Adv Mater
August 2025
Photosystem II (PSII) is a vital photosynthetic enzyme with the potential for sustainable bioelectricity and fuel generation. However, interfacing PSII with intricate, small-scale electrodes for practical applications has been challenging. This study addresses this by creating protonated macroporous carbon nitride (MCN) as support and developing a scalable spray-freeze method to wire PSII with MCN.
View Article and Find Full Text PDFPhotoelectrochemical (PEC) devices offer a promising platform toward direct solar light harvesting and chemical storage through artificial photosynthesis. However, most prototypes employ wide bandgap semiconductors, moisture-sensitive inorganic light absorbers, or corrosive electrolytes. Here, the design and assembly of PEC devices based on an organic donor-acceptor bulk heterojunction (BHJ) using a carbon-based encapsulant are introduced, which demonstrate long-term H evolution and CO reduction in benign aqueous media.
View Article and Find Full Text PDFSolar fuels offer a promising approach to provide sustainable fuels by harnessing sunlight. Following a decade of advancement, CuO photocathodes are capable of delivering a performance comparable to that of photoelectrodes with established photovoltaic materials. However, considerable bulk charge carrier recombination that is poorly understood still limits further advances in performance.
View Article and Find Full Text PDFPhotoelectrochemical devices could play a crucial role toward fuel production in a circular economy. Yet, light absorption suffers losses from thermalization and the inability to use low-energy photons. Here, we demonstrate that photoelectrochemical reactors can utilize this waste heat by integrating thermoelectric modules, which provide additional voltage under concentrated light irradiation.
View Article and Find Full Text PDFArtificial photosynthesis can provide a solution to our current energy needs by converting small molecules such as water or carbon dioxide into useful fuels. This can be accomplished using photochemical diodes, which interface two complementary light absorbers with suitable electrocatalysts. Nanowire semiconductors provide unique advantages in terms of light absorption and catalytic activity, yet great control is required to integrate them for overall fuel production.
View Article and Find Full Text PDFThe sustainable synthesis of fuels and chemicals is key to attaining a carbon-neutral economy. This can be achieved by mimicking the light-harvesting and catalytic processes occurring in plants. Solar fuel production is commonly performed via established approaches, including photovoltaic-electrochemical (PV-EC), photoelectrochemical (PEC), and photocatalytic (PC) systems.
View Article and Find Full Text PDFPhotoelectrochemical (PEC) devices have been developed for direct solar fuel production but the limited stability of submerged light absorbers can hamper their commercial prospects. Here, we demonstrate photocathodes with an operational H evolution activity over weeks, by integrating a BiOI light absorber into a robust, oxide-based architecture with a graphite paste conductive encapsulant. In this case, the activity towards proton and CO reduction is mainly limited by catalyst degradation.
View Article and Find Full Text PDFThe fabrication of mixed-metal oxide films holds promise for the development of practical photoelectrochemical catalyst coatings but currently presents challenges in terms of homogeneity, cost, and scalability. We report a straightforward and versatile approach to produce catalytically active zirconium-based films for electrochemical and photoelectrochemical water oxidation. The mixed-metal oxide catalyst films are derived from novel single-source precursor oxide cage compounds containing Zr with first-row transition metals such as Co, Fe, and Cu.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2021
Semi-artificial photoelectrochemistry can combine state-of-the-art photovoltaic light-absorbers with enzymes evolved for selective fuel-forming reactions such as CO reduction, but the overall performance of such hybrid systems has been limited to date. Here, the electrolyte constituents were first tuned to establish an optimal local environment for a W-formate dehydrogenase to perform electrocatalysis. The CO reductase was then interfaced with a triple cation lead mixed-halide perovskite through a hierarchically structured porous TiO scaffold to produce an integrated photocathode achieving a photocurrent density of -5 mA cm at 0.
View Article and Find Full Text PDFThe development of thin-film thermoelectric applications in sensing and energy harvesting can benefit largely from suitable deposition methods for earth-abundant materials. In this study, p-type copper oxide thin films have been prepared on soda lime silicate glass by direct current (DC) magnetron sputtering at room temperature from a pure copper metallic target in an argon atmosphere, followed by subsequent annealing steps at 300 °C under various atmospheres, namely air (CuO:air), nitrogen (CuO:N) and oxygen (CuO:O). The resultant films have been studied to understand the influence of various annealing atmospheres on the structural, spectroscopic and thermoelectric properties.
View Article and Find Full Text PDFLead halide perovskite solar cells are notoriously moisture-sensitive, but recent encapsulation strategies have demonstrated their potential application as photoelectrodes in aqueous solution. However, perovskite photoelectrodes rely on precious metal co-catalysts, and their combination with biological materials remains elusive in integrated devices. Here, we interface [NiFeSe] hydrogenase from Hildenborough, a highly active enzyme for H generation, with a triple cation mixed halide perovskite.
View Article and Find Full Text PDFThe photoelectrochemical (PEC) production of syngas from water and CO represents an attractive technology towards a circular carbon economy. However, the high overpotential, low selectivity and cost of commonly employed catalysts pose challenges for this sustainable energy-conversion process. Here we demonstrate highly tunable PEC syngas production by integrating a cobalt porphyrin catalyst immobilized on carbon nanotubes with triple-cation mixed halide perovskite and BiVO photoabsorbers.
View Article and Find Full Text PDFACS Appl Mater Interfaces
July 2019
Metal halide perovskites are actively pursued as photoelectrodes to drive solar fuel synthesis. However, currently, these photocathodes suffer from limited stability in water, which hampers their practical application. Here, we report a high-performance solution-processable photocathode composed of cesium formamidinium methylammonium triple-cation lead halide perovskite protected by an Al-doped ZnO (AZO) layer combined with a Field's metal encapsulation.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
August 2018
Hydrogenases (H ases) are benchmark electrocatalysts for H production, both in biology and (photo)catalysis in vitro. We report the tailoring of a p-type Si photocathode for optimal loading and wiring of H ase through the introduction of a hierarchical inverse opal (IO) TiO interlayer. This proton-reducing Si|IO-TiO |H ase photocathode is capable of driving overall water splitting in combination with a photoanode.
View Article and Find Full Text PDFACS Appl Mater Interfaces
September 2017
Although the deposition of alternating layers from poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) and polyaniline (PANI) salts has recently provided a breakthrough in the field of conductive polymers, the cause for the conductivity improvement has remained unclear. In this work, we report a cooperative doping effect between alternating PANI base and PEDOT:PSS layers, resulting in electrical conductivities of 50-100 S cm and power factors of up to 3.0 ± 0.
View Article and Find Full Text PDFAs thermoelectric devices begin to make their way into commercial applications, the emphasis is put on decreasing the thermal conductivity. In this purely theoretical study, finite element analysis is used to determine the effect of a supporting material on the thermal conductivity of a thermoelectric module. The simulations illustrate the heat transfer along a sample, consisting from Cu, Cu2O and PbTe thermoelectric layers on a 1 mm thick Pyrex glass substrate.
View Article and Find Full Text PDFWe present a facile alternative to other well known strategies for synthesizing flexible thermoelectric materials. Instead of printing thin active layers on flexible substrates or doping conductive polymers, we produce thermoelectric pastes, using a mixture of graphite, copper(I) oxide and polychlorotrifluoroethene. The Seebeck coefficient of the investigated pastes varies between 10 and 600 μV K(-1), while the electrical conductivity spans over an even wider range of 10(-4) to 10(2) S m(-1).
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