Citation: Wenting Li, Nina Wu, Chengze Li, Jin Guo, Guangxun Zhang, Huan Pang. Facet engineering of NH₂-MIL-125(Ti) for enhanced synergistic adsorption and photocatalysis reduction of U(Ⅵ) under visible light[J]. Chinese Chemical Letters, ;2026, 37(4): 110733. doi: 10.1016/j.cclet.2024.110733 shu

Facet engineering of NH₂-MIL-125(Ti) for enhanced synergistic adsorption and photocatalysis reduction of U(Ⅵ) under visible light

Wenting Li ^a ,
Nina Wu ^a ,
Chengze Li ^a ,
Jin Guo ^a ,
Guangxun Zhang ^a ,
Huan Pang ^{a, b, *,}

a.
School of Chemistry and Chemical Engineering, Yangzhou University, Yangzhou 225002, China
b.
State Key Laboratory of Coordination Chemistry, Nanjing University, Nanjing 210023, China

panghuan@yzu.edu.cn

Received Date: 4 November 2024
Revised Date: 28 November 2024
Accepted Date: 5 December 2024
Available Online: 6 December 2024

Figures(6)

Modulating the exposed facets of metal-organic frameworks (MOFs) is an effective strategy to enhance the synergistic effects between adsorption and photocatalytic reduction of U(Ⅵ). Herein, we successfully synthesized four morphologically distinct types of NH₂-MIL-125(Ti), offering insights into the impact of facet engineering on the combined adsorption and photoreduction of U(Ⅵ). An elevated exposure ratio of the {001} facet endows NH₂-MIL-125(Ti) with a larger surface area, enhanced light absorption, and efficient separation of photogenerated charge carriers. Among the four photocatalysts (W, D, S and T), T with a high proportion of {001} facets, demonstrated outstanding adsorption-photocatalytic synergy, achieving over 97% of U(Ⅵ) within 20 min of visible light irradiation across a broad concentrations and pH range, without requiring a hole-trapping agent. The uranium extraction mechanism involves U(Ⅵ) coordination and chelation with active sites during adsorption, followed by reduction to U(Ⅳ) via photogenerated electrons during photocatalysis. This study highlights the use of facet engineering to enhance adsorption and photocatalytic efficiency in MOF-based photocatalysts.
- NH₂-MIL-125(Ti),
- Photocatalytic reduction,
- Adsorption,
- Facet engineering,
- U(Ⅵ)
1. [1]
  Y.J. Lim, K. Goh, A. Goto, Y. Zhao, R. Wang, J. Mater. Chem. A 11 (2023) 22551–22589. doi: 10.1039/d3ta05099h
2. [2]
  Z. Niu, Z. Fan, T. Pham, et al., Angew. Chem. Int. Ed. 61 (2022) e202117807. doi: 10.1002/anie.202117807
3. [3]
  M. Chen, T. Liu, S. Tang, et al., Chem. Eng. J. 446 (2022) 137264. doi: 10.1016/j.cej.2022.137264
4. [4]
  T. Liu, J. Yuan, B. Zhang, et al., Environ. Sci. Technol. 53 (2019) 14612–14619. doi: 10.1021/acs.est.9b06790
5. [5]
  S.K. Raj, A.J. Carrier, B.C. Youden, et al., Chem. Eng. J. 492 (2024) 152341. doi: 10.1016/j.cej.2024.152341
6. [6]
  G. Wang, G.M. Shi, S. Zhang, J. Hazard. Mater. 457 (2023) 131822. doi: 10.1016/j.jhazmat.2023.131822
