Skip to main content
SpringerLink
Log in

Constructing dual-functional porphyrin-based thorium metal-organic framework toward photocatalytic uranium(VI) reduction integrated with organic oxidation

  • Articles
  • Published:
Science China Chemistry Aims and scope Submit manuscript

Abstract

The rational fabrication of photocatalysts with dual functions upon visible light, such as photocatalytic radioactive U(VI) reduction and value-added organic oxidation, is highly desirable but remains huge challenge. Here, we couple the photocatalytic U(VI) reduction with the oxidative organic synthesis to one system using novel extended π-conjugated framework (Cu@Th-TCPP) without the expense of sacrificial reagents. Noticeably, the as-prepared Cu@Th-TCPP linked by tetratopic tetrakis(4-carboxyphenyl)porphyrin (TCPP) ligand and unique Th6(μ3-O)2(HCOO)4(H2O)6 secondary building unit (SBU) exhibits significantly enhanced activity when the photocatalytic U(VI) reduction and thioanisole oxidation were integrated to one system. Further experimental characterizations demonstrate that the highly conjugated framework of Cu@Th-TCPP is good for the charge transfer and separation, while incorporating Cu2+ site further accelerates the charge-carrier dynamics, thus giving rise to the dual-functional property. Apparently, this strategy conforms to atomic economy, opens a new horizon to addresses radioactive environmental pollution in natural water systems and soils, and simultaneously produces valuable chemicals.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Similar content being viewed by others

References

  1. Li D, Kassymova M, Cai X, Zang SQ, Jiang HL. Coord Chem Rev, 2020, 412: 213262

    Article  CAS  Google Scholar 

  2. Dong H, Zhang X, Lu Y, Yang Y, Zhang YP, Tang HL, Zhang FM, Yang ZD, Sun X, Feng Y. Appl Catal B-Environ, 2020, 276: 119173

    Article  CAS  Google Scholar 

  3. Méndez-Ardoy A, Bayón-Fernández A, Yu Z, Abell C, Granja JR, Montenegro J. Angew Chem Int Ed, 2020, 59: 6902–6908

    Article  CAS  Google Scholar 

  4. Jiang XH, Zhang LS, Liu HY, Wu DS, Wu FY, Tian L, Liu LL, Zou JP, Luo SL, Chen BB. Angew Chem Int Ed, 2020, 59: 23112–23116

    Article  CAS  Google Scholar 

  5. Hu H, Wang Z, Cao L, Zeng L, Zhang C, Lin W, Wang C. Nat Chem, 2021, 13: 358–366

    Article  CAS  PubMed  Google Scholar 

  6. Wei W, Tian Q, Sun H, Liu P, Zheng Y, Fan M, Zhuang J. Appl Catal B-Environ, 2020, 260: 118153

    Article  CAS  Google Scholar 

  7. Li JY, Li YH, Qi MY, Lin Q, Tang ZR, Xu YJ. ACS Catal, 2020, 10: 6262–6280

    Article  CAS  Google Scholar 

  8. Savateev A, Ghosh I, König B, Antonietti M. Angew Chem Int Ed, 2018, 57: 15936–15947

    Article  CAS  Google Scholar 

  9. Sun K, Lv QY, Chen XL, Qu LB, Yu B. Green Chem, 2021, 23: 232–248

    Article  CAS  Google Scholar 

  10. Shang W, Li Y, Huang H, Lai F, Roeffaers MBJ, Weng B. ACS Catal, 2021, 11: 4613–4632

    Article  CAS  Google Scholar 

  11. Xiao JD, Jiang HL. Acc Chem Res, 2019, 52: 356–366

    Article  CAS  PubMed  Google Scholar 

  12. Liang P, Yuan L, Deng H, Wang X, Wang L, Li Z, Luo S, Shi W. Appl Catal B-Environ, 2020, 267: 118688

    Article  CAS  Google Scholar 

  13. Ren X, Philo D, Li Y, Shi L, Chang K, Ye J. Coord Chem Rev, 2020, 424: 213516

    Article  CAS  Google Scholar 

  14. Qiu X, Zhang Y, Zhu Y, Long C, Su L, Liu S, Tang Z. Adv Mater, 2021, 33: 2001731

    Article  CAS  Google Scholar 

  15. Chen X, Kondo Y, Kuwahara Y, Mori K, Louis C, Yamashita H. Phys Chem Chem Phys, 2020, 22: 14404–14414

    Article  CAS  PubMed  Google Scholar 

  16. Gao Z, Lai Y, Tao Y, Xiao L, Zhang L, Luo F. ACS Cent Sci, 2021, 7: 1066–1072

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  17. Gao Z, Yu ZW, Liu FQ, Yu Y, Su XM, Wang L, Xu ZZ, Yang YL, Wu GR, Feng XF, Luo F. Inorg Chem, 2019, 58: 11500–11507

