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双金属氧磷化物的界面电子修饰作为用于水分解和尿素电解的多功能电催化剂

Interfacial electronic modification of bimetallic oxyphosphides as Multi-functional electrocatalyst for water splitting and urea electrolysis.

作者信息

Yang Lijun, Zhang Lei

机构信息

College of Chemistry, Liaoning University, 66 Chongshan Middle Road, Shenyang, Liaoning 110036, People's Republic of China.

College of Chemistry, Liaoning University, 66 Chongshan Middle Road, Shenyang, Liaoning 110036, People's Republic of China.

出版信息

J Colloid Interface Sci. 2022 Feb;607(Pt 1):546-555. doi: 10.1016/j.jcis.2021.09.013. Epub 2021 Sep 6.

Abstract

Electrochemical water or wastewater splitting is a sustainable development approach for both hydrogen generation and pollutant elimination. Herein, an N-engineering ultrathin bimetallic oxyphosphides nanosheets on Ni foam (CoNiOP/NF) as a multi-functional binder-free electrode was synthesized for hydrogen evolution reaction (HER), oxygen evolution reaction (OER) and urea oxidation reaction (UOR). The catalytic activity of the composites could be improved through introducing N-doping via an in-situ transformation and heterogeneous metals by ion exchange. Both theoretical calculation and experimental investigations confirmed that electrons transferred from metal centers to anion at the interface, which was favor to accelerate the phase transformation to electrochemically active species and optimize the intermediates adsorption dynamics, thus providing greatly enhanced electrocatalytic activities. Assembled an electrolyzer using UOR replaced OER, it required only 1.42 V to achieve 50 mA cm with long-term stability, 214 mV less than that required for HER‖OER. This work would be beneficial for the exploitation of non-noble metal-based electrocatalysts for simultaneous realization of energy-saving urea-assisted electrolytic hydrogen production and urea-containing wastewater purifying.

摘要

电化学水分解或废水分解是一种用于制氢和消除污染物的可持续发展方法。在此,合成了一种负载在泡沫镍上的氮工程超薄双金属氧磷化物纳米片(CoNiOP/NF)作为多功能无粘结剂电极,用于析氢反应(HER)、析氧反应(OER)和尿素氧化反应(UOR)。通过原位转变引入氮掺杂和通过离子交换引入异质金属,可以提高复合材料的催化活性。理论计算和实验研究均证实,电子在界面处从金属中心转移到阴离子,这有利于加速向电化学活性物种的相变并优化中间体吸附动力学,从而大大提高电催化活性。组装了一种使用UOR代替OER的电解槽,在长期稳定性下,实现50 mA cm⁻²仅需1.42 V,比HER‖OER所需电压低214 mV。这项工作将有助于开发用于同时实现节能尿素辅助电解制氢和含尿素废水净化的非贵金属基电催化剂。

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