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受生物启发的镍铁基有机凝胶:一种用于在高电流密度下进行全水分裂的高效稳定双功能电催化剂。

Bio-inspired nickel-iron-based organogel: an efficient and stable bifunctional electrocatalyst for overall water splitting at high current density.

作者信息

Ghosh Debasish, Maharana Subhransu, Panda Asit Baran

机构信息

Functional Materials Group, Advanced Materials and Corrosion Division, National Metallurgical Laboratory (CSIR-NML), Jamshedpur, Jharkhand-831007, India.

Academy of Scientific & Innovative Research (AcSIR), Ghaziabad - 201002, India.

出版信息

Nanoscale. 2025 May 23;17(20):12880-12893. doi: 10.1039/d5nr00589b.

DOI:10.1039/d5nr00589b
PMID:40326852
Abstract

Developing a platinum group metal (PGM) free electrocatalyst remains a prime challenge for cost effective green hydrogen (H) production. Herein, mimicking the PS II catalyst, a bimetallic organogel of nickel (Ni), iron (Fe) and benzotriazole (NiFe-gel) is developed as an efficient electrocatalyst. The developed synthetic strategy is simple and scalable, and most importantly, no binder is required for gel-loaded electrode preparation. The respective gel-based electrode showed excellent bifunctionality, in both the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER), water electrolysis activity in low and high current density (: 110 mV and : 260 mV for the OER and : 88 mV and : 324 mV for the HER), low Tafel slope and outstanding stability for 100 h at a current density of 1 A cm. The two-electrode electrolyser using the developed NiFe-gel in the anode and cathode setups for overall water splitting attained current densities of 10 mA cm and 1 A cm at potentials of 1.49 V and 1.89 V, respectively. Most significantly, NiFe-gel loaded anion exchange membrane based 4 cm alkaline water electrolysis (AEMAWE) attained a current density of 1.08 A cm at 50 °C and 2 V and showed stability for at least 100 h. Very nominal performance reduction was observed upon scale-up of the electrolyser from 4 cm to 9 cm, and the performance was better than the targeted AEMAWE performance of ≥1 A cm at 2 V. This excellent performance is attributed to the synergistic electronic interaction between Fe and Ni, interaction of nitrogen rich triazole moieties attached to the metal site, similar to the PS II system, and porous electrode microstructure. Thus, the NiFe-gel might be a potential PGM-free electrocatalyst for industrial scale hydrogen production through water electrolysis.

摘要

开发一种不含铂族金属(PGM)的电催化剂仍然是实现具有成本效益的绿色制氢面临的主要挑战。在此,模仿光系统II催化剂,开发了一种镍(Ni)、铁(Fe)和苯并三唑的双金属有机凝胶(NiFe-凝胶)作为高效电催化剂。所开发的合成策略简单且可扩展,最重要的是,制备凝胶负载电极时无需粘合剂。相应的基于凝胶的电极在析氧反应(OER)和析氢反应(HER)中均表现出优异的双功能特性,在低电流密度和高电流密度下都具有水电解活性(OER为110 mV和260 mV,HER为88 mV和324 mV),塔菲尔斜率低,在1 A cm-2的电流密度下具有100小时的出色稳定性。在阳极和阴极装置中使用所开发的NiFe-凝胶进行全水解的双电极电解槽在1.49 V和1.89 V的电位下分别达到了10 mA cm-2和1 A cm-2的电流密度。最显著的是,基于负载NiFe-凝胶的阴离子交换膜的4 cm2碱性水电解槽(AEMAWE)在50°C和2 V下达到了1.08 A cm-2的电流密度,并显示出至少100小时的稳定性。将电解槽从4 cm2扩大到9 cm2时,性能下降非常小,并且该性能优于目标AEMAWE在2 V下≥1 A cm-2的性能。这种优异的性能归因于Fe和Ni之间的协同电子相互作用、附着在金属位点上的富氮三唑部分的相互作用(类似于光系统II体系)以及多孔电极微观结构。因此,NiFe-凝胶可能是一种用于通过水电解进行工业规模制氢的潜在无PGM电催化剂。

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