Citation: Lin Yuan, Lei Zhang, Xiao-Xin Li, Jiang Liu, Jing-Jing Liu, Long-Zhang Dong, Dong-Sheng Li, Shun-Li Li, Ya-Qian Lan. Uncovering the synergistic photocatalytic behavior of bimetallic molecular catalysts[J]. Chinese Chemical Letters, ;2023, 34(1): 107146. doi: 10.1016/j.cclet.2022.01.039 shu

Uncovering the synergistic photocatalytic behavior of bimetallic molecular catalysts

Lin Yuan ^{a, 1} ,
Lei Zhang ^{b, 1} ,
Xiao-Xin Li ^c ,
Jiang Liu ^{a, b, *,} ,
Jing-Jing Liu ^b ,
Long-Zhang Dong ^a ,
Dong-Sheng Li ^d ,
Shun-Li Li ^{a, *,} ,
Ya-Qian Lan ^{a, b, *,}

a.
Jiangsu Collaborative Innovation Centre of Biomedical Functional Materials, Jiangsu Key Laboratory of New Power Batteries, College of Chemistry and Materials Science, Nanjing Normal University, Nanjing 210023, China
b.
School of Chemistry, South China Normal University, Guangzhou 510006, China
c.
School of Chemistry and Chemical Engineering, Southeast University, Nanjing 211189, China
d.
Key Laboratory of Inorganic Nonmetallic Crystalline and Energy Conversion Materials, China Three Gorges University, Yichang 443002, China

liuj@njnu.edu.cn

slli@njnu.edu.cn

yqlan@m.scnu.edu.cn

Received Date: 31 December 2021
Revised Date: 12 January 2022
Accepted Date: 16 January 2022
Available Online: 23 January 2022

Figures(4)