7. [7]
  B.K. Sahu, B.C. Pattnayak, S. Mohapatra, Desalination 581 (2024) 117611. doi: 10.1016/j.desal.2024.117611
8. [8]
  N. Smječanin, M. Nuhanović, J. Sulejmanović, E. Mašić, F. Sher, Chemosphere 313 (2023) 137488. doi: 10.1016/j.chemosphere.2022.137488
9. [9]
  F. Gao, J. Bai, H. Yan, et al., Chem. Eng. J. 485 (2024) 149822. doi: 10.1016/j.cej.2024.149822
10. [10]
  C. Zhang, Y. Wang, Y.L. Liu, et al., Chem. Eng. J. 485 (2024) 149856. doi: 10.1016/j.cej.2024.149856
11. [11]
  B. Wang, C. Bao, J. Xu, Y et al., Chem. Eng. J. 486 (2024) 150251. doi: 10.1016/j.cej.2024.150251
12. [12]
  E. Hu, Q. Chen, Q. Gao, et al., Adv. Funct. Mater. 34 (2024) 2312215. doi: 10.1002/adfm.202312215
13. [13]
  J. Pan, B. Xiao, W. Zhu, et al., Nano. Res. 17 (2024) 6713–6720. doi: 10.1007/s12274-024-6654-x
14. [14]
  K. Yu, L. Tang, X. Cao, et al., Adv. Funct. Mater. 32 (2022) 2200315. doi: 10.1002/adfm.202200315
15. [15]
  T. Chen, T. Liu, L. Zhou, et al., Appl. Catal. B: Environ. 318 (2022) 121815. doi: 10.1016/j.apcatb.2022.121815
16. [16]
  X. Ma, K.R. Meihaus, Y. Yang, et al., J. Am. Chem. Soc. 146 (2024) 23566–23573. doi: 10.1021/jacs.4c07699
17. [17]
  Y. Qian, F. Zhang, H. Pang, Adv. Funct. Mater. 31 (2021) 2104231. doi: 10.1002/adfm.202104231
18. [18]
  Z. Qian, R. Zhang, Y. Xiao, et al., Adv. Energy. Mater. 13 (2023) 2300086. doi: 10.1002/aenm.202300086
19. [19]
  P. Dong, K. Gao, L. Zhang, et al., Appl. Catal. B: Environ. Energy 357 (2024) 124297. doi: 10.1016/j.apcatb.2024.124297
20. [20]
  K. Xu, S. Zhang, X. Zhuang, et al., Adv. Colloid. Interf. 323 (2024) 103050. doi: 10.1016/j.cis.2023.103050
21. [21]
  S.W. Lv, Y. Cong, X. Chen, W. Wang, L. Che, Chem. Eng. J. 433 (2022) 133605. doi: 10.1016/j.cej.2021.133605
22. [22]
  K. Sun, H.L. Jiang, Nat. Chem. 16 (2024) 1580–1581. doi: 10.1038/s41557-024-01607-9
23. [23]
  W. Gong, Y. Geng, P. Gao, et al., J. Am. Chem. Soc. 146 (2024) 21806–21814. doi: 10.1021/jacs.4c06046
24. [24]
  L. Li, X.S. Wang, T.F. Liu, J. Ye, Small Methods 4 (2020) 2000486. doi: 10.1002/smtd.202000486
25. [25]
  C. Zhu, Q. Tian, S. Wan, et al., Chem. Eng. J. 497 (2024) 154689. doi: 10.1016/j.cej.2024.154689
26. [26]
  H. Dong, X. Zhang, Y. Lu, et al., Appl. Catal. B: Environ. 276 (2020) 119173. doi: 10.1016/j.apcatb.2020.119173
27. [27]
  J. Huang, Y. Li, R.K. Huang, et al., Angew. Chem. Int. Ed. 57 (2018) 4632–4636. doi: 10.1002/anie.201801029
28. [28]
  S. Bai, L. Wang, Z. Li, Y. Xiong, Adv. Sci. 4 (2016) 1600216.
29. [29]
  J. Wan, D. Liu, H. Xiao, et al., Chem. Commun. 56 (2020) 4316–4319. doi: 10.1039/d0cc00700e
30. [30]
  X. Yuan, Q. Mu, S. Xue, et al., J. Energy. Chem. 60 (2021) 202–208. doi: 10.1016/j.jechem.2020.12.025
31. [31]
  X.Y. Zhang, P. Wang, Y. Zhang, X.M. Cheng, W.Y. Sun, ACS Appl. Mater. Interfaces 15 (2023) 3348–3356. doi: 10.1021/acsami.2c19236
32. [32]
