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 |