Intermarrying MOF Glass and Lead Halide Perovskites for Artificial Photosynthesis.

The development of efficient artificial photosynthesis systems is crucial for sustainable chemical production, as they mimic natural processes to convert solar energy into chemical products, thereby addressing both energy and environmental challenges. The main bottlenecks in current research include fabricating highly selective, stable, and scalable catalysts, as well as effectively harnessing the full spectrum of light, particularly the low-energy, long-wavelength portion. Herein, we report a novel composite photocatalyst system based on lead halide perovskites embedded in functionalized MOF glass.

Organometallic Compound Stabilizes All-Inorganic Tin-Based Perovskite Nanocrystals Against Antisolvent Post-Treatment.

The isolation and purification of all-inorganic Sn-based perovskite nanocrystals (PNCs) remain troublesome, as common antisolvents accelerate the collapse of the optically active perovskite structure. Here, we mitigate such instabilities and endow strong resistance to antisolvent by incorporating the organometallic compound zinc diethyldithiocarbamate, Zn(DDTC), during the solution-based synthesis of all-inorganic CsSnI nanocrystals. Thiourea is shown to form through the thermal-driven conversion of Zn(DDTC) during synthesis, which binds to un-passivated Sn sites on the crystal surface and shields it from irreversible oxidation reactions.

Oxygen vacancy induced defect dipoles in BiVO for photoelectrocatalytic partial oxidation of methane.

A strong driving force for charge separation and transfer in semiconductors is essential for designing effective photoelectrodes for solar energy conversion. While defect engineering and polarization alignment can enhance this process, their potential interference within a photoelectrode remains unclear. Here we show that oxygen vacancies in bismuth vanadate (BiVO) can create defect dipoles due to a disruption of symmetry.

Triple Regulations via Fe Redox Boosting Nitrate Reduction to Ammonia at Industrial Current Densities.

Electrochemical nitrate reduction reaction (NO RR) has promising prospects for green synthesis of ammonia and environmental remediation. However, the performance of catalysts at high current density usually suffers from the high energy barrier for the nitrate (NO ) to nitrite (NO ) and the competitive hydrogen evolution. Herein, we proposed a two-step relay mechanism through spontaneous redox reaction followed electrochemical reaction by introducing low-valence Fe species into NiP nanosheets to significantly enhance the NO RR performance at industrial current density.

Water adsorption on ferroelectric PbTiO (0 0 1) surface: A density functional theory study.

In this work, combining the density functional theory (DFT) calculations and the ab initio molecular dynamics (AIMD) simulations, the water adsorption behavior, including the molecular and the dissociative adsorption on the negatively polarized (0 0 1) surface of ferroelectric PbTiO was comprehensively studied. Our theoretical results show that the dissociative adsorption of water is more energetically favorable than the molecular adsorption on the pristine PbTiO (0 0 1) surface. It has been also found that introducing surface oxygen vacancies (O) can enhance the thermodynamic stability of dissociative adsorption of water molecule.

Insights into Mechanistic Aspect of Organic Materials for Aluminum-Ion Batteries.

Rechargeable aluminum-ion batteries (AIBs) with organic electrode materials have garnered significant attention due to their excellent safety profile, cost-effectiveness, and eco-friendly nature. This review examines the fundamental properties of organic compounds and their effects on battery performance, with a primary focus on how changes in ion interactions and charge storage mechanisms at active sites influence overall performance. The aim is to propose innovative design approaches for AIBs that overcome the constraints associated with various types of organic materials.

Simultaneous Defect Passivation and Co-Catalyst Engineering Leads to Superior Photocatalytic Hydrogen Evolution on Metal Halide Perovskites.

Metal halide perovskites (MHPs) have emerged as attractive candidates for producing green hydrogen via photocatalytic pathway. However, the presence of abundant defects and absence of efficient hydrogen evolution reaction (HER) active sites on MHPs seriously limit the solar-to-chemical (STC) conversion efficiency. Herein, to address this issue, we present a bi-functionalization strategy through decorating MHPs with a molecular molybdenum-sulfur-containing co-catalyst precursor.

