Featured
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Article
| Open AccessPotential window alignment regulating ion transfer in faradaic junctions for efficient photoelectrocatalysis
Band alignment theory has been widely used to design semiconductor heterojunctions for photo(electro)catalysis, but it cannot describe coupled electron and ion transfer process. Here, the authors propose potential window alignment theory to remarkably improve the performance of heterojunctions.
- Hongzheng Dong
- , Xiangyu Pan
- & Zhigang Zou
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Article
| Open AccessImproving the photovoltage of Cu2O photocathodes with dual buffer layers
Increasing the photovoltage of the Cu2O photocathode plays an important role in photocatalytic water splitting. Here the authors construct a dual buffer layer to optimize the band alignment between the n-type layer and the protective layer, which improves the onset potential of the Cu2O photocathode by 0.16 V.
- Jinshui Cheng
- , Linxiao Wu
- & Jingshan Luo
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Article
| Open AccessSolar-driven upgrading of biomass by coupled hydrogenation using in situ (photo)electrochemically generated H2
Green chemical transformations driven by renewable energies are imperative to realize a sustainable energy society. We demonstrate a coupled approach to hydrogenate biomass feedstock into valuable chemicals with high stability using hydrogen generated in situ in a (photo)electrochemical reactor.
- Keisuke Obata
- , Michael Schwarze
- & Fatwa F. Abdi
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Article
| Open AccessSolution-processable polymers of intrinsic microporosity for gas-phase carbon dioxide photoreduction
This works presents a series of solution processable, conjugated polymers of intrinsic microporosity, which are used as photocatalysts for carbon dioxide reduction to carbon monoxide in the presence of hydrogen.
- Floriana Moruzzi
- , Weimin Zhang
- & Iain McCulloch
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Article
| Open AccessCu-based high-entropy two-dimensional oxide as stable and active photothermal catalyst
Synergistically enhancing catalytic stability and activity of Cu-based nanocatalysts is an ongoing challenge. Here the authors report Cu-based high-entropy two-dimensional oxide as stable and active catalyst for photothermal CO2 hydrogenation under ambient sunlight irradiation.
- Yaguang Li
- , Xianhua Bai
- & Jinhua Ye
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Article
| Open AccessPhotothermal-enabled single-atom catalysts for high-efficiency hydrogen peroxide photosynthesis from natural seawater
Photoproduction of solar fuels and important chemicals is of significant interest. Here, the authors construct a cobalt single atom-based photothermal-photocatalytic heterostructure that realizes efficient hydrogen peroxide photosynthesis from earth-abundant seawater.
- Wei Wang
- , Qun Song
- & Ning Wang
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Article
| Open AccessRenewable formate from sunlight, biomass and carbon dioxide in a photoelectrochemical cell
The sustainable production of chemicals and fuels from waste carbon sources holds significant promise for reducing our dependence on fossil resources. Here, the authors demonstrate renewable formate production from biomass wastes and CO2 powered by solar energy.
- Yuyang Pan
- , Huiyan Zhang
- & Sheng Chu
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Article
| Open AccessDecoupling light absorption and carrier transport via heterogeneous doping in Ta3N5 thin film photoanode
While photoelectrochemical water splitting offers a promising means to obtain renewable H2, it is challenging to balance light absorption and carrier transport in semiconductor thin films. Here, authors combine surface doping and bulk gradient doping to decouple these factors to boost performances.
- Yequan Xiao
- , Zeyu Fan
- & Yanbo Li
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Article
| Open AccessLow-bias photoelectrochemical water splitting via mediating trap states and small polaron hopping
While photoelectrochemical water splitting produces fuel from solar energy, a large fraction of photoanode photoexcited charge carriers cannot be extracted efficiently at low bias voltages. Here, authors improve the charge transport in P-doped BiVO4 by mediating polaron hopping and trap states.
- Hao Wu
- , Lei Zhang
- & Yun Hau Ng
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Article
| Open AccessBias-free solar hydrogen production at 19.8 mA cm−2 using perovskite photocathode and lignocellulosic biomass
While light-driven water splitting offers a means to produce renewable H2 fuel, water oxidation limits performances and yields low-value products. Here, authors demonstrate a photoelectrochemical cell that converts lignocellulosic biomass into valuable products alongside H2.
