Subsurface carbon modification of Ni-Ga for improved selectivity in acetylene hydrogenation reaction

doi:10.1016/j.cclet.2024.109525

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	Subsurface carbon modification of Ni-Ga for improved selectivity in acetylene hydrogenation reaction
	Dong, Shaoming 1,2; Niu, Yiming 1,2; Pu, Yinghui 1,2; Wang, Yongzhao 1,2; Zhang, Bingsen 1,2
通讯作者	Niu, Yiming(ymniu14b@imr.ac.cn) ; Zhang, Bingsen(bszhang@imr.ac.cn)
	2024-12-01
发表期刊	CHINESE CHEMICAL LETTERS
ISSN	1001-8417
卷号	35 期号:12 页码:4
摘要	Control of subsurface interstitial atoms in transition metals is an effective approach to modulate selectivity in hydrogenation reactions. In this study, nickel was alloyed with gallium to form Ni-3 Ga, thereby regulating the octahedral interstitial sites. Subsequently, carbon atoms were introduced into the Ni3 Ga (forming Ni-3 GaC0.5 ) via thermal treatment in an acetylene atmosphere, leading to a significant enhancement in selectivity for acetylene hydrogenation reaction. The X-ray diffraction and transmission electron microscopy results demonstrate an increase in the lattice parameter due to the incorporation of carbon atoms and the uniform distribution of carbon in Ni-3 GaC0.5 nanoparticles. The obtained Ni-3 GaC0.5 /oCNT catalyst exhibits significantly improved selectivity in acetylene hydrogenation reaction, with approximately 82% ethylene selectivity at 98% conversion. Furthermore, it maintains good selectivity at various hydrogen-to-alkyne ratios and displays good stability during long-term operation. The introduction of carbon suppresses the formation of the subsurface hydrogen structure under reaction conditions. Additionally, the charge transfer between carbon and nickel results in the electron deficiency of nickel, effectively inhibiting the over-hydrogenation pathway and enhancing the selectivity. These results provide insights for the design of non-precious metal catalysts in selective hydrogenation reactions. (c) 2024 Published by Elsevier B.V. on behalf of Chinese Chemical Society and Institute of Materia Medica, Chinese Academy of Medical Sciences.
关键词	Subsurface structure Interstitial atom Carbide Hydrogenation reaction Nickel alloy
资助者	National Natural Science Foundation of China ; Natural Science Foundation of Liaoning Province ; China Postdoctoral Science Foundation ; LiaoNing Revitalization Talents Program ; Foundations of Shenyang National Laboratory for Materials Science
DOI	10.1016/j.cclet.2024.109525
收录类别	SCI
语种	英语
资助项目	National Natural Science Foundation of China[22002173] ; National Natural Science Foundation of China[22072164] ; National Natural Science Foundation of China[52161145403] ; Natural Science Foundation of Liaoning Province[2022-MS-004] ; China Postdoctoral Science Foundation[2020M680999] ; LiaoNing Revitalization Talents Program[XLYC1807175] ; Foundations of Shenyang National Laboratory for Materials Science
WOS研究方向	Chemistry
WOS类目	Chemistry, Multidisciplinary
WOS记录号	WOS:001314387200001
出版者	ELSEVIER SCIENCE INC
引用统计
文献类型	期刊论文
条目标识符	http://ir.imr.ac.cn/handle/321006/189841
专题	中国科学院金属研究所
通讯作者	Niu, Yiming; Zhang, Bingsen
作者单位	1.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China 2.Univ Sci & Technol China, Sch Mat Sci & Engn, Shenyang 110016, Peoples R China
推荐引用方式 GB/T 7714	Dong, Shaoming,Niu, Yiming,Pu, Yinghui,et al. Subsurface carbon modification of Ni-Ga for improved selectivity in acetylene hydrogenation reaction[J]. CHINESE CHEMICAL LETTERS,2024,35(12):4.
APA	Dong, Shaoming,Niu, Yiming,Pu, Yinghui,Wang, Yongzhao,&Zhang, Bingsen.(2024).Subsurface carbon modification of Ni-Ga for improved selectivity in acetylene hydrogenation reaction.CHINESE CHEMICAL LETTERS,35(12),4.
MLA	Dong, Shaoming,et al."Subsurface carbon modification of Ni-Ga for improved selectivity in acetylene hydrogenation reaction".CHINESE CHEMICAL LETTERS 35.12(2024):4.