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.

Control of Electrons' Spin Eliminates Hydrogen Peroxide Formation during Water Splitting / Mtangi, Wilbert; Tassinari, Francesco; Vankayala, Kiran; Vargas Jentzsch, Andreas; Adelizzi, Beatrice; Palmans, Anja R. A.; Fontanesi, Claudio; Meijer, E. W; Naaman, Ron. - In: JOURNAL OF THE AMERICAN CHEMICAL SOCIETY. - ISSN 0002-7863. - 139:7(2017), pp. 2794-2798. [10.1021/jacs.6b12971]

Control of Electrons' Spin Eliminates Hydrogen Peroxide Formation during Water Splitting

Tassinari, Francesco;FONTANESI, Claudio;
2017

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.
10-feb-2017
139
7
2794
2798
Control of Electrons' Spin Eliminates Hydrogen Peroxide Formation during Water Splitting / Mtangi, Wilbert; Tassinari, Francesco; Vankayala, Kiran; Vargas Jentzsch, Andreas; Adelizzi, Beatrice; Palmans, Anja R. A.; Fontanesi, Claudio; Meijer, E. W; Naaman, Ron. - In: JOURNAL OF THE AMERICAN CHEMICAL SOCIETY. - ISSN 0002-7863. - 139:7(2017), pp. 2794-2798. [10.1021/jacs.6b12971]
Mtangi, Wilbert; Tassinari, Francesco; Vankayala, Kiran; Vargas Jentzsch, Andreas; Adelizzi, Beatrice; Palmans, Anja R. A.; Fontanesi, Claudio; Meijer, E. W; Naaman, Ron
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Utilizza questo identificativo per citare o creare un link a questo documento: http://hdl.handle.net/11380/1141211
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