Evolution of Zn(II) single atom catalyst sites during the pyrolysis-induced transformation of ZIF-8 to N-doped carbons

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dc.contributor.author Wang, Qing en
dc.contributor.author Ina, T en
dc.contributor.author Chen, Wan-Ting en
dc.contributor.author Shang, L en
dc.contributor.author Sun, F en
dc.contributor.author Wei, Shanghai en
dc.contributor.author Sun-Waterhouse, Dongxiao en
dc.contributor.author Telfer, SG en
dc.contributor.author Zhang, T en
dc.contributor.author Waterhouse, Geoffrey en
dc.date.accessioned 2020-07-06T21:50:19Z en
dc.date.issued 2020-06-08 en
dc.identifier.uri http://hdl.handle.net/2292/51887 en
dc.description.abstract The 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 500–900 °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 °C. As the pyrolysis temperature increased in the range 600–900 °C, the Zn atoms moved closer to the N4 coordination plane. This subtle geometry change in the ZnN4 sites alters the electron density on the Zn atoms (formally Zn2+), strongly impacting the catalytic performance for the peroxidase-like decomposition of H2O2. The catalyst obtained at 800 °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. en
dc.relation.ispartofseries Science Bulletin en
dc.rights Items in ResearchSpace are protected by copyright, with all rights reserved, unless otherwise indicated. Previously published items are made available in accordance with the copyright policy of the publisher. en
dc.rights.uri https://researchspace.auckland.ac.nz/docs/uoa-docs/rights.htm en
dc.title Evolution of Zn(II) single atom catalyst sites during the pyrolysis-induced transformation of ZIF-8 to N-doped carbons en
dc.type Journal Article en
dc.identifier.doi 10.1016/j.scib.2020.06.020 en
dc.rights.holder Copyright: The author en
pubs.author-url https://www.sciencedirect.com/science/article/pii/S2095927320304187 en
dc.rights.accessrights http://purl.org/eprint/accessRights/RestrictedAccess en
pubs.subtype Article en
pubs.elements-id 804461 en
pubs.org-id Science en
pubs.org-id Chemistry en
pubs.record-created-at-source-date 2020-06-22 en
pubs.online-publication-date 2020-06-16 en

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