DataVXAdvanced MaterialsPaper
journal article·2024-06Open access

Unveiling the Synergistic Role of Frustrated Lewis Pairs in Carbon‐Encapsulated Ni/NiOx Photothermal Cocatalyst for Enhanced Photocatalytic Hydrogen Production

Zhi Yang, Taiyu Huang, Meng Li, Xudong Wang, Xiaosong Zhou, Siyuan Yang, Qiongzhi Gao, Xin Cai, Yingju Liu, Yueping Fang, Yu Wang, Shanqing Zhang, Shengsen Zhang

Advanced Materials· Volume 36· Issue 24
Publisher pageOpen full text
Source abstract

Abstract

Abstract The development of high‐density and closely spaced frustrated Lewis pairs (FLPs) is crucial for enhancing catalyst activity and accelerating reaction rates. However, constructing efficient FLPs by breaking classical Lewis bonds poses a significant challenge. Here, this work has made a pivotal discovery regarding the Jahn–Teller effect during the formation of grain boundaries in carbon‐encapsulated Ni/NiOx (Ni/NiOx@C). This effect facilitates the formation of high‐density O (VO) and Ni (VNi) vacancy sites with different charge polarities, specifically FLP‐VO‐C basic sites and FLP‐VNi‐C acidic sites. The synergistic interaction between FLP‐VO‐C and FLP‐VNi‐C sites not only reduces energy barriers for water adsorption and splitting, but also induces a strong photothermal effect. This mutually reinforcing effect contributes to the exceptional performance of Ni/NiOx@C as a cocatalyst in photothermal‐assisted photocatalytic hydrogen production. Notably, the Ni/NiOx@C/g‐C3N4 (NOCC) composite photocatalyst exhibits remarkable hydrogen production activity with a rate of 10.7 mmol g−1 h−1, surpassing that of the Pt cocatalyst by 1.76 times. Moreover, the NOCC achieves an impressive apparent quantum yield of 40.78% at a wavelength of 380 nm. This work paves the way for designing novel defect‐state multiphase cocatalysts with high‐density and adjacent FLP sites, which hold promise for enhancing various catalytic reactions.
Source: crossref · Quality: baseline

Research context

CompositesCatalysis & surfaces

OpenAlex topics: Advanced Photocatalysis Techniques · Catalytic Processes in Materials Science · Covalent Organic Framework Applications

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

Affiliations

Guangdong Laboratory for Lingnan Modern Agriculture Key Laboratory for Biobased Materials and Energy of Ministry of Education College of Materials and Energy South China Agricultural University Guangzhou Guangdong 510643 P. R. China

Institute for Sustainable Transformation School of Chemical Engineering and Light Industry Guangdong University of Technology Guangzhou Guangdong 510006 P. R. China

Guangdong Laboratory of Chemistry and Fine Chemical Industry Jieyang Center Jieyang Guangdong 515200 China

SMOE Key Laboratory of Bioinorganic and Synthetic Chemistry Lehn Institute of Functional Materials School of Chemistry Sun Yat‐sen University Guangzhou Guangdong 510275 China

School of Chemistry and Chemical Engineering Key Laboratory of Clean Energy Materials Chemistry of Guangdong Higher Education Institutes Lingnan Normal University Zhanjiang Guangdong 524048 P. R. China

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

Centre for Clean Environment and Energy and School of Environment and Science Gold Coast Campus Griffith University Queensland 4222 Australia

Funding

National Natural Science Foundation of China · Natural Science Foundation of Guangdong Province

References (48)

