共 56 条
Atomic Insight into the Local Structure and Microenvironment of Isolated Co-Motifs in MFI Zeolite Frameworks for Propane Dehydrogenation
被引:121
作者:

Hu, Zhong-Pan
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机构:
Chinese Acad Sci, IChEM Collaborat Innovat Ctr Chem Energy Mat, Natl Engn Res Ctr Lower Carbon Catalysis Technol, Dalian Natl Lab Clean Energy,Dalian Inst Chem Phy, Dalian 116023, Peoples R China Chinese Acad Sci, IChEM Collaborat Innovat Ctr Chem Energy Mat, Natl Engn Res Ctr Lower Carbon Catalysis Technol, Dalian Natl Lab Clean Energy,Dalian Inst Chem Phy, Dalian 116023, Peoples R China

Qin, Gangqiang
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h-index: 0
机构:
Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
Univ Chinese Acad Sci, Beijing 100049, Peoples R China Chinese Acad Sci, IChEM Collaborat Innovat Ctr Chem Energy Mat, Natl Engn Res Ctr Lower Carbon Catalysis Technol, Dalian Natl Lab Clean Energy,Dalian Inst Chem Phy, Dalian 116023, Peoples R China

Han, Jingfeng
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机构:
Chinese Acad Sci, IChEM Collaborat Innovat Ctr Chem Energy Mat, Natl Engn Res Ctr Lower Carbon Catalysis Technol, Dalian Natl Lab Clean Energy,Dalian Inst Chem Phy, Dalian 116023, Peoples R China Chinese Acad Sci, IChEM Collaborat Innovat Ctr Chem Energy Mat, Natl Engn Res Ctr Lower Carbon Catalysis Technol, Dalian Natl Lab Clean Energy,Dalian Inst Chem Phy, Dalian 116023, Peoples R China

Zhang, Wenna
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机构:
Chinese Acad Sci, IChEM Collaborat Innovat Ctr Chem Energy Mat, Natl Engn Res Ctr Lower Carbon Catalysis Technol, Dalian Natl Lab Clean Energy,Dalian Inst Chem Phy, Dalian 116023, Peoples R China Chinese Acad Sci, IChEM Collaborat Innovat Ctr Chem Energy Mat, Natl Engn Res Ctr Lower Carbon Catalysis Technol, Dalian Natl Lab Clean Energy,Dalian Inst Chem Phy, Dalian 116023, Peoples R China

Wang, Nan
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机构:
Chinese Acad Sci, IChEM Collaborat Innovat Ctr Chem Energy Mat, Natl Engn Res Ctr Lower Carbon Catalysis Technol, Dalian Natl Lab Clean Energy,Dalian Inst Chem Phy, Dalian 116023, Peoples R China
Univ Chinese Acad Sci, Beijing 100049, Peoples R China Chinese Acad Sci, IChEM Collaborat Innovat Ctr Chem Energy Mat, Natl Engn Res Ctr Lower Carbon Catalysis Technol, Dalian Natl Lab Clean Energy,Dalian Inst Chem Phy, Dalian 116023, Peoples R China

Zheng, Yijun
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h-index: 0
机构:
Chinese Acad Sci, IChEM Collaborat Innovat Ctr Chem Energy Mat, Natl Engn Res Ctr Lower Carbon Catalysis Technol, Dalian Natl Lab Clean Energy,Dalian Inst Chem Phy, Dalian 116023, Peoples R China Chinese Acad Sci, IChEM Collaborat Innovat Ctr Chem Energy Mat, Natl Engn Res Ctr Lower Carbon Catalysis Technol, Dalian Natl Lab Clean Energy,Dalian Inst Chem Phy, Dalian 116023, Peoples R China

Jiang, Qike
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Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China Chinese Acad Sci, IChEM Collaborat Innovat Ctr Chem Energy Mat, Natl Engn Res Ctr Lower Carbon Catalysis Technol, Dalian Natl Lab Clean Energy,Dalian Inst Chem Phy, Dalian 116023, Peoples R China

Ji, Te
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机构:
Chinese Acad Sci, Shanghai Inst Appl Phys, SSRF, Shanghai 201800, Peoples R China Chinese Acad Sci, IChEM Collaborat Innovat Ctr Chem Energy Mat, Natl Engn Res Ctr Lower Carbon Catalysis Technol, Dalian Natl Lab Clean Energy,Dalian Inst Chem Phy, Dalian 116023, Peoples R China

Yuan, Zhong-Yong
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机构:
Nankai Univ, Sch Mat Sci & Engn, Minist Educ, Key Lab Adv Energy Mat Chem, Tianjin 300350, Peoples R China Chinese Acad Sci, IChEM Collaborat Innovat Ctr Chem Energy Mat, Natl Engn Res Ctr Lower Carbon Catalysis Technol, Dalian Natl Lab Clean Energy,Dalian Inst Chem Phy, Dalian 116023, Peoples R China

