Identifying the Performance Descriptor in Direct Syngas Conversion to Long-Chain α-Olefins over Ruthenium-Based Catalysts Promoted by Alkali Metals

doi:10.1021/acscatal.2c06158

	Identifying the Performance Descriptor in Direct Syngas Conversion to Long-Chain α-Olefins over Ruthenium-Based Catalysts Promoted by Alkali Metals
	Yu, Hailing 1,2; Wei, Yao 2,3; Lin, Tiejun 1; Wang, Caiqi 1; An, Yunlei 1; Yu, Fei 1; Sun, Fanfei 4; Jiang, Zheng 4; Sun, Yuhan1,5 ; Zhong, Liangshu1,5
	2023
发表期刊	ACS CATALYSIS; (IF:11.3[JCR-2023],12.6[5-Year])
ISSN	2155-5435
EISSN	2155-5435
卷号	13 期号:6 页码:3949-3959
发表状态	已发表
DOI	10.1021/acscatal.2c06158
摘要	Fischer-Tropsch synthesis (FTS) provides a nonpetroleum route for the production of value-added α-olefins from syngas. However, regulating the product distribution to promote the formation of long-chain α-olefins while maintaining low selectivity to C1 byproducts (CO2 and CH4) remains a great challenge. Herein, a series of alkali metal-promoted Ru/SiO2 catalysts were synthesized to investigate the effect of alkali metals and identify the performance descriptor for syngas to α-olefins. X-ray absorption and photoelectron spectroscopy as well as CO diffuse reflectance infrared Fourier transformation spectra revealed that Ru’s electronic structure can be tuned by the addition of alkali metal promoters. The Allen scale electronegativity deviation between the metallic Ru and the alkali metal promoter, which was identified as a performance descriptor, was correlated with the initial turnover frequency (TOF) and olefins distribution, as well as the chain growth probability. In addition, the fraction of olefin products was successfully adjusted from lower olefins (50.3%) to long-chain α-olefins (85.8%) by controlling the kinds of alkali metal promoters. Evidences from X-ray absorption spectroscopy and chemisorption characterizations revealed that the controllable Ru electron density could enhance CO adsorption and hinder the reactivity of chemisorbed H species, thus benefiting the α-olefin production. These results offer a comprehensive view of the electronic effect for regulating product selectivity during the Fischer-Tropsch reaction process.
关键词	alkali metal Fischer-Tropsch synthesis long-chain α-olefins ruthenium-based catalyst syngas conversion
学科门类	Catalysis ; Chemistry (all)
URL	查看原文
收录类别	SCOPUS ; EI ; SCI
语种	英语
资助项目	Natural Science Foundation of China["U22B20136","22293023","91945301","22072177","22172188"] ; National Key R&D Program of China[2021YFF0500702] ; Natural Science Foundation of Shanghai["22JC1404200","21ZR1471700"] ; Program of Shanghai Academic/Technology Research Leader[20XD1404000] ; Chinese Academy of Sciences[XDA21020600]
WOS研究方向	Chemistry
WOS类目	Chemistry, Physical
WOS记录号	WOS:000946554600001
出版者	AMER CHEMICAL SOC
EI入藏号	20231113729250
EI主题词	Fischer-Tropsch synthesis
EI分类号	547.1 Precious Metals ; 801.4 Physical Chemistry ; 802.2 Chemical Reactions ; 802.3 Chemical Operations ; 803 Chemical Agents and Basic Industrial Chemicals ; 804 Chemical Products Generally ; 804.1 Organic Compounds ; 921.3 Mathematical Transformations ; 922.1 Probability Theory ; 931.3 Atomic and Molecular Physics
原始文献类型	Article
Scopus 记录号	2-s2.0-85149810183
来源库	SCOPUS
引用统计	正在获取...
文献类型	期刊论文
条目标识符	https://kms.shanghaitech.edu.cn/handle/2MSLDSTB/286520
专题	物质科学与技术学院物质科学与技术学院_特聘教授组_孙予罕组物质科学与技术学院_特聘教授组_钟良枢组
通讯作者	Zhong, Liangshu
作者单位	1.Chinese Acad Sci, Shanghai Adv Res Inst, CAS Key Lab Low Carbon Convers Sci & Engn, Shanghai 201210, Peoples R China 2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 3.Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai 201800, Peoples R China 4.Chinese Acad Sci, Shanghai Adv Res Inst, Shanghai Synchrotron Radiat Facil, Shanghai 201210, Peoples R China 5.ShanghaiTech Univ, Sch Phys Sci & Technol, Shanghai 201210, Peoples R China
通讯作者单位	物质科学与技术学院
推荐引用方式 GB/T 7714	Yu, Hailing,Wei, Yao,Lin, Tiejun,et al. Identifying the Performance Descriptor in Direct Syngas Conversion to Long-Chain α-Olefins over Ruthenium-Based Catalysts Promoted by Alkali Metals[J]. ACS CATALYSIS;,2023,13(6):3949-3959.
APA	Yu, Hailing.,Wei, Yao.,Lin, Tiejun.,Wang, Caiqi.,An, Yunlei.,...&Zhong, Liangshu.(2023).Identifying the Performance Descriptor in Direct Syngas Conversion to Long-Chain α-Olefins over Ruthenium-Based Catalysts Promoted by Alkali Metals.ACS CATALYSIS;,13(6),3949-3959.
MLA	Yu, Hailing,et al."Identifying the Performance Descriptor in Direct Syngas Conversion to Long-Chain α-Olefins over Ruthenium-Based Catalysts Promoted by Alkali Metals".ACS CATALYSIS; 13.6(2023):3949-3959.