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

Haoqiang Song; Min Wu; Zhiyong Tang; John S Tse; Bai Yang; Siyu Lu

doi:10.1002/anie.202017102

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

Angew Chem Int Ed Engl. 2021 Mar 22;60(13):7234-7244. doi: 10.1002/anie.202017102. Epub 2021 Feb 24.

Authors

Haoqiang Song¹, Min Wu², Zhiyong Tang^{1

3}, John S Tse⁴, Bai Yang⁵, Siyu Lu¹

Affiliations

¹ Green Catalysis Center, and College of Chemistry, Zhengzhou University, Zhengzhou, 450000, China.
² College of Materials Science and Engineering, Zhejiang University of Technology, Hangzhou, 310014, China.
³ Henan Institute of Advanced Technology, Zhengzhou University, Zhengzhou, 450000, China.
⁴ Department of Physics and Engineering Physics, University of Saskatchewan, Saskatoon, S7N5E2, Canada.
⁵ State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry, Jilin University, Changchun, 130012, China.

PMID: 33438321
DOI: 10.1002/anie.202017102

Abstract

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 (Ru₁ CoP/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 Ru₁ CoP. 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 Ru₁ CoP/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.

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

Abstract

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