熔融盐法制备Mo2CTx MXene及其电催化析氢性能

引用本文: 李玉琼, 兰冰, 管斌, 代春龙, 张帆, 林紫锋. 熔融盐法制备Mo₂CT_x MXene及其电催化析氢性能[J]. 物理化学学报, 2024, 40(9): 230603. doi: 10.3866/PKU.WHXB202306031 shu

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

熔融盐法制备Mo₂CT_x MXene及其电催化析氢性能

李玉琼 ^1, ,
兰冰 ^2, ,
管斌 ^1, ,
代春龙 ^1, ,
张帆 ^2, ,
林紫锋 ^{1,
,}

1.
四川大学材料科学与工程学院, 成都 610065;
2.
四川大学化学学院, 成都 610065

通讯作者: 林紫锋,Email:linzifeng@scu.edu.cn

基金项目:
国家自然科学基金(52072252)及四川大学自贡市校地科技合作专项资金(2022CDZG-16)资助项目

摘要: 钼基MXenes在电化学生物分子传感、电催化和能源储存等领域具有重要应用潜力。然而，制备钼基MXenes的传统方法是使用强腐蚀性HF溶液刻蚀Mo基MAX相(三元层状碳化物)制得，实验危险性高且制备周期长。本文提出通过路易斯酸熔盐法选择性刻蚀Mo₂Ga₂C前驱体制备Mo₂CT_x MXene，降低危险性并大幅提升制备效率，并研究了刻蚀温度和保温时间对Mo₂CT_x MXene物相和微观结构的影响。研究表明，使用HF无法完全刻蚀Mo₂Ga₂C前驱体制得高纯度Mo₂CT_x MXene，而熔融盐法在600 °C下仅需30 min即实现完全刻蚀。此外，熔融盐法制备的Mo₂CT_x MXene在碱性电解液中具有优异的电催化析氢(HER)电催化活能，并具有长期稳定性，在10 mA∙cm⁻²的电流密度下有着较低的过电位和Tafel斜率，分别为114 mV和124 mV∙dec⁻¹。

关键词:

English

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
Accepted Date: 19 July 2023
Revised Date: 19 July 2023
Available Online: 09 August 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).

Abstract: 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.

Key words:

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1.
沈阳化工大学材料科学与工程学院沈阳 110142

熔融盐法制备Mo₂CT_x MXene及其电催化析氢性能

通讯作者: 林紫锋,Email:linzifeng@scu.edu.cn

English

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

Corresponding author: Zifeng Lin, linzifeng@scu.edu.cn

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