- Yuri Choi
- , Rashmi Mehrotra
- & Jungki Ryu
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Article
| Open AccessA hygroscopic nano-membrane coating achieves efficient vapor-fed photocatalytic water splitting
Although light-driven water vapor splitting may avoid material stability challenges for renewable fuel production, material performances lag behind solution-based studies. Here, authors incorporate metal hydroxides layers into particulate photocatalysts to enhance water vapor splitting activities.
- Takuya Suguro
- , Fuminao Kishimoto
- & Kazuhiro Takanabe
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Article
| Open AccessUnassisted selective solar hydrogen peroxide production by an oxidised buckypaper-integrated perovskite photocathode
It is of high demand yet challenging to boost the efficiency of solar driven hydrogen peroxide synthesis. Herein, the authors intergrade perovskite-based photocathode and oxidised buckypaper for unassisted solar H2O2 production with a solar-to-chemical conversion efficiency of ~1.463 %.
- Rashmi Mehrotra
- , Dongrak Oh
- & Ji-Wook Jang
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Article
| Open AccessEfficient CO2 electroreduction on facet-selective copper films with high conversion rate
Regulation of Cu facets to promote electrocatalytic CO2 reduction is interesting and challenging. Here the authors describe a deposition-etch-bombardment synthetic approach to prepare Cu(100)-rich thin film electrodes for CO2 electroreduction with over 50% ethylene Faradaic efficiency at a total current of 12 A.
- Gong Zhang
- , Zhi-Jian Zhao
- & Jinlong Gong
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Article
| Open AccessVacancy-defect modulated pathway of photoreduction of CO2 on single atomically thin AgInP2S6 sheets into olefiant gas
CO2 conversion driven by light is a promising strategy to synchronously overcome global warming and energy-supply issues. Here the authors show that the sulfur defect engineering on a quaternary AgInP2S6 atomic layer can excitingly change the CO2 photoreduction reaction pathway to the generation of ethene.
- Wa Gao
- , Shi Li
- & Zhigang Zou
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Article
| Open AccessCharacterisation of oxygen defects and nitrogen impurities in TiO2 photocatalysts using variable-temperature X-ray powder diffraction
Nitrogen-doped TiO2 exhibits improved photocatalytic water-splitting activity partially due to enhanced oxygen vacancy formation. Here, authors demonstrate the temperature-dependent lattice distortion of oxygen vacancies, and identify the presence of a titanium oxynitride phase in high activity catalysts.
- Christopher Foo
- , Yiyang Li
- & Shik Chi Edman Tsang
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Article
| Open AccessBismuth atom tailoring of indium oxide surface frustrated Lewis pairs boosts heterogeneous CO2 photocatalytic hydrogenation
Surface frustrated Lewis pairs (SFLPs) provide a unique class of active sites that enable efficient gas-phase CO2 photocatalysis. How to tailor the reactivity of the SFLPs represents a major challenge, which the authors address here by single-site Bi3+ ion substitution of the SFLPs.
- Tingjiang Yan
- , Na Li
- & Geoffrey A. Ozin
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Article
| Open AccessHigh-performance and stable photoelectrochemical water splitting cell with organic-photoactive-layer-based photoanode
While organic semiconductors may be useful in photoelectrochemical water-splitting materials, they show low stability in water. Here, the authors report high-performance and stable organic-semiconductor-based photoanodes passivated using nickel foils, GaIn eutectic, and layered double hydroxides.
- Je Min Yu
- , Jungho Lee
- & Ji-Wook Jang
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Article
| Open AccessDirect growth of uniform carbon nitride layers with extended optical absorption towards efficient water-splitting photoanodes
Photoelectrochemical cells (PEC) can convert sunlight and water directly to a hydrogen fuel. Here a robust metal-free carbon nitride-based layer is used as an efficient photoanode for water-splitting PEC.
