期刊
CHEMICAL SCIENCE
卷 10, 期 16, 页码 4469-4475出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c8sc05006f
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资金
- French National Research Agency (Labex program) [ARCANE - ANR-11-LABX-0003-01, ANR-17-EURE-0003]
Hydrogen production through direct sunlight-driven water splitting in photo-electrochemical cells (PECs) is a promising solution for energy sourcing. PECs need to fulfill three criteria: sustainability, cost-effectiveness and stability. Here we report an efficient and stable photocathode platform for H-2 evolution based on Earthabundant elements. A p-type silicon surface was protected by atomic layer deposition (ALD) with a 15 nm TiO2 layer, on top of which a 300 nm mesoporous TiO2 layer was spin-coated. The cobalt diimine-dioxime molecular catalyst was covalently grafted onto TiO2 through phosphonate anchors and an additional 0.2 nm ALD-TiO2 layer was applied for stabilization. This assembly catalyzes water reduction into H-2 in phosphate buffer (pH 7) with an onset potential of + 0.47 V vs. RHE. The resulting current density is 1.3 0.1 mA cm 2 at 0 V vs. RHE under AM 1.5 solar irradiation, corresponding to a turnover number of 260 per hour of operation and a turnover frequency of 0.071 s(-1).
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