Identifying the Active Site on ZnxCryOz for HC-O Bond Cleavage in Syn-gas Conversion

doi:10.26434/chemrxiv-2024-chrkx

	Identifying the Active Site on Zn_xCr_yO_z for HC-O Bond Cleavage in Syn-gas Conversion
	Wu, Jiawei 1,2,3; Han, Yulan 1; Jia, Menglei 1,3; Xu, Jiayan 1; Hu, Peijun1,4
	2024-04-05
状态	已发表
摘要	The excellent performance of Zn_xCr_yO_z catalysts, used in the process of converting CO/H2 to methanol and light olefins, is highly attractive, but the microstructure of Zn_xCr_yO_z structure under the syngas conversion conditions remains elusive experimentally and theoretically because of the limitation of the detecting facilities/methods. By using the geneticalgorithm -based global structural search accelerated by machine learning in combination with a local cluster sampling strategy in the active learning scheme, we reveal the structure/composition evolution of Zn_xCr_yO_z structures and uncover that the catalytic activities of these catalysts strongly depend on the Zn/Cr ratios under the syngas conversion conditions. The possible active phase at the thermodynamically stable condition is identified and the critical active site influencing the catalytic property is unraveled. We show that the catalyst Zn₂Cr₂O₅, which consists of a thin ZnO layer and the ZnCr₂O₄ structures, achieves a high catalytic activity for syngas conversion and its X-ray diffraction patterns are in agreement with the experimental result. Importantly, the presence of a hexahedral configuration ([ZnCrO₂]_hex) is found to affect the catalyst activity significantly, and this result is further supported by the analysis based on the structure -activity relationship.
关键词	ZnxCryOz catalysts Zn/Cr=1 machine learning syngas conversion
语种	英语
DOI	10.26434/chemrxiv-2024-chrkx
相关网址	查看原文
出处	chemRxiv
收录类别	PPRN.PPRN
WOS记录号	PPRN:88404701
WOS类目	Chemistry, Multidisciplinary
资助项目	EPSRC[EP/P022561/1] ; null[EP/T022175/1] ; null[EP/P020194/1]
文献类型	预印本
条目标识符	https://kms.shanghaitech.edu.cn/handle/2MSLDSTB/372941
专题	物质科学与技术学院物质科学与技术学院_PI研究组_胡培君组
通讯作者	Hu, Peijun
作者单位	1.Queens Univ Belfast, Sch Chem & Chem Engn, Belfast BT9 5AZ, North Ireland 2.Jianghan Univ, Sch Optoelect Mat & Technol, Wuhan 430056, Peoples R China 3.East China Univ Sci & Technol, Res Inst Ind Catalysis, Ctr Computat Chem, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China 4.ShanghaiTech Univ, Sch Phys Sci & Technol, Shanghai 201210, Peoples R China
推荐引用方式 GB/T 7714	Wu, Jiawei,Han, Yulan,Jia, Menglei,et al. Identifying the Active Site on Zn_xCr_yO_z for HC-O Bond Cleavage in Syn-gas Conversion. 2024.