Citation: Zhuo Li, Peng Yu, Di Shen, Xinxin Zhang, Zhijian Liang, Baoluo Wang, Lei Wang. Low-loading Pt anchored on molybdenum carbide-based polyhedral carbon skeleton for enhancing pH-universal hydrogen production[J]. Chinese Chemical Letters, ;2025, 36(4): 109713. doi: 10.1016/j.cclet.2024.109713 shu

Low-loading Pt anchored on molybdenum carbide-based polyhedral carbon skeleton for enhancing pH-universal hydrogen production

Zhuo Li ^{a, 1} ,
Peng Yu ^{b, 1} ,
Di Shen ^a ,
Xinxin Zhang ^a ,
Zhijian Liang ^a ,
Baoluo Wang ^a ,
Lei Wang ^{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.
Key Laboratory for Photonic and Electronic Bandgap Materials, Ministry of Education, School of Physics and Electronic Engineering, Harbin Normal University, Harbin 150025, China

wanglei0525@hlju.edu.cn

Received Date: 4 February 2024
Revised Date: 19 February 2024
Accepted Date: 1 March 2024
Available Online: 11 March 2024

Figures(7)

Developing high-efficient and low-loading Pt based catalyst is significant for the electrocatalytic pH-universal hydrogen evolution reaction (HER). Herein, the molybdenum carbide nanoparticles supported on the polyhedral N-doped carbon nanotube skeleton (MoC/NCT) composite has been synthesized by a pyrolysis of polyacid organo-metallic phosphate framework precursor. Then, only 2.15 wt% Pt are loaded on the MoC/NCT to form Pt-MoC/NCT catalyst, which performs superior HER activity and stability in entire pH range. Specially, the overpotentials of 22 and 74 mV are respectively attained at 10 mA/cm² in 1.0 mol/L KOH and 0.5 mol/L H₂SO₄ electrolytes, approaching or even exceeding commercial Pt/C. More importantly, it can be used as excellent catalyst for efficient hydrogen production at 0–14 pH range. Density functional theory (DFT) calculations demonstrate that the interaction between MoC and Pt leads to the electron redistribution at the corresponding interfaces and the downward shift of the d-band centers, thus optimizing H* adsorption and desorption for promoting the HER activity. Besides, the unique three-dimensional network structure is conductive to the transmission of mass and electrons. In the application of both alkaline and acidic electrolysers, only 1.52 V voltage of solar panel can drive a hydrogen production current density of 10 mA/cm².
- Organo-metallic phosphate framework,
- Low-Pt electrocatalyst,
- Wide-pH,
- Hydrogen evolution reaction,
- Water electrolysis
1. [1]
  Y. Gu, A.P. Wu, Y.Q. Jiao, et al., Angew. Chem. Int. Ed. 60 (2021) 6673–6681. doi: 10.1002/anie.202016102
2. [2]
  T.T. Chao, W.B. Xie, Y.M. Hu, et al., Energy Environ. Sci. 17 (2024) 1397–1406. doi: 10.1039/d3ee02760k
3. [3]
  Y. Cheng, H.Y. Chen, L.F. Zhang, et al., Adv. Mater. 36 (2024) 202313156.
4. [4]
  Y.Q. He, F. Yan, X. Zhang, et al., Adv. Energy Mater. 13 (2023) 2204177. doi: 10.1002/aenm.202204177
5. [5]
  Y.H. Li, C.K. Peng, H.M. Hu, et al., Nat. Commun. 13 (2022) 2204177.
6. [6]
