Interface Engineering of Earth-Abundant Transition Metals Using Boron Nitride for Selective Electroreduction of CO2
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.
- Authors:
-
[2];
[3];
[1]
- Univ. of California, Riverside, CA (United States). Dept. of Chemistry
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division. Center for Nanophase Materials Sciences
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division. Center for Nanophase Materials Sciences; Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemistry
- Publication Date:
- Research Org.:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of California, Riverside, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
- OSTI Identifier:
- 1468197
- Alternate Identifier(s):
- OSTI ID: 1485129
- Grant/Contract Number:
- AC05-00OR22725; AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Applied Materials and Interfaces
- Additional Journal Information:
- Journal Volume: 10; Journal Issue: 7; Journal ID: ISSN 1944-8244
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; earth-abundant transition metals; electrochemical CO2 reduction; first-principles DFT; h-BN monolayer; hydrogen evolution reaction; interfacial materials
Citation Formats
Hu, Guoxiang, Wu, Zili, Dai, Sheng, and Jiang, De-en. Interface Engineering of Earth-Abundant Transition Metals Using Boron Nitride for Selective Electroreduction of CO2. United States: N. p., 2018.
Web. doi:10.1021/acsami.7b17600.
Hu, Guoxiang, Wu, Zili, Dai, Sheng, & Jiang, De-en. Interface Engineering of Earth-Abundant Transition Metals Using Boron Nitride for Selective Electroreduction of CO2. United States. https://doi.org/10.1021/acsami.7b17600
Hu, Guoxiang, Wu, Zili, Dai, Sheng, and Jiang, De-en. Thu .
"Interface Engineering of Earth-Abundant Transition Metals Using Boron Nitride for Selective Electroreduction of CO2". United States. https://doi.org/10.1021/acsami.7b17600. https://www.osti.gov/servlets/purl/1468197.
@article{osti_1468197,
title = {Interface Engineering of Earth-Abundant Transition Metals Using Boron Nitride for Selective Electroreduction of CO2},
author = {Hu, Guoxiang and Wu, Zili and Dai, Sheng and Jiang, De-en},
abstractNote = {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.},
doi = {10.1021/acsami.7b17600},
journal = {ACS Applied Materials and Interfaces},
number = 7,
volume = 10,
place = {United States},
year = {Thu Feb 01 00:00:00 EST 2018},
month = {Thu Feb 01 00:00:00 EST 2018}
}
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Figures / Tables:
Figure 1: Top and side views of the optimized structures for h-BN/Ni, h-BN/Co, and h-BN/Cu. In the side view, the charge density difference plots are also shown. The red color indicates charge accumulation and the green color indicates charge depletion. The value of isosurface for h-BN/Ni(111) and h-BN/Co(0001) is 0.004more »
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Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.