单原子铁在硫化钼上的组装及电催化析氢

doi:10.11896/cldb.21100048

材料导报

2023, Vol. 37

Issue (11): 21100048-5 https://doi.org/10.11896/cldb.21100048

无机非金属及其复合材料

单原子铁在硫化钼上的组装及电催化析氢

秦超, 张鑫, 周奕伦, 孟则达, 刘守清

苏州科技大学化学与生命科学学院,江苏省环境功能材料重点实验室,江苏苏州 215009

Assembly of Single-atom Iron on Molybdenum Disulfide and Electrocatalytic Hydrogen Evolution Reaction

QIN Chao, ZHANG Xin, ZHOU Yilun, MENG Zeda, LIU Shouqing

School of Chemistry and Life Science, Jiangsu Key Laboratory of Environmental Functional Materials, Suzhou University of Science and Technology, Suzhou 215009, Jiangsu, China

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摘要贵金属Pt具有最高的析氢活性,但其高昂的价格限制了大面积推广应用。因此,研究开发高活性、低成本的析氢电催化材料,对发展氢能产业具有重要意义。利用二步水热反应法成功制备单原子铁-硫化钼(Fe-MoS₂)电催化材料,并采用X-射线粉末衍射(XRD)、高角环形暗场扫描透射电子显微镜(HAADF-STEM)成像技术、能量色散X射线光谱(EDX)、电子能谱测定(XPS)对Fe-MoS₂进行了表征。XRD结果表明,所制备Fe-MoS₂样品的粉末衍射曲线与晶态2H-MoS₂的标准卡(JCPDS 37-1492)相一致,表明Fe-MoS₂与2H-MoS₂具有相同的晶型结构;球差电镜分析表明,铁单原子均匀分布于MoS₂表面;EDX与XPS分析进一步表明铁单原子存在于MoS₂结构中。采用线性扫描伏安(LSV)法研究了Fe-MoS₂的析氢性能。结果表明,最佳条件下制备的Fe-MoS₂,其析氢过电位在电流密度为10 mA/cm²时仅为101 mV,而纯MoS₂在相同条件下的析氢过电位为462 mV, 其过电位降低了361 mV;纯MoS₂的塔菲尔斜率为433 mV/dec,而单原子Fe-MoS₂的塔菲尔斜率仅为64 mV/dec。以乙二胺四乙酸(EDTA)和F-离子为探针分子,测试析氢电催化活性位点。结果表明,在KOH溶液中加入强配位能力的EDTA,其析氢过电位迅速升高,显示铁单原子是析氢电催化剂。机理研究表明,Fe-MoS₂的析氢机理为Volmer-Heyrovsky机理。

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关键词: 铁单原子硫化钼组装电催化剂析氢

Abstract: The precious metal Pt has the highest hydrogen evolution activity, but its high price limits its widespread application. Therefore, the research and development of high-activity and low-cost hydrogen evolution electrocatalytic materials is of great significance to the development of the hydrogen energy industry. In this work, a two-step hydrothermal reaction method was used to successfully assemble single-atoms of Fe on molybdenum sulfide, prepared ofresulting in single-atoms of Fe on MoS₂ to form Fe-MoS₂ electrocatalytic hydrogen evolution material. X-ray powder diffraction (XRD), high-angle annular dark field scanning transmission electron microscopy (HAADF-STEM), energy dispersive X-ray spectroscopy (EDX) and electron spectroscopy (XPS) were used to characterize and analyze the synthesized Fe-MoS₂. XRD results showed that the powder diffraction patterns of the as-synthesized Fe-MoS₂ sample are consistent with that of crystalline 2H-MoS₂ (JCPDS 37-1492), indicating that Fe-MoS₂ and 2H-MoS₂ have the same crystal structure;Spherical aberration electron microscope displayed single-atoms of iron were uniformly dispersed on MoS₂;EDX and XPS analysis further showed that the single iron atoms exist on the MoS₂ structure.The hydrogen evolution performance of Fe-MoS₂ was studied by linear sweep voltammetry (LSV).The results showed that the Fe-MoS₂ synthesized under the optimal conditions has a hydrogen evolution overpotential of only 101 mV at the current density of 10 mA·cm^-2, whereas the hydrogen evolution overpotential of pure MoS₂ under the same conditions is 462 mV, its overpotential is reduced by 361 mV. The Tafel slope of pure MoS₂ is 433 mV/dec, while that of single-atom Fe-MoS₂ is only 64 mV/dec. EDTA and F-ion were used as probe molecules to test the active sites of hydrogen evolution, the results show that the hydrogen evolution overpotential rises rapidly, when EDTA and F ions were added to 1.0 mol/L KOH solution. It is concluded that single atoms of iron are active sites for HER. In addition, studies have shown that the hydrogen evolution mechanism of single-atom Fe-MoS₂ follows the Volmer-Heyrovsky mechanism.

Key words: single-atom iron molybdenum disulfide assembly electrocatalyst hydrogen evolution reaction

出版日期: 2023-06-10 发布日期: 2023-06-19

ZTFLH:

TK91

基金资助: 国家自然科学基金(21576175)

通讯作者: 刘守清,通信作者,苏州科技大学教授,分别于武汉大学和南京大学获得理学硕士学位和博士学位,2003—2004年在日本国立物质材料研究所从事博士后研究。现已在Carbon、Chemical Engineering Journal、Journal of Hazardous Materials、Electrochimica Acta、Biosensors & Bioelectronics、《物理化学》《催化学报》等期刊上发表 80多篇学术论文。申请国家发明专利52项,获得授权发明专利35项,转让专利10项。刘守清教授是国家自然科学基金委员会基金项目函评专家、教育部学位中心学位论文评审专家、国家高新技术企业评审专家。其团队的研究方向和研究领域为电催化材料制氢、燃料电池、可充电电池、电化学发光、光催化及压电催化等。

作者简介: 秦超,苏州科技大学硕士研究生。2015—2019年就读于辽宁科技大学金属材料专业,本科期间多次荣获校级奖学金、校三好学生等荣誉称号,并获得学士学位。2019年至今,在苏州科技大学攻读材料学专业硕士研究生,其研究方向是电催化材料的合成与电催化制氢。现已发表一篇期刊论文。

引用本文:

秦超, 张鑫, 周奕伦, 孟则达, 刘守清. 单原子铁在硫化钼上的组装及电催化析氢[J]. 材料导报, 2023, 37(11): 21100048-5.
QIN Chao, ZHANG Xin, ZHOU Yilun, MENG Zeda, LIU Shouqing. Assembly of Single-atom Iron on Molybdenum Disulfide and Electrocatalytic Hydrogen Evolution Reaction. Materials Reports, 2023, 37(11): 21100048-5.

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http://www.mater-rep.com/CN/10.11896/cldb.21100048 或 http://www.mater-rep.com/CN/Y2023/V37/I11/21100048

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