Citation: Yuqiong Li, Bing Lan, Bin Guan, Chunlong Dai, Fan Zhang, Zifeng Lin. Molten Salt Derived Mo₂CT_x MXene with Excellent Catalytic Performance for Hydrogen Evolution Reaction[J]. Acta Physico-Chimica Sinica, ;2024, 40(9): 230603. doi: 10.3866/PKU.WHXB202306031 shu

Molten Salt Derived Mo₂CT_x MXene with Excellent Catalytic Performance for Hydrogen Evolution Reaction

Yuqiong Li ¹ ,
Bing Lan ² ,
Bin Guan ¹ ,
Chunlong Dai ¹ ,
Fan Zhang ² ,
Zifeng Lin ^1,,

1.
College of Materials Science and Engineering, Sichuan University, Chengdu 610065, China;
2.
College of Chemistry, Sichuan University, Chengdu 610065, China

Corresponding author: Zifeng Lin, linzifeng@scu.edu.cn
Received Date: 20 June 2023
Revised Date: 19 July 2023
Accepted Date: 19 July 2023

Fund Project: The project was supported by the National Natural Science Foundation of China (52072252) and Sichuan University-Zigong City Science and Technology Cooperation Special Project (2022CDZG-16).

MXenes are two-dimensional metal carbides, nitrides, and carbonitrides that are typically achieved by selectively etching the A-site elements from their corresponding MAX phase precursors. Thanks to the merits including high mechanical stability, excellent conductivity, and a high specific surface area, MXenes have attracted widespread attention in the field of energy storage and conversion. By far, most studies are focus on the synthesis and applications of Ti- or V-based MXenes. Mo-based MXenes, while less investigated due to the difficulty of synthesis, have shown significant potential in various fields, including electrochemical biomolecular sensing, electrocatalysis, and energy storage. The conventional method of preparing Mo-based MXenes involves etching precursors with hazardous HF-containing solutions, which is not only time-consuming but also poses safety risks. In this study, we present a Lewis molten salt synthesis approach to prepare Mo₂CT_x MXene by etching Mo₂Ga₂C precursor that eliminates the need for hazardous HF and significantly reduces the synthesis time. The impact of etching temperature and time on the phase and microstructure of Mo₂CT_x MXene were carefully investigated, and our findings indicate that the Mo₂Ga₂C precursor can be almost fully etched at 600 °C for just 30 min using the molten salt method, which is a challenging feat to achieve using HF etching. Furthermore, it is found that Mo₂CT_x MXene can be obtained in a wide temperature range from 600 to 800 °C with excellent structural stability. Transmission electron microscopy (TEM) and X-ray diffraction (XRD) confirmed the selective etching of Ga atoms from Mo₂Ga₂C and the successful preparation of Mo₂CT_x MXene, and X-ray photoelectron spectroscopy (XPS) suggests the preservation of Mo-C bonds in the Mo₂CT_x layered structure. The hydrogen evolution reaction (HER) performance of Mo₂CT_x MXene prepared by the molten salt method was investigated in alkaline electrolytes. The molten salt derived Mo₂CT_x MXene displayed exceptional catalytic performance for the HER, maintaining long-term stability in alkaline conditions, and exhibiting a low overpotential of only 114 mV and a Tafel slope of 124 mV∙dec⁻¹ at 10 mA∙cm⁻². The much larger double layer capacitance of molten salt derived Mo₂CT_x MXene as compare to the Mo₂Ga₂C precursor suggests that accordion-like structure can greatly increase the electrochemical active sites and thus plays a key role in boosting the catalytic performance.
