Citation: Zhilong Jiang, Qiaolin Chen, Min Wang, Fengxue Liu, Xiaojie Huang, Bangtang Chen, Qiangqiang Dong, Mingzhao Chen, Yifan Lin, Pingshan Wang, Jun Wang. 3D fractal expanding of a Sierpiński triangular-faced supramolecular cage for enhanced photocatalytic performance[J]. Chinese Chemical Letters, ;2026, 37(1): 111168. doi: 10.1016/j.cclet.2025.111168 shu

3D fractal expanding of a Sierpiński triangular-faced supramolecular cage for enhanced photocatalytic performance

Zhilong Jiang ^{a, 1} ,
Qiaolin Chen ^{a, 1} ,
Min Wang ^a ,
Fengxue Liu ^b ,
Xiaojie Huang ^a ,
Bangtang Chen ^a ,
Qiangqiang Dong ^b ,
Mingzhao Chen ^a ,
Yifan Lin ^{c, *,} ,
Pingshan Wang ^{a, b, **,} ,
Jun Wang ^{a, *,}

a.
Institute of Environmental Research at Greater Bay Area, Key Laboratory for Water Quality and Conservation of the Pearl River Delta, Ministry of Education, Guangzhou University, Guangzhou 510006, China
b.
Hunan Key Laboratory of Micro & Nano Materials Interface Science, College of Chemistry and Chemical Engineering, Central South University, Changsha 410083, China
c.
College of Light Chemical Industry and Materials Engineering, Shunde Polytechnic, Foshan 528300, China

^**

24011@sdpt.edu.cn

chemwps@csu.edu.cn

wangjun@gzhu.edu.cn

Received Date: 15 January 2025
Revised Date: 23 March 2025
Accepted Date: 1 April 2025
Available Online: 1 April 2025

Figures(7)