Bimetallic catalysts usually exhibit better performance than monometallic catalysts due to synergistic effect. However, there is a lack of exploring the synergistic effect on catalytic performance caused by the introduction of inactive metal ion. In this work, we design a molecular model system that can precisely regulate the metal site number and catalytic property. When these molecular metal compounds are used as homogeneous catalysts for photocatalytic CO₂ reduction, the dinuclear heterometallic CuNi-L² shows the highest CO₂-to-CO conversion, which is 2.1 and 3.0 times higher than that of dinuclear homometallic Ni₂-L² and mononuclear Ni-L¹. Density functional theory calculations demonstrate that, in CuNi-L², the introduction of inactive Cu^II is easier to promote the photo-generated electrons transferring to the coupled active Ni^II site to achieve the highest activity. In addition, this work also provides insights to design and construct more efficient bimetallic catalysts in future.
- Dinuclear metal compounds,
- Crystalline photocatalyst,
- Synergistic effect,
- Photocatalytic CO₂RR,
- Artificial photosynthesis
1. [1]
  X. Chang, T. Wang, P. Yang, G. Zhang, J. Gong, Adv. Mater. 31 (2019) 1804710. doi: 10.1002/adma.201804710
2. [2]
  Y. Hu, F. Zhan, Q. Wang, et al., J. Am. Chem. Soc. 142 (2020) 5618–5626. doi: 10.1021/jacs.9b12443
3. [3]
  M. Sun, C. Wang, C.Y. Sun, et al., J Catal. 385 (2020) 70–75. doi: 10.1016/j.jcat.2020.03.005
4. [4]
  S. Navarro-Jaén, M. Virginie, J. Bonin, et al., Nat. Rev. Chem. 5 (2021) 564–579. doi: 10.1038/s41570-021-00289-y
5. [5]
  W. Tu, Y. Zhou and Z. Zou, Adv. Mater. 26 (2014) 4607–4626. doi: 10.1002/adma.201400087
6. [6]
  Y. Wang, N.Y. Huang, J.Q. Shen, et al., J. Am. Chem. Soc. 140 (2018) 38–41. doi: 10.1021/jacs.7b10107
7. [7]
  H. Zhong, R. Sa, H. Lv, et al., Adv. Funct. Mater. 30 (2020) 2002654. doi: 10.1002/adfm.202002654
8. [8]
  M. Ding, H.L. Jiang, ACS Catal. 8 (2018) 3194–3201. doi: 10.1021/acscatal.7b03404
9. [9]
  H. Rao, L.C. Schmidt, J. Bonin, M. Robert, Nature 548 (2017) 74–77. doi: 10.1038/nature23016
10. [10]
  D. Mellmann, P. Sponholz, H. Junge, M. Beller, Chem. Soc. Rev. 45 (2016) 3954–3988. doi: 10.1039/C5CS00618J
11. [11]
  P. Wang, R. Dong, S. Guo, et al., Nat. Sci. Rev. 7 (2020) 1459–1467. doi: 10.1093/nsr/nwaa112
12. [12]
  Z. Guo, S. Cheng, C. Cometto, et al., J. Am. Chem. Soc. 138 (2016) 9413–9416. doi: 10.1021/jacs.6b06002
13. [13]
  Q. Fu and C. Draxl, Phys. Rev. Lett. 122 (2019) 046101. doi: 10.1103/PhysRevLett.122.046101
14. [14]
  T. Ouyang, H.H. Huang, J.W. Wang, D.C. Zhong, T.B. Lu, Angew. Chem. Int. Ed. 56 (2017) 738–743. doi: 10.1002/anie.201610607
15. [15]
  V.S. Thoi, N. Kornienko, C.G. Margarit, P. Yang, C.J. Chang, J. Am. Chem. Soc. 135 (2013) 14413–14424. doi: 10.1021/ja4074003
16. [16]
  T. Ishizuka, A. Watanabe, H. Kotani, et al., Inorg. Chem. 55 (2016) 1154–1164. doi: 10.1021/acs.inorgchem.5b02336
17. [17]
  L. Zhang, X.X. Li, Z.L. Lang, et al., J. Am. Chem. Soc. 143 (2021) 3808–3816. doi: 10.1021/jacs.0c11450
18. [18]
  N. Li, J. Liu, B.X. Dong, Y.Q. Lan, Angew. Chem. Int. Ed. 59 (2020) 20779–20793. doi: 10.1002/anie.202008054
19. [19]
  L. Ma, Q. Wang, W.L. Man, et al., Angew. Chem. Int. Ed. 54 (2015) 5246–5249. doi: 10.1002/anie.201500507
20. [20]
  L.Z. Dong, L. Zhang, J. Liu, et al., Angew. Chem. Int. Ed. 59 (2020) 2659–2663. doi: 10.1002/anie.201913284
21. [21]
  Z. -. H. Yan, M.H. Du, J. Liu, et al., Nat. Commun. 9 (2018) 3353. doi: 10.1038/s41467-018-05659-7
