Selective electrochemical generation of hydrogen peroxide from water oxidation

Viswanathan, Venkatasubramanian; Hansen, Heine A.; Norskov, Jens K.

doi:10.1021/acs.jpclett.5b02178

Title: Selective electrochemical generation of hydrogen peroxide from water oxidation

Journal Article · Thu Oct 08 00:00:00 EDT 2015 · Journal of Physical Chemistry Letters

DOI:https://doi.org/10.1021/acs.jpclett.5b02178· OSTI ID:1263404

Viswanathan, Venkatasubramanian ^[1]; Hansen, Heine A. ^[2]; Norskov, Jens K. ^[3]

Carnegie Mellon Univ., Pittsburgh, PA (United States); Stanford Univ., Stanford, CA (United States)
Technical Univ. of Denmark, Lyngby (Denmark); Stanford Univ., Stanford, CA (United States)
Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)

Water is a life-giving source, fundamental to human existence, yet over a billion people lack access to clean drinking water. The present techniques for water treatment such as piped, treated water rely on time and resource intensive centralized solutions. In this work, we propose a decentralized device concept that can utilize sunlight to split water into hydrogen and hydrogen peroxide. The hydrogen peroxide can oxidize organics while the hydrogen bubbles out. In enabling this device, we require an electrocatalyst that can oxidize water while suppressing the thermodynamically favored oxygen evolution and form hydrogen peroxide. Using density functional theory calculations, we show that the free energy of adsorbed OH* can be used to determine selectivity trends between the 2e– water oxidation to H₂O₂ and the 4e– oxidation to O₂. We show that materials which bind oxygen intermediates sufficiently weakly, such as SnO₂, can activate hydrogen peroxide evolution. Furthermore, we present a rational design principle for the selectivity in electrochemical water oxidation and identify new material candidates that could perform H₂O₂ evolution selectively.

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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:: AC02-76SF00515

OSTI ID:: 1263404

Report Number(s):: SLAC-PUB-16634; arXiv:1509.07444

Journal Information:: Journal of Physical Chemistry Letters, Vol. 6, Issue 21; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 108 works

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