Although sunlight-driven water splitting is a promising route to sustainable hydrogen fuel production, widespread implementation hampered by the expense of necessary photovoltaic and photoelectrochemical apparatus. Here, we describe highly efficient low-cost water-splitting cell combining state-of-the-art solution-processed perovskite tandem solar bifunctional Earth-abundant catalyst. The catalyst electrode, NiFe layered double hydroxide, exhibits high activity toward both oxygen evolution...

Revved-up rust! Light-induced water splitting over iron oxide (hematite) has been achieved by using a particle-assisted deposition technique and IrO2-based surface catalysis. Photocurrents in excess of 3 mA cm−2 were obtained at +1.23 V versus the reversible hydrogen electrode under AM 1.5 G 100 mW simulated sunlight. These photocurrents are unmatched any other oxide-based photoanode. FTO=fluorine-doped tin oxide. Detailed facts importance to specialist readers published as "Supporting...

The kinetic competition between electron-hole recombination and water oxidation is a key consideration for the development of efficient photoanodes solar driven splitting. In this study, we employed three complementary techniques, transient absorption spectroscopy (TAS), photocurrent (TPC), electrochemical impedance (EIS), to address issue one most widely studied photoanode systems: nanostructured hematite thin films. For first time, show quantitative agreement all techniques. particular,...

The utilisation of Cu2O photocathodes for photoelectrochemical water splitting requires their stabilisation due to photocorrosion in aqueous electrolytes. Ultrathin films wide band gap semiconducting oxides deposited by atomic layer deposition (ALD) on top cuprous oxide can perform the dual function both facilitating charge extraction (through creation a p–n junction) and protecting absorber material from electrolyte, thereby suppressing corrosion favor hydrogen generation. factors that...

Recent research on photoanodes for photoelectrochemical water splitting has introduced the concept of under‐ and overlayers activation ultrathin hematite films. Their effects photocatalytic behavior were clearly shown; however, mechanism is thus far not fully understood. Herein, contribution each layer analyzed by means electrochemical impedance spectroscopy, with aim obtaining a general understanding surface interface modifications their influence photoanode performance. This study shows...

Water oxidation is a key chemical reaction, central to both biological photosynthesis and artificial solar fuel synthesis strategies. Despite recent progress on the structure of natural catalytic site, inorganic catalyst function, determining mechanistic details this multiredox reaction remains significant challenge. We report herein rate law analysis order water as function surface hole density hematite photoanode employing photoinduced absorption spectroscopy. Our study reveals transition...

Photocathodes based on cuprous oxide (Cu 2 O) are promising materials for large scale and widespread solar fuel generation due to the abundance of copper, suitable bandgap, favorable band alignments reducing water carbon dioxide. A protective overlayer is required stabilize Cu O in aqueous media under illumination, interface between this catalyst nanoparticles was previously identified as a key source instability. Here, properties titanium dioxide composite photocathodes further...

Abstract Photo‐electrochemical (PEC) solar energy conversion offers the promise of low‐cost renewable fuel generation from abundant sunlight and water. In this Review, recent developments in photo‐electrochemical water splitting are discussed with respect to promise. State‐of‐the‐art device performance is put context current understanding necessary requirements for cost‐effective hydrogen (in terms solar‐to‐hydrogen efficiency system durability, particular). Several important studies at...

Sunlight-driven water splitting to produce hydrogen fuel is an attractive method for renewable energy conversion. Tandem photoelectrochemical devices utilize two photoabsorbers harvest the sunlight and drive reaction. The absorption of by electrocatalysts a severe problem tandem where light needs be transmitted through larger bandgap component illuminate smaller component. Herein, we describe novel deposition optically transparent amorphous iron nickel oxide oxygen evolution electrocatalyst....

Transient absorption spectroscopy on subpicosecond to second time scales is used investigate photogenerated charge carrier recombination in Si-doped nanostructured hematite (α-Fe2O3) photoanodes as a function of applied bias. For unbiased hematite, this exhibits 50% decay ~6 ps, ~10(3) times faster than that TiO2 under comparable conditions. Anodic bias significantly retards dynamics, and causes the appearance electron trapping ps-μs scales. These ultrafast their retardation by bias,...

Through examination of the optoelectronic and photoelectrochemical properties BiVO4 Cu2O photoelectrodes, we evaluate feasibility a BiVO4/Cu2O photoanode/photocathode tandem cell for overall unassisted solar water splitting. Using state-of-the-art photoelectrodes identify current-matching conditions by altering photoanode active layer thickness. By further employing oxidation reduction catalysts (Co-Pi RuOx, respectively) together with an operating point analysis, show that photocurrent...