- Mo₂Ga₂C MAX,
- Mo₂CT_x MXene,
- Molten salt synthesis,
- Hydrogen evolution reaction
1. [1]
  (1) VahidMohammadi, A.; Rosen, J.; Gogotsi, Y. Science 2021, 372, eabf1581. doi: 10.1126/science.abf1581
2. [2]
  (2) Li, X.; Huang, Z.; Shuck, C.E.; Liang, G.; Gogotsi Y.; Zhi, C. Nat. Rev. Chem. 2022, 6, 389. doi: 10.1038/s41570-022-00384-8
3. [3]
  (3) Wang, Y.; Qu, Z.; Geng, S.; Liao, M.; Ye, L.; Shadike, Z.; Zhao, X.; Wang, S.; Xu, Q.; Yuan, B.; et al. Angew. Chem. Int. Ed. 2023, 62, e202304978. doi: 10.1002/anie.202304978
4. [4]
  (4) Wen, C.; Li, X.; Zhang, R.; Xu, C.; You, W.; Liu, Z.; Zhao, B.; Che, R. ACS Nano 2022, 16, 1150. doi: 10.1021/acsnano.1c08957
5. [5]
  (5) Ma, G.; Shao, H.; Xu, J.; Liu, Y.; Huang, Q.; Taberna, P. L.; Simon, P.; Lin, Z. Nat. Commun. 2021, 12, 5085. doi: 10.1038/s41467-021-25306-y
6. [6]
  (6) Lin, Z.; Shao, H.; Xu, K.; Taberna, P. L.; Simon, P. Trends Chem. 2020, 2, 654. doi: 10.1016/j.trechm.2020.04.010
7. [7]
8. [8]
  (8) Naguib, M.; Kurtoglu, M.; Presser, V.; Lu, J.; Niu, J.; Heon, M.; Hultman, L.; Gogotsi, Y.; Barsoum, M. W. Adv. Mater. 2011, 23, 4248. doi: 10.1002/adma.201102306
9. [9]
  (9) Shuck, C. E.; Sarycheva, A.; Anayee, M.; Levitt, A.; Zhu, Y.; Uzun, S.; Balitskiy, V.; Zahorodna, V.; Gogotsi, O.; Gogotsi, Y. Adv. Eng. Mater. 2020, 22, 1901241. doi: 10.1002/adem.201901241
10. [10]
  (10) Naguib, M.; Mochalin, V. N.; Barsoum, M. W.; Gogotsi, Y. Adv. Mater. 2014, 26, 982. doi: 10.1002/adma.201470041
11. [11]
  (11) Yang, X.; Gao, N.; Zhou, S.; Zhao, J. Phys. Chem. Chem. Phys. 2018, 20, 19390. doi: 10.1039/C8CP02635A
12. [12]
  (12) Michalsky, R.; Zhang, Y. J.; Peterson, A. A. ACS Catal. 2014, 4, 1274. doi: 10.1021/cs500056u
13. [13]
  (13) Chen, W. F.; Muckerman, J. T.; Fujita, E. Chem. Commun. 2013, 49, 8896. doi: 10.1039/C3CC44076A
14. [14]
  (14) Vrubel, H.; Hu, X. Angew. Chem. Int. Ed. 2012, 51, 12703. doi: 10.1002/anie.201207111
15. [15]
  (15) Chang, K.; Chen, W. ACS Nano 2011, 5, 4720. doi: 10.1021/nn200659w
16. [16]
  (16) Zribi, R.; Neri, G. Sensors 2020, 20, 5404. doi: 10.3390/s20185404
17. [17]
  (17) Zha, X. H.; Yin, J.; Zhou, Y.; Huang, Q.; Luo, K.; Lang, J.; Francisco, J. S.; He, J.; Du, S. J. Phys. Chem. C 2016, 120, 15082. doi: 10.1021/acs.jpcc.6b04192
18. [18]
  (18) Hu, C.; Lai, C. C.; Tao, Q.; Lu, J.; Halim, J.; Sun, L.; Zhang, J.; Yang, J.; Anasori, B.; Wang, J. Chem. Commun. 2015, 51, 6560. doi: 10.1039/C5CC00980D
19. [19]
  (19) Meshkian, R.; Näslund, L. Å.; Halim, J.; Lu, J.; Barsoum, M. W.; Rosen, J. Scripta Mater. 2015, 108, 147. doi: 10.1016/j.scriptamat.2015.07.003
20. [20]
21. [21]
  (21) Halim, J.; Kota, S.; Lukatskaya, M. R.; Naguib, M.; Zhao, M. Q.; Moon, E. J.; Pitock, J.; Nanda, J.; May, S. J.; Gogotsi, Y. Adv. Funct. Mater. 2016, 26, 3118. doi: 10.1002/adfm.201505328
22. [22]
  (22) Mei, J.; Ayoko, G. A.; Hu, C.; Bell, J. M.; Sun, Z. Sustain. Mater. Technol. 2020, 25, e00156. doi: 10.1016/j.susmat.2020.e00156
23. [23]
  (23) Li, Y.; Shao, H.; Lin, Z.; Lu, J.; Liu, L.; Duployer, B.; Persson, P.; Eklund, P.; Hultman, L.; Li, M.; et al. Nat. Mater. 2020, 19, 894. doi: 10.1038/s41563-020-0657-0
24. [24]
  (24) Sarma, D.; Rao, C. J. Electron. Spectrosc. 1980, 20, 25. doi: 10.1016/0368-2048(80)85003-1
