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Results for “SOLAR WATER SPLITTING”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

Progress on ternary oxide-based photoanodes for use in photoelectrochemical cells for solar water splitting

Solar water splitting using photoelectrochemical cells (PECs) has emerged as one of the most promising routes to produce hydrogen as a clean and renewable fuel source. Among various semiconductors that have been considered as photoelectrodes for use in PECs, oxide-based photoanodes are particularly attractive because of their stability in aqueous media in addition to inexpensive and facile processing compared to other types of semiconductors. However, they typically suffer from poor charge carrier separation and transport. In the past few years, there has been tremendous progress in developing ternary oxide-based photoelectrodes, specifically, photoanodes. The use of ternary oxides provides more opportunities to tune the composition and electronic structure of the photoelectrode compared to binary oxides, thus providing more freedom to tune the photoelectrochemical properties. In this article, we outline the important characteristics to analyze when evaluating photoanodes and review the major recent progress made on the development of ternary oxide-based photoanodes. For each system, we highlight the favorable and unfavorable features and summarize the strategies utilized to address the challenges associated with each material. Finally, by combining our analyses of all the photoanodes surveyed in this review, we provide possible future research directions for each compound and an outlook for constructing more efficient oxide-based PECs. Overall, this review will provide a critical overview of current ternary oxide-based photoanodes and will serve as a platform for the design of future oxide-based PECs.

25 ENERGY STORAGE↗
DOE OSTI2017

Modelling heterogeneous interfaces for solar water splitting

The generation of hydrogen from water and sunlight offers a promising approach for producing scalable and sustainable carbon-free energy. The key of a successful solar-to-fuel technology is the design of efficient, long-lasting and low-cost photoelectrochemicalcells (PECs), which are responsible for absorbing sunlight and driving water splitting reactions. To this end, a detailed understanding and control of heterogeneous interfaces between photoabsorbers, electrolytes and catalysts present in PECs is essential. This paper reviews recent progress and open challenges in predicting physicochemical properties of heterogeneous interfaces for solar water splitting applications using first-principles-based approaches, and highlights the key role of these calculations in interpreting increasingly complex experiments.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Stable Unassisted Solar Water Splitting on Semiconductor Photocathodes Protected by Multifunctional GaN Nanostructures

Producing hydrogen by unassisted solar water splitting is one essential step to make direct solar fuel conversion a viable energy source. To date, however, there has been no demonstration of stable photoelectrodes for high efficiency photoelectrochemical water splitting. In this work, we report that a GaInP2/GaAs/Ge triple-junction (3J) photocathode protected by multi-functional GaN nanostructures can enable both efficient and relatively stable solar water splitting. A 12.6% solar-to-hydrogen (STH) efficiency is measured without any external bias. Of particular importance, we demonstrate relatively stable solar water splitting for 80 hours in three-electrode configuration and 57 hours in two-electrode measurement at zero bias. This is the best reported stability for multi-junction semiconductor photocathodes in two-electrode configuration to our knowledge. Here, the multifunctional GaN nanostructure significantly reduces the charge transfer resistance at semiconductor/electrolyte interface and protects III-V materials against corrosion. Such multi-functional GaN photocatalytic nanostructures provide a new pathway to improve the performance of conventional photoelectrodes to achieve both efficient and stable unassisted solar water splitting.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2013

A Fully Integrated Nanosystem of Semiconductor Nanowires for Direct Solar Water Splitting

Artificial photosynthesis, the biomimetic approach to converting sunlight?s energy directly into chemical fuels, aims to imitate nature by using an integrated system of nanostructures, each of which plays a specific role in the sunlight-to-fuel conversion process. Here we describe a fully integrated system of nanoscale photoelectrodes assembled from inorganic nanowires for direct solar water splitting. Similar to the photosynthetic system in a chloroplast, the artificial photosynthetic system comprises two semiconductor light absorbers with large surface area, an interfacial layer for charge transport, and spatially separated cocatalysts to facilitate the water reduction and oxidation. Under simulated sunlight, a 0.12percent solar-to-fuel conversion efficiency is achieved, which is comparable to that of natural photosynthesis. The result demonstrates the possibility of integrating material components into a functional system that mimics the nanoscopic integration in chloroplasts. It also provides a conceptual blueprint of modular design that allows incorporation of newly discovered components for improved performance.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Hematite‐Based Solar Water Splitting in Acidic Solutions: Functionalization by Mono‐ and Multilayers of Iridium Oxygen‐Evolution Catalysts

Abstract Solar water splitting in acidic solutions has important technological implications, but has not been demonstrated to date in a dual absorber photoelectrochemical cell. The lack of functionally stable water‐oxidation catalysts (WOCs) in acids is a key reason for this slow development. The only WOCs that are stable at low pH are Ir‐based systems, which are typically too expensive to be implemented broadly. It is now shown that this deficiency may be corrected by applying an ultra‐thin monolayer of a molecular Ir WOC to hematite for solar water splitting in acidic solutions. The turn‐on voltage is observed to shift cathodically by 250 mV upon the application of a monolayer of the molecular Ir WOC. When the molecular WOC is replaced by a heterogeneous multilayer derivative, stable solar water splitting for over 5 h is achieved with near‐unity Faradaic efficiency.

