DICP OpenIR
Switchable CO2 electroreduction via engineering active phases of Pd nanoparticles
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
2017-06-01
DOI10.1007/s12274-017-1514-6
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
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
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.
语种英语
WOS记录号WOS:000401320700030
引用统计
文献类型期刊论文
条目标识符http://cas-ir.dicp.ac.cn/handle/321008/152317
专题中国科学院大连化学物理研究所
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
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GB/T 7714
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.
APA Gao, Dunfeng.,Zhou, Hu.,Cai, Fan.,Wang, Dongniu.,Hu, Yongfeng.,...&Bao, Xinhe.(2017).Switchable CO2 electroreduction via engineering active phases of Pd nanoparticles.NANO RESEARCH,10,2181-2191.
MLA Gao, Dunfeng,et al."Switchable CO2 electroreduction via engineering active phases of Pd nanoparticles".NANO RESEARCH 10(2017):2181-2191.
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