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https://hdl.handle.net/2440/124673
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Type: | Journal article |
Title: | Coordination tunes selectivity: two-electron oxygen reduction on high-loading Molybdenum single-atom catalysts |
Author: | Tang, C. Jiao, Y. Shi, B. Liu, J.-N. Xie, Z. Chen, X. Zhang, Q. Qiao, S. |
Citation: | Angewandte Chemie International Edition, 2020; 59(23):9171-9176 |
Publisher: | Wiley |
Issue Date: | 2020 |
ISSN: | 1433-7851 1521-3773 |
Statement of Responsibility: | Cheng Tang, Yan Jiao, Bingyang Shi, Jia‐Ning Liu, Zhenhua Xie, Xiao Chen, Qiang Zhang and Shi-Zhang Qiao |
Abstract: | Single-atom catalysts (SACs) have great potential in electrocatalysis. Their performance can be rationally optimized by tailoring the center metal atoms, adjacent coordinative dopants, and metal loading. However, it is still of great challenge due to the limited synthesis approach and insufficient understanding of the structure-property relation. Herein, we reported a new kind of Mo SAC with a unique O, S-dual coordination and a high metal loading over 10 wt%. The isolation feature and local environment was identified by high-angle annular dark-field scanning transmission electron microscopy and extended X-ray absorption fine structure. The obtained SACs can catalyze oxygen reduction reaction via 2e- pathway with a high H2O2 selectivity above 95% in 0.10 M KOH. The critical role of Mo single atoms and the coordination structure was revealed by both electrochemical tests and theoretical calculations. This work enriches the family of SACs and highlights the importance of local coordination, thus rendering new opportunities to tune the activity and selectivity in multi-electron electrocatalysis. |
Keywords: | Electrosynthesis local coordination oxygen reduction selectivity single atom catalyst |
Rights: | © 2020 Wiley‐VCH Verlag GmbH & Co. KGaA, Weinheim. |
DOI: | 10.1002/anie.202003842 |
Grant ID: | http://purl.org/au-research/grants/arc/DP160104866 http://purl.org/au-research/grants/arc/LP160100927 http://purl.org/au-research/grants/arc/DP190103472 http://purl.org/au-research/grants/arc/FL170100154 |
Published version: | http://dx.doi.org/10.1002/anie.202003842 |
Appears in Collections: | Aurora harvest 4 Chemical Engineering publications |
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