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用于析氢反应、析氧反应、超级电容器及直接甲醇燃料电池应用的多功能电极——CTAB修饰的还原氧化石墨烯改性MXene杂化膜的逐层组装

Layer-by-Layer Assembly of CTAB-rGO-Modified MXene Hybrid Films as Multifunctional Electrodes for Hydrogen Evolution and Oxygen Evolution Reactions, Supercapacitors, and DMFC Applications.

作者信息

Raveendran Asha, Chandran Mijun, Siddiqui Masoom Raza, Wabaidur Saikh Mohammad, Eswaran Muthusankar, Dhanusuraman Ragupathy

机构信息

Nano Electrochemistry Lab (NEL), Department of Chemistry, National Institute of Technology Puducherry, Karaikal 609609, India.

Department of Chemistry, Central University of Tamil Nadu, Thiruvarur 610005, India.

出版信息

ACS Omega. 2023 Sep 14;8(38):34768-34786. doi: 10.1021/acsomega.3c03827. eCollection 2023 Sep 26.

Abstract

Exceptional electrical conductivity and abundance of surface terminations like-F- and OH- leading to hydrophilicity make the family of 2D transition metal carbides/nitrides and carbonitrides (MXene) excellent candidates for energy storage and conversion applications. MXenes, however, undergo restacking of nanosheets via van der Waals interaction, hindering the active sites, leading to slow electronic and ionic kinetics, and ultimately affecting their electrochemical performance. Herein, we report binder-free cetyltrimethylammonium bromide-reduced graphene oxide (CTAB-rGO)-modified MXene hybrid films on nickel foam as a promising noble metal-free multifunctional electrode synthesized via layer-by-layer assembly and dip coating techniques, which effectively reduce restacking while improving the kinetics. The properties of the as-prepared electrocatalysts are investigated using various physiochemical characterizations and electrochemical measurements to accomplish the objective of "creating one kind of electrocatalyst for multiapplication" with a thorough understanding of the relationship between the material structure, morphology, and electrocatalytic performance. In energy conversion, the synergetic effect of MXene and the CTAB-rGO support helped increase the catalytic activity of the composite for electrochemical water splitting, demonstrating a current density of 10 mA/cm at an overpotential (η) of 360 V and a Tafel slope value of 56.6 mV/dec for hydrogen evolution reaction and a current density of 10 mA/cm at an overpotential (η) of 179 mV and a Tafel slope value of 47.03 mV/dec for oxygen evolution reaction in an alkaline medium. The electrode material also exhibited a higher oxidation current density (373.60 mA/cm) compared to that of synthesized MXene toward methanol oxidation reaction in direct methanol fuel cell application. Additionally, the energy storage potential of CTAB-rGO modified MXene as electrode materials for supercapacitors with a high specific capacitance (544.50 F g at 0.5 A g) and a good capacity retention of 87% after 5000 cycles was studied. These findings of this work showcase the potential of the electrocatalyst in both conversion and storage of electrochemical energy.

摘要

二维过渡金属碳化物/氮化物和碳氮化物(MXene)家族具有卓越的导电性以及大量诸如 -F 和 OH- 等表面端基,从而导致亲水性,这使其成为能量存储和转换应用的极佳候选材料。然而,MXene会通过范德华相互作用使纳米片重新堆叠,阻碍活性位点,导致电子和离子动力学缓慢,并最终影响其电化学性能。在此,我们报道了在泡沫镍上通过逐层组装和浸涂技术合成的无粘结剂十六烷基三甲基溴化铵还原氧化石墨烯(CTAB-rGO)修饰的MXene混合薄膜,作为一种有前景的无贵金属多功能电极,它能有效减少重新堆叠,同时改善动力学。使用各种物理化学表征和电化学测量方法研究了所制备的电催化剂的性能,以彻底理解材料结构、形态和电催化性能之间的关系,从而实现“制备一种用于多种应用的电催化剂”这一目标。在能量转换方面,MXene与CTAB-rGO载体的协同效应有助于提高复合材料对电化学水分解的催化活性,在碱性介质中,析氢反应的过电位(η)为360 V时电流密度为10 mA/cm²,塔菲尔斜率值为56.6 mV/dec;析氧反应的过电位(η)为179 mV时电流密度为10 mA/cm²,塔菲尔斜率值为47.03 mV/dec。在直接甲醇燃料电池应用中,与合成的MXene相比,该电极材料对甲醇氧化反应也表现出更高的氧化电流密度(373.60 mA/cm²)。此外,还研究了CTAB-rGO修饰的MXene作为超级电容器电极材料的储能潜力,其具有高比电容(在0.5 A/g时为544.50 F/g),并且在5000次循环后容量保持率良好,为87%。这项工作的这些发现展示了该电催化剂在电化学能量转换和存储方面的潜力。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b113/10536025/1d51f72d1402/ao3c03827_0002.jpg

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