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一种通过界面Ru的电子穿梭制备磷化钌(RuP)/Ru异质结构以实现高效析氢的可持续途径。

A Sustainable Route to Ruthenium Phosphide (RuP)/Ru Heterostructures with Electron-Shuttling of Interfacial Ru for Efficient Hydrogen Evolution.

作者信息

Li Daohao, Cai Rongsheng, Zheng Dongyong, Ren Jun, Dong Chung-Li, Huang Yu-Cheng, Haigh Sarah J, Liu Xien, Gong Feilong, Liu Yiming, Liu Jian, Yang Dongjiang

机构信息

State Key Laboratory of Bio-fibers and Eco-textiles, College of Materials Science and Engineering, School of Environmental Science and Engineering, Institute of Marine Biobased Materials, Qingdao University, Qingdao, 266071, P. R. China.

Department of Materials, University of Manchester, Manchester, M13 9PL, UK.

出版信息

Adv Sci (Weinh). 2024 Jun;11(22):e2309869. doi: 10.1002/advs.202309869. Epub 2024 Mar 28.

DOI:10.1002/advs.202309869
PMID:38544479
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11165549/
Abstract

Ruthenium (Ru) is a promising electrocatalyst for the hydrogen evolution reaction (HER), despite suffering from low activity in non-acidic conditions due to the high kinetic energy barrier of HO dissociation. Herein, the synthesis of carbon nanosheet-supported RuP/Ru heterostructures (RuP/Ru@CNS) from a natural polysaccharide is reported and demonstrates its behavior as an effective HER electrocatalyst in non-acidic conditions. The RuP/Ru@CNS exhibits low overpotential (106 mV at 200 mA·cm) in alkaline electrolyte, exceeding most reported Ru-based electrocatalysts. The electron shuttling between Ru atoms at the RuP/Ru interface results in a lowered energy barrier for HO dissociation by electron-deficient Ru atoms in the pure Ru phase, as well as optimized H adsorption of electron-gaining Ru atoms in the neighboring RuP. A low H spillover energy barrier between Ru atoms at the RuP/Ru interface further boosts HER kinetics. This study demonstrates a sustainable method for the fabrication of efficient Ru-based electrocatalysts and provides a more detailed understanding of interface effects in HER catalysis.

摘要

钌(Ru)是一种很有前景的析氢反应(HER)电催化剂,尽管由于HO解离的高动能垒,在非酸性条件下活性较低。本文报道了由天然多糖合成碳纳米片负载的RuP/Ru异质结构(RuP/Ru@CNS),并证明了其在非酸性条件下作为有效HER电催化剂的性能。RuP/Ru@CNS在碱性电解质中表现出低过电位(200 mA·cm时为106 mV),超过了大多数已报道的Ru基电催化剂。RuP/Ru界面处Ru原子之间的电子穿梭导致纯Ru相中缺电子Ru原子的HO解离能垒降低,以及相邻RuP中得电子Ru原子的H吸附优化。RuP/Ru界面处Ru原子之间的低H溢流能垒进一步促进了HER动力学。本研究展示了一种制备高效Ru基电催化剂的可持续方法,并为HER催化中的界面效应提供了更详细的理解。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f876/11165549/f7a11ed4aea3/ADVS-11-2309869-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f876/11165549/6d969a0922a4/ADVS-11-2309869-g005.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f876/11165549/f886f66f8d3d/ADVS-11-2309869-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f876/11165549/15eab0630a4f/ADVS-11-2309869-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f876/11165549/f7a11ed4aea3/ADVS-11-2309869-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f876/11165549/6d969a0922a4/ADVS-11-2309869-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f876/11165549/c3177849da9c/ADVS-11-2309869-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f876/11165549/f886f66f8d3d/ADVS-11-2309869-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f876/11165549/15eab0630a4f/ADVS-11-2309869-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f876/11165549/f7a11ed4aea3/ADVS-11-2309869-g002.jpg

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本文引用的文献

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Cooperative Ni(Co)-Ru-P Sites Activate Dehydrogenation for Hydrazine Oxidation Assisting Self-powered H Production.协同的镍(钴)-钌-磷位点激活脱氢作用以实现肼氧化辅助自供能制氢。
Angew Chem Int Ed Engl. 2023 Aug 28;62(35):e202308800. doi: 10.1002/anie.202308800. Epub 2023 Jul 20.
2
Boron-induced activation of Ru nanoparticles anchored on carbon nanotubes for the enhanced pH-independent hydrogen evolution reaction.硼诱导锚定在碳纳米管上的钌纳米颗粒活化以增强与pH无关的析氢反应。
J Colloid Interface Sci. 2022 Jun 15;616:338-346. doi: 10.1016/j.jcis.2022.02.072. Epub 2022 Feb 19.
3
Optimizing Hydrogen Binding on Ru Sites with RuCo Alloy Nanosheets for Efficient Alkaline Hydrogen Evolution.
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Angew Chem Int Ed Engl. 2022 Jan 21;61(4):e202113664. doi: 10.1002/anie.202113664. Epub 2021 Dec 7.
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Construction of Dual-Site Atomically Dispersed Electrocatalysts with Ru-C Single Atoms and Ru-O Nanoclusters for Accelerated Alkali Hydrogen Evolution.用于加速碱性析氢反应的具有Ru-C单原子和Ru-O纳米团簇的双位点原子分散电催化剂的构建
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Sodium-Decorated Amorphous/Crystalline RuO with Rich Oxygen Vacancies: A Robust pH-Universal Oxygen Evolution Electrocatalyst.具有丰富氧空位的钠修饰非晶态/晶态RuO:一种强大的pH通用析氧电催化剂。
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