    Article  CAS  PubMed  Google Scholar 

  18. Xiao JD, Han L, Luo J, Yu SH, Jiang HL. Angew Chem Int Ed, 2018, 57: 1103–1107

    Article  CAS  Google Scholar 

  19. Wang Y, Liu W, Bai Z, Zheng T, Silver MA, Li Y, Wang Y, Wang X, Diwu J, Chai Z, Wang S. Angew Chem Int Ed, 2018, 57: 5783–5787

    Article  CAS  Google Scholar 

  20. Li Y, Yang Z, Wang Y, Bai Z, Zheng T, Dai X, Liu S, Gui D, Liu W, Chen M, Chen L, Diwu J, Zhu L, Zhou R, Chai Z, Albrecht-Schmitt TE, Wang S. Nat Commun, 2017, 8: 1354

    Article  PubMed  PubMed Central  CAS  Google Scholar 

  21. Allendorf MD, Bauer CA, Bhakta RK, Houk RJT. Chem Soc Rev, 2009, 38: 1330–1352

    Article  CAS  PubMed  Google Scholar 

  22. Dolgopolova EA, Rice AM, Martin CR, Shustova NB. Chem Soc Rev, 2018, 47: 4710–4728

    Article  CAS  PubMed  Google Scholar 

  23. Zeng L, Guo X, He C, Duan C. ACS Catal, 2016, 6: 7935–7947

    Article  CAS  Google Scholar 

  24. Cichocka MO, Liang Z, Feng D, Back S, Siahrostami S, Wang X, Samperisi L, Sun Y, Xu H, Hedin N, Zheng H, Zou X, Zhou HC, Huang Z. J Am Chem Soc, 2020, 142: 15386–15395

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  25. Wang G, He CT, Huang R, Mao J, Wang D, Li Y. J Am Chem Soc, 2020, 142: 19339–19345

    Article  CAS  PubMed  Google Scholar 

  26. Zeng L, Wang Z, Wang Y, Wang J, Guo Y, Hu H, He X, Wang C, Lin W. J Am Chem Soc, 2020, 142: 75–79

    Article  CAS  PubMed  Google Scholar 

  27. Wang SS, Huang HH, Liu M, Yao S, Guo S, Wang JW, Zhang ZM, Lu TB. Inorg Chem, 2020, 59: 6301–6307

    Article  CAS  PubMed  Google Scholar 

  28. Wu B, Zhang L, Jiang B, Li Q, Tian C, Xie Y, Li W, Fu H. Angew Chem Int Ed, 2021, 60: 4815–4822

    Article  CAS  Google Scholar 

  29. Simon T, Bouchonville N, Berr MJ, Vaneski A, Adrovic A, Volbers D, Wyrwich R, Döblinger M, Susha AS, Rogach AL, Jäckel F, Stolarczyk JK, Feldmann J. Nat Mater, 2014, 13: 1013–1018

    Article  CAS  PubMed  Google Scholar 

  30. Guo Q, Liang F, Li XB, Gao YJ, Huang MY, Wang Y, Xia SG, Gao XY, Gan QC, Lin ZS, Tung CH, Wu LZ. Chem, 2019, 5: 2605–2616

    Article  CAS  Google Scholar 

  31. Kasap H, Caputo CA, Martindale BCM, Godin R, Lau VWH, Lotsch BV, Durrant JR, Reisner E. J Am Chem Soc, 2016, 138: 9183–9192

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  32. Liu H, Xu C, Li D, Jiang HL. Angew Chem Int Ed, 2018, 57: 5379–5383

    Article  CAS  Google Scholar 

  33. Zhang H, Liu W, Li A, Zhang D, Li X, Zhai F, Chen L, Chen L, Wang Y, Wang S. Angew Chem Int Ed, 2019, 58: 16110–16114

    Article  CAS  Google Scholar 

  34. Kumar V, Singh V, Kim KH, Kwon EE, Younis SA. Coord Chem Rev, 2021, 447: 214148

    Article  CAS  Google Scholar 

  35. Li H, Zhai F, Gui D, Wang X, Wu C, Zhang D, Dai X, Deng H, Su X, Diwu J, Lin Z, Chai Z, Wang S. Appl Catal B-Environ, 2019, 254: 47–54

