4.8 Article

Single Atom Ruthenium-Doped CoP/CDs Nanosheets via Splicing of Carbon-Dots for Robust Hydrogen Production

Journal

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 60, Issue 13, Pages 7234-7244

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202017102

Keywords

carbon dots; hydrogen production; single-atom catalysts; transition metal phosphides

Funding

  1. National Natural Science Foundation of China [21905253, 51973200]
  2. China Postdoctoral Science Foundation [2018M640681, 2019T120632]
  3. Natural Science Foundation of Henan [202300410372]

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This study introduces a composite material design with CoP nanoparticles doped with Ru single-atom sites supported on carbon dots (CDs) single-layer nanosheets, forming Ru1CoP/CDs. The catalyst shows high efficiency for the hydrogen evolution reaction over a wide pH range and excellent stability and activity. Through density functional theory calculations, it was revealed that the substituted Ru single atoms enhance catalytic performance by lowering the proton-coupled electron transfer energy barrier and promoting H-H bond formation. This research presents a new approach for developing carbon-based hybridization materials with integrated electrocatalytic performance for water splitting.
Ultrathin two-dimensional catalysts are attracting attention in the field of electrocatalytic hydrogen evolution. This work describe a composite material design in which CoP nanoparticles doped with Ru single-atom sites supported on carbon dots (CDs) single-layer nanosheets formed by splicing CDs (Ru1CoP/CDs). Small CD fragments bore abundant functional groups, analogous to pieces of a jigsaw puzzle, and could provide a high density of binding sites to immobilize Ru1CoP. The single-particle-thick nanosheets formed by splicing CDs acted as supports, which improved the conductivity of the electrocatalyst and the stability of the catalyst during operation. The Ru1CoP/CDs formed from doping atomic Ru dispersed on CoP showed very high efficiency for the hydrogen evolution reaction (HER) over a wide pH range. The catalyst prepared under optimized conditions displayed outstanding stability and activity: the overpotential for the HER at a current density of 10 mA cm(-2) was as low as 51 and 49 mV under alkaline and acidic conditions, respectively. Density functional theory calculations showed that the substituted Ru single atoms lowered the proton-coupled electron transfer energy barrier and promoted H-H bond formation, thereby enhancing catalytic performance for the HER. The findings open a new avenue for developing carbon-based hybridization materials with integrated electrocatalytic performance for water splitting.

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