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

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

doi:10.1021/jacs.8b02798

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

Journal Article · 06 June 2018 · Journal of the American Chemical Society

DOI: https://doi.org/10.1021/jacs.8b02798 · OSTI ID:1459647

^[1]; Chen, Zhihua ^[1];

^[1];

^[1]; Nordlund, Dennis ^[2]; Sokaras, Dimosthenis ^[2]; Kim, Taeho Roy ^[1]; Liu, Yunzhi ^[1];

^[1]; Nilsson, Elisabeth ^[2]; Sinclair, Robert ^[1]; Norskov, Jens K. ^[3];

^[3];

^[1]

Stanford Univ., Stanford, CA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)

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.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0008685; AC02-76SF00515

OSTI ID:: 1459647

Journal Information:: Journal of the American Chemical Society, Vol. 140, Issue 25; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 267 works

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