A solar-to-fuel conversion efficiency of 22% was achieved by using concentrated solar power to run a matched electrolyser based on Earth-abundant materials.

Light-driven conversion of CO2 to chemicals provides a sustainable alternative fossil fuels, but homogeneous systems are typically limited by cross reactivity between different redox half reactions and inefficient charge separation. Herein, we present the bioinspired development amphiphilic photosensitizer catalyst pairs that self-assemble in lipid membranes overcome some these limitations enable photocatalytic reduction liposomes using precious metal-free catalysts. Using sodium ascorbate...

The sunlight-driven reduction of CO2 into fuels and platform chemicals is a promising approach to enable circular economy. However, established optimization approaches are poorly suited multivariable multimetric photocatalytic systems because they aim optimize one performance metric while sacrificing the others thereby limit overall system performance. Herein, we address this challenge by defining for holistic that takes multiple figures merit account, employ machine learning algorithm...

Manganese oxide (MnOx ) electrocatalysts are examined herein by in situ soft X-ray absorption spectroscopy (XAS) and resonant inelastic scattering (RIXS) during the oxidation of water buffered borate (pH 9.2) at potentials from 0.75 to 2.25 V vs. reversible hydrogen electrode. Correlation L-edge XAS data with previous mechanistic studies indicates MnIV is highest state involved catalytic mechanism. MnOx transformed into birnessite 1.45 does not undergo further structural phase changes. At...

A novel architecture for quasi-interdigitated electrodes (QIDEs) allows the fabrication of back-contacted perovskite solar cells.

Detection and quantification of redox transformations involved in water oxidation electrocatalysis is often not possible using conventional techniques. Herein, use large amplitude Fourier transformed ac voltammetry comprehensive analysis the higher harmonics has enabled us to access processes responsible for catalysis. An examination voltammetric data borate buffered solutions (pH 9.2) at electrodes functionalized with systematically varied low loadings cobalt (CoOx), manganese (MnOx),...

Supramolecular surfactants provide a versatile platform to construct systems for solar fuel synthesis, example via the self‐assembly of amphiphilic photosensitizers and catalysts into diverse supramolecular structures. However, utilization in production has predominantly focused on yielding gaseous products, such as molecular hydrogen (H2), carbon monoxide (CO), methane (CH4) with turnover number (TON) synthetic typically range hundreds thousands. Inspired by biological lipid–protein...

Supramolecular surfactants provide a versatile platform to construct systems for solar fuel synthesis, example via the self‐assembly of amphiphilic photosensitizers and catalysts into diverse supramolecular structures. However, utilization in production has predominantly focused on yielding gaseous products, such as molecular hydrogen (H2), carbon monoxide (CO), methane (CH4) with turnover number (TON) synthetic typically range hundreds thousands. Inspired by biological lipid–protein...

Soft X-ray absorption and resonant inelastic scattering at the Mn L-edge are established as tools for gaining electronic structural insights into water oxidation catalysis. The MnOx catalyst with lowest d–d transitions, strongest charge transfer a higher proportion of Mn3+ over Mn2+/4+ produces itinerant electrons that contribute to catalytic activity.

Photocatalytic oxidation of organic compounds on semiconductors provides a mild approach for synthesis and solar energy utilization. Herein, we identify the key points photocatalytic over Pt-loaded Rh-doped strontium titanate allowing conversion alcohols efficiently selectively to aldehydes ketones under anaerobic conditions visible light with an apparent quantum efficiency pure benzyl alcohol at 420 nm ≤49.5%. Mechanistic investigations suggest that thermodynamically controlled valence band...

Abstract The instability and expense of anodes for water electrolyzers with acidic electrolytes can be overcome through the implementation a cobalt‐iron‐lead oxide electrocatalyst, [Co–Fe–Pb]O x , that is self‐healing in presence dissolved metal precursors. However, latter requirement pernicious membrane especially cathode half‐reaction since Pb 2+ Fe 3+ precursors poison state‐of‐the‐art platinum H 2 evolving catalyst. To address this, we demonstrate invariably stable operation solutions...

Abstract Manganese oxide (MnO x ) electrocatalysts are examined herein by in situ soft X‐ray absorption spectroscopy (XAS) and resonant inelastic scattering (RIXS) during the oxidation of water buffered borate (pH 9.2) at potentials from 0.75 to 2.25 V vs. reversible hydrogen electrode. Correlation L‐edge XAS data with previous mechanistic studies indicates Mn IV is highest state involved catalytic mechanism. MnO transformed into birnessite 1.45 does not undergo further structural phase...