- Jiani Qin
- , Jesús Barrio
- & Menny Shalom
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Article
| Open AccessSpontaneous solar water splitting with decoupling of light absorption and electrocatalysis using silicon back-buried junction
The simultaneous management of optical, electrical, and catalytic properties is challenging for photoelectrochemical devices. Here, authors design Si back-buried junction photoelectrodes that can be series connected for unassisted water-splitting with a high solar-to-hydrogen efficiency of 15.62%.
- Hui-Chun Fu
- , Purushothaman Varadhan
- & Jr-Hau He
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Article
| Open AccessDirect and indirect Z-scheme heterostructure-coupled photosystem enabling cooperation of CO2 reduction and H2O oxidation
The stoichiometric photoreaction of CO2 with H2O is one of the big challenges in photocatalysis. An artificial photosynthetic system based on a direct and indirect Z-scheme heterostructure is synthesised, enabling simultaneous CO2 reduction to HCOOH and H2O oxidation to O2.
- Ying Wang
- , Xiaotong Shang
- & Can Li
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Article
| Open AccessBenchmark performance of low-cost Sb2Se3 photocathodes for unassisted solar overall water splitting
While photoelectrochemical water splitting offers an integrated means to convert sunlight to a renewable fuel, cost-effective light-absorbers are rare. Here, authors report Sb2Se3 photocathodes for high-performance photoelectrochemical water splitting devices.
- Wooseok Yang
- , Jin Hyun Kim
- & Jooho Moon
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Article
| Open AccessCu2O photocathodes with band-tail states assisted hole transport for standalone solar water splitting
While solar-to-fuel conversion offers a promising technology to produce energy, device components can limit light absorption and reduce performances. Here, authors show copper thiocyanate to assist hole transport in photoelectrodes and enable a 4.55% solar-to-hydrogen efficiency in tandem devices.
- Linfeng Pan
- , Yuhang Liu
- & Anders Hagfeldt
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Article
| Open AccessAn efficient and stable photoelectrochemical system with 9% solar-to-hydrogen conversion efficiency via InGaP/GaAs double junction
Photoelectrochemical water-splitting devices with III-V semiconductors are efficient for solar-to-hydrogen conversion, but high costs and poor stability limit applications. Here, authors decouple light harvesting from electrolysis to enhance stability without compromising the efficiency.
- Purushothaman Varadhan
- , Hui-Chun Fu
- & Jr-Hau He
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Article
| Open AccessUnassisted solar lignin valorisation using a compartmented photo-electro-biochemical cell
The effective valorisation of lignin is crucial for realizing a sustainable biorefinery. Here, the authors report that a compartmented photo-electro-biochemical design enables unassisted, selective, and stable solar lignin valorisation without the need for any additional bias or chemicals.
- Myohwa Ko
- , Le Thanh Mai Pham
- & Ji-Wook Jang
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Article
| Open AccessCollective excitation of plasmon-coupled Au-nanochain boosts photocatalytic hydrogen evolution of semiconductor
Plasmonic effect offers a valuable opportunity to improve the efficiency of semiconductor, photocatalysts. Here, the authors show that the collective excitation of plasmonic metal, nanoparticles is more favorable for enhancing the utilization of plasmonic energy by, semiconductors.
- Guiyang Yu
- , Jun Qian
- & Gang Liu
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Article
| Open AccessPhotocatalytic water splitting by N-TiO2 on MgO (111) with exceptional quantum efficiencies at elevated temperatures
Chemical fuels, produced from light, afford an alternative to fossil fuel, but conversion materials suffer from low photon-to-fuel efficiencies. Here, authors incorporate gold/N-doped TiO2 on MgO surfaces and show enhanced photocatalytic water splitting performances at elevated temperatures.
