Citation: Hongyang Li, Yue Liu, Xiuwen Wang, Haijing Yan, Guimin Wang, Dongxu Wang, Yilong Wang, Shuo Yang, Yanqing Jiao. Morphology engineering and electronic structure remodeling of manganese-incorporated VN for boosting urea-assisted energy-saving hydrogen production[J]. Chinese Chemical Letters, ;2025, 36(6): 110042. doi: 10.1016/j.cclet.2024.110042 shu

Morphology engineering and electronic structure remodeling of manganese-incorporated VN for boosting urea-assisted energy-saving hydrogen production

Hongyang Li ^a ,
Yue Liu ^a ,
Xiuwen Wang ^b ,
Haijing Yan ^{a, *,} ,
Guimin Wang ^a ,
Dongxu Wang ^a ,
Yilong Wang ^a ,
Shuo Yang ^a ,
Yanqing Jiao ^{a, *,}

a.
Key Laboratory of Functional Inorganic Material Chemistry, Ministry of Education of the People’s Republic of China, Heilongjiang University, Harbin 150080, China
b.
Heilongjiang Provincial Key Laboratory of Surface Active Agent and Auxiliary, School of Chemistry and Chemistry Engineering, Qiqihar University, Qiqihar 161006, China

yanhaijing@hlju.edu.cn

jiaoyanqing@hlju.edu.cn

Received Date: 7 April 2024
Revised Date: 3 May 2024
Accepted Date: 22 May 2024
Available Online: 23 May 2024

Figures(5)

