Baig K Mohamed Yusuf, Marimuthu Sundaramoorthy, Maduraiveeran Govindhan, Kole Goutam Kumar
Department of Chemistry, College of Engineering and Technology, SRM Institute of Science and Technology, Kattankulathur, Tamil Nadu 603203, India.
Department of Physics, College of Arts and Sciences, American University of Sharjah, Sharjah, United Arab Emirates.
Dalton Trans. 2025 Jul 15;54(28):11025-11035. doi: 10.1039/d5dt00760g.
Developing stable, efficient, and affordable Earth-abundant transition metal-based electrocatalysts for water splitting applications is key to producing green hydrogen. This study reports the development of new Ni(II)-based one-dimensional coordination polymers (CPs), namely, [Ni(9-AnBz)(4,4'-bpy)(MeOH)] (CP 1), [Ni(9-AnBz)(4,4'-bpe)(MeOH)] (CP 2), and [Ni(9-AnBz)(3,3'-bpdb)(HO)]·HO (CP 3) (where 9-AnBz = 9-anthracenyl-4'-benzoate, 4,4'-bpy = 4,4'-bipyridine, 4,4'-bpe = -1,2-bis(4'-pyridyl)ethene, and 3,3'-bpdb = 1,4-bis(3'-pyridyl)-2,3-diaza-1,3-butadiene), as novel electrocatalysts. Their structures have been confirmed by single crystal X-ray diffraction. These Ni(II)-based CPs exhibited improved electrocatalytic activity towards both the hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER) in 1.0 M KOH. The CP 1 catalyst was found to deliver a low HER onset potential (∼-0.04 V RHE), a small HER overpotential (∼87 mV at -10 mA cm), a Tafel slope of ∼107.0 mV dec, high current density (-496 mA cm at ∼1.83 V RHE), and high mass activity (∼50.0 A g), comparable to those of commercial Pt/C. Moreover, the CP 1 catalyst also exhibited the best OER activity, with a small overpotential (∼370 mV at 10 mA cm) and a low Tafel slope (∼82 mV dec), showing efficient performance and great promise in hydrogen production systems.
开发用于水分解应用的稳定、高效且经济实惠的地球丰富型过渡金属基电催化剂是生产绿色氢气的关键。本研究报告了新型镍（II）基一维配位聚合物（CPs）的开发，即[Ni(9 - AnBz)(4,4'-bpy)(MeOH)]（CP 1）、[Ni(9 - AnBz)(4,4'-bpe)(MeOH)]（CP 2）和[Ni(9 - AnBz)(3,3'-bpdb)(HO)]·HO（CP 3）（其中9 - AnBz = 9 - 蒽基 - 4'-苯甲酸酯，4,4'-bpy = 4,4'-联吡啶，4,4'-bpe = - 1,2 - 双（4'-吡啶基）乙烯，3,3'-bpdb = 1,4 - 双（3'-吡啶基）- 2,3 - 二氮杂 - 1,3 - 丁二烯），作为新型电催化剂。它们的结构已通过单晶X射线衍射得到证实。这些镍（II）基CPs在1.0 M KOH中对析氢反应（HER）和析氧反应（OER）均表现出改进的电催化活性。发现CP 1催化剂具有低HER起始电位（约 - 0.04 V vs RHE）、小HER过电位（在 - 10 mA cm时约87 mV）、约107.0 mV dec的塔菲尔斜率、高电流密度（在约1.83 V vs RHE时为 - 496 mA cm）和高质量活性（约50.0 A g），与商业Pt/C相当。此外，CP 1催化剂还表现出最佳的OER活性，过电位小（在10 mA cm时约370 mV）且塔菲尔斜率低（约82 mV dec），在制氢系统中显示出高效性能和巨大潜力。
