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A robust ALD-protected silicon-based hybrid photoelectrode for hydrogen evolution under aqueous conditions.

ABSTRACT: 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 H₂ evolution based on Earth-abundant 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 H₂ 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.

SUBMITTER: Chandrasekaran S

PROVIDER: S-EPMC6482884 | biostudies-literature | 2019 Apr

REPOSITORIES: biostudies-literature

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A robust ALD-protected silicon-based hybrid photoelectrode for hydrogen evolution under aqueous conditions.

Chandrasekaran Soundarrajan S Kaeffer Nicolas N Cagnon Laurent L Aldakov Dmitry D Fize Jennifer J Nonglaton Guillaume G Baleras François F Mailley Pascal P Artero Vincent V

Chemical science 20190312 16

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<sub>2</sub> evolution based on Earth-abundant elements. A p-type silicon surface was protected by atomic layer deposition (ALD) with a 15 nm TiO<sub>2</sub> layer, on top of which a 300 nm mesopor ...[more]

PMID: 31057774

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Project description:Together with longer production periods, the commercial transition to day-neutral strawberry (Fragaria × ananassa) varieties has favored the development of diseases such as powdery mildew (Podosphaera aphanis) that thrives in late summer-early fall. In an attempt to find alternative solutions to fungicides currently employed to curb the disease, we wanted to investigate the potential of silicon (Si) amendments that have been associated with prophylactic properties against powdery mildews. To this end, our first objective was to determine if strawberry was a Si-competent species following the recent characterization of the properties of Si transporters that plants must carry to uptake silicic acid. Based on genomic data, we were able to conclude that strawberry contained both functional influx (Lsi1) and efflux (Lsi2) transporters for Si uptake. Subsequently commercial experiments under high tunnel and field conditions were conducted with different Si fertilization regimes: constant soluble Si feeding in high tunnel, and bi-weekly soluble Si feeding or three concentrations of calcium silicate fertilization in the field. Results from high tunnel experiments showed that strawberry could accumulate as much as 3% Si on a dry-weight basis, the highest concentration ever reported for this species. All six tested cultivars contained roughly the same concentration, thereby confirming the limited genetic variability, also observed in other species, associated with the trait. Silicon fertilization under high tunnel led to a significant reduction of powdery mildew severity in both years and on all cultivars, and a significant increase in yield of marketable fruits reaching as much as 300% with cv. Monterey. By contrast, Si fertilization under field conditions in soils deficient in plant available Si, either in soluble or solid form, did not result in significant accumulation of Si in plants, regardless of the cultivars, year or concentrations. Our results have thus provided both genotypic and phenotypic proof that strawberry can greatly benefit from Si fertilization, but have also highlighted the importance of validating the fertilization regime to ensure that Si is properly absorbed and/or available to the plant.

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A robust ALD-protected silicon-based hybrid photoelectrode for hydrogen evolution under aqueous conditions.

Publications

A robust ALD-protected silicon-based hybrid photoelectrode for hydrogen evolution under aqueous conditions.

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