Understanding the Product Selectivity of Syngas Conversion on ZnO Surfaces with Complex Reaction Network and Structural Evolution
被引:42
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作者:
Fu, Xiaoyan
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Zhejiang Univ, Dept Chem, Hangzhou 310058, Peoples R China
Westlake Univ, Sch Sci, Hangzhou 310024, Peoples R China
Chinese Acad Sci, Dalian Natl Lab Clean Energy, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R ChinaZhejiang Univ, Dept Chem, Hangzhou 310058, Peoples R China
Fu, Xiaoyan
[1
,2
,3
]
Li, Jiayi
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机构:
Chinese Acad Sci, Dalian Natl Lab Clean Energy, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R ChinaZhejiang Univ, Dept Chem, Hangzhou 310058, Peoples R China
Li, Jiayi
[3
]
Long, Jun
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机构:
Zhejiang Univ, Dept Chem, Hangzhou 310058, Peoples R China
Westlake Univ, Sch Sci, Hangzhou 310024, Peoples R China
Chinese Acad Sci, Dalian Natl Lab Clean Energy, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R ChinaZhejiang Univ, Dept Chem, Hangzhou 310058, Peoples R China
Long, Jun
[1
,2
,3
]
Guo, Chenxi
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机构:
Chinese Acad Sci, Dalian Natl Lab Clean Energy, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R ChinaZhejiang Univ, Dept Chem, Hangzhou 310058, Peoples R China
Guo, Chenxi
[3
]
Xiao, Jianping
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Chinese Acad Sci, Dalian Natl Lab Clean Energy, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
Univ Chinese Acad Sci, Beijing 100049, Peoples R ChinaZhejiang Univ, Dept Chem, Hangzhou 310058, Peoples R China
Xiao, Jianping
[3
,4
]
机构:
[1] Zhejiang Univ, Dept Chem, Hangzhou 310058, Peoples R China
[2] Westlake Univ, Sch Sci, Hangzhou 310024, Peoples R China
[3] Chinese Acad Sci, Dalian Natl Lab Clean Energy, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
[4] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
Recently, a bifunctional oxide-zeolite (OX-ZEO) catalyst was widely studied experimentally, which can selectively convert syngas to light olefins. The performance of OX-ZEO is exceptional, while the mechanism is controversial. In this work, we have first developed an algorithm based on graph theory to establish a complete reaction network for syngas conversion to methanol, ketene, and methane. Combined with density functional theory (DFT) calculations, the activity and selectivity of syngas conversion over zinc oxide (ZnO) are systematically studied by a reaction phase diagram. The key intermediate, ketene, is observed in experiments, which has been first confirmed theoretically in this work. The evolution of ZnO surfaces is found to be a key factor of diverse product selectivity. It is found that methanol production is more favored over the ZnO surfaces with a low oxygen vacancy concentration. As the oxygen vacancy increases, the main product evolves gradually from methanol to ketene and finally to methane. Accordingly, the overall reaction activity increases too. Our prediction from the reaction phase diagram is finally verified by microkinetic modeling.
