TY - JOUR
T1 - Engineering the synergistic effect of carbon dots-stabilized atomic and subnanometric ruthenium as highly efficient electrocatalysts for robust hydrogen evolution
AU - Liu, Yuan
AU - Chen, Ning
AU - Li, Weidong
AU - Sun, Mingzi
AU - Wu, Tong
AU - Huang, Bolong
AU - Yong, Xue
AU - Zhang, Qinghua
AU - Gu, Lin
AU - Song, Haoqiang
AU - Bauer, Robert
AU - Tse, John S.
AU - Zang, Shuang-Quan
AU - Yang, Bai
AU - Lu, Siyu
PY - 2022/6
Y1 - 2022/6
N2 - 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. © 2021 The Authors. SmartMat published by Tianjin University and John Wiley & Sons Australia, Ltd.
AB - 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. © 2021 The Authors. SmartMat published by Tianjin University and John Wiley & Sons Australia, Ltd.
KW - carbon dots
KW - hydrogen evolution reaction
KW - nanoclusters
KW - ruthenium
KW - single/dual atoms
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UR - https://www.scopus.com/record/pubmetrics.uri?eid=2-s2.0-85168429162&origin=recordpage
U2 - 10.1002/smm2.1067
DO - 10.1002/smm2.1067
M3 - RGC 21 - Publication in refereed journal
SN - 2766-8525
VL - 3
SP - 249
EP - 259
JO - SMARTMAT
JF - SMARTMAT
IS - 2
ER -
