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

文献类型：期刊论文

作者Li, Na1,6,7; Zhu, Yifeng6; Jiao, Feng1,6,7; Pan, Xiulian1,6,7; Jiang, Qike1; Cai, Jun2,5,7; Li, Yifan4,6; Tong, Wei3; Xu, Changqi1; Qu, Shengcheng1
刊名NATURE COMMUNICATIONS
出版日期2022-05-18
卷号13
DOI10.1038/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.
WOS关键词HIGHLY SELECTIVE CONVERSION ; SINGLE-CRYSTALLINE ; CARBON-DIOXIDE ; PARAMAGNETIC-RESONANCE ; OPTICAL-PROPERTIES ; METHANOL SYNTHESIS ; CO HYDROGENATION ; ZINC-OXIDE ; FT-IR ; ZNGA2O4
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研究方向Science & Technology - Other Topics
语种英语
WOS记录号WOS:000798996800008
出版者NATURE PORTFOLIO
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
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.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, 457 Zhongshan Rd, Dalian 116023, Peoples R China
2.Chinese Acad Sci, Shanghai Inst Microsyst & Informat Technol, State Key Lab Funct Mat Informat, Shanghai 200050, Peoples R China
3.Chinese Acad Sci, Hefei Inst Phys Sci, High Magnet Field Lab, Hefei 230031, Peoples R China
4.Univ Sci & Technol China, Dept Chem Phys, Jinzhai Rd 96, Hefei 230026, Peoples R China
5.ShanghaiTech Univ, Sch Phys Sci & Technol, Shanghai 201210, Peoples R China
6.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, 457 Zhongshan Rd, Dalian 116023, Peoples R China
7.Univ Chinese Acad Sci, Beijing 100049, 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).

入库方式： OAI收割

来源：合肥物质科学研究院

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