journal article·2024-04-16

Strain-Induced Self-Assembly at Interface of Two-Dimensional Heterostructures Boosts CO2 Reduction to Methanol by H2O

Ming Cheng, Ning Cao, Zhi Wang, Ke Wang, Tiancheng Pu, Yukun Li, Tulai Sun, Xuanyu Yue, Wenkang Ni, Wenxin Dai, Yi He, Yao Shi, Peng Zhang, Yihan Zhu, Pengfei Xie

ACS Nano· Volume 18· Issue 15
Publisher page

Abstract

CO 2 conversion with pure H 2 O into CH 3 OH and O 2 driven by solar energy can supply fuels and life-essential substances for extraterrestrial exploration. However, the effective production of CH 3 OH is significantly challenging. Here we report an organozinc complex/MoS 2 heterostructure linked by well-defined zinc–sulfur covalent bonds derived by the structural deformation and intensive coupling of d x 2 – y 2 (Zn)-p(S) orbitals at the interface, resulting in distinctive charge transfer behaviors and excellent redox capabilities as revealed by experimental characterizations and first-principle calculations. The synthesis strategy is further generalized to more organometallic compounds, achieving various heterostructures for CO 2 photoreduction. The optimal catalyst delivers a promising CH 3 OH yield of 2.57 mmol g cat –1 h –1 and selectivity of more than 99.5%. The reverse water gas shift mechanism is identified for methanol formation. Meanwhile, energy-unfavorable adsorption of methanol on MoS 2, where the photogenerated holes accumulate, ensures the selective oxidation of water over methanol.
Source: openalex_inverted_index · Quality: baseline

Research context

OpenAlex topics: Perovskite Materials and Applications · Advanced Photocatalysis Techniques · CO2 Reduction Techniques and Catalysts

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

Affiliations

College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310058, China

Center for Electron Microscopy, Institute for Frontier and Interdisciplinary Sciences, State Key Laboratory Breeding Base of Green Chemistry Synthesis Technology and College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, Zhejiang 310014, China

Institute of Zhejiang University-Quzhou, Quzhou 324000, China

State Center for International Cooperation on Designer Low-Carbon and Environmental Materials School of Materials, School of Materials Science and Engineering, Zhengzhou University, Zhengzhou 450001, China

Research Institute of Photocatalysis, State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, Fuzhou 350002, China

State Key Laboratory of Baiyunobo Rare Earth Resource Researches and Comprehensive Utilization, Baotou Research Institute of Rare Earths, Baotou 014030, China

Funding

Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering · National Key Research and Development Program of China · National Natural Science Foundation of China · Natural Science Foundation of Zhejiang Province

References (73)