Xiao, Jianping
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Chinese Acad Sci, IChEM Collaborat Innovat Ctr Chem Energy Mat, Natl Engn Res Ctr Lower Carbon Catalysis Technol, Dalian Natl Lab Clean Energy,Dalian Inst Chem Phy, Dalian 116023, Peoples R China Chinese Acad Sci, IChEM Collaborat Innovat Ctr Chem Energy Mat, Natl Engn Res Ctr Lower Carbon Catalysis Technol, Dalian Natl Lab Clean Energy,Dalian Inst Chem Phy, Dalian 116023, Peoples R China

Wei, Yingxu
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机构:
Chinese Acad Sci, IChEM Collaborat Innovat Ctr Chem Energy Mat, Natl Engn Res Ctr Lower Carbon Catalysis Technol, Dalian Natl Lab Clean Energy,Dalian Inst Chem Phy, Dalian 116023, Peoples R China Chinese Acad Sci, IChEM Collaborat Innovat Ctr Chem Energy Mat, Natl Engn Res Ctr Lower Carbon Catalysis Technol, Dalian Natl Lab Clean Energy,Dalian Inst Chem Phy, Dalian 116023, Peoples R China

Liu, Zhongmin
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h-index: 0
机构:
Chinese Acad Sci, IChEM Collaborat Innovat Ctr Chem Energy Mat, Natl Engn Res Ctr Lower Carbon Catalysis Technol, Dalian Natl Lab Clean Energy,Dalian Inst Chem Phy, Dalian 116023, Peoples R China Chinese Acad Sci, IChEM Collaborat Innovat Ctr Chem Energy Mat, Natl Engn Res Ctr Lower Carbon Catalysis Technol, Dalian Natl Lab Clean Energy,Dalian Inst Chem Phy, Dalian 116023, Peoples R China
机构:
[1] Chinese Acad Sci, IChEM Collaborat Innovat Ctr Chem Energy Mat, Natl Engn Res Ctr Lower Carbon Catalysis Technol, Dalian Natl Lab Clean Energy,Dalian Inst Chem Phy, Dalian 116023, Peoples R China
[2] Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
[3] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
[4] Chinese Acad Sci, Shanghai Inst Appl Phys, SSRF, Shanghai 201800, Peoples R China
[5] Nankai Univ, Sch Mat Sci & Engn, Minist Educ, Key Lab Adv Energy Mat Chem, Tianjin 300350, Peoples R China
基金:
中国博士后科学基金;
中国国家自然科学基金;
关键词:
EFFICIENT EPOXIDATION;
METHANE HYDROXYLATION;
LIGHT ALKANES;
SITES;
CATALYSTS;
ACID;
OXIDATION;
BETA;
NANOPARTICLES;
HYDROCARBONS;
D O I:
10.1021/jacs.2c02636
中图分类号:
O6 [化学];
学科分类号:
0703 ;
摘要:
Embedding metal species into zeolite frameworks can create framework-bond metal sites in a confined microenvironment. The metals sitting in the specific T sites of zeolites and their crystalline surroundings are both committed to the interaction with the reactant, participation in the activation, and transient state achievement during the whole catalytic process. Herein, we construct isolated Co-motifs into purely siliceous MFI zeolite frameworks (Co-MFI) and reveal the location and microenvironment of the isolated Co active center in the MFI zeolite framework particularly beneficial for propane dehydrogenation (PDH). The isolated Co-motif with the distorted tetrahedral stnicture ({( SiO)(2)Co(HO-Si )(2)}, two Co-O-Si bonds, and two pseudo-bridging hydroxyls (Co center dot center dot center dot OH-Si) is located at T-1(7) and T-3(9) sites of the MFI zeolite. DFT calculations and deuterium-labeling reactions verify that the isolated Co-motif together with the MFI microenvironment collectively promotes the PDH reaction by providing an exclusive microenvironment to preactivate C3H8, polarizing the oxygen in Co-O-Si bonds to accept H* ({( SiO)CoH delta- (H delta+O-Si )(3)}), and a scaffold structure to stabilize the C3H7* intermediate. The Co-motif active center in Co-MFI goes through the dynamic evolutions and restoration in electronic states and coordination states in a continuous and repetitive way, which meets the requirements from the series of elementary steps in the PDH catalytic cycle and fulfills the successful catalysis like enzyme catalysis.
引用
收藏
页码:12127 / 12137
页数:11
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Nankai Univ, Sch Mat Sci & Engn, Natl Inst Adv Mat, Tianjin 300350, Peoples R China Nankai Univ, Sch Mat Sci & Engn, Natl Inst Adv Mat, Tianjin 300350, Peoples R China

