Citation: Yamei Li, Ryuhei Nakamura. Structural change of molybdenum sulfide facilitates the electrocatalytic hydrogen evolution reaction at neutral pH as revealed by in situ Raman spectroscopy[J]. Chinese Journal of Catalysis, ;2018, 39(3): 401-406. doi: 10.1016/S1872-2067(17)62945-0 shu

Structural change of molybdenum sulfide facilitates the electrocatalytic hydrogen evolution reaction at neutral pH as revealed by in situ Raman spectroscopy

Yamei Li ^a, ,
Ryuhei Nakamura ^a,b

a Biofunctional Catalyst Research Team, RIKEN Center for Sustainable Resource Science(CSRS), 2-1 Hirosawa, Wako, Saitama 351-0198, Japan;
b Earth-Life Science Institute(ELSI), Tokyo Institute of Technology, 2-12-1-I7 E Ookayama, Meguro-ku, Tokyo 152-8550, Japan

Received Date: 27 September 2017
Revised Date: 26 October 2017

Fund Project: This work was supported by a JSPS Grant-in-Aid for Scientific Research (26288092).

Molybdenum sulfides are promising electrocatalysts for the hydrogen evolution reaction (HER). S-and Mo-related species have been proposed as the active site for forming adsorbed hydrogen to initiate the HER; however, the nature of the interaction between Mo centers and S ligands is unclear. Further, the development of cost-effective water-splitting systems using neutral water as a proton source for H₂ evolution is highly desirable, whereas the mechanism of the HER at neutral pH is rarely discussed. Here, the structural change in the Mo-Mo and S-S species in a synthesized molybdenum sulfide was monitored at neutral pH using in situ electrochemical Raman spectroscopy. Analysis of the potential dependent Raman spectra revealed that the band assigned to a terminal S-S species emerged along with synchronized changes in the frequency of the Mo-Mo, Mo₃-μ₃S, and Mo-S vibrational bands. This indicates that Mo-Mo bonds and terminal S-S ligands play synergistic roles in facilitating hydrogen evolution, likely via the internal reorganization of trinuclear Mo₃-thio species. The nature and role of metal-ligand interactions in the HER revealed in this study demonstrated a mechanism that is distinct from those reported previously in which the S or Mo sites function independently.
- Hydrogen evolution reaction,
- Molybdenum sulfide,
- Electrocatalyst,
- In-situ Raman spectroscopy,
- Artificial photosynthesis,
- Clean energy
1. [1]
2. [2]
3. [3]
4. [4]
5. [5]
6. [6]
7. [7]
8. [8]
9. [9]
10. [10]
11. [11]
12. [12]
13. [13]
14. [14]
15. [15]
16. [16]
17. [17]
18. [18]
19. [19]
20. [20]
21. [21]
22. [22]
23. [23]
24. [24]
25. [25]
26. [26]
27. [27]
28. [28]
29. [29]
30. [30]
31. [31]
32. [32]
33. [33]
1. [1]
  Haodong JIN , Qingqing LIU , Chaoyang SHI , Danyang WEI , Jie YU , Xuhui XU , Mingli XU . NiCu/ZnO heterostructure photothermal electrocatalyst for efficient hydrogen evolution reaction. Chinese Journal of Inorganic Chemistry, 2025, 41(6): 1068-1082. doi: 10.11862/CJIC.20250048
2. [2]
  Qi Wang , Yuqing Liu , Jiefei Wang , Yuan-Yuan Ma , Jing Du , Zhan-Gang Han . Catalysts for electrocatalytic dechlorination of chlorinated aromatic hydrocarbons: synthetic strategies, applications, and challenges. Acta Physico-Chimica Sinica, 2025, 41(10): 100120-0. doi: 10.1016/j.actphy.2025.100120
3. [3]
  Jia Wang , Qing Qin , Zhe Wang , Xuhao Zhao , Yunfei Chen , Liqiang Hou , Shangguo Liu , Xien Liu . P-Doped Carbon-Supported Zn_xP_yO_z for Efficient Ammonia Electrosynthesis under Ambient Conditions. Acta Physico-Chimica Sinica, 2024, 40(3): 2304044-0. doi: 10.3866/PKU.WHXB202304044
4. [4]
  Ruige ZHANG , Zhe ZHANG , He ZHENG , Zhan SHI . Recent advances of metal-organic frameworks for alkaline electrocatalytic oxygen evolution reaction. Chinese Journal of Inorganic Chemistry, 2025, 41(10): 2011-2028. doi: 10.11862/CJIC.20250185
5. [5]
  Sumiya Akter Dristy , Md Ahasan Habib , Shusen Lin , Mehedi Hasan Joni , Rutuja Mandavkar , Young-Uk Chung , Md Najibullah , Jihoon Lee . Exploring Zn doped NiBP microspheres as efficient and stable electrocatalyst for industrial-scale water splitting. Acta Physico-Chimica Sinica, 2025, 41(7): 100079-0. doi: 10.1016/j.actphy.2025.100079
6. [6]
  Bizhu Shao , Huijun Dong , Yunnan Gong , Jianhua Mei , Fengshi Cai , Jinbiao Liu , Dichang Zhong , Tongbu Lu . Metal-Organic Framework-Derived Nickel Nanoparticles for Efficient CO₂ Electroreduction in Wide Potential Windows. Acta Physico-Chimica Sinica, 2024, 40(4): 2305026-0. doi: 10.3866/PKU.WHXB202305026
