journal article·2023-12Open access

Synthesis of 2H/fcc‐Heterophase AuCu Nanostructures for Highly Efficient Electrochemical CO2 Reduction at Industrial Current Densities

Xichen Zhou, An Zhang, Bo Chen, Shangqian Zhu, Yu Cui, Licheng Bai, Jinli Yu, Yiyao Ge, Qinbai Yun, Lujiang Li, Biao Huang, Lingwen Liao, Jiaju Fu, Qingbo Wa, Gang Wang, Zhiqi Huang, Long Zheng, Yi Ren, Siyuan Li, Guangyao Liu, Li Zhai, Zijian Li, Jiawei Liu, Ye Chen, Lu Ma, Chongyi Ling, Jinlan Wang, Zhanxi Fan, Yonghua Du, Minhua Shao, Hua Zhang

Advanced Materials· Volume 35· Issue 51

Abstract

Abstract Structural engineering of nanomaterials offers a promising way for developing high‐performance catalysts toward catalysis. However, the delicate modulation of thermodynamically unfavorable nanostructures with unconventional phases still remains a challenge. Here, the synthesis of hierarchical AuCu nanostructures is reported with hexagonal close‐packed (2H‐type)/face‐centered cubic (fcc) heterophase, high‐index facets, planar defects (e.g., stacking faults, twin boundaries, and grain boundaries), and tunable Cu content. The obtained 2H/fcc Au99Cu1 hierarchical nanosheets exhibit excellent performance for the electrocatalytic CO2 reduction to produce CO, outperforming the 2H/fcc Au91Cu9 and fcc Au99Cu1. The experimental results, especially those obtained by in‐situ differential electrochemical mass spectroscopy and attenuated total reflection Fourier‐transform infrared spectroscopy, suggest that the enhanced catalytic performance of 2H/fcc Au99Cu1 arises from the unconventional 2H/fcc heterophase, high‐index facets, planar defects, and appropriate alloying of Cu. Impressively, the 2H/fcc Au99Cu1 shows CO Faradaic efficiencies of 96.6% and 92.6% at industrial current densities of 300 and 500 mA cm−2, respectively, as well as good durability, placing it among the best CO2 reduction electrocatalysts for CO production. The atomically structural regulation based on phase engineering of nanomaterials (PEN) provides an avenue for the rational design and preparation of high‐performance electrocatalysts for various catalytic applications.
Source: crossref · Quality: baseline

Research context

OpenAlex topics: CO2 Reduction Techniques and Catalysts · Ammonia Synthesis and Nitrogen Reduction · Catalytic Processes in Materials Science

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

Affiliations

Department of Chemistry City University of Hong Kong Hong Kong China

Department of Chemical and Biological Engineering The Hong Kong University of Science and Technology Hong Kong China

School of Physics Southeast University Nanjing 211189 China

Materials Interfaces Center Shenzhen Institute of Advanced Technology Chinese Academy of Sciences Shenzhen 518057 China

Hong Kong Branch of National Precious Metals Material Engineering Research Center (NPMM) City University of Hong Kong Hong Kong China

Key Laboratory of Materials Physics Anhui Key Laboratory of Nanomaterials and Nanotechnology Institute of Solid State Physics Chinese Academy of Sciences Hefei 230031 China

Department of Chemistry The Chinese University of Hong Kong Hong Kong China

Center for Programmable Materials School of Materials Science and Engineering Nanyang Technological University Singapore 639798 Singapore

National Synchrotron Light Source II Brookhaven National Laboratory Upton NY 11973 USA

Shenzhen Research Institute City University of Hong Kong Shenzhen 518057 China

Energy Institute Hong Kong Branch of the Southern Marine Science and Engineering Guangdong Laboratory and Chinese National Engineering Research Center for Control & Treatment of Heavy Metal Pollution The Hong Kong University of Science and Technology Hong Kong China

Funding

City University of Hong Kong

References (55)

