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The construction of efficient and durable electrocatalysts with highly dispersed metal clusters and hydrophilic surface for alkaline hydrogen evolution reaction (HER) remains a great challenge. Herein, we prepared hydrophilic nanocomposites of Ru clusters (~ 1.30 nm) anchored on Na+, K+-decorated porous carbon (Ru/Na+, K+-PC) through hydrothermal method and subsequent annealing treatment at 500 °C. The Ru/Na+, K+-PC exhibits ultralow overpotential of 7 mV at 10 mA·cm−2, mass activity of 15.7 A·mgRu−1 at 100 mV, and long-term durability of 20,000 cycles potential cycling and 200 h chronopotentiometric measurement with a negligible decrease in activity, much superior to benchmarked commercial Pt/C. Density functional theory based calculations show that the energy barrier of H–OH bond breaking is efficiently reduced due to the presence of Na and K ions, thus favoring the Volmer step. Furthermore, the Ru/Na+, K+-PC effectively employs solar energy for obtaining H2 in both alkaline water and seawater electrolyzer. This finding provides a new strategy to construct high-performance and cost-effective alkaline HER electrocatalyst.


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Boosting alkaline hydrogen evolution performance by constructing ultrasmall Ru clusters/Na+, K+-decorated porous carbon composites

Show Author's information Mingxiu Duan1Tie Shu2Jingwei Li3Daliang Zhang3Li-Yong Gan4( )Ke Xin Yao2,3( )Qiang Yuan1( )
State-Local Joint Laboratory for Comprehensive Utilization of Biomass, Center for R&D of Fine Chemicals, College of Chemistry and Chemical Engineering, Guizhou University, Guiyang 550025, China
School of Chemistry and Chemical Engineering, Chongqing University, Chongqing 400044, China
Multi-scale Porous Materials Center, Institute of Advanced Interdisciplinary Studies & School of Chemistry and Chemical Engineering, Chongqing University, Chongqing 400044, China
College of Physics and Center of Quantum Materials and Devices, Chongqing University, Chongqing 401331, China

Abstract

The construction of efficient and durable electrocatalysts with highly dispersed metal clusters and hydrophilic surface for alkaline hydrogen evolution reaction (HER) remains a great challenge. Herein, we prepared hydrophilic nanocomposites of Ru clusters (~ 1.30 nm) anchored on Na+, K+-decorated porous carbon (Ru/Na+, K+-PC) through hydrothermal method and subsequent annealing treatment at 500 °C. The Ru/Na+, K+-PC exhibits ultralow overpotential of 7 mV at 10 mA·cm−2, mass activity of 15.7 A·mgRu−1 at 100 mV, and long-term durability of 20,000 cycles potential cycling and 200 h chronopotentiometric measurement with a negligible decrease in activity, much superior to benchmarked commercial Pt/C. Density functional theory based calculations show that the energy barrier of H–OH bond breaking is efficiently reduced due to the presence of Na and K ions, thus favoring the Volmer step. Furthermore, the Ru/Na+, K+-PC effectively employs solar energy for obtaining H2 in both alkaline water and seawater electrolyzer. This finding provides a new strategy to construct high-performance and cost-effective alkaline HER electrocatalyst.

Keywords: electrocatalysts, hydrogen evolution reaction, decorated porous carbon, ultrasmall Ru clusters, solar-to-hydrogen

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Publication history
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Received: 15 November 2022
Revised: 07 February 2023
Accepted: 09 February 2023
Published: 13 March 2023
Issue date: July 2023

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© Tsinghua University Press 2023

Acknowledgements

Acknowledgements

This work was supported by the National Natural Science Foundation of China (No. 21571038), Education Department of Guizhou Province (No. 2021312), Foundation of Guizhou Province (No. 2019-5666), State Key Laboratory of Coal Mine Disaster Dynamics and Control (Chongqing University, No. 2011DA105287-ZR202101), Science Foundation for After graduated Students of Guizhou Province (No. YJSKYJJ2021023), State Key Laboratory of Physical Chemistry of Solid Surfaces (Xiamen University, No. 202009), and the Open Fund of the Key Lab of Organic Optoelectronics and Molecular Engineering (Tsinghua University). We gratefully acknowledge Analytical and Testing Center of Chongqing University. We also gratefully acknowledge the computing resources provided by Hefei advanced computing center.

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