  M.H. Ning, F.H. Zhang, L.B. Wu, et al., Energy Environ. Sci. 15 (2022) 3945–3957. doi: 10.1039/d2ee01094a
7. [7]
  N.K. Oh, J. Seo, S. Lee, et al., Nat. Commun. 12 (2021) 4606. doi: 10.1038/s41467-021-24829-8
8. [8]
  Z.H. Wang, D.L. Liu, Y. Zhang, et al., Appl. Phys. Lett. 123 (2023) 083901. doi: 10.1063/5.0156504
9. [9]
  M.Q. Liu, J.A. Wang, W. Klysubun, et al., Nat. Commun. 12 (2021) 5260. doi: 10.1038/s41467-021-25647-8
10. [10]
  L.G. Li, S.H. Liu, C.H. Zhan, et al., Energy Environ. Sci. 16 (2023) 157–166. doi: 10.1039/D2EE02076A
11. [11]
  T. Liu, P. Li, N. Yao, et al., Angew. Chem. Int. Ed. 58 (2019) 4679–4684. doi: 10.1002/anie.201901409
12. [12]
  M.Y. Wu, X.L. Fan, W.B. Zhang, et al., Chin. Chem. Lett. 35 (2024) 109258. doi: 10.1016/j.cclet.2023.109258
13. [13]
  Y.P. Zhu, K. Fan, C.S. Hsu, et al., Adv. Mater. 35 (2023) 2301133. doi: 10.1002/adma.202301133
14. [14]
  L.M. Wang, L.L. Zhang, W. Ma, et al., Adv. Funct. Mater. 32 (2022) 2203342. doi: 10.1002/adfm.202203342
15. [15]
  Q. Zhou, Q.H. Bian, L.L. Liao, et al., Chin. Chem. Lett. 34 (2023) 107248. doi: 10.1016/j.cclet.2022.02.053
16. [16]
  L.Y. Zeng, Z.L. Zhao, Q.Z. Huang, et al., J. Am. Chem. Soc. 145 (2023) 21432–21441. doi: 10.1021/jacs.3c06863
17. [17]
  Z.P. Wang, Z.P. Lin, Y.L. Wang, et al., Adv. Mater. 35 (2023) 2302007. doi: 10.1002/adma.202302007
18. [18]
  Y.P. Li, W.T. Wang, M.Y. Cheng, et al., Adv. Mater. 35 (2023) 2206351. doi: 10.1002/adma.202206351
19. [19]
  Y.Q. Sun, K. Xu, Z.H. Zhao, et al., Appl. Catal. B: Environ. 278 (2020) 119284. doi: 10.1016/j.apcatb.2020.119284
20. [20]
  Q.S. Gao, W.B. Zhang, Z.P. Shi, L.C. Yang, Y. Tang, Adv. Mater. 31 (2019) 1802880. doi: 10.1002/adma.201802880
21. [21]
  H.S. Hu, Z.R. Zhang, Y.W. Zhang, et al., Energy Environ. Sci. 16 (2023) 4584–4592. doi: 10.1039/d3ee01541f
22. [22]
  L.Q. Wang, Z.P. Xu, C.H. Kuo, J. Peng, et al., Angew. Chem. Int. Ed. 62 (2023) e202311937. doi: 10.1002/anie.202311937
23. [23]
  J. Wang, T. Liao, Z.Z. Wei, et al., Small Methods 5 (2021) 2000988. doi: 10.1002/smtd.202000988
24. [24]
  T.F. Li, T.Y. Lu, X. Li, et al., ACS Nano 15 (2021) 20032–20041. doi: 10.1021/acsnano.1c07694
25. [25]
  Y.J. Zhang, R.H. Lu, C. Wang, Y. Zhao, L.M. Qi, Adv. Funct. Mater. 33 (2023) 2303073. doi: 10.1002/adfm.202303073
26. [26]
  X.N. Zang, W.S. Chen, X.L. Zou, et al., Adv. Mater. 30 (2018) 1805188. doi: 10.1002/adma.201805188
27. [27]
  W.Q. Han, J. Ning, Y. Long, et al., Adv. Energy Mater. 13 (2023) 2300145. doi: 10.1002/aenm.202300145
28. [28]
  L.B. Wu, F.H. Zhang, S.W. Song, et al., Adv. Mater. 34 (2022) 2201774. doi: 10.1002/adma.202201774
29. [29]
  H.M. Jiang, L.T. Yan, S. Zhang, et al., Nano-Micro Lett. 13 (2021) 215. doi: 10.1007/s40820-021-00737-w
30. [30]
  Y.F. Ma, M. Chen, H.B. Geng, et al., Adv. Funct. Mater. 30 (2020) 2000561. doi: 10.1002/adfm.202000561
31. [31]
  J.B. Wu, J.W. Su, T. Wu, et al., Adv. Mater. 35 (2023) 2209954. doi: 10.1002/adma.202209954
32. [32]