  X.M. Cheng, Y. Gu, X.Y. Zhang, et al., Appl. Catal. B: Environ. 298 (2021) 120524. doi: 10.1016/j.apcatb.2021.120524
33. [33]
  L. Liu, S. Du, Y. Xiao, et al., Appl. Catal. B: Environ. 338 (2023) 123094. doi: 10.1016/j.apcatb.2023.123094
34. [34]
  Y. Zheng, Z. Duan, R. Liang, et al., ChemSusChem 15 (2022) e202200216. doi: 10.1002/cssc.202200216
35. [35]
  C. Fu, F. Li, J. Zhang, et al., Angew. Chem. Int. Ed. 60 (2021) 6160–6169. doi: 10.1002/anie.202014037
36. [36]
  A. Wang, S. Wu, J. Dong, et al., Chem. Eng. J. 404 (2021) 127145. doi: 10.1016/j.cej.2020.127145
37. [37]
  Y. Gao, Q. Wu, X. Liang, et al., Adv. Sci. 7 (2020) 1902820. doi: 10.1002/advs.201902820
38. [38]
  J. Pan, G. Liu, G.Q. Lu, H.M. Cheng, Angew. Chem. Int. Ed. 50 (2011) 2133–2137. doi: 10.1002/anie.201006057
39. [39]
  M. Oveisi, M.A. Asli, N.M. Mahmoodi, J. Hazard. Mater. 347 (2018) 123–140. doi: 10.1016/j.jhazmat.2017.12.057
40. [40]
  S.N. Kim, J. Kim, H.Y. Kim, H.Y. Cho, W.S. Ahn, Catal. Today 204 (2013) 85–93. doi: 10.7583/jkgs.2013.13.3.85
41. [41]
  Y. Fu, D. Sun, Y. Chen, et al., Angew. Chem. Int. Ed. 51 (2012) 3364–3367. doi: 10.1002/anie.201108357
42. [42]
  W. Zhu, P. Liu, S. Xiao, et al., Appl. Catal. B: Environ. 172-173 (2015) 46–51. doi: 10.1016/j.apcatb.2015.02.003
43. [43]
  Q. Huang, Y. Hu, Y. Pei, J. Zhang, M. Fu, Appl. Catal. B: Environ. 259 (2019) 118106. doi: 10.1016/j.apcatb.2019.118106
44. [44]
  R. Liang, L. Shen, F. Jing, et al., Appl. Catal. B: Environ. 162 (2015) 245–251. doi: 10.1016/j.apcatb.2014.06.049
45. [45]
  G. Mo, L. Wang, J. Luo, Sep. Purif. Technol. 277 (2021) 119643. doi: 10.1016/j.seppur.2021.119643
46. [46]
  A.M. Katzenmeyer, J. Canivet, G. Holland, D. Farrusseng, A. Centrone, Angew. Chem. Int. Ed. 53 (2014) 2852–2856. doi: 10.1002/anie.201309295
47. [47]
  X. Li, Z. Le, X. Chen, et al., Appl. Catal. B: Environ. 236 (2018) 501–508. doi: 10.1016/j.apcatb.2018.05.052
48. [48]
  S. Chen, G. Hai, H. Gao, et al., Chem. Eng. J. 406 (2021) 126886. doi: 10.1016/j.cej.2020.126886
49. [49]
  H. Wang, X. Yuan, Y. Wu, et al., J. Hazard. Mater. 286 (2015) 187–194. doi: 10.1007/s10008-014-2598-5
50. [50]
  J. Wang, A.S. Cherevan, C. Hannecart, et al., Appl. Catal. B: Environ. 283 (2021) 119626. doi: 10.1016/j.apcatb.2020.119626
51. [51]
  S. Chen, F. Yang, H. Gao, et al., J. CO2. Util. 48 (2021) 101528. doi: 10.1016/j.jcou.2021.101528
52. [52]
  L. Yuan, C. Zhang, Y. Zou, et al., Adv. Funct. Mater. 33 (2023) 2214627. doi: 10.1002/adfm.202214627
53. [53]
  Z.B. Fang, T.T. Liu, J. Liu, et al., J. Am. Chem. Soc. 142 (2020) 12515–12523. doi: 10.1021/jacs.0c05530
54. [54]
  B. Tu, K. Yu, D. Fu, et al., Appl. Catal. B: Environ. 337 (2023) 122965. doi: 10.1016/j.apcatb.2023.122965
55. [55]
  P. Liang, L. Yuan, K. Du, et al., Chem. Eng. J. 420 (2021) 129831. doi: 10.1016/j.cej.2021.129831
56. [56]
