Switchable CO2 electroreduction via engineering active phases of Pd nanoparticles

doi:10.1007/s12274-017-1514-6

	Switchable CO2 electroreduction via engineering active phases of Pd nanoparticles
	Gao, Dunfeng 2; Zhou, Hu 6; Cai, Fan 2,3; Wang, Dongniu 4; Hu, Yongfeng 4; Jiang, Bei 5; Cai, Wen-Bin 5; Chen, Xiaoqi 2; Si, Rui 1; Yang, Fan 2
刊名	NANO RESEARCH
	2017-06-01
卷号	10 页码:2181-2191
关键词	Carbon-dioxide Electroreduction Pd Nanoparticles Active Phase Selectivity Fluctuation
DOI	10.1007/s12274-017-1514-6
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
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/152317]
专题	大连化学物理研究所_中国科学院大连化学物理研究所
作者单位	1.Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China 2.Chinese Acad Sci, Dalian Inst Chem Phys, CAS Ctr Excellence Nanosci, State Key Lab Catalysis, Dalian 116023, Peoples R China 3.Univ Chinese Acad Sci, Beijing 100039, Peoples R China 4.Univ Saskatchewan, Canadian Light Source Inc, 44 Innovat Blvd, Saskatoon, SK S7N 2V3, Canada 5.Fudan Univ, Shanghai Key Lab Mol Catalysis & Innovat Mat, Collaborat Innovat Ctr Chem Energy Mat, Dept Chem, Shanghai 200433, Peoples R China 6.Zhejiang Univ Technol, Coll Chem Engn, Hangzhou 310032, Zhejiang, Peoples R China
推荐引用方式 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.