Abstract The splitting of water into hydrogen and oxygen molecules using sunlight is an attractive method for solar energy storage. Until now, photoelectrochemical evolution mostly studied in acidic solutions, which the more facile than alkaline solutions. Herein, we report production are favorable solutions complementary half‐reaction. We show first time that amorphous molybdenum sulfide a highly active catalyst basic medium. Ni–Mo then deposited on surface‐protected cuprous oxide...

A new strategy of using forward gradient self-doping to improve the charge separation efficiency in metal oxide photoelectrodes is proposed. Gradient self-doped CuBi2O4 photocathodes are prepared with and reverse gradients copper vacancies a two-step, diffusion-assisted spray pyrolysis process. Decreasing Cu/Bi ratio introduces Cu that increase carrier (hole) concentration lowers Fermi level, as evidenced by shift flat band toward more positive potentials. Thus, leads an internal electric...

A new protein modification reaction has been developed based on a palladium-catalyzed allylic alkylation of tyrosine residues. This technique employs electrophilic π-allyl intermediates derived from acetate and carbamate precursors can be used to modify proteins in aqueous solution at room temperature. To facilitate the detection modified using SDS−PAGE analysis, fluorescent allyl was synthesized coupled chymotrypsinogen bacteriophage MS2. The selectivity confirmed through trypsin digest...

The amount of solar power striking the earth’s surface is vastly superior to humanity’s present day energy needs and can easily meet our increasing demands as world’s population grows. In order make cost competitive with fossil fuels, conversion devices must be made cheaply possible, which necessitates use abundant raw materials low intensity fabrication processes. Cuprous oxide (Cu2O) a promising material capacity for cost, large-scale due nature copper oxygen, suitable bandgap absorption...

Photoelectrochemical water splitting represents an attractive method of capturing and storing the immense energy sunlight in form hydrogen, a clean chemical fuel. Given large energetic demand electrolysis, defined spectrum photons available from incident sunlight, two absorber tandem device is required to achieve high efficiencies. The absorbers should be different complementary bandgaps, connected series necessary voltage, arranged optical stack configuration maximize utilization sunlight....

Cupric oxide (CuO) is a promising material for large-scale, economic solar energy conversion due to the abundance of copper, suitable band gap, and ease fabrication. For application as photocathode water splitting, main challenge prevention inherent photocorrosion in aqueous media. Photoelectrochemical measurements bare CuO thin films prepared by oxidation electroplated Cu indicated that vast majority photocurrent 1 M phosphate buffer solution (pH 7) comes from into metallic Cu, with...

A TiO₂-protected Cu₂O photocathode was paired with a molecular catalyst to drive the efficient and selective reduction of CO₂ CO.

Cu2ZnSnS4 (CZTS) is a promising p-type semiconductor that has not yet been extensively investigated for solar fuel production via water splitting. Here, we optimize and compare two different electrodeposition routes (simultaneous sequential) preparing CZTS electrodes. More consistent results are observed with the simultaneous route. In addition, effect of etching presence CdS buffer layer on photocurrent investigated. Finally, demonstrate first time stabilization these electrodes using...

Given the intermittent nature of solar radiation, large-scale use energy requires an efficient storage solution. So far, only practical way to store such large amounts is in form a chemical carrier, i.e., fuel. Photoelectrochemical (PEC) cells offer ability convert directly into hydrogen. Cuprous oxide (Cu2O) being investigated for photoelectrochemical water splitting since it has band gap 2.0 eV with favorable positions cleavage; abundant and environmentally friendly. A major challenge Cu2O...

Efficient sunlight‐driven water splitting devices can be achieved by pairing two absorbers of different optimized bandgaps in an optical tandem design. With tunable absorption ranges and cell voltages, organic–inorganic metal halide perovskite solar cells provide new opportunities for tailoring top such devices. In this work, semitransparent are developed use as the with a smaller bandgap photocathode to enable panchromatic harvesting spectrum. A CuIn x Ga 1‐ Se 2 multilayer is designed,...

Energy band alignments at heterointerfaces play a crucial role in defining the functionality of semiconductor devices, yet search for material combinations with suitable remains challenge numerous applications. In this work, we demonstrate how changes deposition conditions can dramatically influence functional properties an interface, even within same system. The energy alignment heterointerface between Cu2O and ZnO was studied using photoelectron spectroscopy stepwise onto vice versa. A...

Though Cu2O has demonstrated high performance as a photocathode for solar water splitting, its band gap is too large efficient use the bottom cell in tandem configurations. Accordingly, copper chalcopyrites have recently attracted much attention splitting due to their smaller and tunable gaps. However, fabrication mainly based on vacuum evaporation, which an expensive energy consuming process. Here, we developed novel low-cost solution method, CuInS2 was chosen model material compared...