    Article  CAS  Google Scholar 

  36. Sun K, Chen XL, Zhang YL, Li K, Huang XQ, Peng YY, Qu LB, Yu B. Chem Commun, 2019, 55: 12615–12618

    Article  CAS  Google Scholar 

  37. Liu KJ, Deng JH, Yang J, Gong SF, Lin YW, He JY, Cao Z, He WM. Green Chem, 2020, 22: 433–438

    Article  CAS  Google Scholar 

  38. Li P, Goswami S, Otake KI, Wang X, Chen Z, Hanna SL, Farha OK. Inorg Chem, 2019, 58: 3586–3590

    Article  CAS  PubMed  Google Scholar 

  39. Shi JL, Chen R, Hao H, Wang C, Lang X. Angew Chem Int Ed, 2020, 59: 9088-9093

  40. Gao M, Li H, Liu W, Xu Z, Peng S, Yang M, Ye M, Liu Z. Nat Commun, 2020, 11: 3641

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  41. Zuo Q, Liu T, Chen C, Ji Y, Gong X, Mai Y, Zhou Y. Angew Chem Int Ed, 2019, 58: 10198–10203

    Article  CAS  Google Scholar 

  42. Zhao Y, Wang J, Pei R. J Am Chem Soc, 2020, 142: 10331–10336

    Article  CAS  PubMed  Google Scholar 

  43. Gao Z, Li C, Fan G, Yang L, Li F. Appl Catal B-Environ, 2018, 226: 523–533

    Article  CAS  Google Scholar 

  44. Huang W, Ma BC, Lu H, Li R, Wang L, Landfester K, Zhang KAI. ACS Catal, 2017, 7: 5438–5442

    Article  CAS  Google Scholar 

  45. Xu C, Liu H, Li D, Su JH, Jiang HL. Chem Sci, 2018, 9: 3152–3158

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  46. Li Q, Lan X, An G, Ricardez-Sandoval L, Wang Z, Bai G. ACS Catal, 2020, 10: 6664–6675

    Article  CAS  Google Scholar 

  47. Gao Z, Lai Y, Tao Y, Xiao L, Li Z, Zhang L, Sun L, Luo F. Appl Catal B-Environ, 2021, 297: 120485

    Article  CAS  Google Scholar 

  48. Chappa S, Mhatre AM, Adya VC, Pandey AK. Appl Catal B-Environ, 2017, 203: 53–64

    Article  CAS  Google Scholar 

  49. Chen R, Wang Y, Ma Y, Mal A, Gao XY, Gao L, Qiao L, Li XB, Wu LZ, Wang C. Nat Commun, 2021, 12: 1354

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  50. Jiang L, Yuan X, Zeng G, Wu Z, Liang J, Chen X, Leng L, Wang H, Wang H. Appl Catal B-Environ, 2018, 221: 715–725

    Article  CAS  Google Scholar 

  51. Qin JH, Xu P, Huang YD, Xiao LY, Lu W, Yang XG, Ma LF, Zang SQ. Chem Commun, 2021, 57: 8468–8471

    Article  CAS  Google Scholar 

  52. Liu S, Wang Z, Lu Y, Li H, Chen X, Wei G, Wu T, Maguire DJ, Ye G, Chen J. Appl Catal B-Environ, 2021, 282: 119523

    Article  CAS  Google Scholar 

  53. Feng X, Liu L, Honsho Y, Saeki A, Seki S, Irle S, Dong Y, Nagai A, Jiang D. Angew Chem Int Ed, 2012, 51: 2618–2622

    Article  CAS  Google Scholar 

Download references

Acknowledgements

This work was supported by Jiangxi Province Key Laboratory of Synthetic Chemistry (JXSC202004), the Foundation of Jiangxi Educational Committee (GJJ200731), and the Natural Science Foundation of Jiangxi Province of China (20192BAB213001).

Author information

Authors and Affiliations

  1. Jiangxi Province Key Laboratory of Synthetic Chemistry, East China University of Technology, Nanchang, 330013, China

    Zhi Gao, Yue Wang, Yuzhi Lin, Zhijian Zheng, Yao Liu, Qiqi Jing & Feng Luo

Authors
  1. Zhi Gao
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Yue Wang
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Yuzhi Lin
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Zhijian Zheng
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Yao Liu
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Qiqi Jing
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. Feng Luo
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Feng Luo.

Ethics declarations

Conflict of interest The authors declare no conflict of interest.

Additional information

Supporting information The supporting information is available online at http://chem.scichina.com and http://link.springer.com/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.

Electronic supplementary material

11426_2022_1284_MOESM1_ESM.pdf

Constructing dual-functional porphyrin-based thorium metal-organic framework toward photocatalytic uranium (VI) reduction integrated with organic oxidation

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Gao, Z., Wang, Y., Lin, Y. et al. Constructing dual-functional porphyrin-based thorium metal-organic framework toward photocatalytic uranium(VI) reduction integrated with organic oxidation. Sci. China Chem. 65, 1544–1551 (2022). https://doi.org/10.1007/s11426-022-1284-x

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11426-022-1284-x

Keywords

Search

Navigation