Volume 59, Issue 4 pp. 1718-1726
Research Article

A General Route to Prepare Low-Ruthenium-Content Bimetallic Electrocatalysts for pH-Universal Hydrogen Evolution Reaction by Using Carbon Quantum Dots

Yuan Liu

Yuan Liu

College of Chemistry, College of Materials Science and Engineering, Zhengzhou University, Zhengzhou, 450000 China

These authors contributed equally to this work.

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Xue Li

Xue Li

College of Physics, Jilin University, Jilin, 130012 China

These authors contributed equally to this work.

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Dr. Qinghua Zhang

Dr. Qinghua Zhang

Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing, 100190 China

These authors contributed equally to this work.

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Weidong Li

Weidong Li

College of Chemistry, College of Materials Science and Engineering, Zhengzhou University, Zhengzhou, 450000 China

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Prof. Yu Xie

Prof. Yu Xie

College of Physics, Jilin University, Jilin, 130012 China

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Prof. Hanyu Liu

Prof. Hanyu Liu

College of Physics, Jilin University, Jilin, 130012 China

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Dr. Lu Shang

Dr. Lu Shang

Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing, 100190 China

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Prof. Zhongyi Liu

Prof. Zhongyi Liu

College of Chemistry, College of Materials Science and Engineering, Zhengzhou University, Zhengzhou, 450000 China

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Prof. Zhimin Chen

Prof. Zhimin Chen

College of Chemistry, College of Materials Science and Engineering, Zhengzhou University, Zhengzhou, 450000 China

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Prof. Lin Gu

Prof. Lin Gu

Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing, 100190 China

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Prof. Zhiyong Tang

Prof. Zhiyong Tang

Henan Institute of Advanced Technology, Zhengzhou University, Zhengzhou, 450000 China

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Prof. Tierui Zhang

Corresponding Author

Prof. Tierui Zhang

Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing, 100190 China

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Prof. Siyu Lu

Corresponding Author

Prof. Siyu Lu

College of Chemistry, College of Materials Science and Engineering, Zhengzhou University, Zhengzhou, 450000 China

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First published: 04 December 2019
Citations: 571

Graphical Abstract

How low can Ru go: A scalable and general synthetic method for the preparation of transition-metal-doped RuM/carbon quantum dots (CQDs; M=Ni, Mn, Cu) has been developed through metal-mediated CQD condensation and carbonization. The low-ruthenium-content RuM/CQD catalysts exhibit outstanding activity and stability in catalyzing hydrogen evolution at all pH values.

Abstract

A challenging but pressing task to design and synthesize novel, efficient, and robust pH-universal hydrogen evolution reaction (HER) electrocatalysts for scalable and sustainable hydrogen production through electrochemical water splitting. Herein, we report a facile method to prepare an efficient and robust Ru-M (M=Ni, Mn, Cu) bimetal nanoparticle and carbon quantum dot hybrid (RuM/CQDs) for pH-universal HER. The RuNi/CQDs catalysts exhibit outstanding HER performance at all pH levels. The unexpected low overpotentials of 13, 58, and 18 mV shown by RuNi/CQDs allow a current density of 10 mA cm−2 in 1 m KOH, 0.5 m H2SO4, and 1 m PBS, respectively, for Ru loading at 5.93 μgRu cm−2. This performance is among the best catalytic activities reported for any platinum-free electrocatalyst. Theoretical studies reveal that Ni doping results in a moderate weakening of the hydrogen bonding energy of nearby surface Ru atoms, which plays a critical role in improving the HER activity.

Conflict of interest

The authors declare no conflict of interest.

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