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Title: Regulating the spatial distribution of metal nanoparticles within metal-organic frameworks to enhance catalytic efficiency

Abstract

Composites incorporating metal nanoparticles (MNPs) within metal-organic frameworks (MOFs) have broad applications in many fields. However, the controlled spatial distribution of the MNPs within MOFs remains a challenge for addressing key issues in catalysis, for example, the efficiency of catalysts due to the limitation of molecular diffusion within MOF channels. We report a facile strategy that enables MNPs to be encapsulated into MOFs with controllable spatial localization by using metal oxide both as support to load MNPs and as a sacrificial template to grow MOFs. This strategy is versatile to a variety of MNPs and MOF crystals. By localizing the encapsulated MNPs closer to the surface of MOFs, the resultant MNPs@MOF composites not only exhibit effective selectivity derived from MOF cavities, but also enhanced catalytic activity due to the spatial regulation of MNPs as close as possible to the MOF surface.

Authors:
 [1];  [1];  [1];  [2];  [3];  [1];  [1];  [1];  [4];  [1];  [2]; ORCiD logo [3]
+ Show Author Affiliations
  1. Beijing Univ. of Chemical Technology (China). State Key Lab. of Chemical Resource Engineering
  2. Nanjing Univ. of Technology (China). Key Lab. of Flexible Electronics (KLOFE), Inst. of Advanced Materials (IAM) and Jiangsu National Synergetic Innovation Center for Advanced Materials (SICAM)
  3. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
  4. Argonne National Lab. (ANL), Argonne, IL (United States). X-Ray Science Division
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); National Natural Science Foundation of China (NSFC); Beijing Nova Program; Fundamental Research Funds for the Central Univ. (China); National Basic Research Program of China; Nanjing Tech Univ. (China); Central Committee of the Communist Party of China (CPC)
OSTI Identifier:
1439872
Grant/Contract Number:  
AC02-06CH11357; 21271019; 21574065; 21504043; 21604038; Z121103002512023; YS1406; IRT1205; 2014CB932104; 2015CB932200; 21625401; BK20140044; BK20160975
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 8; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Metal–organic frameworks; Nanoparticles; Organic–inorganic nanostructures

Citation Formats

Yang, Qiu, Liu, Wenxian, Wang, Bingqing, Zhang, Weina, Zeng, Xiaoqiao, Zhang, Cong, Qin, Yongji, Sun, Xiaoming, Wu, Tianpin, Liu, Junfeng, Huo, Fengwei, and Lu, Jun. Regulating the spatial distribution of metal nanoparticles within metal-organic frameworks to enhance catalytic efficiency. United States: N. p., 2017. Web. doi:10.1038/ncomms14429.
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Yang, Qiu, Liu, Wenxian, Wang, Bingqing, Zhang, Weina, Zeng, Xiaoqiao, Zhang, Cong, Qin, Yongji, Sun, Xiaoming, Wu, Tianpin, Liu, Junfeng, Huo, Fengwei, & Lu, Jun. Regulating the spatial distribution of metal nanoparticles within metal-organic frameworks to enhance catalytic efficiency. United States. https://doi.org/10.1038/ncomms14429
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Yang, Qiu, Liu, Wenxian, Wang, Bingqing, Zhang, Weina, Zeng, Xiaoqiao, Zhang, Cong, Qin, Yongji, Sun, Xiaoming, Wu, Tianpin, Liu, Junfeng, Huo, Fengwei, and Lu, Jun. Tue . "Regulating the spatial distribution of metal nanoparticles within metal-organic frameworks to enhance catalytic efficiency". United States. https://doi.org/10.1038/ncomms14429. https://www.osti.gov/servlets/purl/1439872.
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@article{osti_1439872,
title = {Regulating the spatial distribution of metal nanoparticles within metal-organic frameworks to enhance catalytic efficiency},
author = {Yang, Qiu and Liu, Wenxian and Wang, Bingqing and Zhang, Weina and Zeng, Xiaoqiao and Zhang, Cong and Qin, Yongji and Sun, Xiaoming and Wu, Tianpin and Liu, Junfeng and Huo, Fengwei and Lu, Jun},
abstractNote = {Composites incorporating metal nanoparticles (MNPs) within metal-organic frameworks (MOFs) have broad applications in many fields. However, the controlled spatial distribution of the MNPs within MOFs remains a challenge for addressing key issues in catalysis, for example, the efficiency of catalysts due to the limitation of molecular diffusion within MOF channels. We report a facile strategy that enables MNPs to be encapsulated into MOFs with controllable spatial localization by using metal oxide both as support to load MNPs and as a sacrificial template to grow MOFs. This strategy is versatile to a variety of MNPs and MOF crystals. By localizing the encapsulated MNPs closer to the surface of MOFs, the resultant MNPs@MOF composites not only exhibit effective selectivity derived from MOF cavities, but also enhanced catalytic activity due to the spatial regulation of MNPs as close as possible to the MOF surface.},
doi = {10.1038/ncomms14429},
journal = {Nature Communications},
number = ,
volume = 8,
place = {United States},
year = {Tue Feb 14 00:00:00 EST 2017},
month = {Tue Feb 14 00:00:00 EST 2017}
}
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https://doi.org/10.1038/ncomms14429
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    journal, January 2018

