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Evolution of Zn(II) single atom catalyst sites during the pyrolysis-induced transformation of ZIF-8 to N-doped carbons
Wang, Q; Ina, T; Chen, WT; Shang, L; Sun, FF; Wei, SH; Sun-Waterhouse, D; Telfer, SG; Zhang, TR; Waterhouse, GIN
2020
Source PublicationSCIENCE BULLETIN
ISSN2095-9273
Volume65Issue:20Pages:1743-1751
Subtype期刊论文
AbstractThe pyrolysis of zeolitic imidazolate frameworks (ZIFs) is becoming a popular approach for the synthesis of catalysts comprising porphyrin-like metal single atom catalysts (SACs) on N-doped carbons (M-N-C). Understanding the structural evolution of M-N-C as a function of ZIF pyrolysis temperature is important for realizing high performance catalysts. Herein, we report a detailed investigation of the evolution of Zn single atom catalyst sites during the pyrolysis of ZIF-8 at temperatures ranging from 500 to 900 degrees C. Results from Zn L-edge and Zn K-edge X-ray absorption spectroscopy studies reveal that tetrahedral ZnN4 centers in ZIF-8 transform to porphyrin-like ZnN4 centers supported on N-doped carbon at temperatures as low as 600 degrees C. As the pyrolysis temperature increased in the range 600-900 degrees C, the Zn atoms moved closer to the N-4 coordination plane. This subtle geometry change in the ZnN4 sites alters the electron density on the Zn atoms (formally Zn-2(+)), strongly impacting the catalytic performance for the peroxidase-like decomposition of H2O2. The catalyst obtained at 800 degrees C (Zn-N-C-800) offered the best performance for H2O2 decomposition. This work provides valuable new insights about the evolution of porphyrin-like single metal sites on N-doped carbons from ZIF precursors and the factors influencing SAC activity. (C) 2020 Science China Press. Published by Elsevier B.V. and Science China Press. All rights reserved.
KeywordOXYGEN REDUCTION EFFICIENT ELECTROREDUCTION COORDINATION ELECTROCATALYSTS GRAPHENE
DOI10.1016/j.scib.2020.06.020
Indexed BySCI ; EI
Language英语
Citation statistics
Cited Times:20[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.sinap.ac.cn/handle/331007/32865
Collection中科院上海应用物理研究所2011-2020年
Affiliation1.Univ Auckland, Sch Chem Sci, Auckland 1142, New Zealand
2.Japan Synchrotron Radiat Res Inst, Res & Utilizat Div, Kouto 6795148, Japan
3.Chinese Acad Sci, Tech Inst Phys & Chem, Key Lab Photochem Convers & Optoelect Mat, Beijing 100190, Peoples R China
4.Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China
5.Univ Auckland, Fac Engn, Dept Chem & Mat Engn, Auckland 1142, New Zealand
6.Massey Univ, MacDiarmid Inst Adv Mat & Nanotechnol, Palmerston North 4442, New Zealand
Recommended Citation
GB/T 7714
Wang, Q,Ina, T,Chen, WT,et al. Evolution of Zn(II) single atom catalyst sites during the pyrolysis-induced transformation of ZIF-8 to N-doped carbons[J]. SCIENCE BULLETIN,2020,65(20):1743-1751.
APA Wang, Q.,Ina, T.,Chen, WT.,Shang, L.,Sun, FF.,...&Waterhouse, GIN.(2020).Evolution of Zn(II) single atom catalyst sites during the pyrolysis-induced transformation of ZIF-8 to N-doped carbons.SCIENCE BULLETIN,65(20),1743-1751.
MLA Wang, Q,et al."Evolution of Zn(II) single atom catalyst sites during the pyrolysis-induced transformation of ZIF-8 to N-doped carbons".SCIENCE BULLETIN 65.20(2020):1743-1751.
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