中空球形组装体强化Cu0/Cu+界面促进CO2电催化还原为C2+产物
Shaping hollow spherical assemblies for enhanced Cu0/Cu+interface to boost C2+selectivity in CO2 electroreduction
黎雨 1史皓峻 2李聪聪 1刘忠梁 1唐玮峥 1张婷婷 1阴世新 1李会会 1李春忠3
作者信息
- 1. Key Laboratory for Ultrafine Materials of Ministry of Education,School of Chemical Engineering,East China University of Science and Technology,Shanghai 200237,China
- 2. Shanghai Engineering Research Center of Hierarchical Nanomaterials,School of Materials Science and Engineering,East China University of Science and Technology,Shanghai 200237,China
- 3. Key Laboratory for Ultrafine Materials of Ministry of Education,School of Chemical Engineering,East China University of Science and Technology,Shanghai 200237,China;Shanghai Engineering Research Center of Hierarchical Nanomaterials,School of Materials Science and Engineering,East China University of Science and Technology,Shanghai 200237,China
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摘要
在铜基催化剂表面构建Cu0/Cu+界面有利于电催化CO2还原(CO2RR)为多碳(C2+)产物.然而,在高电流密度下,Cu+物种很容易被还原成金属Cu.因此,深入理解并合理设计和构建Cu基催化剂表面Cu0/Cu+界面对提高C2+产物选择性具有重要的意义.基于此,我们提出了一种可控的"纳米粒子组装"策略,以获得由大量Cu2O纳米粒子组成的中空球形组装体(HSA-Cu2O).HSA-Cu2O催化剂显著提高了C2+产物的选择性,其法拉第效率(FE)达到了79.2％±0.7％,C2+产物的部分电流密度为317.1 mA cm-2.在CO2RR过程中,HSA-Cu2O催化剂发生了原位电化学重构,实现了高密度的Cu0/Cu+活性界面位点的构建.俄歇电子能谱、原位拉曼和结构演变过程研究证实,Cu0/Cu+界面与中空球限域结构的结合促进了*CO中间体的富集,从而促进了*CO二聚化,提高了CO2RR中C2+产物的选择性.
Abstract
The creation of Cu0/Cu+interface over Cu-based catalysts is known to facilitate the production of multi-carbon(C2+)products during CO2 reduction reaction(CO2 RR).However,the Cu+moieties exhibit high susceptibility towards reduction into Cu0 at a high current density.Thus,a comprehensive understanding and rational shaping strategy for the construction and stabilization of Cu0/Cu+interface in Cu-based catalysts is imperative.Herein,we proposed a con-trollable"nanoparticle assembly"strategy to obtain hollow spherical assemblies(HSA)composed of numerous Cu2O na-noparticles(HSA-Cu2O).The HSA-Cu2O catalysts sig-nificantly enhance the selectivity of C2+products,resulting in an impressive overall Faraday efficiency(FE)of 79.2％±0.7％at a partial current density of 317.1 mA cm-2.The HSA-Cu2O catalysts undergo in-situ electrochemically reconstruction during CO2RR,achieving Cu0/Cu+interfacial sites with a high density.The Auger electron spectra,in-situ Raman,and morphological evolution studies have confirmed that the combination of the Cu0/Cu+interface and hollow sphere ar-chitecture facilitated the concentration of*CO intermediates,thereby promoting C-C dimerization to boost C2+selectivity in CO2RR.
关键词
Cu0/Cu+interface/hollow spherical assemblies/confinement effect/C-C couplingKey words
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出版年
2024
NETL
NSTL
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