    • Franco, Chris H. J.; Chagas, Poliane; Caldeira, Gabriela S.
    • Dalton Transactions, Vol. 47, Issue 32
    • DOI: 10.1039/c8dt01803k

    Hierarchical branched platinum–copper tripods as highly active and stable catalysts
    journal, January 2018

    In situ synthesized low-PtCo@porous carbon catalyst for highly efficient hydrogen evolution
    journal, January 2019

    • Qin, Yudao; Han, Xiaoyu; Gadipelli, Srinivas
    • Journal of Materials Chemistry A, Vol. 7, Issue 11
    • DOI: 10.1039/c8ta12263f

    High stability of ultra-small and isolated gold nanoparticles in metal–organic framework materials
    journal, January 2019

    • Cure, Jérémy; Mattson, Eric; Cocq, Kévin
    • Journal of Materials Chemistry A, Vol. 7, Issue 29
    • DOI: 10.1039/c8ta12334a

    Atomic-layer-deposition-formed sacrificial template for the construction of an MIL-53 shell to increase selectivity of hydrogenation reactions
    journal, January 2019

    • Xu, Tiantian; Sun, Kai; Gao, Daowei
    • Chemical Communications, Vol. 55, Issue 53
    • DOI: 10.1039/c9cc02727k

    Core–shell-type ZIF-8@ZIF-67@POM hybrids as efficient electrocatalysts for the oxygen evolution reaction
    journal, January 2019

    • Wang, Yan; Wang, Yuyin; Zhang, Li
    • Inorganic Chemistry Frontiers, Vol. 6, Issue 9
    • DOI: 10.1039/c9qi00798a

    Mechanochemistry-assisted encapsulation of metal nanoparticles in MOF matrices via a sacrificial strategy
    journal, January 2019

    • Li, Xiaochen; Zhang, Zhihua; Xiao, Weiming
    • Journal of Materials Chemistry A, Vol. 7, Issue 24
    • DOI: 10.1039/c9ta03578h

    Zeolitic-imidazolate frameworks derived Pt-free counter electrodes for high-performance quantum dot-sensitized solar cells
    journal, May 2018

    • Xu, Wenjiao; Sun, Yuxiu; Ding, Bin
    • Royal Society Open Science, Vol. 5, Issue 5
    • DOI: 10.1098/rsos.180335

    Recent Innovation of Metal-Organic Frameworks for Carbon Dioxide Photocatalytic Reduction
    journal, December 2019

    • Kidanemariam, Alemayehu; Lee, Jiwon; Park, Juhyun
    • Polymers, Vol. 11, Issue 12
    • DOI: 10.3390/polym11122090

    Engineering channels of metal–organic frameworks to enhance catalytic selectivity
    journal, January 2019

    • Liu, Ye; Shen, Yu; Zhang, Weina
    • Chemical Communications, Vol. 55, Issue 78
    • DOI: 10.1039/c9cc06061h

    Multi-shelled Hollow Metal-Organic Frameworks
    journal, March 2017

    • Liu, Wenxian; Huang, Jijiang; Yang, Qiu
    • Angewandte Chemie International Edition, Vol. 56, Issue 20
    • DOI: 10.1002/anie.201701604

    Structural Engineering of Low‐Dimensional Metal–Organic Frameworks: Synthesis, Properties, and Applications
    journal, April 2019

    Zeolitic-imidazolate frameworks derived Pt-free counter electrodes for high-performance quantum dot-sensitized solar cells
    journal, May 2018

    • Xu, Wenjiao; Sun, Yuxiu; Ding, Bin
    • Royal Society Open Science, Vol. 5, Issue 5
    • DOI: 10.1098/rsos.180335

    Recent Innovation of Metal-Organic Frameworks for Carbon Dioxide Photocatalytic Reduction
    journal, December 2019

    • Kidanemariam, Alemayehu; Lee, Jiwon; Park, Juhyun
    • Polymers, Vol. 11, Issue 12
    • DOI: 10.3390/polym11122090
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