

Key words: CO₂ reduction, CO, silver foil, electrocataysis, halides

摘要：

通过在电解液中加入卤族元素，系统地研究了卤族元素对于CO的选择性和反应速率的影响。结果表明，卤族元素对于CO₂的还原反应具有促进作用，并按照Cl^- < Br^- < I^-的顺序递增。Cl^-和Br^-对CO₂还原反应和析氢反应都具有催化作用，而I^-的存在加快了CO的生成，对析氢反应没有明显影响。在过电势为590 mV时，CO在有I-溶液中的选择性是无I^-溶液的28倍。经过表征和分析后得出，I^-具有较强的吸附性能，通过化学吸附使催化剂表面形貌发生改变，CO的活性位增多，加快其反应速率。同时，I^-在反应过程中易向反应表面传输负电荷，增加与碳原子的相互作用，从而提高CO的生成速率。

关键词: CO₂还原, CO, Ag电极, 电催化, 卤族元素

CLC Number:

O646.1

ZHANG Zhipan, CHEN Chengzhen, WANG Qianqian, ZHONG Juhua, ZHANG Bo, CHENG Zhenmin. Effect of halides on catalytic activity and selectivity of silver electrodes for CO₂ electroreduction[J]. CIESC Journal, 2017, 68(2): 687-693.

张志盼, 陈承镇, 王倩倩, 钟菊花, 张波, 程振民. 卤族元素对Ag电极电催化还原CO₂的影响[J]. 化工学报, 2017, 68(2): 687-693.

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Effect of halides on catalytic activity and selectivity of silver electrodes for CO₂ electroreduction

卤族元素对Ag电极电催化还原CO₂的影响

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