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Control of Electrons' Spin Eliminates Hydrogen Peroxide Formation During Water Splitting.


ABSTRACT: The production of hydrogen through water splitting in a photoelectrochemical cell suffers from an overpotential that limits the efficiencies. In addition, hydrogen-peroxide formation is identified as a competing process affecting the oxidative stability of photoelectrodes. We impose spin-selectivity by coating the anode with chiral organic semiconductors from helically aggregated dyes as sensitizers; Zn-porphyrins and triarylamines. Hydrogen peroxide formation is dramatically suppressed, while the overall current through the cell, correlating with the water splitting process, is enhanced. Evidence for a strong spin-selection in the chiral semiconductors is presented by magnetic conducting (mc-)AFM measurements, in which chiral and achiral Zn-porphyrins are compared. These findings contribute to our understanding of the underlying mechanism of spin selectivity in multiple electron-transfer reactions and pave the way toward better chiral dye-sensitized photoelectrochemical cells.

SUBMITTER: Mtangi W 

PROVIDER: S-EPMC5330654 | biostudies-literature | 2017 Feb

REPOSITORIES: biostudies-literature

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Control of Electrons' Spin Eliminates Hydrogen Peroxide Formation During Water Splitting.

Mtangi Wilbert W   Tassinari Francesco F   Vankayala Kiran K   Vargas Jentzsch Andreas A   Adelizzi Beatrice B   Palmans Anja R A AR   Fontanesi Claudio C   Meijer E W EW   Naaman Ron R  

Journal of the American Chemical Society 20170210 7


The production of hydrogen through water splitting in a photoelectrochemical cell suffers from an overpotential that limits the efficiencies. In addition, hydrogen-peroxide formation is identified as a competing process affecting the oxidative stability of photoelectrodes. We impose spin-selectivity by coating the anode with chiral organic semiconductors from helically aggregated dyes as sensitizers; Zn-porphyrins and triarylamines. Hydrogen peroxide formation is dramatically suppressed, while t  ...[more]

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