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Title: Defective Carbon-Based Materials for the Electrochemical Synthesis of Hydrogen Peroxide

Abstract

Hydrogen peroxide (H 2O 2), an important industrial chemical, is currently produced through an energy-intensive anthraquinone process that is limited to large-scale facilities. Small-scale decentralized electrochemical production of H 2O 2 via a two-electron oxygen reduction reaction (ORR) offers unique opportunities for sanitization applications and the purification of drinking water. The development of inexpensive, efficient, and selective catalysts for this reaction remains a challenge. Here in this paper, we examine two different porous carbon-based electrocatalysts and show that they exhibit high selectivity for H 2O 2 under alkaline conditions. By rationally varying synthetic methods, we explore the effect of pore size on electrocatalytic performance. Furthermore, by means of density functional calculations, we point out the critical role of carbon defects. Our theory results show that the majority of defects in graphene are naturally selective for the two-electron reduction of O 2 to H 2O 2, and we identify the types of defects with high activity.

Authors:
ORCiD logo [1];  [1]; ORCiD logo [1];  [2];  [3];  [3];  [3];  [1];  [1];  [2];  [4]; ORCiD logo [1]; ORCiD logo [1]
  1. Stanford Univ., CA (United States). Dept. of Chemical Engineering
  2. Stanford Univ., CA (United States). Dept. of Materials Science and Engineering
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
  4. Stanford Univ., CA (United States). Dept. of Chemical Engineering; SLAC National Accelerator Lab., Menlo Park, CA (United States). SUNCAT Center for Interface Science and Catalysis
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1426186
Grant/Contract Number:
AC02-76SF00515; SC0008685
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ACS Sustainable Chemistry & Engineering
Additional Journal Information:
Journal Volume: 6; Journal Issue: 1; Journal ID: ISSN 2168-0485
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Carbon catalyst; Electrocatalysis; Hydrogen peroxide; Oxygen reduction reaction; Porosity

Citation Formats

Chen, Shucheng, Chen, Zhihua, Siahrostami, Samira, Kim, Taeho Roy, Nordlund, Dennis, Sokaras, Dimosthenis, Nowak, Stanislaw, To, John W. F., Higgins, Drew, Sinclair, Robert, Nørskov, Jens K., Jaramillo, Thomas F., and Bao, Zhenan. Defective Carbon-Based Materials for the Electrochemical Synthesis of Hydrogen Peroxide. United States: N. p., 2017. Web. doi:10.1021/acssuschemeng.7b02517.
Chen, Shucheng, Chen, Zhihua, Siahrostami, Samira, Kim, Taeho Roy, Nordlund, Dennis, Sokaras, Dimosthenis, Nowak, Stanislaw, To, John W. F., Higgins, Drew, Sinclair, Robert, Nørskov, Jens K., Jaramillo, Thomas F., & Bao, Zhenan. Defective Carbon-Based Materials for the Electrochemical Synthesis of Hydrogen Peroxide. United States. doi:10.1021/acssuschemeng.7b02517.
Chen, Shucheng, Chen, Zhihua, Siahrostami, Samira, Kim, Taeho Roy, Nordlund, Dennis, Sokaras, Dimosthenis, Nowak, Stanislaw, To, John W. F., Higgins, Drew, Sinclair, Robert, Nørskov, Jens K., Jaramillo, Thomas F., and Bao, Zhenan. Mon . "Defective Carbon-Based Materials for the Electrochemical Synthesis of Hydrogen Peroxide". United States. doi:10.1021/acssuschemeng.7b02517.
@article{osti_1426186,
title = {Defective Carbon-Based Materials for the Electrochemical Synthesis of Hydrogen Peroxide},
author = {Chen, Shucheng and Chen, Zhihua and Siahrostami, Samira and Kim, Taeho Roy and Nordlund, Dennis and Sokaras, Dimosthenis and Nowak, Stanislaw and To, John W. F. and Higgins, Drew and Sinclair, Robert and Nørskov, Jens K. and Jaramillo, Thomas F. and Bao, Zhenan},
abstractNote = {Hydrogen peroxide (H2O2), an important industrial chemical, is currently produced through an energy-intensive anthraquinone process that is limited to large-scale facilities. Small-scale decentralized electrochemical production of H2O2 via a two-electron oxygen reduction reaction (ORR) offers unique opportunities for sanitization applications and the purification of drinking water. The development of inexpensive, efficient, and selective catalysts for this reaction remains a challenge. Here in this paper, we examine two different porous carbon-based electrocatalysts and show that they exhibit high selectivity for H2O2 under alkaline conditions. By rationally varying synthetic methods, we explore the effect of pore size on electrocatalytic performance. Furthermore, by means of density functional calculations, we point out the critical role of carbon defects. Our theory results show that the majority of defects in graphene are naturally selective for the two-electron reduction of O2 to H2O2, and we identify the types of defects with high activity.},
doi = {10.1021/acssuschemeng.7b02517},
journal = {ACS Sustainable Chemistry & Engineering},
number = 1,
volume = 6,
place = {United States},
year = {Mon Oct 30 00:00:00 EDT 2017},
month = {Mon Oct 30 00:00:00 EDT 2017}
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on October 30, 2018
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