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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.
Publication status:
Published
Peer review status:
Peer reviewed

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Publisher copy:
10.1021/jacs.6b12971

Authors


More by this author
Institution:
University of Oxford
Division:
MPLS
Department:
Chemistry
Sub department:
Organic Chemistry
Role:
Author


Publisher:
American Chemical Society
Journal:
Journal of the American Chemical Society More from this journal
Volume:
139
Issue:
7
Pages:
2794-2798
Publication date:
2017-01-30
Acceptance date:
2017-01-30
DOI:
ISSN:
0002-7863 and 1520-5126
Pmid:
28132505


Language:
English
Keywords:
Pubs id:
pubs:679658
UUID:
uuid:cdf47b04-261d-4ad3-a0e9-7983c3b05249
Local pid:
pubs:679658
Source identifiers:
679658
Deposit date:
2017-11-12

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