Show source-provided references
1. 10.1002/aenm.20160002510.1002/aenm.201600025 ↗
2. 10.20517/cs.2022.2010.20517/cs.2022.20 ↗
3. 10.1002/adma.20180482810.1002/adma.201804828 ↗
4. 10.1002/aenm.20160268410.1002/aenm.201602684 ↗
5. 10.1038/s41929-018-0181-710.1038/s41929-018-0181-7 ↗
6. 10.1002/sus2.4710.1002/sus2.47 ↗
7. 10.1038/s41928-020-00529-x10.1038/s41928-020-00529-x ↗
8. 10.1002/sus2.8310.1002/sus2.83 ↗
9. 10.1016/j.chempr.2018.08.03710.1016/j.chempr.2018.08.037 ↗
10. 10.1021/acs.chemmater.0c0348210.1021/acs.chemmater.0c03482 ↗
11. 10.1038/s41586-021-03338-010.1038/s41586-021-03338-0 ↗
12. 10.1002/adfm.20220258810.1002/adfm.202202588 ↗
13. 10.1039/D0CS01070G10.1039/D0CS01070G ↗
14. 10.1002/cnma.20220015310.1002/cnma.202200153 ↗
15. 10.1002/solr.20200045810.1002/solr.202000458 ↗
16. 10.1039/D0NR09064F10.1039/D0NR09064F ↗
17. 10.1038/nnano.2015.34010.1038/nnano.2015.340 ↗
18. 10.1002/aenm.20200315910.1002/aenm.202003159 ↗
19. 10.1016/j.joule.2021.11.00910.1016/j.joule.2021.11.009 ↗
20. 10.1021/jacs.9b0708810.1021/jacs.9b07088 ↗
21. 10.1021/acscatal.9b0186910.1021/acscatal.9b01869 ↗
22. 10.1038/s41467-022-28987-110.1038/s41467-022-28987-1 ↗
23. 10.1007/s10967-020-07125-510.1007/s10967-020-07125-5 ↗
24. 10.1039/C4CE00123K10.1039/C4CE00123K ↗
25. 10.1039/C2DT31922E10.1039/C2DT31922E ↗
26. 10.1038/nmat485210.1038/nmat4852 ↗
27. 10.1126/science.aao086510.1126/science.aao0865 ↗
28. 10.1038/s41586-019-1013-x10.1038/s41586-019-1013-x ↗
29. 10.1038/natrevmats.2016.4210.1038/natrevmats.2016.42 ↗
30. 10.1016/j.apcatb.2021.12074910.1016/j.apcatb.2021.120749 ↗
31. 10.1002/marc.20190026310.1002/marc.201900263 ↗
32. 10.1002/anie.20210831710.1002/anie.202108317 ↗
33. 10.1002/smtd.20190065310.1002/smtd.201900653 ↗
34. 10.1021/ja512090810.1021/ja5120908 ↗
35. 10.1002/ange.20151021910.1002/ange.201510219 ↗
36. 10.1038/s41598-017-10632-310.1038/s41598-017-10632-3 ↗
37. 10.1021/jacs.7b0888110.1021/jacs.7b08881 ↗
38. 10.1002/smll.20180551110.1002/smll.201805511 ↗
39. 10.1021/acsaem.0c0289910.1021/acsaem.0c02899 ↗
40. 10.1016/j.apsusc.2022.15284210.1016/j.apsusc.2022.152842 ↗
41. 10.1038/s41377-018-0056-310.1038/s41377-018-0056-3 ↗
42. 10.1016/j.apcatb.2016.11.06210.1016/j.apcatb.2016.11.062 ↗
43. 10.1039/C7NR03238B10.1039/C7NR03238B ↗
44. 10.1021/jacs.6b1126310.1021/jacs.6b11263 ↗
45. 10.1016/j.apsusc.2016.06.15510.1016/j.apsusc.2016.06.155 ↗
46. 10.1038/s41467-020-16227-310.1038/s41467-020-16227-3 ↗
47. 10.1016/j.apcatb.2020.11887610.1016/j.apcatb.2020.118876 ↗
48. 10.1016/j.apsusc.2017.01.17110.1016/j.apsusc.2017.01.171 ↗
49. 10.1016/j.cej.2021.12928610.1016/j.cej.2021.129286 ↗
50. 10.1039/D2NR02364D10.1039/D2NR02364D ↗
51. 10.1016/j.apcatb.2021.12069510.1016/j.apcatb.2021.120695 ↗
52. 10.1016/j.jcat.2017.02.00510.1016/j.jcat.2017.02.005 ↗
53. 10.1002/ange.20210889210.1002/ange.202108892 ↗
54. 10.1038/s41560-021-00795-910.1038/s41560-021-00795-9 ↗
55. 10.1016/j.apcatb.2017.03.07710.1016/j.apcatb.2017.03.077 ↗
56. 10.1002/admi.20190180510.1002/admi.201901805 ↗
57. 10.1039/C9GC03323H10.1039/C9GC03323H ↗
58. 10.1016/j.apsusc.2022.15253210.1016/j.apsusc.2022.152532 ↗
59. 10.1021/jacs.1c0791610.1021/jacs.1c07916 ↗
60. 10.1016/j.apcatb.2021.11987710.1016/j.apcatb.2021.119877 ↗
61. 10.1021/jp310516610.1021/jp3105166 ↗
62. 10.1002/smll.20220378710.1002/smll.202203787 ↗
63. 10.1002/smtd.20210070010.1002/smtd.202100700 ↗
64. 10.1039/D2TA02648A10.1039/D2TA02648A ↗
65. 10.1039/C7CY01869J10.1039/C7CY01869J ↗
66. 10.1039/C7TA08766G10.1039/C7TA08766G ↗
67. 10.1038/s41560-019-0431-110.1038/s41560-019-0431-1 ↗
68. 10.1016/j.ijhydene.2022.08.06210.1016/j.ijhydene.2022.08.062 ↗
69. 10.1016/j.jcat.2022.07.03810.1016/j.jcat.2022.07.038 ↗
70. 10.1107/S160053681202386010.1107/S1600536812023860 ↗
71. 10.1107/S160053680101187410.1107/S1600536801011874 ↗
72. 10.1107/S160053680903787810.1107/S1600536809037878 ↗
73. 10.1080/00958972.2015.105848510.1080/00958972.2015.1058485 ↗