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Title: High-efficiency oxygen reduction to hydrogen peroxide catalysed by oxidized carbon materials

Abstract

Hydrogen peroxide (H 2O 2) is a valuable chemical with a wide range of applications, but the current industrial synthesis of H 2O 2 involves an energy-intensive anthraquinone process. The electrochemical synthesis of H 2O 2 from oxygen reduction offers an alternative route for on-site applications; the efficiency of this process depends greatly on identifying cost-effective catalysts with high activity and selectivity. Here, we demonstrate a facile and general approach to catalyst development via the surface oxidation of abundant carbon materials to significantly enhance both the activity and selectivity (~90%) for H 2O 2 production by electrochemical oxygen reduction. We find that both the activity and selectivity are positively correlated with the oxygen content of the catalysts. In conclusion, the density functional theory calculations demonstrate that the carbon atoms adjacent to several oxygen functional groups (–COOH and C–O–C) are the active sites for oxygen reduction reaction via the two-electron pathway, which are further supported by a series of control experiments.

Authors:
ORCiD logo [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1]; ORCiD logo [1];  [1];  [2];  [2]
  1. Stanford Univ., Stanford, CA (United States)
  2. 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
OSTI Identifier:
1458611
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nature Catalysis
Additional Journal Information:
Journal Volume: 1; Journal Issue: 2; Journal ID: ISSN 2520-1158
Publisher:
Springer Nature
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Lu, Zhiyi, Chen, Guangxu, Siahrostami, Samira, Chen, Zhihua, Liu, Kai, Xie, Jin, Liao, Lei, Wu, Tong, Lin, Dingchang, Liu, Yayuan, Jaramillo, Thomas F., Norskov, Jens K., and Cui, Yi. High-efficiency oxygen reduction to hydrogen peroxide catalysed by oxidized carbon materials. United States: N. p., 2018. Web. doi:10.1038/s41929-017-0017-x.
Lu, Zhiyi, Chen, Guangxu, Siahrostami, Samira, Chen, Zhihua, Liu, Kai, Xie, Jin, Liao, Lei, Wu, Tong, Lin, Dingchang, Liu, Yayuan, Jaramillo, Thomas F., Norskov, Jens K., & Cui, Yi. High-efficiency oxygen reduction to hydrogen peroxide catalysed by oxidized carbon materials. United States. doi:10.1038/s41929-017-0017-x.
Lu, Zhiyi, Chen, Guangxu, Siahrostami, Samira, Chen, Zhihua, Liu, Kai, Xie, Jin, Liao, Lei, Wu, Tong, Lin, Dingchang, Liu, Yayuan, Jaramillo, Thomas F., Norskov, Jens K., and Cui, Yi. Mon . "High-efficiency oxygen reduction to hydrogen peroxide catalysed by oxidized carbon materials". United States. doi:10.1038/s41929-017-0017-x. https://www.osti.gov/servlets/purl/1458611.
@article{osti_1458611,
title = {High-efficiency oxygen reduction to hydrogen peroxide catalysed by oxidized carbon materials},
author = {Lu, Zhiyi and Chen, Guangxu and Siahrostami, Samira and Chen, Zhihua and Liu, Kai and Xie, Jin and Liao, Lei and Wu, Tong and Lin, Dingchang and Liu, Yayuan and Jaramillo, Thomas F. and Norskov, Jens K. and Cui, Yi},
abstractNote = {Hydrogen peroxide (H2O2) is a valuable chemical with a wide range of applications, but the current industrial synthesis of H2O2 involves an energy-intensive anthraquinone process. The electrochemical synthesis of H2O2 from oxygen reduction offers an alternative route for on-site applications; the efficiency of this process depends greatly on identifying cost-effective catalysts with high activity and selectivity. Here, we demonstrate a facile and general approach to catalyst development via the surface oxidation of abundant carbon materials to significantly enhance both the activity and selectivity (~90%) for H2O2 production by electrochemical oxygen reduction. We find that both the activity and selectivity are positively correlated with the oxygen content of the catalysts. In conclusion, the density functional theory calculations demonstrate that the carbon atoms adjacent to several oxygen functional groups (–COOH and C–O–C) are the active sites for oxygen reduction reaction via the two-electron pathway, which are further supported by a series of control experiments.},
doi = {10.1038/s41929-017-0017-x},
journal = {Nature Catalysis},
issn = {2520-1158},
number = 2,
volume = 1,
place = {United States},
year = {2018},
month = {1}
}

Journal Article:
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Figures / Tables:

Fig. 1 Fig. 1: Oxygen reduction performance of CNTs and O-CNTs. a,b, Polarization curves at 1,600 r.p.m. (solid lines) and simultaneous H2O2 detection currents at the ring electrode (dashed lines) for both catalysts in 0.1 M KOH (a) or 0.1 M phosphate buffered saline (PBS; b). c,d, Calculated selectivity of these two catalysts atmore » various potentials at 0.1 M KOH (c) and 0.1 M PBS (d). e,f, Stability measurements of O-CNTs at 0.1 M KOH (e) and 0.1 M PBS (f). These results indicate that the O-CNTs possess both higher activity and higher H2O2 selectivity than CNTs towards oxygen reduction to produce H2O2 in alkaline and neutral electrolytes. RHE, reversible hydrogen electrode.« less

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