journal article·2022-09

Molecularly Distorted Local Structure in Bi2CuO4 Oxide to Stabilize Lattice Oxygen for Efficient Formate Electrosynthesis

Yuanwei Liu, Zhen Xin Lou, Xuefeng Wu, Bingbao Mei, Jiacheng Chen, Jia Yue Zhao, Ji Li, Hai Yang Yuan, Minghui Zhu, Sheng Dai, Chenghua Sun, Peng Fei Liu, Zheng Jiang, Hua Gui Yang

Advanced Materials· Volume 34· Issue 39
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Abstract

Abstract The electrochemical CO2 reduction reaction (CO2RR) provides an economically feasible way for converting green energy into valuable chemical feedstocks and fuels. Great progress has been achieved in the understanding and synthesis of oxidized‐based precatalysts; however, their dynamical changes of local structure under operando conditions still hinder their further applications. Here a molecularly distorted Bi2CuO4 precatalyst for efficient CO2‐to‐formate conversion is reported. X‐ray absorption fine structure (XAFS) results and theoretical calculations suggest that the distorted structure with molecularly like [CuO4]6− unit rotation is more conducive to the structural stability of the sample. Operando XAFS and scanning transmission electron microscopy (STEM) results prove that quite a bit of lattice oxygen can remain in the distorted sample after CO2RR. Electrochemical measurements of the distorted sample show an excellent activity and selectivity with a high formate partial current density of 194.6 mA cm−2 at an extremely low overpotential of −400 mV. Further in situ surface‐enhanced infrared absorption spectroscopy (SEIRAS) and density functional theory (DFT) calculations illustrate that the retained oxygen can optimize the adsorption of *OCHO intermediate for the enhanced CO2RR performance.
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Research context

OpenAlex topics: CO2 Reduction Techniques and Catalysts · Advanced battery technologies research · Ionic liquids properties and applications

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

Affiliations

Key Laboratory for Ultrafine Materials of Ministry of Education Shanghai Engineering Research Center of Hierarchical Nanomaterials School of Materials Science and Engineering East China University of Science and Technology Shanghai 200237 China

Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics Chinese Academy of Sciences Shanghai 201204 China

Shanghai Synchrotron Radiation Facility Shanghai Advanced Research Institute Chinese Academy of Sciences Shanghai 201204 China

State Key Laboratory of Chemical Engineering School of Chemical Engineering East China University of Science and Technology Shanghai 200237 China

Key Laboratory for Advanced Materials and Feringa Nobel Prize Scientist Joint Research Center Institute of Fine Chemicals School of Chemistry & Molecular Engineering East China University of Science and Technology Shanghai 200237 China

Department of Chemistry and Biotechnology Center for Translational Atomaterials Swinburne University of Technology Hawthorn Victoria 3122 Australia

Funding

National Natural Science Foundation of China · Science and Technology Commission of Shanghai Municipality

References (51)

Show source-provided references
1. 10.1126/science.aav350610.1126/science.aav3506 ↗
2. 10.1039/C9EE02410G10.1039/C9EE02410G ↗
3. 10.1038/s41929-019-0388-210.1038/s41929-019-0388-2 ↗
4. 10.1038/s41929-019-0266-y10.1038/s41929-019-0266-y ↗
5. 10.1016/j.joule.2019.05.00710.1016/j.joule.2019.05.007 ↗
6. 10.1038/s41467-021-20961-710.1038/s41467-021-20961-7 ↗
7. 10.1021/jacs.1c0344310.1021/jacs.1c03443 ↗
8. 10.1021/acscatal.0c0029710.1021/acscatal.0c00297 ↗
9. 10.1021/acs.chemrev.0c0045410.1021/acs.chemrev.0c00454 ↗
10. 10.1039/C8EE03781G10.1039/C8EE03781G ↗
11. 10.1002/anie.20191483110.1002/anie.201914831 ↗
12. 10.1073/pnas.170240511410.1073/pnas.1702405114 ↗
13. 10.1021/jacs.9b1112610.1021/jacs.9b11126 ↗
14. 10.1038/s41560-018-0308-810.1038/s41560-018-0308-8 ↗
15. 10.1002/adma.20130268510.1002/adma.201302685 ↗
16. 10.1021/ja408329q10.1021/ja408329q ↗
17. 10.1038/s41467-018-07678-w10.1038/s41467-018-07678-w ↗
18. 10.1038/s41560-020-0594-910.1038/s41560-020-0594-9 ↗
19. 10.1021/jacs.0c0169910.1021/jacs.0c01699 ↗
20. 10.1073/pnas.201264911810.1073/pnas.2012649118 ↗
21. 10.1016/j.joule.2017.09.00310.1016/j.joule.2017.09.003 ↗
22. 10.1038/s41565-020-00823-x10.1038/s41565-020-00823-x ↗
23. 10.1038/s41893-021-00739-x10.1038/s41893-021-00739-x ↗
24. 10.1016/j.jallcom.2009.02.06810.1016/j.jallcom.2009.02.068 ↗
25. 10.1007/s11356-015-4946-010.1007/s11356-015-4946-0 ↗
26. Chou C. H. · Chin. J. Phys. · 1991 · 29 · 263
27. 10.1016/j.jssc.2013.04.00810.1016/j.jssc.2013.04.008 ↗
28. 10.1103/PhysRevB.39.154110.1103/PhysRevB.39.1541 ↗
29. 10.1063/1.477358310.1063/1.4773583 ↗
30. 10.1021/acs.jpcc.0c0845510.1021/acs.jpcc.0c08455 ↗
31. 10.1021/acs.chemmater.0c0393010.1021/acs.chemmater.0c03930 ↗
32. 10.1063/1.218945010.1063/1.2189450 ↗
33. 10.1088/0953-8984/21/34/34550110.1088/0953-8984/21/34/345501 ↗
34. 10.1038/s41524-021-00664-910.1038/s41524-021-00664-9 ↗
35. 10.1038/s41467-019-10819-410.1038/s41467-019-10819-4 ↗
36. 10.1038/s41467-020-17403-110.1038/s41467-020-17403-1 ↗
37. 10.1038/s41467-021-25573-910.1038/s41467-021-25573-9 ↗
38. 10.1002/anie.20181053810.1002/anie.201810538 ↗
39. 10.1002/anie.20200557710.1002/anie.202005577 ↗
40. 10.1002/anie.20200065710.1002/anie.202000657 ↗
41. 10.1002/anie.20200831610.1002/anie.202008316 ↗
42. 10.1002/anie.20201434110.1002/anie.202014341 ↗
43. 10.1039/D1EE01495A10.1039/D1EE01495A ↗
44. 10.1002/adma.20180285810.1002/adma.201802858 ↗
45. 10.1002/adma.20200837310.1002/adma.202008373 ↗
46. 10.1016/j.physb.2018.04.03910.1016/j.physb.2018.04.039 ↗
47. 10.1021/acs.jpcc.8b0959810.1021/acs.jpcc.8b09598 ↗
48. 10.1002/anie.20201465510.1002/anie.202014655 ↗
49. 10.1093/nsr/nwaa18710.1093/nsr/nwaa187 ↗
50. 10.1016/j.apcatb.2020.11862510.1016/j.apcatb.2020.118625 ↗
51. 10.1002/anie.20201571310.1002/anie.202015713 ↗