Computational Design of Transition Metal Single-Atom Electrocatalysts on PtS2 for Efficient Nitrogen Reduction

Lejuan Cai, Ning Zhang, Bocheng Qiu, Yang Chai

Research output: Journal article publicationJournal articleAcademic researchpeer-review

55 Citations (Scopus)


Electrocatalytic nitrogen reduction is promising to serve as a sustainable and environmentally friendly strategy to achieve ammonia production. Single-atom catalysts (SACs) hold great promise to convert N2 into NH3 because of the unique molecular catalysis property and ultrahigh atomic utilization ratio. Here, we demonstrate a universal computational design principle to assess the N2 reduction reaction (NRR) performance of SACs anchored on a monolayer PtS2 substrate (SACs-PtS2). Our density functional theory simulations unveil that the barriers of the NRR limiting potential step on different SAC centers are observed to be linearly correlated to the integral of unoccupied d states (UDSs) of SACs. As a result, the Ru SAC-PtS2 catalyst with the largest number of UDSs exhibits a much lower barrier of the limiting step than those of other SACs-PtS2 catalysts and the Ru(0001) benchmark. Our work bridges the apparent NRR activity and intrinsic electronic structure of SAC centers and offers effective guidance to screen and design efficient SACs for the electrochemical NRR process.

Original languageEnglish
Pages (from-to)20448-20455
Number of pages8
JournalACS Applied Materials and Interfaces
Issue number18
Publication statusPublished - 6 May 2020


  • 2D materials
  • DFT
  • electrochemical nitrogen reduction
  • PtS
  • single-atom catalysts

ASJC Scopus subject areas

  • General Materials Science


Dive into the research topics of 'Computational Design of Transition Metal Single-Atom Electrocatalysts on PtS2 for Efficient Nitrogen Reduction'. Together they form a unique fingerprint.

Cite this