Li, Wei↗
DOE OSTI2020

Quantum Theory of Semiconductor Photo-Catalysis and Solar Water Splitting / Theory and Computation for Semiconductor Catalysis of Solar Water Splitting / Static and Dynamic Thermal Effects in Solids. Final Report

This is the final report. The finished research was published in 27 journal papers listed below. The topics fall roughly into seven categories: Photochemistry of water at the GaN ($10\bar{1}0$) surface; Quasiparticles: Band electrons and Anharmonic phonons; Quasiharmonic theory; Anharmonic lattice thermal conductivity; Water and Ice; Electron-phonon effects; and, Alloy theory.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Reduction kinetics of hercynite redox materials for solar thermochemical water splitting

Solar thermochemical water splitting (STWS) using a hercynite redox cycle is a promising technology for producing renewable H 2 . Here, the reduction kinetics of hercynite (FeAl 2 O 4 ) is evaluated using thermogravimetric and XRD analyses. The results indicate that as-prepared hercynite materials undergo reduction via two different reaction mechanisms. The reaction first proceeds by a nucleation and growth mechanism (AE1), followed by a third-order kinetic model (F3). XRD analyses show the occurrence of superstoichiometric oxygen in the spinel structure of FeAl 2 O 4+δ in the second reaction mechanism, which indicates the formation of cationic vacancies. TGA and XRD analyses confirm that hercynite maintains its spinel structure when the materials are thermally reduced and oxidized with steam. Differential scanning calorimetry (DSC) performed on FeAl 2 O 4 particles shows two heats of reaction in agreement with the two observed mechanisms. This is the first kinetics study to report on the thermal reduction of hercynite.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Modulating Carrier Transport via Defect Engineering in Solar Water Splitting Devices

Developing sustainable solar water splitting devices requires efficient separation and transport of photogenerated carriers. In this Perspective, we examine carrier transport in semiconductor photoelectrodes using bismuth vanadate as a primary model system and highlight strategies to significantly improve carrier delivery through defect engineering. To improve electron transport in low-mobility semiconductors, we introduce two distinct bulk doping methods, by homogeneously enhancing the bulk defect level or by forming distributed homojunctions with graded doping. Next, we demonstrate the use of structural boundaries as extrinsic pathways for fast electron transport, thus providing novel insights to engineer materials’ macroscopic conductivity. Third, we describe the importance of interface design in terms of structural, chemical, and electronic matching at the back contact to suppress carrier recombination. Lastly, we highlight the methods for surface defect control via passivation and catalysis and give a brief outlook of research challenges and opportunities for solar water splitting.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2017

Enhancing Mo:BiVO 4 Solar Water Splitting with Patterned Au Nanospheres by Plasmon-Induced Energy Transfer [Rational Nanopositioning for BiVO 4 Solar Water Splitting by Plasmon-induced Energy Transfer]

Here, plasmonic metal nanostructures have been extensively investigated to improve the performance of metal oxide photoanodes for photoelectrochemical (PEC) solar water splitting cells. Most of these studies have focused on the effects of those metal nanostructures on enhancing light absorption and enabling direct energy transfer via hot electrons. However, several recent studies have shown that plasmonic metal nanostructures can improve the PEC performance of metal oxide photoanodes via another mechanism known as plasmon–induced resonant energy transfer (PIRET). However, this PIRET effect has not yet been tested for the molybdenum–doped bismuth vanadium oxide (Mo:BiVO 4 ), regarded as one of the best metal oxide photoanode candidates. Here, this study constructs a hybrid Au nanosphere/Mo:BiVO 4 photoanode interwoven in a hexagonal pattern to investigate the PIRET effect on the PEC performance of Mo:BiVO 4 . This study finds that the Au nanosphere array not only increases light absorption of the photoanode as expected, but also improves both its charge transport and charge transfer efficiencies via PIRET, as confirmed by time–correlated single photon counting and transient absorption studies. As a result, incorporating the Au nanosphere array increases the photocurrent density of Mo:BiVO 4 at 1.23 V versus RHE by ≈2.2–fold (2.83 mA cm –2 ).

