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Single-atom-mediated electron islands boost photocatalytic CO2 chemical fixation

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Abstract

Photocatalytic cycloadditions of CO2 with epoxides are emerging as a significant platform for the green synthesis of valuable carbonates, where efficient catalytic systems with spatially separated charge carriers are demanded. Herein, a single p-block metal atom is proposed to be a candidate for photogenerated electron localization on a metal oxide substrate. By taking the Bi single-atom supported on ZnO nanosheet (Bi1/ZnO) as an example, we show that the Bi atom plays the role of an electron island in the sea of delocalized holes within ZnO. Meanwhile, the as-formed electron island could readily promote the rate-determining ring-opening process of cycloaddition reactions. Benefiting from the unique spatially separated electrons and holes, the Bi1/ZnO achieves a high yield of cyclic carbonates with almost 100% selectivity. This study provides a pioneering strategy for enhancing the performances of photocatalytic CO2 chemical fixation.

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References

  1. Hepburn C, Adlen E, Beddington J, Carter EA, Fuss S, Mac Dowell N, Minx JC, Smith P, Williams CK. Nature, 2019, 575: 87–97

    Article  CAS  PubMed  Google Scholar 

  2. Huang JE, Li F, Ozden A, Sedighian Rasouli A, García de Arquer FP, Liu S, Zhang S, Luo M, Wang X, Lum Y, Xu Y, Bertens K, Miao RK, Dinh CT, Sinton D, Sargent EH. Science, 2021, 372: 1074–1078

    Article  CAS  PubMed  Google Scholar 

  3. Zheng T, Zhang M, Wu L, Guo S, Liu X, Zhao J, Xue W, Li J, Liu C, Li X, Jiang Q, Bao J, Zeng J, Yu T, **a C. Nat Catal, 2022, 5: 388–396

    Article  CAS  Google Scholar 

  4. Sun Q, Chen BWJ, Wang N, He Q, Chang A, Yang C, Asakura H, Tanaka T, Hülsey MJ, Wang C-, Yu J, Yan N. Angew Chem Int Ed, 2020, 59: 20183–20191

    Article  CAS  Google Scholar 

  5. Feng Z, Tang C, Zhang P, Li K, Li G, Wang J, Feng Z, Li C. J Am Chem Soc, 2023, 145: 12663–12672

    Article  CAS  PubMed  Google Scholar 

  6. **n ZK, Gao YJ, Gao Y, Song HW, Zhao J, Fan F, **a AD, Li XB, Tung CH, Wu LZ. Adv Mater, 2022, 34: 2106662

    Article  CAS  Google Scholar 

  7. Li H, Song Q, Wan S, Tung C, Liu C, Pan Y, Luo GQ, Chen HM, Cao S, Yu J, Zhang LM. Small, 2023, 19: 2301711

    Article  CAS  Google Scholar 

  8. Wang Y, Wang S, Lou XWD. Angew Chem Int Ed, 2019, 58: 17236–17240

    Article  CAS  Google Scholar 

  9. Li Y, Wang S, Wang X, He Y, Wang Q, Li Y, Li M, Yang G, Yi J, Lin H, Huang D, Li L, Chen H, Ye J. J Am Chem Soc, 2020, 142: 19259–19267

    Article  CAS  PubMed  Google Scholar 

  10. Wang Y, Fan G, Wang S, Li Y, Guo Y, Luan D, Gu X, Lou XWD. Adv Mater, 2022, 34: 2204865

    Article  CAS  Google Scholar 

  11. **ong X, Mao C, Yang Z, Zhang Q, Waterhouse GIN, Gu L, Zhang T. Adv Energy Mater, 2020, 10: 2002928

    Article  CAS  Google Scholar 

  12. Zhang S, **a Z, Zou Y, Cao F, Liu Y, Ma Y, Qu Y. J Am Chem Soc, 2019, 141: 11353–11357

    Article  CAS  PubMed  Google Scholar 

  13. Cao JP, Xue YS, Li NF, Gong JJ, Kang RK, Xu Y. J Am Chem Soc, 2019, 141: 19487–19497

    Article  CAS  PubMed  Google Scholar 

  14. Hou SL, Dong J, Zhao B. Adv Mater, 2020, 32: 1806163

    Article  CAS  Google Scholar 

  15. Zhang X, Liu H, An P, Shi Y, Han J, Yang Z, Long C, Guo J, Zhao S, Zhao K, Yin H, Zheng L, Zhang B, Liu X, Zhang L, Li G, Tang Z. Sci Adv, 2020, 6: eaaz4824