  K. Sun, M. Liu, J. Pei, et al., Angew. Chem. Int. Ed. 59 (2020) 22749–22755. doi: 10.1002/anie.202011614
57. [57]
  Z. Gao, J. Wang, Y. Muhammad, et al., Chem. Eng. J. 388 (2020) 124389. doi: 10.1016/j.cej.2020.124389
58. [58]
  Z. Feng, H. Fu, Z. Wang, et al., Sep. Purif. Technol. 351 (2024) 128102. doi: 10.1016/j.seppur.2024.128102
59. [59]
  C. Yu, J. Lu, Z. Hou, et al., Sep. Purif. Technol. 255 (2021) 117727. doi: 10.1016/j.seppur.2020.117727
60. [60]
  R. Jiang, G. Lu, Z. Yan, et al., Chem. Eng. J. 374 (2019) 79–90. doi: 10.1016/j.cej.2019.05.176
61. [61]
  L. Yang, X. Luo, L. Yan, et al., Carbohyd. Polym. 285 (2022) 119157. doi: 10.1016/j.carbpol.2022.119157
62. [62]
  S.Y. Chen, J.P. Yu, Z.F. Chai, W.Q. Shi, L.Y. Yuan, Chem. Eng. J. 460 (2023) 141742. doi: 10.1016/j.cej.2023.141742
63. [63]
  J. Yu, H. Zhang, Q. Liu, et al., Chem. Eng. J. 471 (2023) 144705. doi: 10.1016/j.cej.2023.144705
64. [64]
  W. Liu, Z. Yang, B. Zou, et al., Chem. Eng. J. 466 (2023) 143117. doi: 10.1016/j.cej.2023.143117
65. [65]
  M. Li, R. Wang, T. Liu, et al., Sep. Purif. Technol. 309 (2023) 123121. doi: 10.1016/j.seppur.2023.123121
66. [66]
  R. Wang, M. Li, T. Liu, et al., J. Clean. Prod. 364 (2022) 114373.
67. [67]
  J. Wang, Y. Wang, W. Wang, et al., Environ. Pollut. 262 (2020) 114373. doi: 10.1016/j.envpol.2020.114373
68. [68]
  L. Zhang, Y. Yang, N. Zhao, et al., J. Mater. Chem. A 12 (2024) 9651–9660. doi: 10.1039/d3ta07710a
69. [69]
  X. Gong, L. Tang, R. Wang, et al., Chem. Eng. J. 450 (2022) 138044. doi: 10.1016/j.cej.2022.138044
70. [70]
  Z. Lu, G. Zhou, B. Li, et al., Appl. Catal. B: Environ. 301 (2022) 120787. doi: 10.1016/j.apcatb.2021.120787
71. [71]
  J. Lei, H. Liu, C. Yuan, et al., Chem. Eng. J. 416 (2021) 129164. doi: 10.1016/j.cej.2021.129164
72. [72]
  J. Xu, S. He, H. Zhang, et al., J. Mater. Chem. A 3 (2015) 24261–24271. doi: 10.1039/C5TA06838J
73. [73]
  Y. Liu, D. Cui, T. Zhang, et al., Chem. Eng. J. 497 (2024) 154416. doi: 10.1016/j.cej.2024.154416
1. [1]
  Maosen Xu , Pengfei Zhu , Qinghong Cai , Meichun Bu , Chenghua Zhang , Hong Wu , Youzhou He , Min Fu , Siqi Li , Xingyan Liu . In-situ fabrication of TiO₂/NH₂−MIL-125(Ti) via MOF-driven strategy to promote efficient interfacial effects for enhancing photocatalytic NO removal activity. Chinese Chemical Letters, 2024, 35(10): 109524-. doi: 10.1016/j.cclet.2024.109524
2. [2]
  Shouchao Zhong , Yue Wang , Mingshu Xie , Yiqian Wu , Jiuqiang Li , Jing Peng , Liyong Yuan , Maolin Zhai , Weiqun Shi . Radiation reduction modification of sp² carbon-conjugated covalent organic frameworks for enhanced photocatalytic chromium(VI) removal. Chinese Chemical Letters, 2025, 36(5): 110312-. doi: 10.1016/j.cclet.2024.110312
3. [3]
