All-inorganic cesium lead bromide (CsPbBr3) perovskite is attracting growing interest as functional materials in photovoltaics and other optoelectronic devices due to its superb stability. However, the fabrication of high-quality CsPbBr3 films still remains a big challenge by solution-process because of the low solubility of the cesium precursor in common solvents. Herein, we report a facile solution-processed approach to prepare high-quality CsPbBr3 perovskite films via a two-step spin-coating method, in which the CsBr methanol/H2O mixed solvent solution is spin-coated onto the lead bromide films, followed by an isopropanol-assisted post-treatment to regulate the crystallization process and to control the film morphology. In this fashion, dense and uniform CsPbBr3 films are obtained consisting of large crystalline domains with sizes up to microns and low defect density. The effectiveness of the resulting CsPbBr3 films is further examined in perovskite solar cells (PSCs) with a simplified planar architecture of fluorine‒doped tin oxide/compact TiO2/CsPbBr3/carbon, which deliver a maximum power conversion efficiency of 8.11% together with excellent thermal and humidity stability. The present work offers a simple and effective strategy in fabrication of high-quality CsPbBr3 films for efficient and stable PSCs as well as other optoelectronic devices.

A novel flame-assisted deposition (FAD) method was used to generate and immobilize cobalt oxide (CoOx) on the surface of fluorine-doped tin oxide (FTO) and TiO2 modified hematite (TiO2/Fe2O3) for electrochemical and photoelectrochemical (PEC) water oxidation, respectively, with significant performance.

Materials design of efficient electrochemical micro-reactors is challenging, although hierarchically structured, self-standing electrodes with catalyst arrays offer promise. Herein, catalyst function in compact micro-reactor electrodes is designed by nanostructural tailoring of carbonized wood for efficient water splitting. Specifically, NiFe rod tipped, N-doped graphitic carbon nanocapsule arrays are self-assembled in hierarchical wood, and the benefit of this unique presentation and its promotive effect on accessibility of the catalyst surfaces is apparent. This report also comprises the first wood based micro-reactor electrodes for electrocatalytic water oxidation demonstrating excellent performance. The overpotential for oxygen evolution reaction was as low as 180 mV for 10 mA cm−2 current density and TOFredox was high at a level of 5.8 s−1 (at 370 mV overpotential). This hierarchical electrode can also work as bifunctional catalyst (both as anodic and as cathodic electrode) for total water splitting with a cell potential of 1.49 V for 10 mA cm−2 in alkaline solution, suggestive of their potential also in other electrochemical applications.

Single crystals of Spiro(TFSI)2 were grown, the optical and electronic properties were characterized and compared with neutral Spiro-OMeTAD. Density-functional theory was used to get insights into binding and band structure properties. The flat valence bands indicate a rather limited orbital overlap in Spiro(TFSI)2.

In the past few years, the photovoltaic community has witnessed a fast growth of inorganic-organic hybrid perovskite solar cells (PSCs) due to their exceptional power conversion efficiencies with a certified record value exceeding 25%, which rivals the established commercial solar cell technologies. In the stateof-the-art PSCs, a hole-transporting layer (HTL) typically consisting of an active hole-transporting material (HTM) and some additives or dopants, takes the responsibility of transporting the photo-generated holes from the perovskite to the selective contact electrode, and is a key component for achieving high-performance and stable PSCs. In this review article, recent advances in the development of transition metal complexes in HTLs for PSCs including HTMs and p-type dopants are presented.

The electron-injection energy losses of dye-sensitized solar cells (DSSCs) are among the fundamental problems hindering their successful breakthrough application. Two triazatruxene (TAT)-based sensitizers, with one containing a flexible Z-type double bond and another a rigid single bond, coded as ZL001 and ZL003, respectively, have been synthesized and applied in DSSCs to probe the energy losses in the process of electron injection. Using time-resolved laser spectroscopic techniques in the kinetic study, ZL003 with the rigid single bond promotes much faster electron injection into the conductive band of TiO2 especially in the locally excited state (hot injection), which leads to higher electron density in TiO2 and a higher V-oc. The devices based on ZL003 exhibited a champion power conversion efficiency (PCE) of 13.6% with V-oc = 956 mV, J(sc) = 20.73 mA cm(-2), and FF = 68.5%, which are among the highest recorded results to date on single dye-sensitized DSSCs. An independent certified PCE of 12.4% has been obtained for devices based on ZL003.

First-row transition metal-based catalysts have been developed for the oxygen evolution reaction (OER) during the past years, however, such catalysts typically operate at overpotentials (eta) significantly above thermodynamic requirements. Here, we report an iron/ nickel terephthalate coordination polymer on nickel form (NiFeCP/NF) as catalyst for OER, in which both coordinated and uncoordinated carboxylates were maintained after electrolysis. NiFeCP/NF exhibits outstanding electro-catalytic OER activity with a low overpotential of 188 mV at 10 mA cm(-2) in 1.0 KOH, with a small Tafel slope and excellent stability. The pH-independent OER activity of NiFeCP/NF on the reversible hydrogen electrode scale suggests that a concerted proton-coupled electron transfer (c-PET) process is the rate-determining step (RDS) during water oxidation. Deuterium kinetic isotope effects, proton inventory studies and atom-proton-transfer measurements indicate that the uncoordinated carboxylates are serving as the proton transfer relays, with a similar function as amino acid residues in photosystem II (PSII), accelerating the proton-transfer rate.

In this series of articles, the board members of ChemSusChem discuss recent research articles that they consider of exceptional quality and importance for sustainability. This entry features Prof. L. Sun, who proposes a special mechanism for O-O bond formation in photosystem II with involvement of an Mn-VII-oxo species induced by charge- and structural rearrangements. In this viewpoint, Proton transfer is involved in changes of the first coordination spheres around the Mn-VII-oxo site on the dangling Mn4 with de- and re-coordination of carboxylates (Glu333 and Asp170).

Molecular catalysis plays an essential role in both natural and artificial photosynthesis (AP). However, the field of molecular catalysis for AP has gradually declined in recent years because of doubt about the long-term stability of molecular-catalyst-based devices. This review summarizes the development history of molecular-catalyst-based AP, including the fundamentals of AP, molecular catalysts for water oxidation, proton reduction and CO2 reduction, and molecular-catalyst-based AP devices, and it provides an analysis of the advantages, challenges, and stability of molecular catalysts. With this review, we aim to highlight the following points: (i) an investigation on molecular catalysis is one of the most promising ways to obtain atom-efficient catalysts with outstanding intrinsic activities; (ii) effective heterogenization of molecular catalysts is currently the primary challenge for the application of molecular catalysis in AP devices; (iii) development of molecular catalysts is a promising way to solve the problems of catalysis involved in practical solar fuel production. In molecular-catalysis-based AP, much has been attained, but more challenges remain with regard to long-term stability and heterogenization techniques.

A facile preparation of bio-inspired and morphology controllable catalytic electrode FeS@MoS2/CFC, featuring a carbon fiber cloth (CFC) covered with FeS dotted MoS2 nanosheets, has been established. Synergy between the CFC as a self-standing conductive substrate and the FeS nanoparticle dotted MoS2 nanosheets with abundant active sites makes the noble-metal-free catalytic electrode FeS@MoS2/CFC highly efficient in nitrogen reduction reaction (NRR), with an ammonia production rate of 8.45 mu g h(-1) cm(-2) and excellent long-term stability at -0.5 V in pH neutral electrolyte. Further electrolysis in acidic and alkaline electrolytes revealed the overall NRR catalytic activity of this electrode over a wide pH range.