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Title: 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:
 [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [1]
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  1. Univ. of California, Riverside, CA (United States). Dept. of Chemistry
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division. Center for Nanophase Materials Sciences
  3. 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
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & 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.
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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. doi:10.1021/acsami.7b17600.
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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. doi:10.1021/acsami.7b17600. https://www.osti.gov/servlets/purl/1468197.
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@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 = {2018},
month = {2}
}
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Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI:  10.1021/acsami.7b17600
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Cited by: 7 works
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Figures / Tables:

Figure 1 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 » eV/Å3, while for h-BN/Cu(111) it is 0.0006 eV/Å3. B, yellow; N, blue; Ni, green; Co, magenta; Cu, orange.« less
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Works referencing / citing this record:

Mo-doped boron nitride monolayer as a promising single-atom electrocatalyst for CO 2 conversion
journal, January 2019

  • Cui, Qianyi; Qin, Gangqiang; Wang, Weihua
  • Beilstein Journal of Nanotechnology, Vol. 10
  • DOI: 10.3762/bjnano.10.55

Mo-doped boron nitride monolayer as a promising single-atom electrocatalyst for CO 2 conversion
journal, January 2019

  • Cui, Qianyi; Qin, Gangqiang; Wang, Weihua
  • Beilstein Journal of Nanotechnology, Vol. 10
  • DOI: 10.3762/bjnano.10.55

Fabrication and application of BN nanoparticles, nanosheets and their nanohybrids
journal, January 2018

  • Shtansky, Dmitry V.; Firestein, Konstantin L.; Golberg, Dmitri V.
  • Nanoscale, Vol. 10, Issue 37
  • DOI: 10.1039/c8nr05027a
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