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题名: Switchable CO2 electroreduction via engineering active phases of Pd nanoparticles
作者: Gao, Dunfeng1;  Zhou, Hu2;  Cai, Fan1, 6;  Wang, Dongniu3;  Hu, Yongfeng3;  Jiang, Bei4;  Cai, Wen-Bin4;  Chen, Xiaoqi1;  Si, Rui5;  Yang, Fan1;  Miao, Shu1;  Wang, Jianguo2;  Wang, Guoxiong1;  Bao, Xinhe1
关键词: carbon-dioxide electroreduction ;  Pd nanoparticles ;  active phase ;  selectivity fluctuation
刊名: NANO RESEARCH
发表日期: 2017-06-01
DOI: 10.1007/s12274-017-1514-6
卷: 10, 页:2181-2191
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences ;  Technology
类目[WOS]: Chemistry, Physical ;  Nanoscience & Nanotechnology ;  Materials Science, Multidisciplinary ;  Physics, Applied
研究领域[WOS]: Chemistry ;  Science & Technology - Other Topics ;  Materials Science ;  Physics
英文摘要: Active-phase engineering is regularly utilized to tune the selectivity of metal nanoparticles (NPs) in heterogeneous catalysis. However, the lack of understanding of the active phase in electrocatalysis has hampered the development of efficient catalysts for CO2 electroreduction. Herein, we report the systematic engineering of active phases of Pd NPs, which are exploited to select reaction pathways for CO2 electroreduction. In situ X-ray absorption spectroscopy, in situ attenuated total reflection-infrared spectroscopy, and density functional theory calculations suggest that the formation of a hydrogen-adsorbed Pd surface on a mixture of the a-and a-phases of a palladium-hydride core (alpha+beta PdHx@PdHx) above -0.2 V (vs. a reversible hydrogen electrode) facilitates formate production via the HCOO* intermediate, whereas the formation of a metallic Pd surface on the a-phase Pd hydride core (beta PdHx@Pd) below -0.5 V promotes CO production via the COOH* intermediate. The main product, which is either formate or CO, can be selectively produced with high Faradaic efficiencies (> 90%) and mass activities in the potential window of 0.05 to -0.9 V with scalable application demonstration.
关键词[WOS]: INFRARED-ABSORPTION SPECTROSCOPY ;  ELECTROCHEMICAL REDUCTION ;  CARBON-DIOXIDE ;  FORMIC-ACID ;  ELECTROCATALYTIC REDUCTION ;  AU NANOPARTICLES ;  SELECTIVE CONVERSION ;  HYDRIDE FORMATION ;  ENHANCED ACTIVITY ;  IONIC LIQUID
语种: 英语
WOS记录号: WOS:000401320700030
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/152317
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, CAS Ctr Excellence Nanosci, State Key Lab Catalysis, Dalian 116023, Peoples R China
2.Zhejiang Univ Technol, Coll Chem Engn, Hangzhou 310032, Zhejiang, Peoples R China
3.Univ Saskatchewan, Canadian Light Source Inc, 44 Innovat Blvd, Saskatoon, SK S7N 2V3, Canada
4.Fudan Univ, Shanghai Key Lab Mol Catalysis & Innovat Mat, Collaborat Innovat Ctr Chem Energy Mat, Dept Chem, Shanghai 200433, Peoples R China
5.Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China
6.Univ Chinese Acad Sci, Beijing 100039, Peoples R China

Recommended Citation:
Gao, Dunfeng,Zhou, Hu,Cai, Fan,et al. Switchable CO2 electroreduction via engineering active phases of Pd nanoparticles[J]. NANO RESEARCH,2017,10:2181-2191.
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