Fractal assembly in discrete structures, especially for artificial supramolecular species, has attracted significantly increased interest over the past two decades. In this study, we present the precisely controlled fractal expanding synthesis of a novel triangular prism supramolecule featuring Sierpiński triangular face, which was achieved through a module-intervened self-expansion strategy. The homoleptic S1 was firstly synthesized through the assembly of ligand L1 with Zn²⁺ ions. Based on the triangular-faced prism S1, we further introduced Sierpiński triangular faces on the section of the heteroleptic supramolecular cage S2 with an expanded inner cavity and more abundant active sites for photocatalytic properties. The topotactic architectures for both S1 and S2 were fully characterized by nuclear magnetic resonance spectroscopy, high-resolution electrospray ionization mass spectrometry, transmission electron microscopy, and atomic force microscopy. Furthermore, the enhanced photocatalytic activity of the fractal expanded S2 was performed via the superior amine oxidative efficiency over S1. This study proposes the unprecedented fractal expanding strategy for three-dimensional supramolecular species with higher complexity, potentially opening new avenues for structural regulation of artificial fractal molecules.
- Fractal-expansion,
- Metallo-organic ligands,
- Sierpiński triangles,
- Triangular prisms,
- Photocatalysis
1. [1]
  J.W. Cannon, Amer. Math. Monthly 91 (1984) 594–598.
2. [2]
  A. Rieger, Philos. Math. 26 (2017) 234–250.
3. [3]
  J. Liu, Comp. Cont. Philos. 14 (2022) 315–317. doi: 10.1080/17570638.2022.2158432
4. [4]
  C.A. Reiter, Comput. Graph. 18 (1994) 885–891. doi: 10.1016/0097-8493(94)90015-9
5. [5]
  R. Canyellas, C. Liu, R. Arouca, et al., Nat. Phys. 20 (2024) 1421–1428. doi: 10.1038/s41567-024-02551-8
6. [6]
  J. Dai, X. Zhao, Z. Peng, et al., J. Am. Chem. Soc. 145 (2023) 13531–13536. doi: 10.1021/jacs.3c03691
7. [7]
  Z. Jiang, Y. Li, M. Wang, et al., Angew. Chem. Int. Ed. 56 (2017) 11450–11455. doi: 10.1002/anie.201705480
8. [8]
  Z. Jiang, D. Liu, M. Chen, et al., iScience 23 (2020) 101064. doi: 10.1016/j.isci.2020.101064
9. [9]
  N. Li, X. Zhang, G.C. Gu, et al., Chin. Chem. Lett. 26 (2015) 1198–1202. doi: 10.1109/ICEPT.2015.7236794
10. [10]
  Y. Sun, C. Chen, J. Liu, et al., Chem. Soc. Rev. 49 (2020) 3889–3919. doi: 10.1039/d0cs00038h
11. [11]
  E.G. Percástegui, V. Jancik, Coord. Chem. Rev. 407 (2020) 213165. doi: 10.1016/j.ccr.2019.213165
12. [12]
  Y. Li, S.S. Rajasree, G.Y. Lee, et al., J. Am. Chem. Soc. 143 (2021) 2908–2919. doi: 10.1021/jacs.0c12853
13. [13]
  X. Yan, P. Wei, Y. Liu, et al., J. Am. Chem. Soc. 141 (2019) 9673–9679. doi: 10.1021/jacs.9b03885
14. [14]
  H. Zhu, Q. Li, B. Shi, et al., Angew. Chem. Int. Ed. 59 (2020) 20208–20214. doi: 10.1002/anie.202009442
15. [15]
  Y. Ye, T.R. Cook, S.P. Wang, et al., J. Am. Chem. Soc. 137 (2015) 11896–11899. doi: 10.1021/jacs.5b07529
16. [16]
  K. Iizuka, H. Takezawa, M. Fujita, J. Am. Chem. Soc. 146 (2024) 32311–32316. doi: 10.1021/jacs.4c14509