In situ experiments combining X-ray absorption spectroscopy (XAS) and electrochemistry have now become an indispensable tool for understanding the mechanisms of operation, structure, modes degradation electrocatalysts under operational conditions. Herein, design a gas- liquid-tight spectroelectrochemical cell (SEC) experimental protocol simultaneous collection high-quality XAS electrochemical data are introduced. The effects working electrode, loading active material, damage demonstrated...

Fukuyama reduction of thioesters has been achieved using a polymer-supported Pd[0] catalyst (Pd/XAD-4), and continuous flow conditions. The generality this reaction is good with range aldehydes prepared in excellent yields. In addition, an integrated multistep thioesterfication/Fukuyama developed that allows acyl chlorides to be directly converted the corresponding aldehydes. Integral process use amine isocyanate reagents achieve thioesterification scavenge unreacted thiol. catch-and-release...

NaNbO3 enriched with oxygen vacancies by Ni doping was successfully synthesized via a polymerized complex method and applied as photocatalyst in the oxidation of cinnamyl alcohol (CA) to cinnamaldehyde air. Reaction rates high 45 μmol h–1 were achieved under visible light apparent quantum efficiency 67.2% excellent chemoselectivity larger than 99%. UV–vis, electron paramagnetic resonance, attenuated total reflectance infrared spectroscopy results indicate that CA molecules preferentially...

Abstract Amongst the most promising materials designed to catalyse water oxidation from earth‐abundant are metal oxides. Despite success of these materials, understanding relationship structure function has been very challenging. It noted that many oxide water‐oxidation catalysts best in a proton‐accepting electrolyte, such as borate or phosphate buffer. However, same electrolytes known significantly affect structures by imparting level “disorder” “molecular nature” materials. The well‐known...

Abstract Efficient catalysis of water oxidation represents one the major challenges en route to efficient sunlight‐driven splitting. Cobalt oxides (CoO x ) have been widely investigated as catalysts, although incorporation these materials into photoelectrochemical devices has hindered by a lack transparency. Herein, electrosynthesis transparent CoO catalyst films is described utilizing cobalt(II) aminopolycarboxylate complexes precursors oxide. These allow control over deposition rate and...

Dye-sensitized photocathodes have been observed on several occasions to sustain light-driven H2 generation without intentionally introduced catalysts. Herein, plausible mechanisms addressing this phenomenon are probed by a combination of long-term photoelectrochemical measurements with concurrent gas chromatography, transient absorption spectroscopy, and inductively coupled mass spectrometry using perylenemonoimide–sexithiophene–triphenylamine (PMI-6T-TPA) sensitized NiO electrode. The...

We focus on a novel concept of photosynthetic soft membranes, possibly able to allow the conversion solar energy and carbon dioxide (CO[Formula: see text]) into green fuels. The considered membranes rely self-assembled functional molecules in form soap films. elaborate multi-scale multi-physics model describe relevant phenomena, investigating expected performance single membrane. First, we present macroscale continuum model, which accounts for transport gaseous ionic species within film,...

The term amorphous metal oxide is becoming widely used in the catalysis community. generally when there are no apparent peaks an X-ray diffraction pattern. However, absence of such features can mean that material either truly or it better described as nanocrystalline. By coprecipitating a sodium birnessite-like phase with and without phosphate (1.5 %), we able to engineer two very similar but distinct materials – one nanocrystalline other amorphous. closely related phases were characterized...

The possibility of efficient water electrooxidation sustained by continuous (re)generation catalysts derived from the oxidative electrodeposition transition-metal contaminants is examined herein for three natural samples Australia and China. metal composition solutions has been determined inductively coupled plasma optical emission spectrometry, a range strategies to produce water-splitting means in situ have applied. performance resulting electrocatalysts below state-of-the-art level owing...

Abstract Diblock copolymers have been used in sol–gel synthesis to successfully tailor the nanoscale morphology of thin ZnO films. As fabrication several‐micron‐thick mesoporous films such as those required dye‐sensitized solar cells (DSSCs) was difficult with this approach, we exploited benefits diblock‐copolymer‐directed that made it compatible screen printing. The simple conversion diblock copolymer precursor sol a screen‐printing paste not possible resulted poor film properties. To...