Oxygen Vacancy: How Will Poling History Affect Its Role in Photoelectrocatalysis.

Oxygen vacancy (V) has been recognized to possess an effect to promote the charge separation and transfer (CST) in various n-type semiconductor based photoelectrodes. But how external stimulus will change this V effect has not been investigated. In this work, external polarization is applied to investigate the effect of V on the CST process of a typical ferroelectric BiFeO photoelectrode.

Oxygen-Mediated (0D) CsPbX Formation during Open-Air Thermal Processing Improves Inorganic Perovskite Solar Cell Performance.

The desire to commercialize perovskite solar cells continues to mount, motivating the development of scalable production. Evaluations of the impact of open-air processing have revealed a variety of physical changes in the fabricated devices─with few changes having the capacity to be functionalized. Here, we highlight the beneficial role of ambient oxygen during the open-air thermal processing of metastable γ-CsPbI-based perovskite thin films and devices.

'Accelerated' Deactivation of Carbon Nitride Photocatalyst for Solar Hydrogen Evolution.

Carbon nitride photocatalysts are among the most studied candidates for efficient solar hydrogen (H) production due to their abundance of precursors, suitable bandgap, and visible light utilization. However, the polymeric nature of carbon nitride materials raises concerns regarding the self-decomposition during photocatalytic redox processes. Yet, the operational stability of carbon nitride photocatalysts for solar H production remains under-explored.

Na/Mo co-doped PbTiO for photocatalytic water oxidation and Z-scheme overall water splitting under visible light.

Herein, we demonstrate a sodium/molybdenum (Na/Mo) co-doped ferroelectric PbTiO for efficient photocatalysis under visible light. Doped with a high concentration of Mo, quasi-continuous new energy levels are successfully introduced below the conduction band minimum of PbTiO, giving rise to a band-to-band redshift of the absorption edge. The valence state difference of Mo and Ti in the doped PbTiO is compensated by the Na dopant, thus effectively suppressing the formation of the recombination centres caused by Mo.

High-Voltage Spinel Cathode Materials: Navigating the Structural Evolution for Lithium-Ion Batteries.

High-voltage LiNiMnO (LNMO) spinel oxides are highly promising cobalt-free cathode materials to cater to the surging demand for lithium-ion batteries (LIBs). However, commercial application of LNMOs is still challenging despite decades of research. To address the challenge, the understanding of their crystallography and structural evolutions during synthesis and electrochemical operation is critical.

Advancements in Interfacial Engineering for Perovskite Light-Emitting Diodes.

Perovskite light-emitting diodes (PeLEDs) have gained significant attention due to their promising optoelectronic properties and potential applications in the fields of lighting and display devices. Despite their potential, PeLEDs face challenges related to stability, high turn-on voltage, and low external quantum efficiency (EQE) which has restricted their broad acceptance. Most research efforts have predominantly focused on refining the properties of the perovskite films.

Thermally Evaporated Metal Halide Perovskites and Their Analogues: Film Fabrication, Applications and Beyond.

Metal halide perovskites emerge as promising semiconductors for optoelectronic devices due to ease of fabrication, attractive photophysical properties, their low cost, highly tunable material properties, and high performance. High-quality thin films of metal halide perovskites are the basis of most of these applications including solar cells, light-emitting diodes, photodetectors, and electronic memristors. A typical fabrication method for perovskite thin films is the solution method, which has several limitations in device reproducibility, adverse environmental impact, and utilization of raw materials.

Unveiling the Role of Water in Heterogeneous Photocatalysis of Methanol Conversion for Efficient Hydrogen Production.

Water molecules, which act as both solvent and reactant, play critical roles in photocatalytic reactions for methanol conversion. However, the influence of water on the adsorption of methanol and desorption of liquid products, which are two essential steps that control the performance in photocatalysis, has been well under-explored. Herein, we reveal the role of water in heterogeneous photocatalytic processes of methanol conversion on the platinized carbon nitride (Pt/CN) model photocatalyst.

