Interface Engineering of Earth-Abundant Transition Metals Using Boron Nitride for Selective Electroreduction of CO2

Guoxiang Hu, Zili Wu, Sheng Dai, De En Jiang

Research output: Contribution to journalArticlepeer-review

53 Scopus citations

Abstract

Two-dimensional atomically thin hexagonal boron nitride (h-BN) monolayers have attracted considerable research interest. Given the tremendous progress in the synthesis of h-BN monolayers on transition metals and their potential as electrocatalysts, we investigate the electrocatalytic activities of h-BN/Ni, h-BN/Co, and h-BN/Cu interfaces for CO2 reduction by the first-principles density functional theory. We find that with the h-BN monolayer on the metal, electrons transfer from the metal to the interface and accumulate under the B atoms. By calculating the binding energies of three key intermediates (H, HCOO, and COOH) for hydrogen evolution and CO2 reduction, we find that H binding on the metal can be significantly weakened by the h-BN monolayer, preventing the hydrogen evolution reaction (HER). However, the binding strength of HCOO is strong on both the metal and h-BN/metal, especially for Ni and Co, promoting the CO2 reduction channel. On the basis of the free-energy diagrams, we predict that h-BN/Ni and h-BN/Co will have very good electrocatalytic activities for CO2 reduction to HCOOH, while the competitive HER channel is filtered out by the surface h-BN monolayer. Our study opens a new way for selective electroreduction of CO2 via the interface engineering of the h-BN/metal system.

Original languageEnglish
Pages (from-to)6694-6700
Number of pages7
JournalACS Applied Materials and Interfaces
Volume10
Issue number7
DOIs
StatePublished - Feb 21 2018

Funding

This work was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences. This research used resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under contract no. DE-AC02-05CH11231.

Keywords

  • earth-abundant transition metals
  • electrochemical CO reduction
  • first-principles DFT
  • h-BN monolayer
  • hydrogen evolution reaction
  • interfacial materials

Fingerprint

Dive into the research topics of 'Interface Engineering of Earth-Abundant Transition Metals Using Boron Nitride for Selective Electroreduction of CO2'. Together they form a unique fingerprint.

Cite this