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  16. Li XB, **n ZK, **a SG, Gao XY, Tung CH, Wu LZ. Chem Soc Rev, 2020, 49: 9028–9056

    Article  CAS  PubMed  Google Scholar 

  17. Liu W, Li L, Shao W, Wang H, Dong Y, Zuo M, Liu J, Zhang H, Ye B, Zhang X, **e Y. Chem Sci, 2023, 14: 1397–1402

    Article  CAS  PubMed  Google Scholar 

  18. Xu J, Xu H, Dong A, Zhang H, Zhou Y, Dong H, Tang B, Liu Y, Zhang L, Liu X, Luo J, Bie L, Dai S, Wang Y, Sun X, Li Y. Adv Mater, 2022, 34: 2206991

    Article  CAS  Google Scholar 

  19. Yang Q, Peng H, Zhang Q, Qian X, Chen X, Tang X, Dai S, Zhao J, Jiang K, Yang Q, Sun J, Zhang L, Zhang N, Gao H, Lu Z, Chen L. Adv Mater, 2021, 33: 2103186

    Article  CAS  Google Scholar 

  20. Yang Q, Yang C, Lin C, Jiang H. Angew Chem Int Ed, 2019, 58: 3511–3515

    Article  CAS  Google Scholar 

  21. Wang G, Huang R, Zhang J, Mao J, Wang D, Li Y. Adv Mater, 2021, 33: 2105904

    Article  CAS  Google Scholar 

  22. Liu W, Wang Y, Huang H, Wang J, He G, Feng J, Yu T, Li Z, Zou Z. J Am Chem Soc, 2023, 145: 7181–7189

    Article  CAS  PubMed  Google Scholar 

  23. Shi A, Sun D, Zhang X, Ji S, Wang L, Li X’, Zhao Q, Niu X. ACS Catal, 2022, 12: 9570–9578

    Article  CAS  Google Scholar 

  24. **a B, Zhang Y, Ran J, Jaroniec M, Qiao SZ. ACS Cent Sci, 2021, 7: 39–54

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  25. Zhang Y, Johannessen B, Zhang P, Gong J, Ran J, Qiao SZ. Adv Mater, 2023, 35: 2306923

    Article  CAS  Google Scholar 

  26. Zhang Y, Zhi X, Harmer JR, Xu H, Davey K, Ran J, Qiao S. Angew Chem Int Ed, 2022, 61: e202212355

    Article  CAS  Google Scholar 

  27. Yan T, Li N, Wang L, Ran W, Duchesne PN, Wan L, Nguyen NT, Wang L, **a M, Ozin GA. Nat Commun, 2020, 11: 6095

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  28. Singh M, Chakraborty B. Phys Chem Chem Phys, 2023, 25: 16018–16029

    Article  CAS  PubMed  Google Scholar 

  29. Zhang W, Li QS, Li ZS. J Phys Chem Lett, 2022, 13: 6686–6693

    Article  CAS  PubMed  Google Scholar 

  30. Yao X, Wang L, Sun Y, Li X, Sun J, Wang B, He M, Zhang X. Phys Rev B, 2022, 105: 214421

    Article  CAS  Google Scholar 

  31. Liu J, Wang S, Kawazoe Y, Sun Q. ACS Mater Lett, 2022, 4: 860–867

    Article  CAS  Google Scholar 

  32. Wu S, Su B, Ni K, Pan F, Wang C, Zhang K, Yu DYW, Zhu Y, Zhang W. Adv Energy Mater, 2021, 11: 2002737

    Article  CAS  Google Scholar 

  33. Wu Y, Yu XF, Du Y, **a L, Guo Q, Zhang K, Zhang W, Liu S, Peng Y, Li Z, Yang X. Appl Catal B-Environ, 2023, 331: 122732