Urea-assisted water electrolysis offers a promising route to reduce energy consumption for hydrogen production and meanwhile treat urea-rich wastewater. Herein, we devised a shear force-involved polyoxometalate-organic supramolecular self-assembly strategy to fabricate 3D hierarchical porous nanoribbon assembly Mn-VN cardoons. A bimetallic polyoxovanadate (POV) with the inherent structural feature of Mn surrounded by [VO₆] octahedrons was introduced to trigger precise Mn incorporation in VN lattice, thereby achieving simultaneous morphology engineering and electronic structure modulation. The lattice contraction of VN caused by Mn incorporation drives electron redistribution. The unique hierarchical architecture with modulated electronic structure that provides more exposed active sites, facilitates mass and charge transfer, and optimizes the associated adsorption behavior. Mn-VN exhibits excellent activity with low overpotentials of 86 mV and 1.346 V at 10 mA/cm² for hydrogen evolution reaction (HER) and urea oxidation reaction (UOR), respectively. Accordingly, in the two-electrode urea-assisted water electrolyzer utilizing Mn-VN as a bifunctional catalyst, hydrogen production can occur at low voltage (1.456 V@10 mA/cm²), which has the advantages of energy saving and competitive durability over traditional water electrolysis. This work provides a simple and mild route to construct nanostructures and modulate electronic structure for designing high-efficiency electrocatalysts.
- Morphology engineering,
- Electronic structure regulation,
- Metal nitrides,
- Hydogen evolution reaction,
- Urea oxidation reaction
1. [1]
  Y. Zhang, J. Liu, S.L. Li, et al., Energy Chem. 1 (2019) 100021. doi: 10.1016/j.enchem.2019.100021
2. [2]
  H.G. Cha, K.S. Choi, Nat. Chem. 7 (2015) 328–333. doi: 10.1038/nchem.2194
3. [3]
  Z.W. Seh, J. Kibsgaard, C.F. Dickens, et al., Science 355 (2017) eaad4998. doi: 10.1126/science.aad4998
4. [4]
  Y.K. Zhang, Y.X. Lin, T. Duan, et al., Mater. Today 48 (2021) 115–134. doi: 10.1016/j.mattod.2021.02.004
5. [5]
  Y. Jiao, Y. Zheng, M. Jaroniec, et al., Chem. Soc. Rev. 44 (2015) 2060–2086. doi: 10.1039/C4CS00470A
6. [6]
  R. Yang, X.Z. Shi, Y.Y. Wang, et al., Chin. Chem. Lett. 33 (2022) 4930–4935. doi: 10.1016/j.cclet.2021.12.058
7. [7]
  G.C. Yang, Y.Q. Jiao, H.J. Yan, et al., Nat. Commun. 13 (2022) s41467.
8. [8]
  S. Xu, X.W. Ruan, M. Ganesan, et al., Adv. Funct. Mater. 34 (2024) 2313309. doi: 10.1002/adfm.202313309
9. [9]
  W.S. Tang, L.N. Zhang, T.Y. Qiu, et al., Angew. Chem. Int. Ed. 62 (2023) e202305843. doi: 10.1002/anie.202305843
10. [10]
  P. Guo, S.F. Cao, W.J. Huang, et al., Adv. Mater. 36 (2024) 2311766. doi: 10.1002/adma.202311766
11. [11]
  S.K. Geng, Y. Zheng, S.Q. Li, Nat. Energy 6 (2021) 904–912. doi: 10.1038/s41560-021-00899-2
12. [12]
  S. Chen, J.J. Duan, A. Vasileff, et al., Angew. Chem. Int. Ed. 55 (2016) 3804–3808. doi: 10.1002/anie.201600387
13. [13]
  X.T. Gao, S. Zhang, P.T. Wang, et al., Chem. Soc. Rev. 53 (2024) 1552–1591. doi: 10.1039/d3cs00963g
14. [14]
  S.L. Wang, J.Y. Zhu, X. Wu, et al., Chin. Chem. Lett. 33 (2022) 1105–1109. doi: 10.1021/acs.orglett.2c00084
15. [15]
  L.W. Lin, S.Q. Piao, Y.J. Choi, et al., Energy Chem. 4 (2022) 100072. doi: 10.1016/j.enchem.2022.100072
16. [16]
  Y. Zhong, D.L. Chao, S.J. Deng, et al., Adv. Funct. Mater. 28 (2018) 1706391. doi: 10.1002/adfm.201706391
17. [17]
  S.Q. Li, X. Sun, Z.H. Yao, et al., Adv. Funct. Mater. 29 (2019) 1904780. doi: 10.1002/adfm.201904780
