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题名: Size-Dependent Electrocatalytic Reduction of CO2 over Pd Nanoparticles
作者: Gao, Dunfeng1, 3;  Zhou, Hu2;  Wang, Jing1, 3;  Miao, Shu1;  Yang, Fan1;  Wang, Guoxiong1;  Wang, Jianguo2;  Bao, Xinhe1
刊名: JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
发表日期: 2015-04-08
DOI: 10.1021/jacs.5b00046
卷: 137, 期:13, 页:4288-4291
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences
类目[WOS]: Chemistry, Multidisciplinary
研究领域[WOS]: Chemistry
英文摘要: Size effect has been regularly utilized to tune the catalytic activity and selectivity of metal nanoparticles (NPs). Yet, there is a lack of understanding of the size effect in the electrocatalytic reduction of CO2, an important reaction that couples with intermittent renewable energy storage and carbon cycle utilization. We report here a prominent size-dependent activity/selectivity in the electrocatalytic reduction of CO2 over differently sized Pd NPs, ranging from 2.4 to 10.3 nm. The Faradaic efficiency for CO production varies from 5.8% at -0.89 V (vs reversible hydrogen electrode) over 10.3 nm NPs to 91.2% over 3.7 nm NPs, along with an 18.4-fold increase in current density. Based on the Gibbs free energy diagrams from density functional theory calculations, the adsorption of CO2 and the formation of key reaction intermediate COOH* are much easier on edge and corner sites than on terrace sites of Pd NPs. In contrast, the formation of H* for competitive hydrogen evolution reaction is similar on all three sites. A volcano-like curve of the turnover frequency for CO production within the size range suggests that CO2 adsorption, COOH* formation, and CO* removal during CO2 reduction can be tuned by varying the size of Pd NPs due to the changing ratio of corner, edge, and terrace sites.
关键词[WOS]: ELECTROCHEMICAL REDUCTION ;  CARBON-DIOXIDE ;  SELECTIVE CONVERSION ;  ENHANCED ACTIVITY ;  AU NANOPARTICLES ;  CATALYSTS ;  ELECTROREDUCTION ;  ELECTRODES ;  FORMATE
语种: 英语
WOS记录号: WOS:000352752000004
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/146162
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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作者单位: 1.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
2.Zhejiang Univ Technol, Coll Chem Engn, Hangzhou 310032, Zhejiang, Peoples R China
3.Univ Chinese Acad Sci, Beijing 100039, Peoples R China

Recommended Citation:
Gao, Dunfeng,Zhou, Hu,Wang, Jing,et al. Size-Dependent Electrocatalytic Reduction of CO2 over Pd Nanoparticles[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2015,137(13):4288-4291.
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