Yuan, Zhong-Yong
论文数: 0 引用数: 0
h-index: 0
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Nankai Univ, Sch Mat Sci & Engn, Natl Inst Adv Mat, Tianjin 300350, Peoples R China
Nankai Univ, Key Lab Adv Energy Mat Chem, Minist Educ, Tianjin 300071, Peoples R China Nankai Univ, Sch Mat Sci & Engn, Natl Inst Adv Mat, Tianjin 300350, Peoples R China
[50]
Direct Mechanism of the First Carbon-Carbon Bond Formation in the Methanol-to-Hydrocarbons Process
[J].
Wu, Xinqiang
;
Xu, Shutao
;
Zhang, Wenna
;
Huang, Jindou
;
Li, Jinzhe
;
Yu, Bowen
;
Wei, Yingxu
;
Liu, Zhongmin
.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,
2017, 56 (31)
:9039-9043

Wu, Xinqiang
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机构:
Chinese Acad Sci, Natl Engn Lab Methanol Olefins, Dalian Natl Lab Clean Energy,iChEM, State Key Lab Cataysis,Dalian Inst Chem Phys, Dalian 116023, Peoples R China
Univ Chinese Acad Sci, Beijing 100049, Peoples R China Chinese Acad Sci, Natl Engn Lab Methanol Olefins, Dalian Natl Lab Clean Energy,iChEM, State Key Lab Cataysis,Dalian Inst Chem Phys, Dalian 116023, Peoples R China

Xu, Shutao
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h-index: 0
机构:
Chinese Acad Sci, Natl Engn Lab Methanol Olefins, Dalian Natl Lab Clean Energy,iChEM, State Key Lab Cataysis,Dalian Inst Chem Phys, Dalian 116023, Peoples R China Chinese Acad Sci, Natl Engn Lab Methanol Olefins, Dalian Natl Lab Clean Energy,iChEM, State Key Lab Cataysis,Dalian Inst Chem Phys, Dalian 116023, Peoples R China

Zhang, Wenna
论文数: 0 引用数: 0
h-index: 0
机构:
Chinese Acad Sci, Natl Engn Lab Methanol Olefins, Dalian Natl Lab Clean Energy,iChEM, State Key Lab Cataysis,Dalian Inst Chem Phys, Dalian 116023, Peoples R China
Univ Chinese Acad Sci, Beijing 100049, Peoples R China Chinese Acad Sci, Natl Engn Lab Methanol Olefins, Dalian Natl Lab Clean Energy,iChEM, State Key Lab Cataysis,Dalian Inst Chem Phys, Dalian 116023, Peoples R China

Huang, Jindou
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h-index: 0
机构:
Chinese Acad Sci, Natl Engn Lab Methanol Olefins, Dalian Natl Lab Clean Energy,iChEM, State Key Lab Cataysis,Dalian Inst Chem Phys, Dalian 116023, Peoples R China Chinese Acad Sci, Natl Engn Lab Methanol Olefins, Dalian Natl Lab Clean Energy,iChEM, State Key Lab Cataysis,Dalian Inst Chem Phys, Dalian 116023, Peoples R China

Li, Jinzhe
论文数: 0 引用数: 0
h-index: 0
机构:
Chinese Acad Sci, Natl Engn Lab Methanol Olefins, Dalian Natl Lab Clean Energy,iChEM, State Key Lab Cataysis,Dalian Inst Chem Phys, Dalian 116023, Peoples R China Chinese Acad Sci, Natl Engn Lab Methanol Olefins, Dalian Natl Lab Clean Energy,iChEM, State Key Lab Cataysis,Dalian Inst Chem Phys, Dalian 116023, Peoples R China

Yu, Bowen
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h-index: 0
机构:
Chinese Acad Sci, Natl Engn Lab Methanol Olefins, Dalian Natl Lab Clean Energy,iChEM, State Key Lab Cataysis,Dalian Inst Chem Phys, Dalian 116023, Peoples R China
Univ Chinese Acad Sci, Beijing 100049, Peoples R China Chinese Acad Sci, Natl Engn Lab Methanol Olefins, Dalian Natl Lab Clean Energy,iChEM, State Key Lab Cataysis,Dalian Inst Chem Phys, Dalian 116023, Peoples R China

Wei, Yingxu
论文数: 0 引用数: 0
h-index: 0
机构:
Chinese Acad Sci, Natl Engn Lab Methanol Olefins, Dalian Natl Lab Clean Energy,iChEM, State Key Lab Cataysis,Dalian Inst Chem Phys, Dalian 116023, Peoples R China Chinese Acad Sci, Natl Engn Lab Methanol Olefins, Dalian Natl Lab Clean Energy,iChEM, State Key Lab Cataysis,Dalian Inst Chem Phys, Dalian 116023, Peoples R China

Liu, Zhongmin
论文数: 0 引用数: 0
h-index: 0
机构:
Chinese Acad Sci, Natl Engn Lab Methanol Olefins, Dalian Natl Lab Clean Energy,iChEM, State Key Lab Cataysis,Dalian Inst Chem Phys, Dalian 116023, Peoples R China Chinese Acad Sci, Natl Engn Lab Methanol Olefins, Dalian Natl Lab Clean Energy,iChEM, State Key Lab Cataysis,Dalian Inst Chem Phys, Dalian 116023, Peoples R China