- Yiyang Li
- , Yung-Kang Peng
- & Shik Chi Edman Tsang
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Article
| Open AccessA high-performance oxygen evolution catalyst in neutral-pH for sunlight-driven CO2 reduction
Solar-to-fuel conversion under mild conditions offers a renewable means to store energy. Here authors report a Brownmillerite oxide for neutral-pH oxygen evolution that, when integrated with an anodized silver cathode, enables a 13.9% energy-conversion efficiency for light-driven CO2 reduction
- Li Qin Zhou
- , Chen Ling
- & Hongfei Jia
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Article
| Open AccessIn situ observation of picosecond polaron self-localisation in α-Fe2O3 photoelectrochemical cells
The efficiency of Hematite (α-Fe2O3) photo-anodes is thought to be limited by ultrafast lattice distortions or polarons. Here, we use an optical-control method with photocurrent detection to track small polarons in real time and demonstrate that they impact photoelectrochemical cell activity
- Ernest Pastor
- , Ji-Sang Park
- & Artem A. Bakulin
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Article
| Open AccessTailoring the photoelectrochemistry of catalytic metal-insulator-semiconductor (MIS) photoanodes by a dissolution method
Designing synthetic systems to convert light into fuel is crucial in renewable energy development. Here, authors study electrodissolution in nickel thin films from metal-insulator-semiconductor junctions and find decreased homogeneity to improve junction properties and catalytic performances.
- G. Loget
- , C. Mériadec
- & S. Ababou-Girard
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Article
| Open AccessIsolated single atom cobalt in Bi3O4Br atomic layers to trigger efficient CO2 photoreduction
While the conversion of CO2 to high-value products provides a promising means to remove and utilize atmospheric carbon, few materials can do so without wasteful, sacrificial reagents. Here, authors prepare single-atom Co on Bi3O4Br nanosheets as CO2 reduction catalysts using water and light.
- Jun Di
- , Chao Chen
- & Zheng Liu
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Article
| Open AccessGraphite-protected CsPbBr3 perovskite photoanodes functionalised with water oxidation catalyst for oxygen evolution in water
While photoelectrochemical cells may offer access to solar fuels from a single integrated device, halide perovskite photoelectrodes are difficult to use due to their inherent moisture sensitivity. Here, the authors protect perovskite photoanodes with graphite sheets to boost their stability in water.
- Isabella Poli
- , Ulrich Hintermair
- & Petra J. Cameron
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Article
| Open AccessModulating the mechanism of electrocatalytic CO2 reduction by cobalt phthalocyanine through polymer coordination and encapsulation
Understanding the mechanism behind CO2 reduction catalysis is crucial in the development of high efficiency and activity catalysts. Here, authors employ kinetic isotope effects and proton inventory studies to assess catalyst mechanism and proton delivery in molecular CO2 electroreduction materials.
- Yingshuo Liu
- & Charles C. L. McCrory
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Article
| Open AccessEfficient photocatalytic hydrogen evolution with ligand engineered all-inorganic InP and InP/ZnS colloidal quantum dots
While quantum dots show high efficiency solar-to-fuel conversion for renewable energy, the frequently toxic elements employed present severe safety concerns. Here, authors demonstrate indium phosphide quantum dots as low-toxicity alternatives alongside efficient hydrogen evolution photocatalysis.
- Shan Yu
- , Xiang-Bing Fan
- & Greta R. Patzke
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Article
| Open AccessGallium nitride nanowire as a linker of molybdenum sulfides and silicon for photoelectrocatalytic water splitting
Sunlight-harvesting materials require the clean integration of light-absorbing and catalytic components to be efficient. Here, authors link silicon photoelectrodes and molybdenum sulfide catalysts with defect-free gallium nitride nanowire to improve photoelectrochemical hydrogen evolution.
- Baowen Zhou
- , Xianghua Kong
- & Zetian Mi
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Article
| Open AccessCrystalline TiO2 protective layer with graded oxygen defects for efficient and stable silicon-based photocathode
While silicon-based materials can convert sunlight directly to fuel and electricity, balancing their stability and efficiency constrains usage. Here, authors protect silicon photocathodes with crystalline titanium dioxide layers with graded oxygen defects to improve both durability and efficiency.
- Jianyun Zheng
- , Yanhong Lyu
- & Shuangyin Wang
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Article
| Open AccessHalf-metallic carbon nitride nanosheets with micro grid mode resonance structure for efficient photocatalytic hydrogen evolution
The “storage” of sunlight as a chemical fuel can provide renewable on-demand energy, although current earth-abundant materials usually show low activities. Here, authors construct a carbon nitride material whose half-metallicity and micro grid resonance structure boost light-driven H2 evolution.
