Engineering the Coordination Environment of Single-Atom Platinum Anchored on Graphdiyne for Optimizing Electrocatalytic Hydrogen Evolution

Xue-Peng Yin; Hong-Juan Wang; Shang-Feng Tang; Xiu-Li Lu; Miao Shu; Rui Si; Tong-Bu Lu

doi:10.1002/anie.201804817

Engineering the Coordination Environment of Single-Atom Platinum Anchored on Graphdiyne for Optimizing Electrocatalytic Hydrogen Evolution

Angew Chem Int Ed Engl. 2018 Jul 20;57(30):9382-9386. doi: 10.1002/anie.201804817. Epub 2018 Jun 28.

Authors

Xue-Peng Yin¹, Hong-Juan Wang¹, Shang-Feng Tang¹, Xiu-Li Lu¹, Miao Shu², Rui Si², Tong-Bu Lu¹

Affiliations

¹ Institute for New Energy Materials & Low Carbon Technologies, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin, 300384, China.
² Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai, 201204, China.

PMID: 29885267
DOI: 10.1002/anie.201804817

Abstract

Two Pt single-atom catalysts (SACs) of Pt-GDY1 and Pt-GDY2 were prepared on graphdiyne (GDY)supports. The isolated Pt atoms are dispersed on GDY through the coordination interactions between Pt atoms and alkynyl C atoms in GDY, with the formation of five-coordinated C₁ -Pt-Cl₄ species in Pt-GDY1 and four-coordinated C₂ -Pt-Cl₂ species in Pt-GDY2. Pt-GDY2 shows exceptionally high catalytic activity for the hydrogen evolution reaction (HER), with a mass activity up to 3.3 and 26.9 times more active than Pt-GDY1 and the state-of-the-art commercial Pt/C catalysts, respectively. Pt-GDY2 possesses higher total unoccupied density of states of Pt 5d orbital and close to zero value of Gibbs free energy of the hydrogen adsorption (|ΔGPtH* |) at the Pt active sites, which are responsible for its excellent catalytic performance. This work can help better understand the structure-catalytic activity relationship in Pt SACs.

Keywords: electrocatalysis; graphdiyne; hydrogen evolution; platinum; single-atom catalysts.