18. [18]
  W.Q. Jia, B.W. Liu, R. Gong, et al., Small 19 (2023) 2302025. doi: 10.1002/smll.202302025
19. [19]
  Y. Wang, Y.Q. Jiao, H.J. Yan, et al., Angew. Chem. Int. Ed. 61 (2022) e202116233. doi: 10.1002/anie.202116233
20. [20]
  X. Dong, H.J. Yan, Y.Q. Jiao, et al., J. Mater. Chem. A 7 (2019) 15823–15830. doi: 10.1039/c9ta04742e
21. [21]
  H.J. Yan, Y. Xie, A.P. Wu, et al., Adv. Mater. 31 (2019) 1901174. doi: 10.1002/adma.201901174
22. [22]
  M.R. Kandel, U.N. Pan, P.P. Dhakal, et al., Small 20 (2023) 2307241.
23. [23]
  L.X. Dai, Y. Wang, L. Sun, et al., Adv. Sci. 8 (2021) 2004995. doi: 10.1002/advs.202004995
24. [24]
  Y. Liu, L. Bai, Q.Q. Jia, et al., Chin. Chem. Lett. 34 (2023) 107855. doi: 10.1016/j.cclet.2022.107855
25. [25]
  W.M. Li, R. Liu, G.T. Yu, et al., Small 20 (2023) 2307164.
26. [26]
  L. Li, J. Zhou, X. Wang, et al., Adv. Mater. 35 (2023) 2302966. doi: 10.1002/adma.202302966
27. [27]
  F. Chen, F. Yang, C. Sheng, et al., J. Colloid Interface Sci. 626 (2022) 445– 452. doi: 10.1016/j.jcis.2022.06.173
28. [28]
  P. Li, Y.Q. Huang, Q.H. Huang, et al., J. Energy Chem. 87 (2023) 479–490. doi: 10.1016/j.jechem.2023.09.006
29. [29]
  Y.Q. Jiao, H.J. Yan, C.G. Tian, et al., Acc. Mater. Res. 4 (2022) 42–56. doi: 10.1093/ajh/hpab137
30. [30]
  Y.Q. Jiao, H.J. Yan, R.H. Wang, et al., ACS Appl. Mater. Interfaces 12 (2020) 49596–49606. doi: 10.1021/acsami.0c13533
31. [31]
  D. He, L. Cao, L. Feng, et al., Chin. Chem. Lett. 33 (2022) 4781–4785. doi: 10.1016/j.cclet.2022.01.006
32. [32]
  Y.Y. Ma, Z.L. Lang, L.K. Yan, et al., Energ. Environ. Sci. 11 (2018) 2114–2123. doi: 10.1039/c8ee01129j
33. [33]
  Y.C. Bai, H. Zhang, B. Xiang, et al., Nano Energy 89 (2021) 106386. doi: 10.1016/j.nanoen.2021.106386
34. [34]
  Z.X. Xu, X.D. Zhuang, C.Q. Yang, et al., Adv. Mater. 28 (2016) 1981–1987. doi: 10.1002/adma.201505131
35. [35]
  C.R. Xu, J.L. Mu, T. Zhou, et al., Adv. Funct. Mater. 32 (2022) 2206501. doi: 10.1002/adfm.202206501
36. [36]
  Y. Gu, A.P. Wu, Y.Q. Jiao, et al., Angew. Chem. Int. Ed. 60 (2021) 6673– 6681. doi: 10.1002/anie.202016102
37. [37]
  W.L. Li, E.F. Ni, X.H. Li, et al., T. Nonferr. Metal. Soc. 26 (2016) 2372–2379. doi: 10.1016/S1003-6326(16)64375-3
38. [38]
  Y.N. Zhao, W.L. Li, Y.Q. Li, et al., Adv. Funct. Mater. 33 (2023) 2306598. doi: 10.1002/adfm.202306598
39. [39]
  Q. Li, Y.Q. Jiao, Y.Q. Tang, et al., J. Am. Chem. Soc. 145 (2023) 20837–20848. doi: 10.1021/jacs.3c05234
40. [40]
  T.C. Liu, J.X. Ge, Y. Xu, et al., Energy Storage Mater. 32 (2020) 261–271. doi: 10.1016/j.ensm.2020.07.007
41. [41]
  H. Jiang, M.Z. Sun, S.L. Wu, et al., Adv. Funct. Mater. 31 (2021) 2104951. doi: 10.1002/adfm.202104951
42. [42]
  W. Zhang, H.J. Yan, Y. Liu, et al., J. Mater. Chem. A. 11 (2023) 15033–15043. doi: 10.1039/d3ta01789c
43. [43]
  X.M. Li, Q.Y. Hu, H.Y. Wang, et al., Appl. Catal. B 292 (2021) 120172. doi: 10.1016/j.apcatb.2021.120172
44. [44]
  J.Z. Feng, R.X. Tang, G.F. Liu, et al., Chem. Eng. J. 452 (2023) 139131. doi: 10.1016/j.cej.2022.139131
45. [45]
  Y.Q. Jiao, H.J. Yan, D.X. Wang, et al., Sci. China Mater. 65 (2022) 1225–1236. doi: 10.1007/s40843-021-1894-4
46. [46]
  H.J. Yan, Y. Xie, Y.Q. Jiao, et al., Adv. Mater. 30 (2017) 1704156.
47. [47]
  J.C. Hao, Z.C. Zhuang, K.C. Cao, et al., Nat. Commun. 13 (2022) s41467.
48. [48]
  Y. Li, Y.Q. Jiao, H.J. Yan, et al., Angew. Chem. Int. Ed. 62 (2023) e202306640. doi: 10.1002/anie.202306640
49. [49]
