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Nano Research 2021, 14(7): 2353-2362 https://doi.org/10.1007/s12274-020-3234-6
Research Article | Issue | Published: 05 July 2021

Tuning the dual-active sites of ZIF-67 derived porous nanomaterials for boosting oxygen catalysis and rechargeable Zn-air batteries

Show Author's Information Zeyi Zhang1,§,  Yangyang Tan1,§,  Tang Zeng1,  Liyue Yu1,  Runzhe Chen1,  Niancai Cheng1( ),  Shichun Mu2( ),  Xueliang Sun3( )
College of Materials Science and Engineering, Fuzhou University, Fuzhou 350108, China
State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, China
Department of Mechanical and Materials Engineering, University of Western Ontario, London, ON N6A 5B9, Canada

§ Zeyi Zhang and Yangyang Tan contributed equally to this work.

Keywords:
metal-organic frameworks, density functional theory (DFT), Zn-air batteries, dual-active sites, bifunctional oxygen electrocatalysts
Topics:
Catalyst activityElectrolytic reduction MetalsNanocrystalsNanostructured materialsOrganic frameworks OrganometallicsOxygenOxygen reduction reaction Platinum compoundsRuthenium compoundsSodium Borohydride
Cite this article:
Zhang Z, Tan Y, Zeng T, et al. Tuning the dual-active sites of ZIF-67 derived porous nanomaterials for boosting oxygen catalysis and rechargeable Zn-air batteries. Nano Research, 2021, 14(7): 2353-2362. https://doi.org/10.1007/s12274-020-3234-6
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Abstract Full text Electronic supplementary material About this article

The rational control of the active site of metal-organic frameworks (MOFs) derived nanomaterials is essential to build efficient bifunctional oxygen reduction/evolution reaction (ORR/OER) catalysts. Accordingly, through designing and constructing a Co3O4-Co heterostructure embedded in Co, N co-doped carbon polyhedra derived (Co3O4-Co@NC) from the in-situ compositions of ZIF-67 and cobalt nanocrystals synthesized by the strategy of in-situ NaBH4 reduction, the dual-active site (Co3O4-Co and Co-Nx) is synchronously realized in a MOFs derived nanomaterials. The formed Co3O4-Co@NC shows excellent bifunctional electrocatalytic activity with ultra-small potential gap (ΔE = Ej=10 (OER) - E1/2 (ORR)) of 0.72 V, which surpasses the commercial Pt/C and RuO2 catalysts. The theory calculation results reveal that the excellent bifunctional electrocatalytic activity can be attributed to the charge redistribution of Co of Co-Nx induced by the synergistic effects of well-tuned active sites of Co3O4-Co nanoparticle and Co-Nx, thus optimizing the rate-determining step of the desorption of O2* intermediate in ORR and OH* intermediate in OER. The rechargeable Zn-air batteries with our bifunctional catalysts exhibit superior performance as well as high cycling stability. This simple-effective optimization strategy offers prospects for tuning the active site of MOF derived bifunctional catalyst in electrochemical energy devices.


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About this article

Tuning the dual-active sites of ZIF-67 derived porous nanomaterials for boosting oxygen catalysis and rechargeable Zn-air batteries

Show Author's information Zeyi Zhang1,§, Yangyang Tan1,§, Tang Zeng1, Liyue Yu1, Runzhe Chen1, Niancai Cheng1( ), Shichun Mu2( ), Xueliang Sun3( )
College of Materials Science and Engineering, Fuzhou University, Fuzhou 350108, China
State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, China
Department of Mechanical and Materials Engineering, University of Western Ontario, London, ON N6A 5B9, Canada

§ Zeyi Zhang and Yangyang Tan contributed equally to this work.

Abstract

The rational control of the active site of metal-organic frameworks (MOFs) derived nanomaterials is essential to build efficient bifunctional oxygen reduction/evolution reaction (ORR/OER) catalysts. Accordingly, through designing and constructing a Co3O4-Co heterostructure embedded in Co, N co-doped carbon polyhedra derived (Co3O4-Co@NC) from the in-situ compositions of ZIF-67 and cobalt nanocrystals synthesized by the strategy of in-situ NaBH4 reduction, the dual-active site (Co3O4-Co and Co-Nx) is synchronously realized in a MOFs derived nanomaterials. The formed Co3O4-Co@NC shows excellent bifunctional electrocatalytic activity with ultra-small potential gap (ΔE = Ej=10 (OER) - E1/2 (ORR)) of 0.72 V, which surpasses the commercial Pt/C and RuO2 catalysts. The theory calculation results reveal that the excellent bifunctional electrocatalytic activity can be attributed to the charge redistribution of Co of Co-Nx induced by the synergistic effects of well-tuned active sites of Co3O4-Co nanoparticle and Co-Nx, thus optimizing the rate-determining step of the desorption of O2* intermediate in ORR and OH* intermediate in OER. The rechargeable Zn-air batteries with our bifunctional catalysts exhibit superior performance as well as high cycling stability. This simple-effective optimization strategy offers prospects for tuning the active site of MOF derived bifunctional catalyst in electrochemical energy devices.

Keywords: metal-organic frameworks, density functional theory (DFT), Zn-air batteries, dual-active sites, bifunctional oxygen electrocatalysts

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Publication history
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Acknowledgements

Publication history

Received: 08 October 2020
Revised: 09 November 2020
Accepted: 10 November 2020
Published: 05 July 2021
Issue date: July 2021

Copyright

© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2021

Acknowledgements

The authors acknowledge support from the National Natural Science Foundation of China (No. 21875039), Minjiang Professorship (XRC-1677), Fujian province’s high level innovative and entrepreneurial talents (No. 50012709), the Open Project Program of the State Key Laboratory of Photocatalysis on Energy and Environment (No. SKLPEE-201814), Fuzhou University.

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