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Dynamic semiconductor-electrolyte interface for sustainable solar water splitting over 600 hours under neutral conditions.

ABSTRACT: Photoelectrochemical (PEC) water splitting that functions in pH-neutral electrolyte attracts increasing attention to energy demand sustainability. Here, we propose a strategy to in situ form a NiB layer by tuning the composition of the neutral electrolyte with the additions of nickel and borate species, which improves the PEC performance of the BiVO₄ photoanode. The NiB/BiVO₄ exhibits a photocurrent density of 6.0 mA cm^-2 at 1.23 V_RHE with an onset potential of 0.2 V_RHE under 1 sun illumination. The photoanode displays a photostability of over 600 hours in a neutral electrolyte. The additive of Ni²⁺ in the electrolyte, which efficiently inhibits the dissolution of NiB, can accelerate the photogenerated charge transfer and enhance the water oxidation kinetics. The borate species with B─O bonds act as a promoter of catalyst activity by accelerating proton-coupled electron transfer. The synergy effect of both species suppresses the surface charge recombination and inhibits the photocorrosion of BiVO₄.

SUBMITTER: Gao RT

PROVIDER: S-EPMC9812387 | biostudies-literature | 2023 Jan

REPOSITORIES: biostudies-literature

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Dynamic semiconductor-electrolyte interface for sustainable solar water splitting over 600 hours under neutral conditions.

Gao Rui-Ting RT Nguyen Nhat Truong NT Nakajima Tomohiko T He Jinlu J Liu Xianhu X Zhang Xueyuan X Wang Lei L Wu Limin L

Science advances 20230104 1

Photoelectrochemical (PEC) water splitting that functions in pH-neutral electrolyte attracts increasing attention to energy demand sustainability. Here, we propose a strategy to in situ form a NiB layer by tuning the composition of the neutral electrolyte with the additions of nickel and borate species, which improves the PEC performance of the BiVO4 photoanode. The NiB/BiVO4 exhibits a photocurrent density of 6.0 mA cm-2 at 1.23 VRHE with an onset pot ...[more]

PMID: 36598972

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Project description:The relentless consumption of fossil fuels and soaring CO2 emissions have plunged the world into an energy and environmental crisis. As society grapples with these challenges, the demand for clean, renewable, and sustainable energy solutions has never been more urgent. However, even though many efforts have been made in this field, there is still room for improvement concerning efficiency, material stability, and catalytic enhancement regarding kinetics and selectivity of photoelectrochemical (PEC) processes. Herein, we provide the experimental proof for the enhancement of the photocurrent efficiency by the critical focus on semiconductor-electrolyte interface (SEI) properties. By tailoring electrolyte composition, researchers can unlock significant improvements in catalytic efficiency and stability, paving the way for advanced PEC technologies. In this study, we investigate the influence of electrolyte composition on SEI properties and its impact on PEC performance. By employing electrolytes enriched with carbonates, borates, sulphates, and alkali cations, we demonstrate their profound role in optimising photoelectrochemical CO2 reduction reaction (CO2RR) efficiency. Central to this work is Cu2O-an affordable, highly promising photocatalyst. While its potential is undeniable, Cu2O's inherent instability and diverse reduction products, ranging from CH3OH to CO, HCOOH, CH3COOH, and CH3CH2OH, have hindered its widespread adoption in PEC CO2 reduction (CO2RR). Our approach leverages a straightforward yet powerful electrodeposition method, enabling a deeper exploration of SEI dynamics during photocatalysis. Key parameters, such as carbonate concentration, local pH, alkali cation presence, anionic geometry, CO2 solubility, and electrolyte conductivity, are systematically investigated. The findings reveal the formation of a unique "rigid layer" at the photocatalyst surface, driven by specific cation-anion interactions. This rigid layer plays a pivotal role in boosting PEC performance, offering a new perspective on optimising, among other PEC processes, CO2RR catalytic efficiency. This profound study bridges a critical knowledge gap, shedding light on the dual influence of cations and anions on SEI properties and PEC CO2RR. By unravelling these intricate interactions, we provide a roadmap for designing next-generation PEC systems. These insights pave the way for sustainable energy advancements, inspiring innovative strategies to tackle one of the most pressing challenges of our time.

Project description:IntroductionHydrogen is considered as a clean alternative green energy future fuel. Since the Honda-Fujishima effect for photoelectrochemical water splitting is known, there has been a substantial boost in this field. Numerous photocatalysts based on metals, semiconductors, and organic-inorganic hybrid-systems have been proposed. Several factors limit their efficiency, e.g., a stable PEC-WS setup, absorbing visible light, well-aligned band energy for charge transfer, electrons and holes, and their separation to avoid recombination and limited water redox reactions. Metallic doping and impregnation of stable and efficient co-catalysts such as Pt, Ag, and Au showed enhanced PEC-WS. We used Cobalt-based co-catalyst with molybdenum oxysulfide photocatalyst for effectual solar-driven water splitting.ObjectivesTo develop photocatalysts for efficient PEC processes capable of absorbing sufficient visible light, good band energy for effective charge transfer, inexpensive, significant solar-to-chemical energy conversion efficiencies. Above all, it is developing such PEC-WS systems that will be commercially viable for renewable energy resources.MethodsWe prepared Molybdenum oxysulphide-cobalt phosphate photocatalyst for PEC-WS through a facile hydrothermal route using ammonium heptamolybdate, thiourea, and metallic Cobalt precursors.ResultsAn effectual photocatalyst is produced for solar-driven water splitting. The conformal morphology of MoOxSy-CoPi nanoflowers is a significant feature, as observed under FE-SEM and HR-TEM. XRD confirmed the degree of purity and orthorhombic crystal structure of MoOxSy-CoPi. EDX and XPS identify the elemental compositions and corresponding oxidation states of each atom. A 2.44 eV band-gap energy is calculated for MoOxSy-CoPi from the diffused reflectance spectrum. Photo- Electrochemical Studies (PEC) under 1-SUN solar irradiation revealed 7-8 folds enhanced photocurrent (∼ 3.5 mA/cm2) generated from MoOxSy-CoPi/FTO in comparison to Co-PI/FTO (∼ 0.5 mA/cm2) and MoOxSy-/FTO respectively, within 0.5 M Na2SO4 electrolyte (@pH=7) and standard three electrodes electrochemical cell.ConclusionOur results showed MoOxSy-CoPi as promising photocatalyst material for improved solar-driven photoelectrochemical water splitting system.

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Dynamic semiconductor-electrolyte interface for sustainable solar water splitting over 600 hours under neutral conditions.

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Dynamic semiconductor-electrolyte interface for sustainable solar water splitting over 600 hours under neutral conditions.

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