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Bilayer Vesicles as a Noncovalent Immobilization Platform of Electrocatalysts for Energy Conversion in Neutral Aqueous Media
Author(s) -
Chung MinWen,
Liu YuChiao,
Yen TaoHung,
Chiang MingHsi
Publication year - 2018
Publication title -
chemelectrochem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.182
H-Index - 59
ISSN - 2196-0216
DOI - 10.1002/celc.201701051
Subject(s) - overpotential , electrocatalyst , aqueous solution , bilayer , chemistry , electron transfer , catalysis , water splitting , vesicle , electrode , oxygen evolution , chemical engineering , inorganic chemistry , electrochemistry , combinatorial chemistry , photochemistry , membrane , organic chemistry , photocatalysis , engineering , biochemistry
We show that synthetic [FeFe]‐hydrogenase mimics embedded within liposomes can be immobilized on high‐surface‐area carbon blacks for the construction of a three‐dimensional (3D) electrode for H 2 production in neutral aqueous media. In this design, the bilayer vesicles (liposomes) serve as a water‐insoluble electrocatalyst carrier, facilitating access of the embedded catalysts to aqueous solution. Fast electron‐transfer rates and low overpotentials are achieved compared to water‐soluble catalysts. The electron‐transfer rate constant between the embedded [(μ‐bdt)Fe 2 (CO) 6 ] (bdt=1,2‐benzenedithiolate; 1 ) and the electrode is estimated to be 1.33±0.15 s −1 . Immobilized [(μ,κ 2 ‐bdt‐Me)(μ‐PPh 2 )Fe 2 (CO) 5 ] (Me=methyl; 3 ) is able to catalyze H 2 production in Na 2 SO 4(aq) solution (pH=7) at −1.06 V (vs. SHE) with an overpotential of approximately 400 mV. The reported general method for the construction of 3D electrodes paves the way to potential applications of molecular catalysts in energy devices.