  M.H. Hu, B.C. Liu, H.Y. Chen, et al., Appl. Catal. B: Environ. 322 (2023) 122131. doi: 10.1016/j.apcatb.2022.122131
33. [33]
  C. Wan, Y.N. Regmi, B.M. Leonard, Angew. Chem. Int. Ed. 53 (2014) 6407–6410. doi: 10.1002/anie.201402998
34. [34]
  M. Zhou, X.L. Jiang, W.J. Kong, et al., Nano-Micro Lett. 15 (2023) 166. doi: 10.1007/s40820-023-01135-0
35. [35]
  Y. Yang, Y.M. Qian, Z.P. Luo, et al., Nat. Commun. 13 (2022) 7225. doi: 10.1038/s41467-022-34976-1
36. [36]
  C.F. Yang, R. Zhao, H. Xiang, et al., Nano Energy 98 (2022) 107232. doi: 10.1016/j.nanoen.2022.107232
37. [37]
  W. Wang, Y.X. Wu, Y.X. Lin, et al., Adv. Funct. Mater. 32 (2022) 2108464. doi: 10.1002/adfm.202108464
38. [38]
  M. Chen, L.H. Hu, L. Xu, et al., Small Methods 7 (2023) 2300308. doi: 10.1002/smtd.202300308
39. [39]
  X. Liu, L. Wang, G.Y. Zhang, et al., Chem. Eng. J. 414 (2021) 127569.
40. [40]
  T. Ouyang, Y.Q. Ye, C.Y. Wu, K. Xiao, Z.Q. Liu, Angew. Chem. Int. 58 (2019) 4923–4928. doi: 10.1002/anie.201814262
41. [41]
  X. Huang, J. Wang, H.B. Tao, et al., J. Catal. 389 (2020) 461–467. doi: 10.1016/j.jcat.2020.06.020
42. [42]
  P. Liu, X. Zhang, J. Fei, et al., Adv. Mater. 36 (2024) e2310591. doi: 10.1002/adma.202310591
43. [43]
  A. Mosallanezhad, C. Wei, P.A. Koudakan, et al., Appl. Catal. B: Environ. 315 (2022) 121534.
1. [1]
  Haibin Yang , Duowen Ma , Yang Li , Qinghe Zhao , Feng Pan , Shisheng Zheng , Zirui Lou . Mo doped Ru-based cluster to promote alkaline hydrogen evolution with ultra-low Ru loading. Chinese Journal of Structural Chemistry, 2023, 42(11): 100031-100031. doi: 10.1016/j.cjsc.2023.100031
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]
  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
4. [4]
  Weiping Xiao , Yuhang Chen , Qin Zhao , Danil Bukhvalov , Caiqin Wang , Xiaofei Yang . Constructing the synergistic active sites of nickel bicarbonate supported Pt hierarchical nanostructure for efficient hydrogen evolution reaction. Chinese Chemical Letters, 2024, 35(12): 110176-. doi: 10.1016/j.cclet.2024.110176
5. [5]
  Xiangyuan Zhao , Jinjin Wang , Jinzhao Kang , Xiaomei Wang , Hong Yu , Cheng-Feng Du . Ni nanoparticles anchoring on vacuum treated Mo2TiC2Tx MXene for enhanced hydrogen evolution activity. Chinese Journal of Structural Chemistry, 2023, 42(10): 100159-100159. doi: 10.1016/j.cjsc.2023.100159
6. [6]
  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
7. [7]
  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
8. [8]
  Ji Chen , Yifan Zhao , Shuwen Zhao , Hua Zhang , Youyu Long , Lingfeng Yang , Min Xi , Zitao Ni , Yao Zhou , Anran Chen . Heterogeneous bimetallic oxides/phosphides nanorod with upshifted d band center for efficient overall water splitting. Chinese Chemical Letters, 2024, 35(9): 109268-. doi: 10.1016/j.cclet.2023.109268
9. [9]
  Ziyang Yin , Lingbin Xie , Weinan Yin , Ting Zhi , Kang Chen , Junan Pan , Yingbo Zhang , Jingwen Li , Longlu Wang . Advanced development of grain boundaries in TMDs from fundamentals to hydrogen evolution application. Chinese Chemical Letters, 2024, 35(5): 108628-. doi: 10.1016/j.cclet.2023.108628
