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
KeywordCarbon-dioxide Electroreduction Pd Nanoparticles Active Phase Selectivity Fluctuation
Source PublicationNANO RESEARCH
2017-06-01
DOI10.1007/s12274-017-1514-6
Volume10Pages:2181-2191
Indexed BySCI
SubtypeArticle
WOS HeadingsScience & Technology ; Physical Sciences ; Technology
WOS SubjectChemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied
WOS Research AreaChemistry ; Science & Technology - Other Topics ; Materials Science ; Physics
WOS KeywordINFRARED-ABSORPTION SPECTROSCOPY ; ELECTROCHEMICAL REDUCTION ; CARBON-DIOXIDE ; FORMIC-ACID ; ELECTROCATALYTIC REDUCTION ; AU NANOPARTICLES ; SELECTIVE CONVERSION ; HYDRIDE FORMATION ; ENHANCED ACTIVITY ; IONIC LIQUID
AbstractActive-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.
Language英语
WOS IDWOS:000401320700030
Citation statistics
Cited Times:39[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://cas-ir.dicp.ac.cn/handle/321008/152317
Collection中国科学院大连化学物理研究所
Affiliation1.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
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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