7. [7]
  Huafeng SHI . Construction of MnCoNi layered double hydroxide@Co-Ni-S amorphous hollow polyhedron composite with excellent electrocatalytic oxygen evolution performance. Chinese Journal of Inorganic Chemistry, 2025, 41(7): 1380-1386. doi: 10.11862/CJIC.20240378
8. [8]
  Jiajie Li , Xiaocong Ma , Jufang Zheng , Qiang Wan , Xiaoshun Zhou , Yahao Wang . Recent Advances in In-Situ Raman Spectroscopy for Investigating Electrocatalytic Organic Reaction Mechanisms. University Chemistry, 2025, 40(4): 261-276. doi: 10.12461/PKU.DXHX202406117
9. [9]
  Ying Chen , Ronghua Yan , Weiyan Yin . Research Progress on the Synthesis of Metal Single-Atom Catalysts and Their Applications in Electrocatalytic Hydrogen Evolution Reactions. University Chemistry, 2025, 40(9): 344-353. doi: 10.12461/PKU.DXHX202503066
10. [10]
  Qiangqiang SUN , Pengcheng ZHAO , Ruoyu WU , Baoyue CAO . Multistage microporous bifunctional catalyst constructed by P-doped nickel-based sulfide ultra-thin nanosheets for energy-efficient hydrogen production from water electrolysis. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1151-1161. doi: 10.11862/CJIC.20230454
11. [11]
  Wei Sun , Yongjing Wang , Kun Xiang , Saishuai Bai , Haitao Wang , Jing Zou , Arramel , Jizhou Jiang . CoP Decorated on Ti₃C₂T_x MXene Nanocomposites as Robust Electrocatalyst for Hydrogen Evolution Reaction. Acta Physico-Chimica Sinica, 2024, 40(8): 2308015-0. doi: 10.3866/PKU.WHXB202308015
12. [12]
  Lutian Zhao , Yangge Guo , Liuxuan Luo , Xiaohui Yan , Shuiyun Shen , Junliang Zhang . Electrochemical Synthesis for Metallic Nanocrystal Electrocatalysts: Principle, Application and Challenge. Acta Physico-Chimica Sinica, 2024, 40(7): 2306029-0. doi: 10.3866/PKU.WHXB202306029
13. [13]
  Jiapei Zou , Junyang Zhang , Xuming Wu , Cong Wei , Simin Fang , Yuxi Wang . A Comprehensive Experiment Based on Electrocatalytic Nitrate Reduction into Ammonia: Synthesis, Characterization, Performance Exploration, and Applicable Design of Copper-based Catalysts. University Chemistry, 2024, 39(6): 373-382. doi: 10.3866/PKU.DXHX202312081
14. [14]
  Zelong LIANG , Shijia QIN , Pengfei GUO , Hang XU , Bin ZHAO . Synthesis and electrocatalytic CO₂ reduction performance of metal-organic framework catalysts loaded with silver particles. Chinese Journal of Inorganic Chemistry, 2025, 41(1): 165-173. doi: 10.11862/CJIC.20240409
15. [15]
  Wei Zhong , Dan Zheng , Yuanxin Ou , Aiyun Meng , Yaorong Su . Simultaneously Improving Inter-Plane Crystallization and Incorporating K Atoms in g-C₃N₄ Photocatalyst for Highly-Efficient H₂O₂ Photosynthesis. Acta Physico-Chimica Sinica, 2024, 40(11): 2406005-0. doi: 10.3866/PKU.WHXB202406005
16. [16]
  Mian Wei , Chang Cheng , Bowen He , Bei Cheng , Kezhen Qi , Chuanbiao Bie . Inorganic-organic CdS/YBTPy S-scheme photocatalyst for efficient hydrogen production and its mechanism. Acta Physico-Chimica Sinica, 2025, 41(12): 100158-0. doi: 10.1016/j.actphy.2025.100158
17. [17]
  Linjie ZHU , Xufeng LIU . Synthesis, characterization and electrocatalytic hydrogen evolution of two di-iron complexes containing a phosphine ligand with a pendant amine. Chinese Journal of Inorganic Chemistry, 2025, 41(5): 939-947. doi: 10.11862/CJIC.20240416
18. [18]
  Xi YANG , Chunxiang CHANG , Yingpeng XIE , Yang LI , Yuhui CHEN , Borao WANG , Ludong YI , Zhonghao HAN . Co-catalyst Ni₃N supported Al-doped SrTiO₃: Synthesis and application to hydrogen evolution from photocatalytic water splitting. Chinese Journal of Inorganic Chemistry, 2025, 41(3): 440-452. doi: 10.11862/CJIC.20240371
19. [19]
  Kangjuan Cheng , Chunxiao Liu , Youpeng Wang , Qiu Jiang , Tingting Zheng , Xu Li , Chuan Xia . Design of noble metal catalysts and reactors for the electrosynthesis of hydrogen peroxide. Acta Physico-Chimica Sinica, 2025, 41(10): 100112-0. doi: 10.1016/j.actphy.2025.100112
20. [20]
  Jiali Lei , Juan Wang , Wenhui Zhang , Guohong Wang , Zihui Liang , Jinmao Li . TiO₂/CdIn₂S₄ S-scheme heterojunction photocatalyst promotes photocatalytic hydrogen evolution coupled vanillyl alcohol oxidation. Acta Physico-Chimica Sinica, 2025, 41(12): 100174-0. doi: 10.1016/j.actphy.2025.100174

Get Citation

PDF

XML

Metrics

PDF Downloads(11)
Abstract views(2114)
HTML views(129)

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