  C.C. Li, Y.W. Liu, Z.W. Zhuo, et al., Adv. Energy Mater. 8 (2018) 1801775. doi: 10.1002/aenm.201801775
50. [50]
  M. Yang, Y.M. Jiang, M.J. Qu, et al., Appl. Catal. B 269 (2020) 118803. doi: 10.1016/j.apcatb.2020.118803
51. [51]
  J. Zhang, R.J. Cui, C.C. Gao, et al., Small 15 (2019) 1904688. doi: 10.1002/smll.201904688
52. [52]
  W.B. Li, J.F. Huang, L.L. Feng, et al., J. Mater. Chem. A 5 (2017) 20217–20227. doi: 10.1039/C7TA05205G
1. [1]
  Tao Tang , Chen Li , Sipu Li , Zhong Qiu , Tianqi Yang , Beirong Ye , Shaojun Shi , Chunyang Wu , Feng Cao , Xinhui Xia , Minghua Chen , Xinqi Liang , Xinping He , Xin Liu , Yongqi Zhang . One-step constructing advanced N-doped carbon@metal nitride as ultra-stable electrocatalysts via urea plasma under room temperature. Chinese Chemical Letters, 2024, 35(11): 109887-. doi: 10.1016/j.cclet.2024.109887
2. [2]
  Rui Deng , Wenjie Jiang , Tianqi Yu , Jiali Lu , Boyao Feng , Panagiotis Tsiakaras , Shibin Yin . Cycad-leaf-like crystalline-amorphous heterostructures for efficient urea oxidation-assisted water splitting. Chinese Journal of Structural Chemistry, 2024, 43(7): 100290-100290. doi: 10.1016/j.cjsc.2024.100290
3. [3]
  Wenjie Jiang , Zhixiang Zhai , Xiaoyan Zhuo , Jia Wu , Boyao Feng , Tianqi Yu , Huan Wen , Shibin Yin . Revealing the reactant adsorption role of high-valence WO3 for boosting urea-assisted water splitting. Chinese Journal of Structural Chemistry, 2025, 44(3): 100519-100519. doi: 10.1016/j.cjsc.2025.100519
4. [4]
  Qian-Qian Tang , Li-Fang Feng , Zhi-Peng Li , Shi-Hao Wu , Long-Shuai Zhang , Qing Sun , Mei-Feng Wu , Jian-Ping Zou . Single-atom sites regulation by the second-shell doping for efficient electrochemical CO₂ reduction. Chinese Chemical Letters, 2024, 35(9): 109454-. doi: 10.1016/j.cclet.2023.109454
5. [5]
  Tengjia Ni , Xianbiao Hou , Huanlei Wang , Lei Chu , Shuixing Dai , Minghua Huang . Controllable defect engineering based on cobalt metal-organic framework for boosting oxygen evolution reaction. Chinese Journal of Structural Chemistry, 2024, 43(1): 100210-100210. doi: 10.1016/j.cjsc.2023.100210
6. [6]
  Xiao Li , Wanqiang Yu , Yujie Wang , Ruiying Liu , Qingquan Yu , Riming Hu , Xuchuan Jiang , Qingsheng Gao , Hong Liu , Jiayuan Yu , Weijia Zhou . Metal-encapsulated nitrogen-doped carbon nanotube arrays electrode for enhancing sulfion oxidation reaction and hydrogen evolution reaction by regulating of intermediate adsorption. Chinese Chemical Letters, 2024, 35(8): 109166-. doi: 10.1016/j.cclet.2023.109166
7. [7]
  Fenglin Wang , Chengwei Kuang , Zhicheng Zheng , Dan Wu , Hao Wan , Gen Chen , Ning Zhang , Xiaohe Liu , Renzhi Ma . Noble metal clusters substitution in porous Ni substrate renders high mass-specific activities toward oxygen evolution reaction and methanol oxidation reaction. Chinese Chemical Letters, 2025, 36(6): 109989-. doi: 10.1016/j.cclet.2024.109989
8. [8]
  Guoliang Gao , Guangzhen Zhao , Guang Zhu , Bowen Sun , Zixu Sun , Shunli Li , Ya-Qian Lan . Recent advancements in noble-metal electrocatalysts for alkaline hydrogen evolution reaction. Chinese Chemical Letters, 2025, 36(1): 109557-. doi: 10.1016/j.cclet.2024.109557
9. [9]
  Lizhang Chen , Yu Fang , Mingxin Pang , Ruoxu Sun , Lin Xu , Qixing Zhou , Yawen Tang . Interfacial engineering of core/satellite-structured RuP/RuP2 heterojunctions for enhanced pH-universal hydrogen evolution reaction. Chinese Journal of Structural Chemistry, 2025, 44(1): 100461-100461. doi: 10.1016/j.cjsc.2024.100461
10. [10]
