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Substantial lifetime enhancement for Si-based photoanodes enabled by amorphous TiO₂ coating with improved stoichiometry.

ABSTRACT: Amorphous titanium dioxide (TiO₂) film coating by atomic layer deposition (ALD) is a promising strategy to extend the photoelectrode lifetime to meet the industrial standard for solar fuel generation. To realize this promise, the essential structure-property relationship that dictates the protection lifetime needs to be uncovered. In this work, we reveal that in addition to the imbedded crystalline phase, the presence of residual chlorine (Cl) ligands is detrimental to the silicon (Si) photoanode lifetime. We further demonstrate that post-ALD in-situ water treatment can effectively decouple the ALD reaction completeness from crystallization. The as-processed TiO₂ film has a much lower residual Cl concentration and thus an improved film stoichiometry, while its uniform amorphous phase is well preserved. As a result, the protected Si photoanode exhibits a substantially improved lifetime to ~600 h at a photocurrent density of more than 30 mA/cm². This study demonstrates a significant advancement toward sustainable hydrogen generation.

SUBMITTER: Dong Y

PROVIDER: S-EPMC10073107 | biostudies-literature | 2023 Apr

REPOSITORIES: biostudies-literature

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Substantial lifetime enhancement for Si-based photoanodes enabled by amorphous TiO<sub>2</sub> coating with improved stoichiometry.

Dong Yutao Y Abbasi Mehrdad M Meng Jun J German Lazarus L Carlos Corey C Li Jun J Zhang Ziyi Z Morgan Dane D Hwang Jinwoo J Wang Xudong X

Nature communications 20230404 1

Amorphous titanium dioxide (TiO<sub>2</sub>) film coating by atomic layer deposition (ALD) is a promising strategy to extend the photoelectrode lifetime to meet the industrial standard for solar fuel generation. To realize this promise, the essential structure-property relationship that dictates the protection lifetime needs to be uncovered. In this work, we reveal that in addition to the imbedded crystalline phase, the presence of residual chlorine (Cl) ligands is detrimental to the silicon (Si ...[more]

PMID: 37015923

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Project description:The heterostructure WO3/BiVO4-based photoanodes have garnered significant interest for photoelectrochemical (PEC) solar-driven water splitting to produce hydrogen. However, challenges such as inadequate charge separation and photocorrosion significantly hinder their performance, limiting overall solar-to-hydrogen conversion efficiency. The incorporation of cocatalysts has shown promise in improving charge separation at the photoanode, yet mitigating photocorrosion remains a formidable challenge. Amorphous metal oxide-based passivation layers offer a potential solution to safeguard semiconductor catalysts. We examine the structural, surface morphological, and optical properties of two-step-integrated sputter and spray-coated TiO2 thin films and their integration onto WO3/BiVO4, both with and without NiOOH cocatalyst deposition. The J-V experiments reveal that the NiOOH cocatalyst enhances the photocurrent density of the WO3/BiVO4 photoanode in water splitting reactions from 2.81 to 3.87 mA/cm2. However, during prolonged operation, the photocurrent density degrades by 52%. In contrast, integrated sputter and spray-coated TiO2 passivation layer-coated WO3/BiVO4/NiOOH samples demonstrate a ∼88% enhancement in photocurrent density (5.3 mA/cm2) with minimal degradation, emphasizing the importance of a strategic coating protocol to sustain photocurrent generation. We further explore the feasibility of using natural mine wastewater as an electrolyte feedstock in PEC generation. Two-compartment PEC cells, utilizing both fresh water and metal mine wastewater feedstocks exhibit 66.6 and 74.2 μmol/h cm2 hydrogen generation, respectively. Intriguingly, the recovery of zinc (Zn2+) heavy metals on the cathode surface in the mine wastewater electrolyte is confirmed through surface morphology and elemental analysis. This work underscores the significance of passivation layer and cocatalyst coating methodologies in a sequential order to enhance charge separation and protect the photoanode from photocorrosion, contributing to sustainable hydrogen generation. Additionally, it suggests the potential of utilizing wastewater in electrolyzers as an alternative to freshwater resources.

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Substantial lifetime enhancement for Si-based photoanodes enabled by amorphous TiO₂ coating with improved stoichiometry.

Publications

Substantial lifetime enhancement for Si-based photoanodes enabled by amorphous TiO<sub>2</sub> coating with improved stoichiometry.

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Substantial lifetime enhancement for Si-based photoanodes enabled by amorphous TiO2 coating with improved stoichiometry.

Publications

Substantial lifetime enhancement for Si-based photoanodes enabled by amorphous TiO<sub>2</sub> coating with improved stoichiometry.

Similar Datasets

OmicsDI is part of the ELIXIR infrastructure

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Substantial lifetime enhancement for Si-based photoanodes enabled by amorphous TiO₂ coating with improved stoichiometry.