Steering the reaction pathway of syngas-to-light olefins with coordination unsaturated sites of ZnGaOx spinel

doi:10.1038/s41467-022-30344-1

	Steering the reaction pathway of syngas-to-light olefins with coordination unsaturated sites of ZnGaOx spinel
	Li, Na 2,3,7; Zhu, Yifeng 7; Jiao, Feng 2,3,7; Pan, Xiulian 2,3,7; Jiang, Qike 2; Cai, Jun 3,4,5; Li, Yifan 1,7; Tong, Wei 6; Xu, Changqi 2; Qu, Shengcheng 2
刊名	NATURE COMMUNICATIONS
	2022-05-18
卷号	13
DOI	10.1038/s41467-022-30344-1
通讯作者	Pan, Xiulian(panxl@dicp.ac.cn) ; Bao, Xinhe(xhbao@dicp.ac.cn)
英文摘要	Significant progress has been demonstrated in the development of bifunctional oxide-zeolite catalyst concept to tackle the selectivity challenge in syngas chemistry. Despite general recognition on the importance of defect sites of metal oxides for CO/H-2 activation, the actual structure and catalytic roles are far from being well understood. We demonstrate here that syngas conversion can be steered along a highly active and selective pathway towards light olefins via ketene-acetate (acetyl) intermediates by the surface with coordination unsaturated metal species, oxygen vacancies and zinc vacancies over ZnGaOx spinel-SAPO-34 composites. It gives 75.6% light-olefins selectivity and 49.5% CO conversion. By contrast, spinel-SAPO-34 containing only a small amount of oxygen vacancies and zinc vacancies gives only 14.9% light olefins selectivity at 6.6% CO conversion under the same condition. These findings reveal the importance to tailor the structure of metal oxides with coordination unsaturated metal sites/oxygen vacancies in selectivity control within the oxide-zeolite framework for syngas conversion and being anticipated also for CO2 hydrogenation. Great progress has been made in the development of bifunctional oxide-zeolite catalysts to tackle the selectivity challenge in syngas chemistry. Here the authors show syngas conversion can be steered along a highly active and selective pathway towards light olefins via ketene acetate (acetyl) intermediates.
资助项目	Ministry of Science and Technology of China[2018YFA0704503] ; Chinese Academy of Sciences[XDA21020400] ; National Natural Science Foundation of China[91945302] ; National Natural Science Foundation of China[22002153] ; National Natural Science Foundation of China[22008234] ; National Natural Science Foundation of China[11227902] ; Youth Innovation Promotion Association of Chinese Academy of Sciences[2019184] ; Dalian Science and Technology Innovation Fund[2020JJ26GX028] ; Natural Science Foundation of Liaoning[2020-BS-019]
WOS关键词	HIGHLY SELECTIVE CONVERSION ; SINGLE-CRYSTALLINE ; CARBON-DIOXIDE ; PARAMAGNETIC-RESONANCE ; OPTICAL-PROPERTIES ; METHANOL SYNTHESIS ; CO HYDROGENATION ; ZINC-OXIDE ; FT-IR ; ZNGA2O4
WOS研究方向	Science & Technology - Other Topics
语种	英语
出版者	NATURE PORTFOLIO
WOS记录号	WOS:000798996800008
资助机构	Ministry of Science and Technology of China ; Chinese Academy of Sciences ; National Natural Science Foundation of China ; Youth Innovation Promotion Association of Chinese Academy of Sciences ; Dalian Science and Technology Innovation Fund ; Natural Science Foundation of Liaoning
内容类型	期刊论文
源URL	[http://ir.hfcas.ac.cn:8080/handle/334002/131089]
专题	中国科学院合肥物质科学研究院
通讯作者	Pan, Xiulian; Bao, Xinhe
作者单位	1.Univ Sci & Technol China, Dept Chem Phys, Jinzhai Rd 96, Hefei 230026, Peoples R China 2.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, 457 Zhongshan Rd, Dalian 116023, Peoples R China 3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 4.Chinese Acad Sci, Shanghai Inst Microsyst & Informat Technol, State Key Lab Funct Mat Informat, Shanghai 200050, Peoples R China 5.ShanghaiTech Univ, Sch Phys Sci & Technol, Shanghai 201210, Peoples R China 6.Chinese Acad Sci, Hefei Inst Phys Sci, High Magnet Field Lab, Hefei 230031, Peoples R China 7.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, 457 Zhongshan Rd, Dalian 116023, Peoples R China
推荐引用方式 GB/T 7714	Li, Na,Zhu, Yifeng,Jiao, Feng,et al. Steering the reaction pathway of syngas-to-light olefins with coordination unsaturated sites of ZnGaOx spinel[J]. NATURE COMMUNICATIONS,2022,13.
APA	Li, Na.,Zhu, Yifeng.,Jiao, Feng.,Pan, Xiulian.,Jiang, Qike.,...&Bao, Xinhe.(2022).Steering the reaction pathway of syngas-to-light olefins with coordination unsaturated sites of ZnGaOx spinel.NATURE COMMUNICATIONS,13.
MLA	Li, Na,et al."Steering the reaction pathway of syngas-to-light olefins with coordination unsaturated sites of ZnGaOx spinel".NATURE COMMUNICATIONS 13(2022).