25. [25]
  (25) Toby, B. H. J. Appl. Crystallogr. 2001, 34, 210. doi: 10.1107/S0021889801002242
26. [26]
  (26) Song, H.; Wu, M.; Tang, Z.; Tse, J. S.; Yang, B.; Lu, S. Angew. Chem. Int. Ed. 2021, 60, 7234. doi: 10.1002/anie.202017102
27. [27]
  (27) Wang, C.; Shou, H.; Chen, S.; Wei, S.; Lin, Y.; Zhang, P.; Liu, Z.; Zhu, K.; Guo, X.; Wu, X. Adv. Mater. 2021, 33, 2101015. doi: 10.1002/adma.202101015
28. [28]
  (28) Dong, H.; Xiao, P.; Jin, N.; Wang, B.; Liu, Y.; Lin, Z. ChemElectroChem 2021, 8, 957. doi: 10.1002/celc.202100142
29. [29]
  (29) Cheng, H.; Ding, L. X.; Chen, G. F.; Zhang, L.; Xue, J.; Wang, H. Adv. Mater. 2018, 30, 1803694. doi: 10.1002/adma.201803694
30. [30]
  (30) Yue, X.; Yi, S.; Wang, R.; Zhang, Z.; Qiu, S. J. Mater. Chem. A 2017, 5, 10591. doi: 10.1039/C7TA02655B
31. [31]
  (31) Halim, J.; Cook, K. M.; Naguib, M.; Eklund, P.; Gogotsi, Y.; Rosen, J.; Barsoum, M. W. Appl. Surf. Sci. 2016, 362, 406. doi: 10.1016/j.apsusc.2015.11.089
1. [1]
  Yuchen Guo , Xiangyu Zou , Xueling Wei , Weiwei Bao , Junjun Zhang , Jie Han , Feihong Jia . Fe regulating Ni3S2/ZrCoFe-LDH@NF heterojunction catalysts for overall water splitting. Chinese Journal of Structural Chemistry, 2024, 43(2): 100206-100206. doi: 10.1016/j.cjsc.2023.100206
2. [2]
  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
3. [3]
  Jiao Li , Chenyang Zhang , Chuhan Wu , Yan Liu , Xuejian Zhang , Xiao Li , Yongtao Li , Jing Sun , Zhongmin Su . Defined organic-octamolybdate crystalline superstructures derived Mo₂C@C as efficient hydrogen evolution electrocatalysts. Chinese Chemical Letters, 2024, 35(6): 108782-. doi: 10.1016/j.cclet.2023.108782
4. [4]
  Yue Zhang , Xiaoya Fan , Xun He , Tingyu Yan , Yongchao Yao , Dongdong Zheng , Jingxiang Zhao , Qinghai Cai , Qian Liu , Luming Li , Wei Chu , Shengjun Sun , Xuping Sun . Ambient electrosynthesis of urea from carbon dioxide and nitrate over Mo₂C nanosheet. Chinese Chemical Letters, 2024, 35(8): 109806-. doi: 10.1016/j.cclet.2024.109806
5. [5]
  Heng Chen , Longhui Nie , Kai Xu , Yiqiong Yang , Caihong Fang . 两步焙烧法制备大比表面积和结晶性增强超薄g-C₃N₄纳米片及其高效光催化产H₂O₂. Acta Physico-Chimica Sinica, 2024, 40(11): 2406019-. doi: 10.3866/PKU.WHXB202406019
6. [6]
  Ke Wang , Jia Wu , Shuyi Zheng , Shibin Yin . NiCo Alloy Nanoparticles Anchored on Mesoporous Mo2N Nanosheets as Efficient Catalysts for 5-Hydroxymethylfurfural Electrooxidation and Hydrogen Generation. Chinese Journal of Structural Chemistry, 2023, 42(10): 100104-100104. doi: 10.1016/j.cjsc.2023.100104
7. [7]
  Guoqiang Chen , Zixuan Zheng , Wei Zhong , Guohong Wang , Xinhe Wu . 熔融中间体运输导向合成富氨基g-C₃N₄纳米片用于高效光催化产H₂O₂. Acta Physico-Chimica Sinica, 2024, 40(11): 2406021-. doi: 10.3866/PKU.WHXB202406021
8. [8]
  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
9. [9]
  Jun-Jie Fang , Zheng Liu , Yun-Peng Xie , Xing Lu . Superatomic Ag₅₈ nanoclusters incorporating a [MS₄@Ag₁₂]²⁺ (M = Mo or W) kernel show aggregation-induced emission. Chinese Chemical Letters, 2024, 35(10): 109345-. doi: 10.1016/j.cclet.2023.109345
10. [10]
  Xuanzhu Huo , Yixi Liu , Qiyu Wu , Zhiqiang Dong , Chanzi Ruan , Yanping Ren . Integrated Experiment of “Electrolytic Preparation of Cu₂O and Gasometric Determination of Avogadro’s Constant: Implementation, Results, and Discussion: A Micro-Experiment Recommended for Freshmen in Higher Education at Various Levels Across the Nation. University Chemistry, 2024, 39(3): 302-307. doi: 10.3866/PKU.DXHX202308095