  Zixuan Zhu , Xianjin Shi , Yongfang Rao , Yu Huang . Recent progress of MgO-based materials in CO₂ adsorption and conversion: Modification methods, reaction condition, and CO₂ hydrogenation. Chinese Chemical Letters, 2024, 35(5): 108954-. doi: 10.1016/j.cclet.2023.108954
4. [4]
  Yue Li , Minghao Fan , Conghui Wang , Yanxun Li , Xiang Yu , Jun Ding , Lei Yan , Lele Qiu , Yongcai Zhang , Longlu Wang . 3D layer-by-layer amorphous MoS_x assembled from [Mo₃S₁₃]^2- clusters for efficient removal of tetracycline: Synergy of adsorption and photo-assisted PMS activation. Chinese Chemical Letters, 2024, 35(9): 109764-. doi: 10.1016/j.cclet.2024.109764
5. [5]
  Xiangyang Ji , Yishuang Chen , Peng Zhang , Shaojia Song , Jian Liu , Weiyu Song . Boosting the first C–H bond activation of propane on rod-like V/CeO₂ catalyst by photo-assisted thermal catalysis. Chinese Chemical Letters, 2025, 36(5): 110719-. doi: 10.1016/j.cclet.2024.110719
6. [6]
  Zhemi Xu , Haolin Cui , Shule Zhang , Peiyuan Guan , Tianhao Ji , Jin Yan , Qianyu Li , Dewei Chu , Yunxuan Weng , Zhimin Ao , Yang Liu , Jian Jin . Facet engineering of metal-organic frameworks enables high piezoelectricity and piezocatalysis: A case study of ZIF-8. Chinese Chemical Letters, 2026, 37(4): 111667-. doi: 10.1016/j.cclet.2025.111667
7. [7]
  Xiaojuan Sun , Ke Kong , Jun Liang , Dan Wang , Beibei Dong , Ruihu Wang . Periodic Janus structure based on ionic covalent organic framework for selective removal of perfluoroalkyl substances. Chinese Journal of Structural Chemistry, 2025, 44(9): 100652-100652. doi: 10.1016/j.cjsc.2025.100652
8. [8]
  Hong-Rui Li , Xia Kang , Rui Gao , Miao-Miao Shi , Bo Bi , Ze-Yu Chen , Jun-Min Yan . Interfacial interactions of Cu/MnOOH enhance ammonia synthesis from electrochemical nitrate reduction. Chinese Chemical Letters, 2025, 36(2): 109958-. doi: 10.1016/j.cclet.2024.109958
9. [9]
  Haodong Wang , Xiaoxu Lai , Chi Chen , Pei Shi , Houzhao Wan , Hao Wang , Xingguang Chen , Dan Sun . Novel 2D bifunctional layered rare-earth hydroxides@GO catalyst as a functional interlayer for improved liquid-solid conversion of polysulfides in lithium-sulfur batteries. Chinese Chemical Letters, 2024, 35(5): 108473-. doi: 10.1016/j.cclet.2023.108473
10. [10]
  Hui Liu , Baoying Xiao , Yaming Zhao , Wei Wang , Qiong Jia . Adsorption of heavy metals with hyper crosslinked polymers: Progress, challenges and perspectives. Chinese Chemical Letters, 2025, 36(8): 110619-. doi: 10.1016/j.cclet.2024.110619
11. [11]
  Jiaxuan Wang , Tonghe Liu , Bingxiang Wang , Ziwei Li , Yuzhong Niu , Hou Chen , Ying Zhang . Synthesis of polyhydroxyl-capped PAMAM dendrimer/silica composites for the adsorption of aqueous Hg(II) and Ag(I). Chinese Chemical Letters, 2024, 35(12): 109900-. doi: 10.1016/j.cclet.2024.109900
12. [12]
  Fengxing Liang , Yongzheng Zhu , Nannan Wang , Meiping Zhu , Huibing He , Yanqiu Zhu , Peikang Shen , Jinliang Zhu . Recent advances in copper-based materials for robust lithium polysulfides adsorption and catalytic conversion. Chinese Chemical Letters, 2024, 35(11): 109461-. doi: 10.1016/j.cclet.2023.109461
