Abstract
Single-atom catalysts (SACs), as promising alternatives to Pt-based catalysts, suffer from the limited choice of center metals and low single-atom loading. Here, we report a pentacoordinated Zr-based SAC with nontrivial axial O ligands (denoted O−Zr−N−C) for oxygen reduction reaction (ORR). The O ligand downshifts the d-band center of Zr and confers Zr sites with stable local structure and proper adsorption capability for intermediates. Consequently, the ORR performance of O−Zr−N−C prominently surpasses that of commercial Pt/C, achieving a half-wave potential of 0.91 V vs. reversible hydrogen electrode and outstanding durability (92 % current retention after 130-hour operation). Moreover, the Zr site shows good resistance towards aggregation, enabling the synthesis of Zr-based SAC with high loading (9.1 wt%). With the high-loading catalyst, the zinc-air battery (ZAB) delivers a record-high power density of 324 mW cm−2 among those of SAC-based ZABs.
| Original language | English |
|---|---|
| Article number | e202209746 |
| Journal | Angewandte Chemie - International Edition |
| Volume | 61 |
| Issue number | 36 |
| DOIs | |
| Publication status | Published - 2022 Sept 5 |
Bibliographical note
Funding Information:This work was financially supported by European Union's Horizon 2020 research and innovation programme (GrapheneCore3 881603), Sächsisches Staatsministerium für Wissenschaft und Kunst (Sonderzuweisung zur Unterstützung profilbestimmender Struktureinheiten), German Research Foundation (DFG) within the Cluster of Excellence, and CRC 1415 (grant no. 417590517). X.W. gratefully acknowledges funding from China Scholarship Council. The authors acknowledge the use of the facilities in the Dresden Center for Nanoanalysis at the Technische Universität Dresden, the beamline B18 at Diamond Light Source (Didcot, England), and the Center for Information Services and High-Performance Computing (ZIH) at TU Dresden for generous allocations of compute resources. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. AC02-06CH11357. The authors also thank Dongqi Li, Qiongqiong Lu, Peng Chen, Boya Sun, Junjie Wang, and Dr. Maximilian Springer for the insightful discussions. Open Access funding enabled and organized by Projekt DEAL.
Funding Information:
This work was financially supported by European Union's Horizon 2020 research and innovation programme (GrapheneCore3 881603), Sächsisches Staatsministerium für Wissenschaft und Kunst (Sonderzuweisung zur Unterstützung profilbestimmender Struktureinheiten), German Research Foundation (DFG) within the Cluster of Excellence, and CRC 1415 (grant no. 417590517). X.W. gratefully acknowledges funding from China Scholarship Council. The authors acknowledge the use of the facilities in the Dresden Center for Nanoanalysis at the Technische Universität Dresden, the beamline B18 at Diamond Light Source (Didcot, England), and the Center for Information Services and High‐Performance Computing (ZIH) at TU Dresden for generous allocations of compute resources. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. AC02‐06CH11357. The authors also thank Dongqi Li, Qiongqiong Lu, Peng Chen, Boya Sun, Junjie Wang, and Dr. Maximilian Springer for the insightful discussions. Open Access funding enabled and organized by Projekt DEAL.
Publisher Copyright:
© 2022 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.
All Science Journal Classification (ASJC) codes
- Catalysis
- Chemistry(all)