17. [17]
  Y. Domoto, M. Abe, G.R. Genov, et al., Angew. Chem. Int. Ed. 62 (2023) e202303714. doi: 10.1002/anie.202303714
18. [18]
  Y. Domoto, M. Abe, M. Fujita, J. Am. Chem. Soc. 143 (2021) 8578–8582. doi: 10.1021/jacs.1c03208
19. [19]
  D. Fujita, Y. Ueda, S. Sato, et al., Nature 540 (2016) 563–566. doi: 10.1038/nature20771
20. [20]
  Y. Domoto, M. Abe, T. Kikuchi, et al., Angew. Chem. Int. Ed. 59 (2020) 3450–3454. doi: 10.1002/anie.201913142
21. [21]
  J.A. Davies, T.K. Ronson, J.R. Nitschke, J. Am. Chem. Soc. 146 (2024) 5215–5223. doi: 10.1021/jacs.3c11320
22. [22]
  H.K. Liu, T.K. Ronson, K. Wu, et al., J. Am. Chem. Soc. 145 (2023) 15990–15996. doi: 10.1021/jacs.3c03981
23. [23]
  C.F. Espinosa, T.K. Ronson, J.R. Nitschke, J. Am. Chem. Soc. 145 (2023) 9965–9969. doi: 10.1021/jacs.3c00661
24. [24]
  K. Wu, T.K. Ronson, P. Su, et al., Nat. Synth. 2 (2023) 789–797. doi: 10.1038/s44160-023-00276-9
25. [25]
  D. Zhang, Q. Gan, A.J. Plajer, et al., J. Am. Chem. Soc. 144 (2022) 1106–1112. doi: 10.1021/jacs.1c11536
26. [26]
  Y.Q. Zou, D. Zhang, T.K. Ronson, et al., J. Am. Chem. Soc. 143 (2021) 9009–9015. doi: 10.1021/jacs.1c05172
27. [27]
  W.M. Bloch, S. Horiuchi, J.J. Holstein, et al., Chem. Sci. 14 (2023) 1524–1531. doi: 10.1039/d2sc06629g
28. [28]
  E. Benchimol, J. Tessarolo, G.H. Clever, Nat. Chem. 16 (2024) 13–21. doi: 10.1038/s41557-023-01387-8
29. [29]
  K. Hema, A.B. Grommet, M.J. Białek, et al., J. Am. Chem. Soc. 145 (2023) 24755–24764.
30. [30]
  T.R. Schulte, J.J. Holstein, G.H. Clever, Angew. Chem. Int. Ed. 58 (2019) 5562–5566. doi: 10.1002/anie.201812926
31. [31]
  S. Pullen, J. Tessarolo, G.H. Clever, Chem. Sci. 12 (2021) 7269–7293. doi: 10.1039/d1sc01226f
32. [32]
  T.Z. Xie, X. Wu, K.J. Endres, et al., J. Am. Chem. Soc. 139 (2017) 15652–15655. doi: 10.1021/jacs.7b10328
33. [33]
  T.Z. Xie, K.J. Endres, Z. Guo, et al., J. Am. Chem. Soc. 138 (2016) 12344–12347. doi: 10.1021/jacs.6b07969
34. [34]
  T.Z. Xie, K. Guo, Z. Guo, et al., Angew. Chem. Int. Ed. 54 (2015) 9224–9229. doi: 10.1002/anie.201503609
35. [35]
  T.Z. Xie, S.Y. Liao, K. Guo, et al., J. Am. Chem. Soc. 136 (2014) 8165–8168. doi: 10.1021/ja502962j
36. [36]
  D. Chakraborty, N. Kaur, J. Sahoo, et al., J. Am. Chem. Soc. 146 (2024) 24901–24910. doi: 10.1021/jacs.4c05899
37. [37]
  R. Banerjee, D. Chakraborty, P.S. Mukherjee, J. Am. Chem. Soc. 145 (2023) 7692–7711. doi: 10.1021/jacs.3c01084
38. [38]
  J. Chen, Y.H. Huang, J. Yang, et al., J. Am. Chem. Soc. 146 (2024) 32738–32747. doi: 10.1021/jacs.4c12290
39. [39]
  W. Yang, Q. Mo, Q.T. He, et al., Angew. Chem. Int. Ed. 63 (2024) e202406564. doi: 10.1002/anie.202406564
40. [40]
  Y.L. Lai, M. Xie, X.C. Zhou, et al., Angew. Chem. Int. Ed. 63 (2024) e202402829. doi: 10.1002/anie.202402829
41. [41]
  F. Yin, J. Yang, L.P. Zhou, et al., J. Am. Chem. Soc. 146 (2024) 7811–7821. doi: 10.1021/jacs.4c00705
42. [42]
  S.P. Zheng, Y.W. Xu, P.Y. Su, et al., Chin. Chem. Lett. 35 (2024) 108477. doi: 10.1016/j.cclet.2023.108477
43. [43]
