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

被引：293

作者：

Mtangi, Wilbert ^{[1
]}

Tassinari, Francesco ^{[1
]}

Vankayala, Kiran ^{[1
]}

Jentzsch, Andreas Vargas ^{[2
]}

Adelizzi, Beatrice ^{[2
]}

Palmans, Anja R. A. ^{[2
]}

Fontanesi, Claudio ^{[3
]}

Meijer, E. W. ^{[2
]}

Naaman, Ron ^{[1
]}

机构：

[1] Weizmann Inst Sci, Dept Chem Phys, IL-76100 Rehovot, Israel

[2] Eindhoven Univ Technol, Inst Complex Mol Syst, NL-5600 MB Eindhoven, Netherlands

[3] Univ Modena & Reggio Emilia, Dept Engn, Via Vivarelli 10, I-41125 Modena, Italy

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2017年 / 139卷 / 07期

基金：

欧洲研究理事会; 欧盟地平线“2020”;

关键词：

ARTIFICIAL PHOTOSYNTHESIS; OXYGEN EVOLUTION; CATALYSIS; RUO2;

D O I：

10.1021/jacs.6b12971

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

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.

引用

页码：2794 / 2798

页数：5

共 43 条

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