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Title: Designing Boron Nitride Islands in Carbon Materials for Efficient Electrochemical Synthesis of Hydrogen Peroxide

Abstract

Heteroatom-doped carbons have drawn increasing research interest as catalysts for various electrochemical reactions due to their unique electronic and surface structures. In particular, co-doping of carbon with boron and nitrogen has been shown to provide significant catalytic activity for oxygen reduction reaction (ORR). However, limited experimental work has been done to systematically study these materials, and much remains to be understood about the nature of the active site(s), particularly with regards to the factors underlying the activity enhancements of these boron–carbon–nitrogen (BCN) materials. Herein, we prepare several BCN materials experimentally with a facile and controlled synthesis method, and systematically study their electrochemical performance. We demonstrate the existence of h-BN domains embedded in the graphitic structures of these materials using X-ray spectroscopy. These synthesized structures yield higher activity and selectivity toward the 2e ORR to H2O2 than structures with individual B or N doping. We further employ density functional theory calculations to understand the role of a variety of h-BN domains within the carbon lattice for the ORR and find that the interface between h-BN domains and graphene exhibits unique catalytic behavior that can preferentially drive the production of H2O2. Here, to the best of our knowledge, this is the firstmore » example of h-BN domains in carbon identified as a novel system for the electrochemical production of H2O2.« less

Authors:
ORCiD logo [1];  [1]; ORCiD logo [1]; ORCiD logo [1];  [2];  [2];  [1];  [1]; ORCiD logo [1];  [2];  [1];  [3]; ORCiD logo [3]; ORCiD logo [1]
  1. Stanford Univ., Stanford, CA (United States)
  2. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  3. Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1459647
Grant/Contract Number:  
SC0008685; AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 140; Journal Issue: 25; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Chen, Shucheng, Chen, Zhihua, Siahrostami, Samira, Higgins, Drew, Nordlund, Dennis, Sokaras, Dimosthenis, Kim, Taeho Roy, Liu, Yunzhi, Yan, Xuzhou, Nilsson, Elisabeth, Sinclair, Robert, Norskov, Jens K., Jaramillo, Thomas F., and Bao, Zhenan. Designing Boron Nitride Islands in Carbon Materials for Efficient Electrochemical Synthesis of Hydrogen Peroxide. United States: N. p., 2018. Web. doi:10.1021/jacs.8b02798.
Chen, Shucheng, Chen, Zhihua, Siahrostami, Samira, Higgins, Drew, Nordlund, Dennis, Sokaras, Dimosthenis, Kim, Taeho Roy, Liu, Yunzhi, Yan, Xuzhou, Nilsson, Elisabeth, Sinclair, Robert, Norskov, Jens K., Jaramillo, Thomas F., & Bao, Zhenan. Designing Boron Nitride Islands in Carbon Materials for Efficient Electrochemical Synthesis of Hydrogen Peroxide. United States. doi:10.1021/jacs.8b02798.
Chen, Shucheng, Chen, Zhihua, Siahrostami, Samira, Higgins, Drew, Nordlund, Dennis, Sokaras, Dimosthenis, Kim, Taeho Roy, Liu, Yunzhi, Yan, Xuzhou, Nilsson, Elisabeth, Sinclair, Robert, Norskov, Jens K., Jaramillo, Thomas F., and Bao, Zhenan. Wed . "Designing Boron Nitride Islands in Carbon Materials for Efficient Electrochemical Synthesis of Hydrogen Peroxide". United States. doi:10.1021/jacs.8b02798. https://www.osti.gov/servlets/purl/1459647.
@article{osti_1459647,
title = {Designing Boron Nitride Islands in Carbon Materials for Efficient Electrochemical Synthesis of Hydrogen Peroxide},
author = {Chen, Shucheng and Chen, Zhihua and Siahrostami, Samira and Higgins, Drew and Nordlund, Dennis and Sokaras, Dimosthenis and Kim, Taeho Roy and Liu, Yunzhi and Yan, Xuzhou and Nilsson, Elisabeth and Sinclair, Robert and Norskov, Jens K. and Jaramillo, Thomas F. and Bao, Zhenan},
abstractNote = {Heteroatom-doped carbons have drawn increasing research interest as catalysts for various electrochemical reactions due to their unique electronic and surface structures. In particular, co-doping of carbon with boron and nitrogen has been shown to provide significant catalytic activity for oxygen reduction reaction (ORR). However, limited experimental work has been done to systematically study these materials, and much remains to be understood about the nature of the active site(s), particularly with regards to the factors underlying the activity enhancements of these boron–carbon–nitrogen (BCN) materials. Herein, we prepare several BCN materials experimentally with a facile and controlled synthesis method, and systematically study their electrochemical performance. We demonstrate the existence of h-BN domains embedded in the graphitic structures of these materials using X-ray spectroscopy. These synthesized structures yield higher activity and selectivity toward the 2e– ORR to H2O2 than structures with individual B or N doping. We further employ density functional theory calculations to understand the role of a variety of h-BN domains within the carbon lattice for the ORR and find that the interface between h-BN domains and graphene exhibits unique catalytic behavior that can preferentially drive the production of H2O2. Here, to the best of our knowledge, this is the first example of h-BN domains in carbon identified as a novel system for the electrochemical production of H2O2.},
doi = {10.1021/jacs.8b02798},
journal = {Journal of the American Chemical Society},
number = 25,
volume = 140,
place = {United States},
year = {2018},
month = {6}
}

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Figures / Tables:

Figure 1 Figure 1: (a) A schematic of the BCN configuration models examined in this study. Color code: C(gray), N(blue), B(pink). %X composition is defined as the number of Catoms substituted in $h$-BN substrate over the total number of substrate atoms. Similarly, for BN domains %X composition is defined as the numbermore » of BN pairs substituted in graphene substrate over the total number of substrate atoms. (b) Theoretical activity volcano maps for two- (red) and four- (black) electron reduction of O2 to hydrogen peroxide and water, respectively. Both volcano plots are based on the RHE scale. The equilibrium potentials for both two- and four-electron ORR are shown as dashed red and black lines, respectively. Triangles or diamonds represent the activity of the N- or B-doped in the pristine (N-Gr or B-Gr) and defect (N-Gr-D or B-Gr-D) graphene, respectively. The activity of N-Gr-D is adapted from Ref. [34] while the activity of Pt(111) and PtHg4 alloy are adapted from Refs. [37], and [24], respectively.« less

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