36 MATERIALS SCIENCE↗
DOE OSTI2017

Investigation of Pristine and (Mo, W)-Doped Cu 11 V 6 O 26 for Use as Photoanodes for Solar Water Splitting

The development of new and inexpensive semiconductor electrodes that possess suitable bandgap energies and band positions for solar water splitting is of great interest in the field of solar fuel production. In this study, n-type Cu 11 V 6 O 26 that has a bandgap energy of 1.9 eV was produced as a pure, high quality photoanode and its properties and stability for photoelectrochemical water splitting were systematically investigated in pH 9.2 and pH 13 solutions. As Cu 11 V 6 O 26 photoanodes appeared to suffer from poor charge transport properties, Mo and W-doping into the V site were also examined, which considerably improved the photocurrent generation of Cu 11 V 6 O 26 . Furthermore, the bandgap energy, band edge positions, flatband potential, photocurrent generation, and photostability of pristine and doped Cu 11 V 6 O 26 electrodes are discussed in comparison to elucidate the effect of Mo- and W-doping and to evaluate the promise and limitations of Cu 11 V 6 O 26 as a photoanode for use in a water splitting photoelectrochemical cell.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Integrating computation and experiment to investigate photoelectrodes for solar water splitting at the microscopic scale.

CONSPECTUS: Photoelectrochemical water-splitting is a promising and sustainable way to store the energy of the sun in chemical bonds and use it to produce hydrogen gas, a clean fuel. The key components in photoelectrochemical cells (PECs) are photoelectrodes, including a photocathode that reduces water to hydrogen gas and a photoanode that oxidizes water to oxygen gas. Materials used in photoelectrodes for PECs must effectively absorb sunlight, yield photogenerated carriers, and exhibit electronic properties that enable the efficient shuttling of carriers to the surface to participate in relevant water-splitting reactions. Discovering and understanding the key characteristics of optimal photoelectrode materials is paramount to the realization of PEC technologies. Oxide-based photoelectrodes can satisfy many of these materials requirements, including stability in aqueous environments, band edges with reasonable alignment with the redox potentials for water splitting, and ease of synthesis. However, oxide photoelectrodes generally suffer from poor charge transport properties and considerable bulk electron-hole separation, and they have relatively large band gaps. Numerous strategies have been proposed to improve these aspects and understand how these improvements are reflected in the photoelectrochemical performance. Unfortunately, the structural and compositional complexity of multinary oxides accompanied by the inherent complexity of photoelectrochemical processes makes it challenging to understand the individual effects of composition, structure, and defects in the bulk and on the surface on a material's photoelectrochemical properties. The integration of experiment and theory has great potential to increase our atomic-level understanding of structure-composition-property relationships in oxide photoelectrodes. In this Account, we describe how integrating experiment and theory is beneficial for achieving scientific insights at the microscopic scale. We highlight studies focused on understanding the role of (i) bulk composition via solid-state solutions, intercalation, and comparison with isoelectronic compounds, (ii) dopants for both the anion and cation and their interactions with oxygen vacancies, and (iii) surface/interface structure in the photocurrent generation and photoelectrochemical performance in oxide photoelectrodes. In each instance, we outline strategies and considerations for integrating experiment and theory and describe how this integration led to valuable insights and new directions in uncovering structure-composition-property relationships. Our aim is to demonstrate the unique value of combining experiment and theory in studying photoelectrodes and to encourage the continued effort to bring experiment and theory in closer step with each other.

Wang, Wennie↗
DOE OSTI2025

Pulsed laser deposition of delafossite oxide thin films on YSZ (001) substrates as solar water splitting photocathodes

Development of solar energy converters with earth-abundant and environmentally friendly materials is one of the key routes explored towards a sustainable future. In this work, crystalline delafossite-phase CuAlO 2 and CuFeO 2 thin film solar water splitting photocathodes were fabricated using pulsed laser deposition. It was found that the desired delafossite phase was formed only after high temperature annealing in an oxygen-free atmosphere. Further, the homogeneous delafossite bulk structure of the films was determined by correlating simulation results from first-principles calculations with synchrotron-based X-ray absorption near edge structure (XANES) spectroscopy. Both CuAlO 2 and CuFeO 2 photocathodes are active for solar water splitting, with the latter more efficient due to its narrower band gap and improved light absorption.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Hematite‐Based Solar Water Splitting in Acidic Solutions: Functionalization by Mono‐ and Multilayers of Iridium Oxygen‐Evolution Catalysts

Abstract Solar water splitting in acidic solutions has important technological implications, but has not been demonstrated to date in a dual absorber photoelectrochemical cell. The lack of functionally stable water‐oxidation catalysts (WOCs) in acids is a key reason for this slow development. The only WOCs that are stable at low pH are Ir‐based systems, which are typically too expensive to be implemented broadly. It is now shown that this deficiency may be corrected by applying an ultra‐thin monolayer of a molecular Ir WOC to hematite for solar water splitting in acidic solutions. The turn‐on voltage is observed to shift cathodically by 250 mV upon the application of a monolayer of the molecular Ir WOC. When the molecular WOC is replaced by a heterogeneous multilayer derivative, stable solar water splitting for over 5 h is achieved with near‐unity Faradaic efficiency.

Li, Wei↗