Precious-metal free photoelectrochemical water splitting with immobilised molecular Ni and Fe redox catalysts

Chemical Science
Timothy E RosserErwin Reisner

Abstract

Splitting water into hydrogen and oxygen with molecular catalysts and light has been a long-established challenge. Approaches in homogeneous systems have been met with little success and the integration of molecular catalysts in photoelectrochemical cells is challenging due to inaccessibility and incompatibility of functional hybrid molecule/material electrodes with long-term stability in aqueous solution. Here, we present the first example of light-driven water splitting achieved with precious-metal-free molecular catalysts driving both oxygen and hydrogen evolution reactions. Mesoporous TiO2 was employed as a low-cost scaffold with long-term stability for anchoring a phosphonic acid-modified nickel(ii) bis-diphosphine catalyst (NiP) for electrocatalytic proton reduction. A turnover number of 600 mol H2 per mol NiP was achieved after 8 h controlled-potential electrolysis at a modest overpotential of 250 mV. X-ray photoelectron, UV-vis and IR spectroscopies confirmed that the molecular structure of the Ni catalyst remains intact after prolonged hydrogen production, thereby reasserting the suitability of molecular catalysts in the development of effective, hydrogen-evolving materials. The relatively mild operating conditions of ...Continue Reading

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Citations

Oct 27, 2018·Chemistry, an Asian Journal·Tianqi LiuLicheng Sun
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Dec 11, 2020·Chemical Communications : Chem Comm·Hao-Lin WuLi-Zhu Wu
Dec 22, 2020·Dalton Transactions : an International Journal of Inorganic Chemistry·Elisabetta BenazziMirco Natali
Mar 27, 2021·Nature Chemistry·Laurent SéveryS David Tilley
Jun 25, 2021·Chemical Science·Carlota Bozal-GinestaJames R Durrant
Nov 20, 2018·Journal of the American Chemical Society·Katarzyna P SokolErwin Reisner
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Oct 1, 2021·Chemical Society Reviews·Ana Belén Muñoz-GarcíaMarina Freitag
Oct 23, 2021·Journal of the American Chemical Society·Jérémy SchildVincent Artero
Dec 9, 2021·Journal of the American Chemical Society·Bethany M StratakesAlexander J M Miller

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Methods Mentioned

BETA
scanning electron microscopy
X-ray
column chromatography

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