Bhargav Rajbongshi, Pragyan Tripathi, Abhishek Kumar Singh, Manikoth M. Shaijumon
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引用次数: 0
Abstract
Implantation of foreign elements into a host lattice can enhance catalytic activity by modulating electronic properties. Copper (Cu), a low-cost and abundant material, shows great potential in energy conversion applications. However, its high water dissociation energy barrier limits its catalytic performance in alkaline hydrogen evolution reactions (HER). Herein, a highly scalable co-electrodeposition method is presented to enhance the electrocatalytic performance of copper for alkaline HER by incorporating rhenium (Re) into the copper lattice. The incorporated Re improves electrocatalytic activity by promoting exothermic water dissociation and enhancing water adsorption. The optimized catalyst, CuRe-10/CP, achieves an overpotential of 46 mV to drive a current density of 10 mA cm−2, demonstrating excellent electrochemical stability for 450 h at 50 mA cm−2 in an alkaline medium (1.0 m KOH). Additionally, the electrochemical activity of the CuRe-10/CP is evaluated in simulated seawater and alkaline seawater, where it exhibited exceptional activity and stability. Electrochemical impedance spectroscopy (EIS), electrochemical surface area measurement (ECSA), and turnover frequency (TOF) analyses confirm the significant enhancement in catalytic performance following Re incorporation. Furthermore, in situ Raman spectroscopy, EIS, and density functional theory (DFT) studies reveal that the Re incorporation into the copper lattice significantly improves the water dissociation and intermediate adsorption. This study gives a scalable strategy for designing platinum group element free electrocatalysts for alkaline hydrogen evolution.
外来元素注入主晶格可以通过调制电子性质来提高催化活性。铜(Cu)是一种储量丰富、成本低廉的材料,在能量转换方面具有巨大的应用潜力。但其较高的水解离能垒限制了其在碱性析氢反应中的催化性能。本文提出了一种高度可扩展的共电沉积方法,通过在铜晶格中加入铼(Re)来提高铜对碱性HER的电催化性能。掺入的稀土通过促进放热水解离和增强水吸附来提高电催化活性。优化后的催化剂CuRe-10/CP实现了46 mV的过电位,驱动电流密度为10 mA cm-2,在碱性介质(1.0 m KOH)中,在50 mA cm-2下表现出450小时的优异电化学稳定性。此外,还对CuRe-10/CP在模拟海水和碱性海水中的电化学活性进行了评价,结果表明其具有优异的活性和稳定性。电化学阻抗谱(EIS)、电化学表面积测量(ECSA)和周转频率(TOF)分析证实了稀土掺入后催化性能的显著增强。此外,原位拉曼光谱、EIS和密度泛函理论(DFT)研究表明,稀土掺入铜晶格显著改善了水解离和中间吸附。本研究为无铂族元素碱性析氢电催化剂的设计提供了一种可扩展的策略。
期刊介绍:
Small serves as an exceptional platform for both experimental and theoretical studies in fundamental and applied interdisciplinary research at the nano- and microscale. The journal offers a compelling mix of peer-reviewed Research Articles, Reviews, Perspectives, and Comments.
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