Induced dipole moments in amorphous ZnCdS catalysts facilitate photocatalytic H evolution.

Amorphous semiconductors without perfect crystalline lattice structures are usually considered to be unfavorable for photocatalysis due to the presence of enriched trap states and defects. Here we demonstrate that breaking long-range atomic order in an amorphous ZnCdS photocatalyst can induce dipole moments and generate strong electric fields within the particles which facilitates charge separation and transfer. Loading 1 wt.

Liquid metal-embraced photoactive films for artificial photosynthesis.

The practical applications of solar-driven water splitting pivot on significant advances that enable scalable production of robust photoactive films. Here, we propose a proof-of-concept for fabricating robust photoactive films by a particle-implanting technique (PiP) which embeds semiconductor photoabsorbers in the liquid metal. The strong semiconductor/metal interaction enables resulting films efficient collection of photogenerated charges and superior photoactivity.

Scientific issues of zinc-bromine flow batteries and mitigation strategies.

Zinc-bromine flow batteries (ZBFBs) are promising candidates for the large-scale stationary energy storage application due to their inherent scalability and flexibility, low cost, green, and environmentally friendly characteristics. ZBFBs have been commercially available for several years in both grid scale and residential energy storage applications. Nevertheless, their continued development still presents challenges associated with electrodes, separators, electrolyte, as well as their operational chemistry.

Bilayer 2D-3D Perovskite Heterostructures for Efficient and Stable Solar Cells.

With a stacking-layered architecture, the bilayer two-dimensional-three-dimensional (2D-3D) perovskite heterostructure (PHS) not only eliminates surface defects but also protects the 3D perovskite matrix from external stimuli. However, these bilayer 2D-3D PHSs suffer from impaired interfacial charge carrier transport due to the relatively insulating 2D perovskite fragments with a random phase distribution. Over the past decade, substantial efforts have been devoted to pioneering molecular and structural designs of the 2D perovskite interlayers for improving their charge carrier mobility, which enables state-of-the-art perovskite solar cells with high power conversion efficiency and exceptional operational stability.

The role of ion migration, octahedral tilt, and the A-site cation on the instability of CsFAPbI.

Organic-inorganic hybrid perovskites are promising materials for the next generation photovoltaics and optoelectronics; however, their practical application has been hindered by poor structural stability mainly caused by ion migration and external stimuli. Understanding the mechanism(s) of ion migration and structure decomposition is thus critical. Here we observe the sequence of structural changes at the atomic level that precede structural decomposition in the technologically important CsFAPbI using ultralow dose transmission electron microscopy.

Modulating the Structure and Composition of Single-Atom Electrocatalysts for CO reduction.

Electrochemical CO reduction reaction (eCO RR) is a promising strategy to achieve carbon cycling by converting CO into value-added products under mild reaction conditions. Recently, single-atom catalysts (SACs) have shown enormous potential in eCO RR due to their high utilization of metal atoms and flexible coordination structures. In this work, the recent progress in SACs for eCO RR is outlined, with detailed discussions on the interaction between active sites and CO , especially the adsorption/activation behavior of CO and the effects of the electronic structure of SACs on eCO RR.

Gradient tungsten-doped BiTiNbO ferroelectric photocatalysts with additional built-in electric field for efficient overall water splitting.

BiTiNbO, a layered ferroelectric photocatalyst, exhibits great potential for overall water splitting through efficient intralayer separation of photogenerated carriers motivated by a depolarization field along the in-plane a-axis. However, the poor interlayer transport of carriers along the out-of-plane c-axis, caused by the significant potential barrier between layers, leads to a high probability of carrier recombination and consequently results in low photocatalytic activity. Here, we have developed an efficient photocatalyst consisting of BiTiNbO nanosheets with a gradient tungsten (W) doping along the c-axis.