  Xiaoxia WANG , Ya'nan GUO , Feng SU , Chun HAN , Long SUN . Synthesis, structure, and electrocatalytic oxygen reduction reaction properties of metal antimony-based chalcogenide clusters. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1201-1208. doi: 10.11862/CJIC.20230478
11. [11]
  Haoying ZHAI , Lanzong WEN , Wenjie LIAO , Qin LI , Wenjun ZHOU , Kun CAO . Metal-organic framework-derived sulfur-doped iron-cobalt tannate nanorods for efficient oxygen evolution reaction performance. Chinese Journal of Inorganic Chemistry, 2025, 41(5): 1037-1048. doi: 10.11862/CJIC.20240320
12. [12]
  Shiqi Peng , Yongfang Rao , Tan Li , Yufei Zhang , Jun-ji Cao , Shuncheng Lee , Yu Huang . Regulating the electronic structure of Ir single atoms by ZrO₂ nanoparticles for enhanced catalytic oxidation of formaldehyde at room temperature. Chinese Chemical Letters, 2024, 35(7): 109219-. doi: 10.1016/j.cclet.2023.109219
13. [13]
  Xianxu Chu , Lu Wang , Junru Li , Hui Xu . Surface chemical microenvironment engineering of catalysts by organic molecules for boosting electrocatalytic reaction. Chinese Chemical Letters, 2024, 35(8): 109105-. doi: 10.1016/j.cclet.2023.109105
14. [14]
  Mingjie Lei , Wenting Hu , Kexin Lin , Xiujuan Sun , Haoshen Zhang , Ye Qian , Tongyue Kang , Xiulin Wu , Hailong Liao , Yuan Pan , Yuwei Zhang , Diye Wei , Ping Gao . Co/Mn/Mo掺杂加速NiSe₂重构以提高其电催化尿素氧化性能. Acta Physico-Chimica Sinica, 2025, 41(8): 100083-. doi: 10.1016/j.actphy.2025.100083
15. [15]
  Yu-Yao Li , Xiao-Hui Li , Zhi-Xuan An , Yang Chu , Xiu-Li Wang . Room-temperature olefin epoxidation reaction by two 2D cobalt metal-organic complexes under O₂ atmosphere: Coordination and structural regulation. Chinese Chemical Letters, 2025, 36(4): 109716-. doi: 10.1016/j.cclet.2024.109716
16. [16]
  Ziyi Liu , Xunying Liu , Lubing Qin , Haozheng Chen , Ruikai Li , Zhenghua Tang . Alkynyl ligand for preparing atomically precise metal nanoclusters: Structure enrichment, property regulation, and functionality enhancement. Chinese Journal of Structural Chemistry, 2024, 43(11): 100405-100405. doi: 10.1016/j.cjsc.2024.100405
17. [17]
  Yi Zhang , Biao Wang , Chao Hu , Muhammad Humayun , Yaping Huang , Yulin Cao , Mosaad Negem , Yigang Ding , Chundong Wang . Fe–Ni–F electrocatalyst for enhancing reaction kinetics of water oxidation. Chinese Journal of Structural Chemistry, 2024, 43(2): 100243-100243. doi: 10.1016/j.cjsc.2024.100243
18. [18]
  Jing Cao , Dezheng Zhang , Bianqing Ren , Ping Song , Weilin Xu . Mn incorporated RuO₂ nanocrystals as an efficient and stable bifunctional electrocatalyst for oxygen evolution reaction and hydrogen evolution reaction in acid and alkaline. Chinese Chemical Letters, 2024, 35(10): 109863-. doi: 10.1016/j.cclet.2024.109863
19. [19]
  Yi Liu , Peng Lei , Yang Feng , Shiwei Fu , Xiaoqing Liu , Siqi Zhang , Bin Tu , Chen Chen , Yifan Li , Lei Wang , Qing-Dao Zeng . Topologically engineering of π-conjugated macrocycles: Tunable emission and photochemical reaction toward multi-cyclic polymers. Chinese Chemical Letters, 2024, 35(10): 109571-. doi: 10.1016/j.cclet.2024.109571
20. [20]
  Xiaoya Cui , Yanchang Liu , Qiang Li , He Zhu , Shibo Xi , Jianrong Zeng . Ultrafast crystallinity engineering of PtCo₃ alloy for enhanced oxygen reduction reaction. Chinese Chemical Letters, 2025, 36(5): 110069-. doi: 10.1016/j.cclet.2024.110069

Get Citation

PDF

XML

Metrics

PDF Downloads(0)
Abstract views(156)
HTML views(4)

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