化工进展 ›› 2023, Vol. 42 ›› Issue (8): 4136-4142.DOI: 10.16085/j.issn.1000-6613.2023-0273

• 专栏:化学产品工程 • 上一篇    下一篇

Ag/Cu耦合催化剂的Cu晶面调控用于电催化二氧化碳还原

刘毅1,2(), 房强1,2, 钟达忠1,2, 赵强1,2(), 李晋平1,2()   

  1. 1.太原理工大学化学工程与技术学院,山西 太原 030024
    2.气体能源高效利用山西省重点实验室,山西 太原 030024
  • 收稿日期:2023-02-27 修回日期:2023-04-10 出版日期:2023-08-15 发布日期:2023-09-19
  • 通讯作者: 赵强,李晋平
  • 作者简介:刘毅(1996—),男,硕士研究生,研究方向为电催化CO2还原。E-mail:liuyi0649@link.tyut.edu.cn
  • 基金资助:
    国家自然科学基金(21878202);山西省基础研究计划(202203021212266)

Cu facets regulation of Ag/Cu coupled catalysts for electrocatalytic reduction of carbon dioxide

LIU Yi1,2(), FANG Qiang1,2, ZHONG Dazhong1,2, ZHAO Qiang1,2(), LI Jinping1,2()   

  1. 1.College of Chemical Engineering and Technology, Taiyuan University of Technology, Taiyuan 030024, Shanxi, China
    2.Shanxi Key Laboratory of Gas Energy Efficient and Clean Utilization, Taiyuan 030024, Shanxi, China
  • Received:2023-02-27 Revised:2023-04-10 Online:2023-08-15 Published:2023-09-19
  • Contact: ZHAO Qiang, LI Jinping

摘要:

电催化二氧化碳还原是降低大气中二氧化碳浓度和缓解温室效应的有效方法。然而,将CO2电还原为具有高附加值和高能量密度的碳氢化合物或燃料(C2+产物)仍然具有十足的挑战性。为了降低大气中二氧化碳浓度和将其转换为有价值的工业品,本文通过优化Ag/Cu耦合催化剂中Cu的晶面,有效地促进了其还原CO2至C2H4和C2H5OH等C2+产物。利用暴露Cu2O(100)晶面的Ag/Cu2O-(100),暴露Cu2O(111)晶面的Ag/Cu2O-(111)以及具有Cu2O(100)和(111)晶面的Ag/Cu2O-(100/111)还原制备得到了三种具有不同Cu晶面的Ag/Cu耦合催化剂。控制Cu/Ag比均为30∶1,采用H型电解槽,在CO2饱和的0.1mol/L KHCO3电解液中,评估了其CO2电化学还原性能。其中,具有Cu(100)和Cu(111)晶面的Ag/Cu-(100/111)催化剂展现出最优异的将CO2还原为C2+产物的性能,Cu(100)晶面和(111)晶面的界面有效地促进了C—C耦合,其在-1.3V、-1.5V(vs.RHE)时,C2+产物的法拉第效率(FE)均在50%以上,在电位为-1.5V(vs. RHE)时,C2+产物的最大FE为57.7%,部分电流密度为8.92mA/cm2

关键词: Ag/Cu2O催化剂, 电化学, 二氧化碳, 还原, 形貌, 晶面, C2+产物

Abstract:

Electrocatalytic carbon dioxide reduction is an effective method to reduce atmospheric carbon dioxide concentration and mitigate the greenhouse effect. However, electroreduction of CO2 to hydrocarbons or fuels with high-added value and high energy density(C2+ products) remains extremely challenging, which however could be effectively promoted by optimizing the facets of Cu in the Ag/Cu coupled catalysts. Three Ag/Cu coupled catalysts with different Cu facets were obtained by reduction of Ag/Cu2O-(100) with exposed Cu2O-(100) facets, Ag/Cu2O-(111) with exposed Cu2O-(111) facets, and Ag/Cu2O-(100/111) with Cu2O(100) and (111) facets. The CO2 electrochemical reduction performance was evaluated in an H-type electrolytic cell filled with CO2-saturated 0.1 M KHCO3 electrolyte, and the Cu/Ag ratio was controlled as 30∶1. Among them, Ag/Cu-(100/111) catalyst with Cu(100) and Cu(111) facets showed the best performance of reduction CO2 to C2+ productswith aFE of C2+ products above 50% at -1.3V and -1.5V vs. RHE. When the potential was -1.5V vs. RHE, the maximum FE of C2+ products was 57.7% and the partial current density was 8.92mA/cm2.

Key words: Ag/Cu2O catalyst, electrochemistry, carbon dioxide, reduction, morphology, facets, C2+ products

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