10. [10]
  Bin Dong , Ning Yu , Qiu-Yue Wang , Jing-Ke Ren , Xin-Yu Zhang , Zhi-Jie Zhang , Ruo-Yao Fan , Da-Peng Liu , Yong-Ming Chai . Double active sites promoting hydrogen evolution activity and stability of CoRuOH/Co₂P by rapid hydrolysis. Chinese Chemical Letters, 2024, 35(7): 109221-. doi: 10.1016/j.cclet.2023.109221
11. [11]
  Yanan Zhou , Li Sheng , Lanlan Chen , Wenhua Zhang , Jinlong Yang . Axial coordinated iron-nitrogen-carbon as efficient electrocatalysts for hydrogen evolution and oxygen redox reactions. Chinese Chemical Letters, 2025, 36(1): 109588-. doi: 10.1016/j.cclet.2024.109588
12. [12]
  Xinyu Hou , Xuelian Yu , Meng Liu , Hengxing Peng , Lijuan Wu , Libing Liao , Guocheng Lv . Ultrafast synthesis of Mo₂N with highly dispersed Ru for efficient alkaline hydrogen evolution. Chinese Chemical Letters, 2025, 36(4): 109845-. doi: 10.1016/j.cclet.2024.109845
13. [13]
  Ping Wang , Ting Wang , Ming Xu , Ze Gao , Hongyu Li , Bowen Li , Yuqi Wang , Chaoqun Qu , Ming Feng . Keplerate polyoxomolybdate nanoball mediated controllable preparation of metal-doped molybdenum disulfide for electrocatalytic hydrogen evolution in acidic and alkaline media. Chinese Chemical Letters, 2024, 35(7): 108930-. doi: 10.1016/j.cclet.2023.108930
14. [14]
  Lanfang Wang , Jiangnan Lv , Yujia Li , Yanqing Hao , Wenjiao Liu , Hui Zhang , Xiaohong Xu . One-step synthesis of nanowoven ball-like NiS-WS₂ for high-efficiency hydrogen evolution. Chinese Chemical Letters, 2025, 36(1): 109597-. doi: 10.1016/j.cclet.2024.109597
15. [15]
  Gu Gong , Mengzhu Li , Ning Sun , Ting Zhi , Yuhao He , Junan Pan , Yuntao Cai , Longlu Wang . Versatile oxidized variants derived from TMDs by various oxidation strategies and their applications. Chinese Chemical Letters, 2024, 35(6): 108705-. doi: 10.1016/j.cclet.2023.108705
16. [16]
  Xiaoli Deng , Xiangchao Lu , Yang Cao , Qianjin Chen . Electrochemical imaging uncovers the heterogeneity of HER activity by sulfur vacancies in molybdenum disulfide monolayer. Chinese Chemical Letters, 2025, 36(3): 110379-. doi: 10.1016/j.cclet.2024.110379
17. [17]
  Chuyuan Lin , Hui Lin , Lingxing Zeng . Optimization strategy for rechargeable Zn metal batteries over wide-pH aqueous electrolytes. Chinese Journal of Structural Chemistry, 2025, 44(1): 100407-100407. doi: 10.1016/j.cjsc.2024.100407
18. [18]
  Hongliang Zeng , Yuan Ji , Jinfeng Wen , Xu Li , Tingting Zheng , Qiu Jiang , Chuan Xia . Pt nanocluster-catalyzed hydrogen evolution reaction: Recent advances and future outlook. Chinese Chemical Letters, 2025, 36(3): 109686-. doi: 10.1016/j.cclet.2024.109686
19. [19]
  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
20. [20]
  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

Get Citation

PDF

XML

Metrics

PDF Downloads(2)
Abstract views(88)
HTML views(11)

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