Impact of Surface Modulation of Two-Dimensional Ni-MOF and Its Derivatives on Electrochemical Energy Storage and Electrocatalytic Performance

Balaji Chettiannan, Gowdhaman Arumugam, Stanleydhinakar Mathan, Kavitha Kandiah and Ramesh Rajendran*, 
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Abstract

This research introduces an innovative approach to enhancing materials for supercapacitors, as well as hydrogen evolution reactions. The study involves synthesizing two-dimensional nickel metal–organic frameworks on nickel foam and the oxide-based materials derived from them and investigating the influence of various surfactants on structural architecture. Among the surfactants, sodium dodecyl sulfate (SDS) displayed the most effective outcomes. The SDS-assisted Ni-MOF-derived NiO demonstrated better electrochemical characteristics when served as one of the electrodes in a supercapacitor exhibiting a high specific capacity of 841.2 C·g–1 (equivalent to 1682.4 F·g–1) when tested at 1 A·g–1, and maintained 92.9% of this capacity after 5000 charge–discharge cycles. This represents significant improvements over surfactant-free materials, with a 26% increase in specific capacitance. In an asymmetric supercapacitor setup, the material demonstrated an impressive energy density (67.89 Wh·kg–1) coupled with a power density of 750 W·kg–1. When applied to the hydrogen evolution reaction, it reached 10 mA·cm–2 with an overpotential of only 87 mV. It also showed a consistent performance over 24 h. The findings highlight how surfactant-assisted synthesis of Ni-MOF and subsequent derivation resulted in interlinked nanoparticle assemblies arranged in a hierarchical, blossom-like superstructure, which significantly enhances both electrochemical and hydrogen evolution performance. The study underscores the potential of tailored MOF synthesis in developing advanced materials for sustainable energy applications.

Abstract Image

二维 Ni-MOF 及其衍生物的表面调制对电化学储能和电催化性能的影响
这项研究引入了一种创新方法,用于增强超级电容器材料以及氢进化反应。研究涉及在泡沫镍上合成二维镍金属有机框架及其衍生的氧化物基材料,并研究各种表面活性剂对结构架构的影响。在各种表面活性剂中,十二烷基硫酸钠(SDS)的效果最好。SDS 辅助的 Ni-MOF 衍生氧化镍在作为超级电容器的电极之一时表现出更好的电化学特性,在 1 A-g-1 的测试条件下,比容量高达 841.2 C-g-1(相当于 1682.4 F-g-1),并在 5000 次充放电循环后保持了 92.9% 的比容量。与不含表面活性剂的材料相比,这种材料的性能有了显著提高,比电容增加了 26%。在非对称超级电容器设置中,该材料表现出惊人的能量密度(67.89 Wh-kg-1)和 750 W-kg-1 的功率密度。当应用于氢进化反应时,它的过电位仅为 87 mV,而能量密度却达到了 10 mA-cm-2。研究结果突显了表面活性剂辅助合成 Ni-MOF 及其衍生如何产生了相互连接的纳米粒子组装体,这些组装体排列成层次分明、像花朵一样的上层结构,从而显著提高了电化学和氢进化性能。这项研究强调了定制 MOF 合成在开发可持续能源应用先进材料方面的潜力。
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期刊介绍: ACS Applied Engineering Materials is an international and interdisciplinary forum devoted to original research covering all aspects of engineered materials complementing the ACS Applied Materials portfolio. Papers that describe theory simulation modeling or machine learning assisted design of materials and that provide new insights into engineering applications are welcomed. The journal also considers experimental research that includes novel methods of preparing characterizing and evaluating new materials designed for timely applications. With its focus on innovative applications ACS Applied Engineering Materials also complements and expands the scope of existing ACS publications that focus on materials science discovery including Biomacromolecules Chemistry of Materials Crystal Growth & Design Industrial & Engineering Chemistry Research Inorganic Chemistry Langmuir and Macromolecules.The scope of ACS Applied Engineering Materials includes high quality research of an applied nature that integrates knowledge in materials science engineering physics mechanics and chemistry.
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