Engineering the synergistic effect of carbon dots‐stabilized atomic and subnanometric ruthenium as highly efficient electrocatalysts for robust hydrogen evolution
Yuan Liu,
Ning Chen,
Weidong Li,
Mingzi Sun,
Tong Wu,
Bolong Huang,
Xue Yong,
Qinghua Zhang,
Lin Gu,
Haoqiang Song,
Robert Bauer,
John S. Tse,
Shuang‐Quan Zang,
Bai Yang,
Siyu Lu
Affiliations
Yuan Liu
Green Catalysis Center, and College of Chemistry Zhengzhou University Zhengzhou China
Ning Chen
Canadian Light Source University of Saskatchewan Saskatoon Canada
Weidong Li
Green Catalysis Center, and College of Chemistry Zhengzhou University Zhengzhou China
Mingzi Sun
Department of Applied Biology and Chemical Technology The Hong Kong Polytechnic University Hong Kong China
Tong Wu
Department of Applied Biology and Chemical Technology The Hong Kong Polytechnic University Hong Kong China
Bolong Huang
Department of Applied Biology and Chemical Technology The Hong Kong Polytechnic University Hong Kong China
Xue Yong
Department of Physics and Engineering Physics University of Saskatchewan Saskatoon Canada
Qinghua Zhang
State Key Lab of Supramolecular Structure and Materials College of Chemistry Jilin University Changchun China
Lin Gu
State Key Lab of Supramolecular Structure and Materials College of Chemistry Jilin University Changchun China
Haoqiang Song
Green Catalysis Center, and College of Chemistry Zhengzhou University Zhengzhou China
Robert Bauer
Department of Physics and Engineering Physics University of Saskatchewan Saskatoon Canada
John S. Tse
Department of Physics and Engineering Physics University of Saskatchewan Saskatoon Canada
Shuang‐Quan Zang
Green Catalysis Center, and College of Chemistry Zhengzhou University Zhengzhou China
Bai Yang
Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences Beijing China
Siyu Lu
Green Catalysis Center, and College of Chemistry Zhengzhou University Zhengzhou China
Abstract Currently, the most efficient electrocatalyst for the hydrogen evolution reaction (HER) in water dissociation is Pt‐based catalyst. Unfortunately, the high cost and less than perfect efficiency hinder wide‐range industrial/technological applications. Here, by controlling the treatment temperature of tris (2,2‐bipyridine) ruthenium dichloride hexahydrate, synthesis of compounds with novel ruthenium single/dual atoms (Ru S/DAs) mixed with Ru nanoclusters (Ru S/DAs + Ru NCs) and supported by carbon dots is demonstrated. These compounds are shown to be highly efficient and competitive catalysts for hydrogen evolution. Ru S/DAs + Ru NCs exhibit very high activity, with overpotentials of 15 and 40 mV at a current density of 10 mA/cm2 in 1.0 mol/L KOH and 0.5 mol/L H2SO4, respectively. Furthermore, the composites are found to possess outstanding stability and rapid HER kinetics. X ray absorption fine structure analysis, supported by density functional theory calculations, shows charge rearrangement in single‐atomic Ru, and the Ru dual sites promote active hydrogen adsorption and recombination. Ru S/DAs and Ru NCs demonstrate high electroactivity due to the electroactive Ru 4d orbitals. The introduction of Ru NCs activates the carbon support, providing a high electronic conductivity to transfer electrons from Ru NCs to Ru S/DAs, and facilitates water dissociation for the HER process.