Show source-provided references
1. 10.1021/acsenergylett.2c0188910.1021/acsenergylett.2c01889 ↗
2. 10.1038/nmat231710.1038/nmat2317 ↗
3. 10.1016/j.ccr.2022.21451610.1016/j.ccr.2022.214516 ↗
4. 10.1038/s41467-022-29076-z10.1038/s41467-022-29076-z ↗
5. 10.1016/j.cej.2022.13467310.1016/j.cej.2022.134673 ↗
6. 10.1016/j.apcatb.2016.07.03310.1016/j.apcatb.2016.07.033 ↗
7. 10.1002/adfm.20221274610.1002/adfm.202212746 ↗
8. 10.1038/s41467-023-37451-710.1038/s41467-023-37451-7 ↗
9. Yan Y. · Adv. Energy Mater. · 2022 · 12
10. 10.1016/j.nanoen.2018.08.05810.1016/j.nanoen.2018.08.058 ↗
11. 10.1016/j.apcatb.2023.12236910.1016/j.apcatb.2023.122369 ↗
12. 10.1126/science.aaf722910.1126/science.aaf7229 ↗
13. 10.1021/jacs.1c1084510.1021/jacs.1c10845 ↗
14. 10.1021/jacs.8b0826710.1021/jacs.8b08267 ↗
15. 10.1002/anie.20221449010.1002/anie.202214490 ↗
16. 10.1021/acsnano.6b0234610.1021/acsnano.6b02346 ↗
17. 10.1103/PhysRev.87.83510.1103/PhysRev.87.835 ↗
18. 10.1103/PhysRevB.45.145010.1103/PhysRevB.45.1450 ↗
19. 10.1021/acsnano.5b0593410.1021/acsnano.5b05934 ↗
20. 10.1002/adma.20170116510.1002/adma.201701165 ↗
21. 10.1002/anie.20171039910.1002/anie.201710399 ↗
22. 10.1021/acsnano.3c0065710.1021/acsnano.3c00657 ↗
23. 10.1016/j.nanoen.2022.10813810.1016/j.nanoen.2022.108138 ↗
24. 10.1021/jacs.3c0831110.1021/jacs.3c08311 ↗
25. 10.1002/adma.20210847510.1002/adma.202108475 ↗
26. 10.1038/s41467-020-14462-210.1038/s41467-020-14462-2 ↗
27. 10.1088/0034-4885/38/1/00110.1088/0034-4885/38/1/001 ↗
28. 10.1016/j.jechem.2022.06.01110.1016/j.jechem.2022.06.011 ↗
29. 10.1016/j.jcat.2018.11.00310.1016/j.jcat.2018.11.003 ↗
30. 10.1016/j.carbon.2010.01.02910.1016/j.carbon.2010.01.029 ↗
31. 10.1002/anie.20130682510.1002/anie.201306825 ↗
32. 10.1016/j.jcat.2019.09.00710.1016/j.jcat.2019.09.007 ↗
33. 10.1016/j.apcatb.2021.12013910.1016/j.apcatb.2021.120139 ↗
34. 10.1002/adma.20221100810.1002/adma.202211008 ↗
35. 10.1038/s41578-022-00433-010.1038/s41578-022-00433-0 ↗
36. 10.1002/adfm.20211022410.1002/adfm.202110224 ↗
37. 10.1016/j.nanoen.2021.10648810.1016/j.nanoen.2021.106488 ↗
38. 10.1016/j.apcatb.2023.12273810.1016/j.apcatb.2023.122738 ↗
39. 10.1002/aenm.20220043410.1002/aenm.202200434 ↗
40. 10.1002/adfm.20180013610.1002/adfm.201800136 ↗
41. 10.1002/adfm.20211174010.1002/adfm.202111740 ↗
42. 10.1002/adma.20190340410.1002/adma.201903404 ↗
43. 10.1038/ncomms1422410.1038/ncomms14224 ↗
44. 10.1016/j.nanoen.2022.10702810.1016/j.nanoen.2022.107028 ↗
45. 10.1016/j.apcatb.2019.03.07410.1016/j.apcatb.2019.03.074 ↗
46. 10.1016/j.apcatb.2017.04.02910.1016/j.apcatb.2017.04.029 ↗
47. 10.1016/S1872-2067(20)63559-810.1016/S1872-2067(20)63559-8 ↗
48. 10.1039/C3NR03998F10.1039/C3NR03998F ↗