journal article·2019-01-09Open access

Oxygen Electrocatalysis at MnIII–Ox–C Hybrid Heterojunction: An Electronic Synergy or Cooperative Catalysis?

Kuang-Hsu Wu, Xing Huang, Hassan Tahini, Peter Kappen, Rui Huang, Xin Tan, Ling-Yun Jang, Yuxiao Ding, Sean C. Smith, Wei Qi, Ian R. Gentle, Dang-Sheng Su, Rose Amal, Da-Wei Wang

Abstract

The interface at the metal oxide–carbon hybrid heterojunction is the source to the well-known “synergistic effect” in catalysis. Understanding the structure–function properties is key for designing more advanced catalyst–support systems. Using a model MnIII–Ox single-layer catalyst on carbon, we herein report a full elucidation to the catalytic synergism at the hybrid heterojunction in the oxygen reduction reaction (ORR). The successful fabrication of the single-layer catalyst from bottom-up is fully characterized by the X-ray absorption fine structure and high-resolution transmission electron microscopy. For oxygen electrocatalysis over this model hybrid heterostructure, our results, from both theory and experiment, show that the synergistic ORR truly undergoes a cooperated two-step electrocatalysis with catalytic promotion (ΔEonset = 60 mV) near the heterojunction and over the single-layer catalyst through an interfacial electronic interplay, rather than an abstruse transition towards a one-step dissociative pathway. Finally, we report a superior peroxide-reducing activity of 432.5 mA cm–2 mg(M)–1 over the MnIII–Ox single-layer.
Source: openalex_inverted_index · Quality: baseline

Research context

OpenAlex topics: Electrocatalysts for Energy Conversion · Catalytic Processes in Materials Science · CO2 Reduction Techniques and Catalysts

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

PartCat Research Group, School of Chemical Engineering, The University of New South Wales, Sydney, NSW 2052, Australia

School of Chemistry and Molecular Biosciences, The University of Queensland, Brisbane, QLD 4072, Australia

AC Department, Fritz-Haber Institute of Max-Planck Society, 14195 Berlin, Germany

Integrated Materials Design Laboratory, Research School of Physics and Engineering, The Australian National University, Canberra, ACT 2601, Australia

Synchrotron Light Source, Australian Synchrotron, Melbourne, VIC 3168, Australia

Institute of Metal Research, Chinese Academy of Sciences, Shenyang, Liaoning 110016, China

Research Division, National Synchrotron Radiation Research Centre, Hsinchu 300, Taiwan

Max-Planck Institute for Chemical Energy Conversion, 45470 Mülheim, Germany

Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, Liaoning 116023, China

Funding

Australian Research Council · University of Queensland · University of New South Wales · Chinese Academy of Sciences

References (30)

Show source-provided references
1. 10.1021/ar300361m10.1021/ar300361m ↗
2. 10.1021/acscatal.6b0153410.1021/acscatal.6b01534 ↗
3. 10.1002/anie.20130924810.1002/anie.201309248 ↗
4. 10.1039/C3CS60389J10.1039/C3CS60389J ↗
5. 10.1021/ja308992310.1021/ja3089923 ↗
6. 10.1038/nature1645510.1038/nature16455 ↗
7. 10.1021/ja305623m10.1021/ja305623m ↗
8. 10.1021/acsnano.8b0105610.1021/acsnano.8b01056 ↗
9. 10.1038/nmat308710.1038/nmat3087 ↗
10. 10.1021/ja210924t10.1021/ja210924t ↗
11. 10.1002/cssc.20150037210.1002/cssc.201500372 ↗
12. 10.1021/nl202907810.1021/nl2029078 ↗
13. 10.1039/c2cc17537a10.1039/c2cc17537a ↗
14. 10.1002/ange.20120615210.1002/ange.201206152 ↗
15. 10.1038/srep4363810.1038/srep43638 ↗
16. 10.1002/celc.20180008610.1002/celc.201800086 ↗
17. 10.1039/c2ee23844f10.1039/c2ee23844f ↗
18. 10.1002/celc.20170121510.1002/celc.201701215 ↗
19. 10.1016/j.carbon.2014.09.06010.1016/j.carbon.2014.09.060 ↗
20. 10.2138/am.2012.390310.2138/am.2012.3903 ↗
21. 10.2138/am-1998-3-41410.2138/am-1998-3-414 ↗
22. Radovic L. R. · 2010 · 203
23. 10.1002/celc.20150048010.1002/celc.201500480 ↗
24. 10.1007/s10008-008-0670-810.1007/s10008-008-0670-8 ↗
25. 10.1107/S090904950501271910.1107/S0909049505012719 ↗
26. 10.1107/S090904950001696410.1107/S0909049500016964 ↗
27. 10.1103/PhysRevB.54.1116910.1103/PhysRevB.54.11169 ↗
28. 10.1103/PhysRevB.50.1795310.1103/PhysRevB.50.17953 ↗
29. 10.1103/PhysRevLett.77.386510.1103/PhysRevLett.77.3865 ↗
30. 10.1063/1.338234410.1063/1.3382344 ↗