MOFs衍生的黄铁矿型纳米电催化剂析氧性能研究  

Study on the Electrochemical Oxidation Performance of MOF-derived Pyrite Nano-electrocatalysts

作　　者：韩家生 李芷萌 李杰[1] 凌琪 严魁 张苗[2] 吴明在[1] HAN Jiasheng;LI Zhimeng;LI Jie;LING Qi;YAN Kui;ZHANG Miao;WU Mingzai(Stony Brook Institute,Anhui University,Hefei 230039,China;School of Materials Science and Engineering,Anhui University,Hefei 230601,China)

机构地区：[1]安徽大学纽约石溪学院,安徽合肥230039 [2]安徽大学材料科学与工程学院,安徽合肥230601

出　　处：《金属矿山》2024年第7期261-267,共7页Metal Mine

基　　金：安徽省重点研究与开发计划项目(编号:202104a05020061);安徽大学纽约石溪学院科研发展基金项目(编号:Y010440001)。

摘　　要：廉价、高效且耐用的非贵金属电催化剂的可控制备,对于推动电解水这项能源转换技术的大规模应用至关重要。以水热法制备的MIL-101(Fe)为前驱体,热解得到金属有机框架(MOFs)衍生铁碳化合物,经原位硫化还原,成功制备了纳米黄铁矿型催化剂(MIL-101(Fe)-D-FeS_(2))。采用X射线衍射仪(XRD)、冷场发射式扫描电镜(SEM)、X射线光电子能谱(XPS)对样品进行了物相表征,发现FeS_(2)纳米球均匀衍生在前驱物形成的八面体碳框架上;通过循环伏安法和线性扫描伏安法研究了该材料在电化学反应过程中的可逆性和活性。结果表明:在10 mA/cm^(2)和100 mA/cm^(2)的电流密度下,MIL-101(Fe)-D-FeS_(2)的过电位分别为260 mV和307 mV,双层电容值为3.82 mF/cm^(2),塔菲尔斜率为48.4 mV/dec。该新型催化剂表现出优越的相关性能,优于传统商用电极RuO2和市售黄铁矿粉。此外MIL-101(Fe)-D-FeS_(2)在高电流密度下保持长期的稳定性。这种优异的活性得益于MOFs与FeS_(2)材料的结合,增加催化剂活性位点的暴露,提高整体催化剂的活性和导电性。研究结果为MIL-101(Fe)-D-FeS_(2)型电催化剂的开发和研究提供了新思路。The large-scale use of electrolytic water as an energy conversion technique is contingent upon the carefully managed production of non-precious metal electrocatalysts that are affordable,effective and long-lasting.MIL-101(Fe)was synthesized via a hydrothermal method and employed as a precursor for the production of iron carbon-based metal-organic frameworks(MOFs)through pyrolysis.This iron carbon compound was further transformed into a nano pyrite-type catalyst(MIL-101(Fe)-D-FeS_(2))through in-situ sulfurization reduction.The sample was characterized through X-ray diffraction(XRD),field-emission scanning electron microscopy(SEM)and high-resolution X-ray photoelectron spectroscopy(XPS).The analysis revealed uniform distribution of FeS_(2)nanospheres on the octahedral carbon framework derived from the precursor.Cyclic voltammetry(CV)and linear sweep voltammetry(LSV)were utilized to assess the reversibility and activity of MIL-101(Fe)-D-FeS_(2)in electrochemical reactions.The overpotentials of the material at current densities of 10 mA/cm^(2)and 100 mA/cm^(2)were measured at 260 mV and 307 mV,respectively.Notably,the double-layer capacitance was determined to be 3.82 mF/cm^(2),with a Tafel slope of 48.4 mV/dec.When compared to commercial pyrite powder and the conventional commercial electrode RuO2,the novel catalyst demonstrated better performance metrics.Furthermore,long-term stability is preserved in MIL-101(Fe)-D-FeS_(2)at high current densities.The combination of MOFs and FeS_(2)material,which raises the catalyst active site′s exposure and enhances the catalyst′s overall activity and conductivity,is responsible for this remarkable activity.The findings demonstrate that a novel strategy for the synthesis and investigation of electrocatalysts is provided by the creation of the MIL-101(Fe)-D-FeS_(2)catalyst.

关 键 词：黄铁矿 MOFS 析氧反应 电解水 电催化 

分 类 号：O643[理学—物理化学] O644[理学—化学]