  Y. Ding, C. Shen, F. Gan, et al., Chin. Chem. Lett. 32 (2021) 3988–3992. doi: 10.1016/j.cclet.2021.05.033
44. [44]
  D. Luo, B. Pan, J. Zhang, et al., Chin. Chem. Lett. 32 (2021) 1397–1399. doi: 10.1016/j.cclet.2020.11.002
45. [45]
  Y.L. Lai, J. Su, L.X. Wu, et al., Chin. Chem. Lett. 35 (2024) 108326. doi: 10.1016/j.cclet.2023.108326
46. [46]
  R. Sarkar, T.Z. Xie, K.J. Endres, et al., J. Am. Chem. Soc. 142 (2020) 5526–5530. doi: 10.1021/jacs.0c01168
47. [47]
  J. Wang, Z. Jiang, W. Liu, et al., Angew. Chem. Int. Ed. 62 (2023) e202214237. doi: 10.1002/anie.202214237
48. [48]
  Q. Dong, F. Liu, J. Wang, et al., Angew. Chem. Int. Ed. 64 (2025) e202416327. doi: 10.1002/anie.202416327
49. [49]
  Z. Jiang, Z. Wu, J. Wang, et al., Nano Res. 16 (2023) 9584–9590. doi: 10.1007/s12274-023-5607-0
50. [50]
  F. Su, S. Zhang, Z. Chen, et al., J. Am. Chem. Soc. 144 (2022) 16559–16571. doi: 10.1021/jacs.2c06251
51. [51]
  L. He, H.K. Hsu, L. Li, et al., Chem 8 (2022) 494–507. doi: 10.1016/j.chempr.2021.11.013
52. [52]
  Y.S. Chen, E. Solel, Y.F. Huang, et al., Nat. Commun. 10 (2019) 3443. doi: 10.1038/s41467-019-11457-6
53. [53]
  J. Shi, W. Xu, H. Yu, et al., J. Am. Chem. Soc. 145 (2023) 24081–24088. doi: 10.1021/jacs.3c07477
54. [54]
  T. Wu, Z. Jiang, Q. Bai, et al., Chem 7 (2021) 2429–2441. doi: 10.1016/j.chempr.2021.06.003
55. [55]
  D. Liu, M. Chen, K. Li, et al., J. Am. Chem. Soc. 142 (2020) 7987–7994. doi: 10.1021/jacs.0c02366
56. [56]
  Z. Jiang, H. Zhao, J. Wang, et al., Chin. Chem. Lett. 34 (2023) 108334. doi: 10.1016/j.cclet.2023.108334
57. [57]
  T. Wu, Z. Jiang, X. Xue, et al., Chin. Chem. Lett. 32 (2021) 1911–1914. doi: 10.1016/j.cclet.2021.01.052
58. [58]
  G. Wang, M. Chen, J. Wang, et al., J. Am. Chem. Soc. 142 (2020) 7690–7698. doi: 10.1021/jacs.0c00754
59. [59]
  Z. Zhang, Y. Li, B. Song, et al., Nat. Chem. 12 (2020) 468–474. doi: 10.1038/s41557-020-0454-z
60. [60]
  J. Wang, H. Zhao, M. Chen, et al., J. Am. Chem. Soc. 142 (2020) 21691–21701. doi: 10.1021/jacs.0c08020
61. [61]
  Z. Li, Y. Li, Y. Zhao, et al., J. Am. Chem. Soc. 142 (2020) 6196–6205. doi: 10.1021/jacs.0c00110
62. [62]
  Z. Jiang, B. Chen, H. Zhao, et al., J. Am. Chem. Soc. 146 (2024) 16721–16728. doi: 10.1021/jacs.4c04310
63. [63]
  B. Song, Z. Zhang, K. Wang, et al., Angew. Chem. Int. Ed. 56 (2017) 5258–5262. doi: 10.1002/anie.201701417
64. [64]
  X. Lang, W. Ma, Y. Zhao, et al., Chem. Eur. J. 18 (2012) 2624–2631. doi: 10.1002/chem.201102779
65. [65]
  G.J. Chen, H.C. Ma, W.L. Xin, et al., Inorg. Chem. 56 (2017) 654–660. doi: 10.1021/acs.inorgchem.6b02592
66. [66]
  K. Wu, X.Y. Liu, P.W. Cheng, et al., J. Am. Chem. Soc. 145 (2023) 18931–18938. doi: 10.1021/jacs.3c05585
67. [67]
  H. Hao, J.L. Shi, H. Xu, et al., Appl. Catal. B: Environ 246 (2019) 149–155. doi: 10.1016/j.apcatb.2019.01.037
68. [68]
  H. Yin, J. Yuan, J. Wang, et al., Energy Environ. Sci. 18 (2025) 2231–2242. doi: 10.1039/d4ee05796a
69. [69]
  E.M. Han, W.D. Yu, L.J. Li, et al., Chem. Commun. 57 (2021) 2792–2795. doi: 10.1039/d1cc00019e
1. [1]
