journal article·2024-10

Defect‐Expedited Photocarrier Separation in Zn2In2S5 for High‐Efficiency Photocatalytic C─C Coupling Synchronized with H2 Liberation from Benzyl Alcohol

Minmin Ma, Ran Wang, Li Shi, Ronghua Li, Jie Huang, Zhuo Li, Peng Li, Elena Yu. Konysheva, Yanbo Li, Gang Liu, Xiaoxiang Xu

Advanced Functional Materials· Volume 34· Issue 44
Publisher page

Abstract

Abstract Photocatalytic carbon‐carbon (C─C) coupling of benzyl alcohol is a promising means to coproduce the value‐added chemicals with H2 but is generally subject to low efficiency in terms of photon utilization. Here, efficient benzyl alcohol C─C coupling is achieved over Zn2In2S5 containing a tunable content of Zn vacancies (VZn). The VZn tends to form shallow defect states below the conduction band that can expedite photocarrier separation by collecting the photo‐generated electrons. The VZn‐collected electrons are essential for a high selectivity of the C─C coupling reactions because they enable a fast elimination of the byproduct benzaldehyde by catalyzing its reduction back to the ketyl radicals. Under simulated sunlight, the VZn‐containing Zn2In2S5 accomplishes ≈100% conversion of benzyl alcohol for merely 1 h and attains ≈100% selectivity for the C─C coupling compounds for 2 h, delivering an apparent quantum yield as high as 7.7% at 420 ± 20 nm. The benefits of VZn have also been verified by the theoretical calculations that indicate reduced energy barriers for various surface reactions in the presence of VZn. This work brings fresh mechanistic insights into the role of VZn and can serve as a useful guideline in the design of efficient photocatalysts.
Source: crossref · Quality: baseline

Research context

OpenAlex topics: Advanced Photocatalysis Techniques · Perovskite Materials and Applications · TiO2 Photocatalysis and Solar Cells

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

Affiliations

Clinical and Central Lab, Putuo People’s Hospital Tongji University Shanghai 200060 China

Shanghai Key Lab of Chemical Assessment and Sustainability School of Chemical Science and Engineering Tongji University Shanghai 200092 China

State Key Laboratory of Organic Electronics and Information Displays & Institute of Advanced Materials (IAM) Nanjing University of Posts and Telecommunications Nanjing 210023 China

Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of China Chengdu 610054 China

Shenyang National Laboratory for Materials Science Institute of Metal Research Chinese Academy of Sciences 72 Wenhua Road Shenyang 110016 China

College of Environment Science and Engineering Tongji University Shanghai 200092 China

Shaanxi Huaqin Technology Industry Co., Ltd Xi'an 710055 China

Institute of Metallurgy of the Ural Branch of the Russian Academy of Sciences Ekaterinburg 620016 Russia

Funding

Fundamental Research Funds for the Central Universities · Nanjing University of Posts and Telecommunications · National Natural Science Foundation of China

References (44)

Show source-provided references
1. 10.1021/acs.chemrev.1c0019710.1021/acs.chemrev.1c00197 ↗
2. Xu Q. C. · Angew. Chem., Int. Ed. · 2023 · 62
3. 10.1021/acscatal.0c0348010.1021/acscatal.0c03480 ↗
4. 10.1016/j.isci.2021.10220910.1016/j.isci.2021.102209 ↗
5. 10.1021/acscatal.0c0359710.1021/acscatal.0c03597 ↗
6. 10.1039/D0GC03447A10.1039/D0GC03447A ↗
7. 10.1021/acs.joc.3c0081210.1021/acs.joc.3c00812 ↗
8. 10.1016/j.jhazmat.2022.13036310.1016/j.jhazmat.2022.130363 ↗
9. 10.1002/anie.20230305410.1002/anie.202303054 ↗
10. 10.34133/research.007310.34133/research.0073 ↗
11. 10.1016/j.cattod.2022.04.00710.1016/j.cattod.2022.04.007 ↗
12. 10.1039/D0CS00314J10.1039/D0CS00314J ↗
13. 10.1038/s41929-020-0423-310.1038/s41929-020-0423-3 ↗
14. 10.1021/acscatal.0c0171510.1021/acscatal.0c01715 ↗
15. 10.1021/acs.accounts.8b0026710.1021/acs.accounts.8b00267 ↗
16. 10.1038/s41467-018-03543-y10.1038/s41467-018-03543-y ↗
17. 10.1039/C7EE02951A10.1039/C7EE02951A ↗
18. 10.1021/acsnano.2c0865210.1021/acsnano.2c08652 ↗
19. 10.1021/ja500411910.1021/ja5004119 ↗
20. 10.1016/j.chempr.2019.01.00510.1016/j.chempr.2019.01.005 ↗
21. 10.1002/anie.20230430610.1002/anie.202304306 ↗
22. 10.1016/j.apcatb.2022.12201910.1016/j.apcatb.2022.122019 ↗
23. 10.1016/j.apcatb.2020.11878310.1016/j.apcatb.2020.118783 ↗
24. 10.1021/jacs.2c0741010.1021/jacs.2c07410 ↗
25. 10.1021/acscatal.9b0365110.1021/acscatal.9b03651 ↗
26. 10.1021/acsaem.8b0165210.1021/acsaem.8b01652 ↗
27. 10.1021/acscatal.0c0423710.1021/acscatal.0c04237 ↗
28. 10.1016/S1872-2067(21)63931-110.1016/S1872-2067(21)63931-1 ↗
29. 10.1016/j.mcat.2022.11242910.1016/j.mcat.2022.112429 ↗
30. 10.1016/j.apcatb.2021.12096710.1016/j.apcatb.2021.120967 ↗
31. 10.1016/j.tet.2011.01.04410.1016/j.tet.2011.01.044 ↗
32. 10.1021/jacs.6b0292910.1021/jacs.6b02929 ↗
33. 10.1016/S0040-4020(02)01475-810.1016/S0040-4020(02)01475-8 ↗
34. 10.1021/ol025811h10.1021/ol025811h ↗
35. 10.1016/j.cej.2023.14797010.1016/j.cej.2023.147970 ↗
36. 10.1002/adfm.20220135710.1002/adfm.202201357 ↗
37. 10.1039/D2TA08336A10.1039/D2TA08336A ↗
38. 10.1002/aenm.20210245210.1002/aenm.202102452 ↗
39. 10.1021/ja058084510.1021/ja0580845 ↗
40. 10.1039/c3ta01685d10.1039/c3ta01685d ↗
41. 10.1021/jacs.7b0229010.1021/jacs.7b02290 ↗
42. 10.1088/0953-8984/21/39/39550210.1088/0953-8984/21/39/395502 ↗
43. 10.1103/PhysRevLett.77.386510.1103/PhysRevLett.77.3865 ↗
44. 10.1002/jcc.2175910.1002/jcc.21759 ↗