无机材料学报 ›› 2022, Vol. 37 ›› Issue (1): 29-37.DOI: 10.15541/jim20210547

所属专题: 【能源环境】CO2绿色转换 2022年度中国知网高下载论文

• 专栏: CO 2 绿色转化(特邀编辑: 欧阳述昕, 王文中) • 上一篇    下一篇

调控CuO表面性质选择性电催化还原CO2制HCOOH

郭李娜(), 何雪冰, 吕琳, 吴丹, 原弘()   

  1. 华中师范大学 化学学院, 农药与化学生物学教育部重点实验室, 武汉 430079
  • 收稿日期:2021-09-04 修回日期:2021-10-22 出版日期:2022-01-20 网络出版日期:2021-11-01
  • 通讯作者: 原 弘, 教授. E-mail: yuanhong@mail.ccnu.edu.cn
  • 作者简介:郭李娜(1998-), 女, 硕士研究生. E-mail: gln@mails.ccnu.edu.cn
  • 基金资助:
    软物质材料化学与功能制造重庆市重点实验室开放经费(20191002)

Modulation of CuO Surface Properties for Selective Electrocatalytic Reduction of CO2 to HCOOH

GUO Lina(), HE Xuebing, LYU Lin, WU Dan, YUAN Hong()   

  1. Key Laboratory of Pesticide and Chemical Biology, Ministry of Education, College of Chemistry, Central China Normal University, Wuhan 430079, China
  • Received:2021-09-04 Revised:2021-10-22 Published:2022-01-20 Online:2021-11-01
  • Contact: YUAN Hong, professor. E-mail: yuanhong@mail.ccnu.edu.cn
  • About author:GUO Lina (1998-), female, Master candidate. E-mail: gln@mails.ccnu.edu.cn
  • Supported by:
    Chongqing Key Laboratory of Soft-Matter Material Chemistry and Function Manufacturing(20191002)

摘要:

电催化二氧化碳还原反应可将温室气体二氧化碳转化为化工原料或者有机燃料, 为克服全球变暖和电能向化学能转化提供了一条可行途径。该技术的主要挑战是产物分布广, 导致单一产物选择性低, 而调控催化剂的表面性质是解决这一难题的可行策略。本研究通过对氧化亚铜、硫化亚铜进行氧化制备表面性质不同的氧化铜, 其中, 氧化硫化亚铜制得的CuO-FS催化剂提高了电还原二氧化碳的活性和还原产物甲酸的选择性。该催化剂表现出较高的总电流密度, 而且在一个较大的测试电压范围(-0.8 ~ -1.1 V)内, 甲酸的法拉第效率可以保持在70%以上, 在-0.9 V时达到最大值78.4%。反应机理探究表明, CuO-FS优异的电还原二氧化碳性能归因于其较大的电化学活性表面积提供了大量表面活性位点, 产生较高的总电流密度; 而且电催化过程中催化剂表面产生较少的零价Cu, 减少了乙烯的生成, 使产物更集中于甲酸。

关键词: 电还原二氧化碳, 铜基催化剂, 表面性质, 产物选择性, 甲酸

Abstract:

The electrocatalytic carbon dioxide reduction reaction can convert the greenhouse gas carbon dioxide into chemical raw materials or organic fuels, providing a feasible way to overcome global warming and the conversion of electrical energy to chemical energy. The main challenge of this technology is the wide product distribution, resulting in low selectivity of a single product, however, modulating the surface properties of the catalyst is an efficient strategy to solve this problem. In this study, the precursors of Cu2O and Cu2S were oxidized to the CuO catalysts with different surface properties. The CuO-FS catalyst derived from Cu2S delivered the improved activity of electro-reduction of carbon dioxide and selectivity for formic acid product. This catalyst exhibited a higher total current density and the Faraday efficiency of formic acid > 70% in a wide test voltage range of -0.8 - -1.1 V; the Faraday efficiency for formic acid could reach a maximum of 78.4% at -0.9 V. The mechanism study indicated that the excellent performance of CuO-FS for electro-reduction of carbon dioxide could be attributed to the large electrochemically active surface area, which provided a large number of surface active sites, resulting in a higher total current density; moreover, the less zero-valent Cu was produced over the surface of CuO-FS during the electrocatalytic process, which reduced the production of ethylene and thus promoted the production of formic acid.

Key words: CO2 electroreduction, Cu-based catalyst, surface properties, product selectivity, formic acid

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