  Jiaqi Ma , Lan Li , Yiming Zhang , Jinjie Qian , Xusheng Wang . Covalent organic frameworks: Synthesis, structures, characterizations and progress of photocatalytic reduction of CO2. Chinese Journal of Structural Chemistry, 2024, 43(12): 100466-100466. doi: 10.1016/j.cjsc.2024.100466
2. [2]
  Weixu Li , Yuexin Wang , Lin Li , Xinyi Huang , Mengdi Liu , Bo Gui , Xianjun Lang , Cheng Wang . Promoting energy transfer pathway in porphyrin-based sp2 carbon-conjugated covalent organic frameworks for selective photocatalytic oxidation of sulfide. Chinese Journal of Structural Chemistry, 2024, 43(7): 100299-100299. doi: 10.1016/j.cjsc.2024.100299
3. [3]
  Jia-Cheng Hou , Wei Cai , Hong-Tao Ji , Li-Juan Ou , Wei-Min He . Recent advances in semi-heterogenous photocatalysis in organic synthesis. Chinese Chemical Letters, 2025, 36(2): 110469-. doi: 10.1016/j.cclet.2024.110469
4. [4]
  Zhen Shi , Wei Jin , Yuhang Sun , Xu Li , Liang Mao , Xiaoyan Cai , Zaizhu Lou . Interface charge separation in Cu2CoSnS4/ZnIn2S4 heterojunction for boosting photocatalytic hydrogen production. Chinese Journal of Structural Chemistry, 2023, 42(12): 100201-100201. doi: 10.1016/j.cjsc.2023.100201
5. [5]
  Qiang Zhang , Weiran Gong , Huinan Che , Bin Liu , Yanhui Ao . S doping induces to promoted spatial separation of charge carriers on carbon nitride for efficiently photocatalytic degradation of atrazine. Chinese Journal of Structural Chemistry, 2023, 42(12): 100205-100205. doi: 10.1016/j.cjsc.2023.100205
6. [6]
  Ziruo Zhou , Wenyu Guo , Tingyu Yang , Dandan Zheng , Yuanxing Fang , Xiahui Lin , Yidong Hou , Guigang Zhang , Sibo Wang . Defect and nanostructure engineering of polymeric carbon nitride for visible-light-driven CO2 reduction. Chinese Journal of Structural Chemistry, 2024, 43(3): 100245-100245. doi: 10.1016/j.cjsc.2024.100245
7. [7]
  Mengjun Zhao , Yuhao Guo , Na Li , Tingjiang Yan . Deciphering the structural evolution and real active ingredients of iron oxides in photocatalytic CO2 hydrogenation. Chinese Journal of Structural Chemistry, 2024, 43(8): 100348-100348. doi: 10.1016/j.cjsc.2024.100348
8. [8]
  Jiangqi Ning , Junhan Huang , Yuhang Liu , Yanlei Chen , Qing Niu , Qingqing Lin , Yajun He , Zheyuan Liu , Yan Yu , Liuyi Li . Alkyl-linked TiO2@COF heterostructure facilitating photocatalytic CO2 reduction by targeted electron transport. Chinese Journal of Structural Chemistry, 2024, 43(12): 100453-100453. doi: 10.1016/j.cjsc.2024.100453
9. [9]
  Yanghanbin Zhang , Dongxiao Wen , Wei Sun , Jiahe Peng , Dezhong Yu , Xin Li , Yang Qu , Jizhou Jiang . State-of-the-art evolution of g-C3N4-based photocatalytic applications: A critical review. Chinese Journal of Structural Chemistry, 2024, 43(12): 100469-100469. doi: 10.1016/j.cjsc.2024.100469
10. [10]
  Tianhao Li , Wenguang Tu , Zhigang Zou . In situ photocatalytically enhanced thermogalvanic cells for electricity and hydrogen production. Chinese Journal of Structural Chemistry, 2024, 43(1): 100195-100195. doi: 10.1016/j.cjsc.2023.100195
11. [11]
