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

Yuan Liu; Xue Li; Qinghua Zhang; Weidong Li; Yu Xie; Hanyu Liu; Lu Shang; Zhongyi Liu; Zhimin Chen; Lin Gu; Zhiyong Tang; Tierui Zhang; Siyu Lu

doi:10.1002/anie.201913910

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

Angew Chem Int Ed Engl. 2020 Jan 20;59(4):1718-1726. doi: 10.1002/anie.201913910. Epub 2019 Dec 19.

Authors

Yuan Liu¹, Xue Li², Qinghua Zhang³, Weidong Li¹, Yu Xie², Hanyu Liu², Lu Shang⁴, Zhongyi Liu¹, Zhimin Chen¹, Lin Gu³, Zhiyong Tang⁵, Tierui Zhang⁴, Siyu Lu¹

Affiliations

¹ College of Chemistry, College of Materials Science and Engineering, Zhengzhou University, Zhengzhou, 450000, China.
² College of Physics, Jilin University, Jilin, 130012, China.
³ Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing, 100190, China.
⁴ Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing, 100190, China.
⁵ Henan Institute of Advanced Technology, Zhengzhou University, Zhengzhou, 450000, China.

PMID: 31799763
DOI: 10.1002/anie.201913910

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 H₂ SO₄ , 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.

Keywords: carbon quantum dots; hydrogen evolution reaction; pH-universal; ruthenium; transition-metal doping.

Abstract

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