Surface Segregation in CuNi Nanoparticle Catalysts During CO2 Hydrogenation: The Role of CO in the Reactant Mixture

doi:10.1021/acs.jpcc.8b09912

CORC > 上海应用物理研究所 > 中国科学院上海应用物理研究所 > 中科院上海应用物理研究所2011-2017年

	Surface Segregation in CuNi Nanoparticle Catalysts During CO2 Hydrogenation: The Role of CO in the Reactant Mixture
	Zegkinoglou, I ; Pielsticker, L ; Han, ZK ; Divins, NJ ; Kordus, D ; Chen, YT ; Escudero, C ; Perez-Dieste, V ; Zhu, BE ; Gao, Y
刊名	JOURNAL OF PHYSICAL CHEMISTRY C
	2019
卷号	123 期号:13 页码:8421—8428
关键词	RAY PHOTOELECTRON-SPECTROSCOPY TOTAL-ENERGY CALCULATIONS METHANOL SYNTHESIS PARTICLE-SIZE NICKEL NI METHANATION GAS DEPOSITION OXIDE
ISSN号	1932-7447
DOI	10.1021/acs.jpcc.8b09912
文献子类	期刊论文
英文摘要	Surface segregation and restructuring in size-selected CuNi nanoparticles were investigated via near-ambient pressure X-ray photoelectron spectroscopy (NAP-XPS) at various temperatures in different gas environments. Particularly in focus were structural and morphological changes occurring under CO2 hydrogenation conditions in the presence of carbon monoxide (CO) in the reactant gas mixture. Nickel surface segregation was observed when only CO was present as adsorbate. The segregation trend is inverted in a reaction gas mixture consisting of CO2, H-2, and CO, resulting in an increase of copper concentration on the surface. Density functional theory calculations attributed the inversion of the segregation trend to the formation of a stable intermediate on the nanocatalyst surface (CH3O) in the CO-containing reactant mixture, which modifies the nickel segregation energy, thus driving copper to the surface. The promoting role of CO for the synthesis of methanol was demonstrated by catalytic characterization measurements of silica-supported CuNi NPs in a fixed-bed reactor, revealing high methanol selectivity (over 85%) at moderate pressures (20 bar). The results underline the important role of intermediate reaction species in determining the surface composition of bimetallic nanocatalysts and help understand the effect of CO cofeed on the properties of CO2 hydrogenation catalysts.
语种	英语
内容类型	期刊论文
源URL	[http://ir.sinap.ac.cn/handle/331007/31843]
专题	上海应用物理研究所_中科院上海应用物理研究所2011-2017年
作者单位	1.Ruhr Univ Bochum, Dept Phys, D-44780 Bochum, Germany; 2.Chinese Acad Sci, Shanghai Inst Appl Phys, Div Interfacial Water, Shanghai 201800, Peoples R China; 3.Chinese Acad Sci, Shanghai Inst Appl Phys, Key Lab Interfacial Phys & Technol, Shanghai 201800, Peoples R China; 4.ALBA Synchrotron Light Source, Carrer Llum 2-26, Barcelona 08290, Spain; 5.Max Planck Gesell, Fritz Haber Inst, Dept Interface Sci, D-14195 Berlin, Germany
推荐引用方式 GB/T 7714	Zegkinoglou, I,Pielsticker, L,Han, ZK,et al. Surface Segregation in CuNi Nanoparticle Catalysts During CO2 Hydrogenation: The Role of CO in the Reactant Mixture[J]. JOURNAL OF PHYSICAL CHEMISTRY C,2019,123(13):8421—8428.
APA	Zegkinoglou, I.,Pielsticker, L.,Han, ZK.,Divins, NJ.,Kordus, D.,...&Cuenya, BR.(2019).Surface Segregation in CuNi Nanoparticle Catalysts During CO2 Hydrogenation: The Role of CO in the Reactant Mixture.JOURNAL OF PHYSICAL CHEMISTRY C,123(13),8421—8428.
MLA	Zegkinoglou, I,et al."Surface Segregation in CuNi Nanoparticle Catalysts During CO2 Hydrogenation: The Role of CO in the Reactant Mixture".JOURNAL OF PHYSICAL CHEMISTRY C 123.13(2019):8421—8428.