Photoproduction of Hydrogen by Decamethylruthenocene Combined with Electrochemical Recycling

Lucie Rivier; Pekka Peljo; Laurent A.C. Vannay; Grégoire C. Gschwend; Manuel A. Méndez; Clémence Corminboeuf; Micheál D. Scanlon; Hubert H. Girault

doi:10.1002/anie.201610240

Photoproduction of Hydrogen by Decamethylruthenocene Combined with Electrochemical Recycling

Lucie Rivier
, Pekka Peljo
, Laurent A.C. Vannay
, Grégoire C. Gschwend
, Manuel A. Méndez
, Clémence Corminboeuf
, Micheál D. Scanlon
, Hubert H. Girault

Swiss Federal Institute of Technology Lausanne
University College Cork

Research output: Contribution to journal › Article › peer-review

Abstract

The photoinduced hydrogen evolution reaction (HER) by decamethylruthenocene, Cp₂*Ru^II(Cp*=C₅Me₅), is reported. The use of a metallocene to photoproduce hydrogen is presented as an alternative strategy to reduce protons without involving an additional photosensitizer. The mechanism was investigated by (spectro)electrochemical and spectroscopic (UV/Vis and¹H NMR) measurements. The photoactivated hydride involved was characterized spectroscopically and the resulting [Cp₂*Ru^III]⁺species was electrochemically regenerated in situ on a fluorinated tin oxide electrode surface. A promising internal quantum yield of 25 % was obtained. Optimal experimental conditions— especially the use of weakly coordinating solvent and counterions—are discussed.

Original language	English
Pages (from-to)	2324-2327
Number of pages	4
Journal	Angewandte Chemie - International Edition
Volume	56
Issue number	9
DOIs	https://doi.org/10.1002/anie.201610240
Publication status	Published - 20 Feb 2017
Externally published	Yes

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

SDG 7 Affordable and Clean Energy

Keywords

decamethylruthenocene
electrocatalysis
hydrogen evolution reaction
metallocenes

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10.1002/anie.201610240

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title = "Photoproduction of Hydrogen by Decamethylruthenocene Combined with Electrochemical Recycling",

abstract = "The photoinduced hydrogen evolution reaction (HER) by decamethylruthenocene, Cp2*RuII(Cp*=C5Me5), is reported. The use of a metallocene to photoproduce hydrogen is presented as an alternative strategy to reduce protons without involving an additional photosensitizer. The mechanism was investigated by (spectro)electrochemical and spectroscopic (UV/Vis and1H NMR) measurements. The photoactivated hydride involved was characterized spectroscopically and the resulting [Cp2*RuIII]+species was electrochemically regenerated in situ on a fluorinated tin oxide electrode surface. A promising internal quantum yield of 25 \% was obtained. Optimal experimental conditions— especially the use of weakly coordinating solvent and counterions—are discussed.",

keywords = "decamethylruthenocene, electrocatalysis, hydrogen evolution reaction, metallocenes",

author = "Lucie Rivier and Pekka Peljo and Vannay, \{Laurent A.C.\} and Gschwend, \{Gr{\'e}goire C.\} and M{\'e}ndez, \{Manuel A.\} and Cl{\'e}mence Corminboeuf and Scanlon, \{Miche{\'a}l D.\} and Girault, \{Hubert H.\}",

note = "Publisher Copyright: {\textcopyright} 2017 Wiley-VCH Verlag GmbH \& Co. KGaA, Weinheim",

year = "2017",

month = feb,

day = "20",

doi = "10.1002/anie.201610240",

language = "English",

volume = "56",

pages = "2324--2327",

journal = "Angewandte Chemie - International Edition",

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TY - JOUR

T1 - Photoproduction of Hydrogen by Decamethylruthenocene Combined with Electrochemical Recycling

AU - Rivier, Lucie

AU - Peljo, Pekka

AU - Vannay, Laurent A.C.

AU - Gschwend, Grégoire C.

AU - Méndez, Manuel A.

AU - Corminboeuf, Clémence

AU - Scanlon, Micheál D.

AU - Girault, Hubert H.

PY - 2017/2/20

Y1 - 2017/2/20

N2 - The photoinduced hydrogen evolution reaction (HER) by decamethylruthenocene, Cp2*RuII(Cp*=C5Me5), is reported. The use of a metallocene to photoproduce hydrogen is presented as an alternative strategy to reduce protons without involving an additional photosensitizer. The mechanism was investigated by (spectro)electrochemical and spectroscopic (UV/Vis and1H NMR) measurements. The photoactivated hydride involved was characterized spectroscopically and the resulting [Cp2*RuIII]+species was electrochemically regenerated in situ on a fluorinated tin oxide electrode surface. A promising internal quantum yield of 25 % was obtained. Optimal experimental conditions— especially the use of weakly coordinating solvent and counterions—are discussed.

AB - The photoinduced hydrogen evolution reaction (HER) by decamethylruthenocene, Cp2*RuII(Cp*=C5Me5), is reported. The use of a metallocene to photoproduce hydrogen is presented as an alternative strategy to reduce protons without involving an additional photosensitizer. The mechanism was investigated by (spectro)electrochemical and spectroscopic (UV/Vis and1H NMR) measurements. The photoactivated hydride involved was characterized spectroscopically and the resulting [Cp2*RuIII]+species was electrochemically regenerated in situ on a fluorinated tin oxide electrode surface. A promising internal quantum yield of 25 % was obtained. Optimal experimental conditions— especially the use of weakly coordinating solvent and counterions—are discussed.

KW - decamethylruthenocene

KW - electrocatalysis

KW - hydrogen evolution reaction

KW - metallocenes

UR - https://www.scopus.com/pages/publications/85011319768

U2 - 10.1002/anie.201610240

DO - 10.1002/anie.201610240

M3 - Article

C2 - 28124825

AN - SCOPUS:85011319768

SN - 1433-7851

VL - 56

SP - 2324

EP - 2327

JO - Angewandte Chemie - International Edition

JF - Angewandte Chemie - International Edition

IS - 9

ER -

Photoproduction of Hydrogen by Decamethylruthenocene Combined with Electrochemical Recycling

Abstract

UN SDGs

Keywords

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