11. [11]
  Yaping Wang , Pengcheng Yuan , Zeyuan Xu , Xiong-Xiong Liu , Shengfa Feng , Mufan Cao , Chen Cao , Xiaoqiang Wang , Long Pan , Zheng-Ming Sun . Ti₃C₂T_x MXene in-situ transformed Li₂TiO₃ interface layer enabling 4.5 V-LiCoO₂/sulfide all-solid-state lithium batteries with superior rate capability and cyclability. Chinese Chemical Letters, 2024, 35(6): 108776-. doi: 10.1016/j.cclet.2023.108776
12. [12]
  Xinpeng LIU , Liuyang ZHAO , Hongyi LI , Yatu CHEN , Aimin WU , Aikui LI , Hao HUANG . Ga₂O₃ coated modification and electrochemical performance of Li_1.2Mn_0.54Ni_0.13Co_0.13O₂ cathode material. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1105-1113. doi: 10.11862/CJIC.20230488
13. [13]
  Min LI , Xianfeng MENG . Preparation and microwave absorption properties of ZIF-67 derived Co@C/MoS₂ nanocomposites. Chinese Journal of Inorganic Chemistry, 2024, 40(10): 1932-1942. doi: 10.11862/CJIC.20240065
14. [14]
  Lei Wan , Yizhou Tong , Xi Lu , Yao Fu . Cobalt-catalyzed reductive alkynylation to construct C(sp)-C(sp³) and C(sp)-C(sp²) bonds. Chinese Chemical Letters, 2024, 35(7): 109283-. doi: 10.1016/j.cclet.2023.109283
15. [15]
  Tong Su , Yue Wang , Qizhen Zhu , Mengyao Xu , Ning Qiao , Bin Xu . Multiple conductive network for KTi₂(PO₄)₃ anode based on MXene as a binder for high-performance potassium storage. Chinese Chemical Letters, 2024, 35(8): 109191-. doi: 10.1016/j.cclet.2023.109191
16. [16]
  Jiajun Wang , Guolin Yi , Shengling Guo , Jianing Wang , Shujuan Li , Ke Xu , Weiyi Wang , Shulai Lei . Computational design of bimetallic TM₂@g-C₉N₄ electrocatalysts for enhanced CO reduction toward C₂ products. Chinese Chemical Letters, 2024, 35(7): 109050-. doi: 10.1016/j.cclet.2023.109050
17. [17]
  Yongheng Ren , Yang Chen , Hongwei Chen , Lu Zhang , Jiangfeng Yang , Qi Shi , Lin-Bing Sun , Jinping Li , Libo Li . Electrostatically driven kinetic Inverse CO2/C2H2 separation in LTA-type zeolites. Chinese Journal of Structural Chemistry, 2024, 43(10): 100394-100394. doi: 10.1016/j.cjsc.2024.100394
18. [18]
  Dong-Xue Jiao , Hui-Li Zhang , Chao He , Si-Yu Chen , Ke Wang , Xiao-Han Zhang , Li Wei , Qi Wei . Layered (C5H6ON)2[Sb2O(C2O4)3] with a large birefringence derived from the uniform arrangement of π-conjugated units. Chinese Journal of Structural Chemistry, 2024, 43(6): 100304-100304. doi: 10.1016/j.cjsc.2024.100304
19. [19]
  Wenhao Chen , Muxuan Wu , Han Chen , Lue Mo , Yirong Zhu . Cu₂Se@C thin film with three-dimensional braided structure as a cathode material for enhanced Cu²⁺ storage. Chinese Chemical Letters, 2024, 35(5): 108698-. doi: 10.1016/j.cclet.2023.108698
20. [20]
  Yi Luo , Lin Dong . Multicomponent remote C(sp²)-H bond addition by Ru catalysis: An efficient access to the alkylarylation of 2H-imidazoles. Chinese Chemical Letters, 2024, 35(10): 109648-. doi: 10.1016/j.cclet.2024.109648

Get Citation

PDF

XML

Metrics

PDF Downloads(0)
Abstract views(558)
HTML views(52)

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

Molten Salt Derived Mo2CTx MXene with Excellent Catalytic Performance for Hydrogen Evolution Reaction

Metrics

通讯作者: 陈斌, bchen63@163.com

Molten Salt Derived Mo₂CT_x MXene with Excellent Catalytic Performance for Hydrogen Evolution Reaction