  Guixu Pan , Zhiling Xia , Ning Wang , Hejia Sun , Zhaoqi Guo , Yunfeng Li , Xin Li . Preparation of high-efficient donor-π-acceptor system with crystalline g-C3N4 as charge transfer module for enhanced photocatalytic hydrogen evolution. Chinese Journal of Structural Chemistry, 2024, 43(12): 100463-100463. doi: 10.1016/j.cjsc.2024.100463
12. [12]
  Yue Pan , Wenping Si , Yahao Li , Haotian Tan , Ji Liang , Feng Hou . Promoting exciton dissociation by metal ion modification in polymeric carbon nitride for photocatalysis. Chinese Chemical Letters, 2024, 35(12): 109877-. doi: 10.1016/j.cclet.2024.109877
13. [13]
  Shujun Ning , Zhiyuan Wei , Zhening Chen , Tianmin Wu , Lu Zhang . Curvature and defect formation synergistically promote the photocatalysis of ZnO slabs. Chinese Chemical Letters, 2025, 36(7): 111057-. doi: 10.1016/j.cclet.2025.111057
14. [14]
  Chaoqun Ma , Yuebo Wang , Ning Han , Rongzhen Zhang , Hui Liu , Xiaofeng Sun , Lingbao Xing . Carbon dot-based artificial light-harvesting systems with sequential energy transfer and white light emission for photocatalysis. Chinese Chemical Letters, 2024, 35(4): 108632-. doi: 10.1016/j.cclet.2023.108632
15. [15]
  Jing Wang , Zenghui Li , Xiaoyang Liu , Bochao Su , Honghong Gong , Chao Feng , Guoping Li , Gang He , Bin Rao . Fine-tuning redox ability of arylene-bridged bis(benzimidazolium) for electrochromism and visible-light photocatalysis. Chinese Chemical Letters, 2024, 35(9): 109473-. doi: 10.1016/j.cclet.2023.109473
16. [16]
  Yusong Bi , Rongzhen Zhang , Kaikai Niu , Shengsheng Yu , Hui Liu , Lingbao Xing . Construction of a three-step sequential energy transfer system with selective enhancement of superoxide anion radicals for photocatalysis. Chinese Chemical Letters, 2025, 36(5): 110311-. doi: 10.1016/j.cclet.2024.110311
17. [17]
  Yan Fan , Jiao Tan , Cuijuan Zou , Xuliang Hu , Xing Feng , Xin-Long Ni . Unprecedented stepwise electron transfer and photocatalysis in supramolecular assembly derived hybrid single-layer two-dimensional nanosheets in water. Chinese Chemical Letters, 2025, 36(4): 110101-. doi: 10.1016/j.cclet.2024.110101
18. [18]
  Lihua Ma , Song Guo , Zhi-Ming Zhang , Jin-Zhong Wang , Tong-Bu Lu , Xian-Shun Zeng . Sensitizing photoactive metal–organic frameworks via chromophore for significantly boosting photosynthesis. Chinese Chemical Letters, 2024, 35(5): 108661-. doi: 10.1016/j.cclet.2023.108661
19. [19]
  Xiao-Ya Yuan , Cong-Cong Wang , Bing Yu . Recent advances in FeCl₃-photocatalyzed organic reactions via hydrogen-atom transfer. Chinese Chemical Letters, 2024, 35(9): 109517-. doi: 10.1016/j.cclet.2024.109517
20. [20]
  Rongxin Zhu , Shengsheng Yu , Xuanzong Yang , Ruyu Zhu , Hui Liu , Kaikai Niu , Lingbao Xing . Construction of pyrene-based hydrogen-bonded organic frameworks as photocatalysts for photooxidation of styrene in water. Chinese Chemical Letters, 2024, 35(10): 109539-. doi: 10.1016/j.cclet.2024.109539

Get Citation

PDF

XML

Metrics

PDF Downloads(0)
Abstract views(7)
HTML views(1)

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142