13. [13]
  Congyan Liu , Xueyao Zhou , Fei Ye , Bin Jiang , Bo Liu . Confined electric field in nano-sized channels of ionic porous framework towards unique adsorption selectivity. Chinese Chemical Letters, 2025, 36(2): 109969-. doi: 10.1016/j.cclet.2024.109969
14. [14]
  Huazhe Wang , Chenghuan Qiao , Chuchu Chen , Bing Liu , Juanshan Du , Qinglian Wu , Xiaochi Feng , Shuyan Zhan , Wan-Qian Guo . Synergistic adsorption and singlet oxygenation of humic acid on alkali-activated biochar via peroxymonosulfate activation. Chinese Chemical Letters, 2025, 36(5): 110244-. doi: 10.1016/j.cclet.2024.110244
15. [15]
  Chong Liu , Nanthi Bolan , Anushka Upamali Rajapaksha , Hailong Wang , Paramasivan Balasubramanian , Pengyan Zhang , Xuan Cuong Nguyen , Fayong Li . Critical review of biochar for the removal of emerging inorganic pollutants from wastewater. Chinese Chemical Letters, 2025, 36(2): 109960-. doi: 10.1016/j.cclet.2024.109960
16. [16]
  Ping Wang , Chunmao Chen , Hongwei Ren , Erhong Duan . A review of carbon dots in synthesis strategies, photoluminescence mechanisms, and applications in wastewater treatment. Chinese Chemical Letters, 2025, 36(9): 110725-. doi: 10.1016/j.cclet.2024.110725
17. [17]
  Yaohua Wu , Yihong Chen , Juanshan Du , Huazhe Wang , Chuchu Chen , Wenrui Jia , Yongqi Liang , Qinglian Wu , Wan-Qian Guo . Ice-assisted synthesis of functional materials: Strategies and environmental applications. Chinese Chemical Letters, 2025, 36(12): 110944-. doi: 10.1016/j.cclet.2025.110944
18. [18]
  Linshan Peng , Qihang Peng , Tianxiang Jin , Zhirong Liu , Yong Qian . Highly efficient capture of thorium ion by citric acid-modified chitosan gels from aqueous solution. Chinese Chemical Letters, 2024, 35(5): 108891-. doi: 10.1016/j.cclet.2023.108891
19. [19]
  Xiao-Hong Yi , Chong-Chen Wang . Metal-organic frameworks on 3D interconnected macroporous sponge foams for large-scale water decontamination: A mini review. Chinese Chemical Letters, 2024, 35(5): 109094-. doi: 10.1016/j.cclet.2023.109094
20. [20]
  Dan Luo , Jinya Tian , Jianqiao Zhou , Xiaodong Chi . Anthracene-bridged "Texas-sized" box for the simultaneous detection and uptake of tryptophan. Chinese Chemical Letters, 2024, 35(9): 109444-. doi: 10.1016/j.cclet.2023.109444

Get Citation

PDF

XML

Metrics

PDF Downloads(0)
Abstract views(95)
HTML views(10)

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

Facet engineering of NH2-MIL-125(Ti) for enhanced synergistic adsorption and photocatalysis reduction of U(Ⅵ) under visible light

Metrics

通讯作者: 陈斌, bchen63@163.com

Facet engineering of NH₂-MIL-125(Ti) for enhanced synergistic adsorption and photocatalysis reduction of U(Ⅵ) under visible light