- Gang Zhou
- , Yun Shan
- & Xinglong Wu
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Article
| Open AccessNanoscale imaging of charge carrier transport in water splitting photoanodes
The performance of energy materials is affected by structural defects, as well as physicochemical heterogeneity over different length scales. Here the authors map nanoscale correlations between morphological and functional heterogeneity, quantifying the trap states limiting electronic transport in bismuth vanadate thin films.
- Johanna Eichhorn
- , Christoph Kastl
- & Francesca M. Toma
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Article
| Open AccessEfficient solar hydrogen generation in microgravity environment
While renewable energy production is a terrestrial concern, far less attention is devoted to solar-to-fuel conversion for long-term space missions. Here, the authors explore photoelectrochemical hydrogen generation in microgravity and overcome microgravity’s limitations by electrode nanostructuring.
- Katharina Brinkert
- , Matthias H. Richter
- & Hans-Joachim Lewerenz
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Article
| Open AccessA photochemical diode artificial photosynthesis system for unassisted high efficiency overall pure water splitting
A major challenge facing solar-to-fuel technologies is the integration of light-absorbing and catalytic components into efficient water-splitting devices. Here, the authors construct a photochemical diode array to harvest visible light and split pure water at high solar-to-hydrogen efficiencies.
- Faqrul A. Chowdhury
- , Michel L. Trudeau
- & Zetian Mi
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Article
| Open AccessRETRACTED ARTICLE: Supported black phosphorus nanosheets as hydrogen-evolving photocatalyst achieving 5.4% energy conversion efficiency at 353 K
In order to displace fossil fuel technologies, it is crucial to develop efficient solar-to-fuel conversion materials using abundant, cheap elements. Here, the authors prepare few-layer black phosphorous with amorphous cobalt phosphide and produce hydrogen gas with light at high efficiencies.
- Bin Tian
- , Bining Tian
- & Yue Tian
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Article
| Open AccessSize-dependent activity and selectivity of carbon dioxide photocatalytic reduction over platinum nanoparticles
Light-driven carbon dioxide conversion into fuels provides a nature-inspired strategy to combat climate change, but how materials do so remains a challenge. Here, the authors prepare metal–semiconductor composites and find platinum-nanoparticle size controls fuel selectivity and activity.
- Chunyang Dong
- , Cheng Lian
- & Jinlong Zhang
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Article
| Open AccessCarbon-doped SnS2 nanostructure as a high-efficiency solar fuel catalyst under visible light
Photocatalytic reduction of CO2 to hydrocarbons is a promising route to both CO2 utilization and renewable fuel production. Here the authors identify that carbon-doped SnS2 possesses a high catalytic efficiency towards CO2 reduction owing to low photogenerated charge recombination rates.
- Indrajit Shown
- , Satyanarayana Samireddi
- & Kuei-Hsien Chen
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Article
| Open AccessTi3C2 MXene co-catalyst on metal sulfide photo-absorbers for enhanced visible-light photocatalytic hydrogen production
Solar hydrogen production through photocatalytic water splitting requires active and stable co-catalysts to replace platinum. Here, the authors use DFT to identify Ti3C2nanoparticles as potential co-catalysts, and assess their photocatalytic hydrogen production activity.
- Jingrun Ran
- , Guoping Gao
- & Shi-Zhang Qiao
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Article
| Open AccessEfficiency limits for photoelectrochemical water-splitting
Theoretical limiting efficiencies play a critical role in determining technological viability and expectations for device prototypes. Here, the authors present a unified framework for photoelectrochemical device performance through which previous limiting efficiencies can be understood and contextualized.
- Katherine T. Fountaine
- , Hans Joachim Lewerenz
- & Harry A. Atwater
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Article
| Open AccessUpscaling of integrated photoelectrochemical water-splitting devices to large areas
The realization of photoelectrochemical water splitting requires the upscale of associated technologies. Here, the authors report a scalable design based on independent photovoltaic and electrochemical silicon thin-film modules and assess its solar hydrogen generation performance.
- Bugra Turan
- , Jan-Philipp Becker
- & Stefan Haas