    Article  CAS  Google Scholar 

  34. Haldavnekar R, Venkatakrishnan K, Tan B. Nat Commun, 2018, 9: 3065

    Article  PubMed  PubMed Central  Google Scholar 

  35. Lahann J, Choi IS, Lee J, Jensen KF, Langer R. Angew Chem Intl Ed, 2001, 40: 3166–3169

    Article  CAS  Google Scholar 

  36. Guidelli EJ, Ramos AP, Zaniquelli MED, Nicolucci P, Baffa O. ACS Appl Mater Interfaces, 2012, 4: 5844–5851

    Article  CAS  PubMed  Google Scholar 

  37. Zhou D, Tang X, Guo X, Li P, Shanmukaraj D, Liu H, Gao X, Wang Y, Rojo T, Armand M, Wang G. Angew Chem Int Ed, 2020, 59: 16725–16734

    Article  CAS  Google Scholar 

  38. Wang Y, Hu J, Ge T, Chen F, Lu Y, Chen R, Zhang H, Ye B, Wang S, Zhang Y, Ma T, Huang H. Adv Mater, 2023, 35: 2302538

    Article  CAS  Google Scholar 

  39. Chen S, Wang H, Kang Z, ** S, Zhang X, Zheng X, Qi Z, Zhu J, Pan B, **e Y. Nat Commun, 2019, 10: 788

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  40. Wang P, Shi R, Zhao Y, Li Z, Zhao J, Zhao J, Waterhouse GIN, Wu L-, Zhang T. Angew Chem Int Ed, 2023, 62: e202304301

    Article  CAS  Google Scholar 

  41. Song S, Song H, Li L, Wang S, Chu W, Peng K, Meng X, Wang Q, Deng B, Liu Q, Wang Z, Weng Y, Hu H, Lin H, Kako T, Ye J. Nat Catal, 2021, 4: 1032–1042

    Article  CAS  Google Scholar 

  42. Zhu S, Li X, Pan Z, Jiao X, Zheng K, Li L, Shao W, Zu X, Hu J, Zhu J, Sun Y, **e Y. Nano Lett, 2021, 21: 4122–4128

    Article  CAS  PubMed  Google Scholar 

  43. Surdhar PS, Mezyk SP, Armstrong DA. J Phys Chem, 1989, 93: 3360–3363

    Article  CAS  Google Scholar 

Download references

Acknowledgements

This work was supported by the National Key R&D Program of China (2022YFA1502903, 2021YFA1501502), the Strategic Priority Research Program of Chinese Academy of Sciences (XDB0450000, XDB36000000), the National Natural Science Foundation of China (92163105, T2122004, U2032212, 22275179, 22305058), the Anhui Provincial Key Research and Development Program (2022a05020054), the Fundamental Research Funds for the Central Universities (WK2060000039, WK2060000068), the China Postdoctoral Science Foundation (2023TQ0341, 2023M743369), and the Postdoctoral Fellowship Program of CPSF (GZB20230706). The numerical calculations in this paper have been done on the supercomputing system in the Supercomputing Center of the University of Science and Technology of China. We also thank the Infrared Spectroscopy and Microspectroscopy Endstation (BL01B), the Catalysis and Surface Science Endstation (BL11U) at the National Synchrotron Radiation Laboratory (NSRL) and the beamline 1W1B station in the Bei**g Synchrotron Radiation Facility (BSRF) for help in characterizations. This work was partially carried out at the Instruments Center for Physical Science, University of Science and Technology of China.

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Authors and Affiliations

  1. Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, 230026, China

    Shu Shang, Lei Li, **n He, Hui Wang, **aodong Zhang & Yi **e

  2. Institute of Energy, Hefei Comprehensive National Science Center, Hefei, 230031, China

    Hui Wang, **aodong Zhang & Yi **e

  3. Bei**g Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Bei**g, 100049, China

    Lirong Zheng

  4. School of Chemistry and Chemical Engineering, Hefei Normal University, Hefei, 230031, China

    Wei Shao

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  1. Shu Shang
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  2. Lei Li
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  3. **n He
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  4. Hui Wang
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  7. **aodong Zhang
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Correspondence to Lirong Zheng or **aodong Zhang.

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Conflict of interest The authors declare no conflict of interest.

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Supporting information The supporting information is available online at chem.scichina.com and springer.longhoe.net/journal/11426. The supporting materials are published as submitted, without typesetting or editing. The responsibility for scientific accuracy and content remains entirely with the authors.

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Shang, S., Li, L., He, X. et al. Single-atom-mediated electron islands boost photocatalytic CO2 chemical fixation. Sci. China Chem. (2024). https://doi.org/10.1007/s11426-024-1970-5

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  • DOI: https://doi.org/10.1007/s11426-024-1970-5

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