机构:
China Univ Min & Technol, Sch Mines, Dept Ind Engn, Xuzhou, Jiangsu, Peoples R ChinaChina Univ Min & Technol, Sch Mines, Dept Ind Engn, Xuzhou, Jiangsu, Peoples R China
Li, Yupeng
Ni, Yongbo
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China Univ Min & Technol, Sch Mines, Dept Ind Engn, Xuzhou, Jiangsu, Peoples R ChinaChina Univ Min & Technol, Sch Mines, Dept Ind Engn, Xuzhou, Jiangsu, Peoples R China
Ni, Yongbo
Zhang, Na
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China Univ Min & Technol, Sch Mines, Dept Ind Engn, Xuzhou, Jiangsu, Peoples R ChinaChina Univ Min & Technol, Sch Mines, Dept Ind Engn, Xuzhou, Jiangsu, Peoples R China
Zhang, Na
Liu, Qinming
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机构:
Univ Shanghai Sci & Technol, Dept Ind Engn, Business Sch, Shanghai, Peoples R ChinaChina Univ Min & Technol, Sch Mines, Dept Ind Engn, Xuzhou, Jiangsu, Peoples R China
Liu, Qinming
Cao, Jin
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机构:
Shanghai Highly Grp Co Ltd, Dept Sci & Dev, Shanghai, Peoples R ChinaChina Univ Min & Technol, Sch Mines, Dept Ind Engn, Xuzhou, Jiangsu, Peoples R China
机构:
Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA
BASF Corp, Calif Res Alliance CARA, Berkeley, CA 94720 USAUniv Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA
Maulana, Arifin Luthfi
Chen, Peng-Cheng
论文数: 0引用数: 0
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机构:
BASF Corp, Calif Res Alliance CARA, Berkeley, CA 94720 USA
Univ Calif Berkeley, Kavli Energy Nanosci Inst, Berkeley, CA 94720 USA
Fudan Univ, Dept Mat Sci, Shanghai 200438, Peoples R China
Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USAUniv Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA
Chen, Peng-Cheng
Shi, Zixiao
论文数: 0引用数: 0
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Cornell Univ, Dept Chem & Chem Biol, Ithaca, NY 14850 USA
Cornell Univ, Sch Appl & Engn Phys, Ithaca, NY 14850 USAUniv Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA
Shi, Zixiao
Yang, Yao
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Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA
Univ Calif Berkeley, Miller Inst Basic Res Sci, Berkeley, CA 94720 USAUniv Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA
Yang, Yao
Lizandara-Pueyo, Carlos
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BASF Corp, Calif Res Alliance CARA, Berkeley, CA 94720 USAUniv Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA
Lizandara-Pueyo, Carlos
Seeler, Fabian
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BASF SE, D-67056 Ludwigshafen Am Rhein, GermanyUniv Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA
Seeler, Fabian
Abruna, Hector D.
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Cornell Univ, Dept Chem & Chem Biol, Ithaca, NY 14850 USAUniv Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA
Abruna, Hector D.
Muller, David
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Cornell Univ, Sch Appl & Engn Phys, Ithaca, NY 14850 USA
Cornell Univ, Kavli Inst Cornell Nanoscale Sci, Ithaca, NY 14850 USAUniv Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA
Muller, David
Schierle-Arndt, Kerstin
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BASF SE, D-67056 Ludwigshafen Am Rhein, GermanyUniv Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA
Schierle-Arndt, Kerstin
Yang, Peidong
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机构:
Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA
BASF Corp, Calif Res Alliance CARA, Berkeley, CA 94720 USA
Univ Calif Berkeley, Kavli Energy Nanosci Inst, Berkeley, CA 94720 USA
Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USAUniv Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA
机构:
Univ Malaya, Nanotechnol & Catalysis Res Ctr NANOCAT, Inst Postgrad Studies, Leuel 3,Block A, Kuala Lumpur 50603, MalaysiaUniv Malaya, Nanotechnol & Catalysis Res Ctr NANOCAT, Inst Postgrad Studies, Leuel 3,Block A, Kuala Lumpur 50603, Malaysia
机构:
Inst Natl Rech Sci Energie Mat & Telecommun, Varennes, PQ J3X 1S2, Canada
Simon Fraser Univ, Dept Chem, Burnaby, BC VSA 1S6, Canada
Forschungszentrum Julich, Theory & Computat Energy Mat IEK 13, Inst Energy & Climate Res, D-52425 Julich, GermanyInst Natl Rech Sci Energie Mat & Telecommun, Varennes, PQ J3X 1S2, Canada
机构:
Forschungszentrum Julich, Theory & Computat Energy Mat IEK 13, Inst Energy & Climate Res, D-52425 Julich, GermanyInst Natl Rech Sci Energie Mat & Telecommun, Varennes, PQ J3X 1S2, Canada
Eikerling, Michael
Guay, Daniel
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Inst Natl Rech Sci Energie Mat & Telecommun, Varennes, PQ J3X 1S2, CanadaInst Natl Rech Sci Energie Mat & Telecommun, Varennes, PQ J3X 1S2, Canada