Show source-provided references
1. 10.1021/acs.chemrev.0c0045410.1021/acs.chemrev.0c00454 ↗
2. 10.1038/s41586-021-03870-z10.1038/s41586-021-03870-z ↗
3. 10.1126/science.abj998010.1126/science.abj9980 ↗
4. 10.1038/s41586-019-1603-710.1038/s41586-019-1603-7 ↗
5. 10.1021/acs.chemrev.6b0021110.1021/acs.chemrev.6b00211 ↗
6. 10.1038/ncomms594810.1038/ncomms5948 ↗
7. 10.1126/sciadv.abd664710.1126/sciadv.abd6647 ↗
8. 10.1021/acs.chemrev.7b0072710.1021/acs.chemrev.7b00727 ↗
9. 10.1038/s41929-019-0397-110.1038/s41929-019-0397-1 ↗
10. 10.1002/anie.20210283210.1002/anie.202102832 ↗
11. 10.1126/science.aax584310.1126/science.aax5843 ↗
12. 10.1038/s41929-020-00504-x10.1038/s41929-020-00504-x ↗
13. 10.1002/anie.20181142210.1002/anie.201811422 ↗
14. 10.1021/acs.chemrev.9b0022010.1021/acs.chemrev.9b00220 ↗
15. 10.1038/s41570-020-0173-410.1038/s41570-020-0173-4 ↗
16. 10.1126/science.aaw800710.1126/science.aaw8007 ↗
17. 10.1038/s41578-020-0183-310.1038/s41578-020-0183-3 ↗
18. 10.1038/ncomms129110.1038/ncomms1291 ↗
19. 10.1038/ncomms868410.1038/ncomms8684 ↗
20. 10.1038/s41586-021-04391-510.1038/s41586-021-04391-5 ↗
21. 10.1038/s41929-018-0072-y10.1038/s41929-018-0072-y ↗
22. 10.1002/adma.20190296410.1002/adma.201902964 ↗
23. 10.1021/jacs.1c1131310.1021/jacs.1c11313 ↗
24. 10.1038/s41467-020-17068-w10.1038/s41467-020-17068-w ↗
25. 10.1021/jacs.0c0946110.1021/jacs.0c09461 ↗
26. 10.1002/adma.20180323410.1002/adma.201803234 ↗
27. 10.1038/s41557-018-0012-010.1038/s41557-018-0012-0 ↗
28. 10.1021/acscatal.1c0333310.1021/acscatal.1c03333 ↗
29. 10.1002/adma.20200048210.1002/adma.202000482 ↗
30. 10.1002/smll.20210676610.1002/smll.202106766 ↗
31. 10.1038/s41467-021-23699-410.1038/s41467-021-23699-4 ↗
32. 10.1021/acs.jpcc.8b0623410.1021/acs.jpcc.8b06234 ↗
33. 10.1002/anie.20191599210.1002/anie.201915992 ↗
34. 10.1021/acs.nanolett.1c0348310.1021/acs.nanolett.1c03483 ↗
35. 10.1002/chem.20190461910.1002/chem.201904619 ↗
36. 10.1021/jacs.2c0051810.1021/jacs.2c00518 ↗
37. 10.1021/jacs.8b1177110.1021/jacs.8b11771 ↗
38. S. D.Ross Inorganic infrared and Raman spectra. McGraw‐Hill Book Company London1972 p.140.
39. 10.1038/s41467-021-26053-w10.1038/s41467-021-26053-w ↗
40. 10.1038/s41565-021-00974-510.1038/s41565-021-00974-5 ↗
41. 10.1038/s41467-020-14914-910.1038/s41467-020-14914-9 ↗
42. 10.1039/C8TA03784A10.1039/C8TA03784A ↗
43. 10.1002/anie.20220456310.1002/anie.202204563 ↗
44. 10.1126/science.aao369110.1126/science.aao3691 ↗
45. 10.1021/ja513051310.1021/ja5130513 ↗
46. 10.1021/acscatal.6b0041210.1021/acscatal.6b00412 ↗
47. 10.1021/acsenergylett.7b0109610.1021/acsenergylett.7b01096 ↗
48. 10.1038/s41467-021-24936-610.1038/s41467-021-24936-6 ↗
49. 10.1002/cphc.20170081510.1002/cphc.201700815 ↗
50. 10.1080/21663831.2020.184253410.1080/21663831.2020.1842534 ↗
51. 10.1002/cssc.20210197210.1002/cssc.202101972 ↗
52. 10.1002/anie.20210288710.1002/anie.202102887 ↗
53. 10.1039/C9EE01204D10.1039/C9EE01204D ↗
54. 10.1021/acsaem.1c0157710.1021/acsaem.1c01577 ↗
55. 10.1021/acsenergylett.1c0226710.1021/acsenergylett.1c02267 ↗