22. [22]
  D. Hong, Y. Tsukakoshi, H. Kotani, T. Ishizuka, T. Kojima, J. Am. Chem. Soc. 139 (2017) 6538–6541. doi: 10.1021/jacs.7b01956
23. [23]
  N. Elgrishi, M.B. Chambers, X. Wang, M. Fontecave, Chem. Soc. Rev. 46 (2017) 761–796. doi: 10.1039/C5CS00391A
24. [24]
  J.J. Liu, N. Li, J.W. Sun, et al., ACS Catal. 11 (2021) 4510–4519. doi: 10.1021/acscatal.0c04495
25. [25]
  N. Bakharev, D. Bono, H.B. Brom, et al., Phys. Rev. Lett. 96 (2006) 117002. doi: 10.1103/PhysRevLett.96.117002
26. [26]
  N. Zheng, X. Bu, P. Feng, J. Am. Chem. Soc. 124 (2002) 9688–9689. doi: 10.1021/ja020480p
27. [27]
  H. Rao, J. Bonin and M. Robert, ChemSusChem. 10 (2017) 4447–4450. doi: 10.1002/cssc.201701467
28. [28]
  H.X. Zhang, Q.L. Hong, J. Li, et al., Angew. Chem. Int. Ed. 58 (2019) 11752–11756. doi: 10.1002/anie.201905869
29. [29]
  X.X. Li, L. Zhang, J. Liu, et al., JACS Au. 1 (2021) 1288–1295. doi: 10.1021/jacsau.1c00186
30. [30]
  Y. Chen, S. Fan, B. Qiu, et al., ACS Appl. Mater. Interfaces 13 (2021) 24795–24803. doi: 10.1021/acsami.1c04155
31. [31]
  B. Guo, Q. Li, J. Lin, et al., ACS Appl. Nano Mater. 4 (2021) 1849–1857. doi: 10.1021/acsanm.0c03224
32. [32]
  Kashid, D.J. Patil, R.D. Mali, et al., Catal Letters. 151 (2021) 353–358. doi: 10.1007/s10562-020-03330-9
33. [33]
  C. Liu, C.L. Ji, T. Zhou, X. Hong, M. Szostak, Angew. Chem. Int. Ed. 60 (2021) 10690–10699. doi: 10.1002/anie.202100949
34. [34]
  J. Xu, Z. Ju, W. Zhang, et al., Angew. Chem. Int. Ed. 60 (2021) 8705–8709. doi: 10.1002/anie.202017041
35. [35]
  T. Ouyang, H.J. Wang, H.H. Huang, et al., Angew. Chem. Int. Ed. 57 (2018) 16480–16485. doi: 10.1002/anie.201811010
36. [36]
  S.M. Liu, Z. Zhang, X. Li, et al., Adv. Mater. Interfaces 5 (2018) 1801062. doi: 10.1002/admi.201801062
37. [37]
  J.Z. Bloh, R. Dillert, D.W. Bahnemann, J. Phys. Chem. C 116 (2012) 25558–25562. doi: 10.1021/jp307313z
38. [38]
  X. Feng, F. Pan, H. Zhao, et al., Appl. Catal. B 238 (2018) 274–283. doi: 10.1016/j.apcatb.2018.07.027
39. [39]
  Z. Jiang, J. Liu, M. Gao, et al., Adv. Mater. 29 (2017) 1603369. doi: 10.1002/adma.201603369
40. [40]
  B. Tang, X. Yang, Z. Kang, L. Feng, Appl. Catal. B 278 (2020) 119281. doi: 10.1016/j.apcatb.2020.119281
41. [41]
  B. Liu, Y.F. Zhao, H.Q. Peng, et al., Adv. Mater. 29 (2017) 1606521. doi: 10.1002/adma.201606521
42. [42]
  Z. Li, H. Dong, Y. Zhang, et al., J. Phys. Chem. C 112 (2008) 16046–16051. doi: 10.1021/jp805475a
43. [43]
  B. Zhang, J. Zhang, F. Zhang, et al., Adv. Funct. Mater. 30 (2020) 1906194. doi: 10.1002/adfm.201906194
44. [44]
  L. Feng, K.Y. Wang, E. Joseph, H.C. Zhou, Trends Chem. 2 (2020) 555–568. doi: 10.1016/j.trechm.2020.01.003
45. [45]
  S.N. Habisreutinger, L. Schmidt-Mende, J.K. Stolarczyk, Angew. Chem. Int. Ed. 52 (2013) 7372–7408. doi: 10.1002/anie.201207199
46. [46]
  J.P. Beale, J.A. Cunningham, D.J. Philips, Inorg. Chim. Acta. 33 (1979) 113–118. doi: 10.1016/S0020-1693(00)89463-3
47. [47]
  N. Pilkington, R. Robson, Aust. J. Chem. 23 (1970) 2225–2236.
48. [48]
  X. Chang, T. Wang, J. Gong, Energy Environ. Sci. 9 (2016) 2177–2196. doi: 10.1039/C6EE00383D
49. [49]
  X.K. Wang, J. Liu, L. Zhang, et al., ACS Catal. 9 (2019) 1726–1732. doi: 10.1021/acscatal.8b04887
50. [50]
  Y. Fu, D. Sun, Y. Chen, et al., Angew. Chem. Int. Ed. 51 (2012) 3364–3367. doi: 10.1002/anie.201108357
51. [51]
  N. Li, J.J. Liu, J.W. Sun, et al., Green Chem. 22 (2020) 5325–5332. doi: 10.1039/D0GC01497D
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