Regulating Interfacial Hydrogen-Bonding Networks by Implanting Cu Sites with Perfluorooctane to Accelerate CO Electroreduction to Ethanol.

Efficient CO electroreduction (CORR) to ethanol holds promise to generate value-added chemicals and harness renewable energy simultaneously. Yet, it remains an ongoing challenge due to the competition with thermodynamically more preferred ethylene production. Herein, we presented a CO reduction predilection switch from ethylene to ethanol (ethanol-to-ethylene ratio of ~5.

Unsymmetric Protonation Driven Highly Efficient HO Photosynthesis in Supramolecular Photocatalysts via One-Step Two-Electron Oxygen Reduction.

Photocatalytic hydrogen peroxide (HO) production has emerged as an attractive alternative to the traditional anthraquinone process. However, its performance is often hindered by low selectivity and sluggish kinetics of oxygen reduction reaction (ORR). Herein, we report an anthrazoline-based supramolecular photocatalyst, SA-SADF-H, featuring an unsymmetric protonation structure for HO photosynthesis from water and air.

Rate Constants of the H + HCF → H + CF Reaction from Ring Polymer Molecular Dynamics on a Highly Accurate Potential Energy Surface.

The reaction between H and HCF is the primary consumption pathway of HCF in the atmosphere and combustion. In this work, ring polymer molecular dynamics (RPMD) calculations are performed to calculate the rate constants of the reaction on a recently developed accurate potential energy surface. 36, 20, and 8 beads are used to compute the rate constants at 350 K ≤ < 800 K, 800 K ≤ ≤ 1000 K, and > 1000 K, respectively.

Enhanced Methanol Electrooxidation and Supercapacitive Performance via Compositional Engineering of Colloidal Ni-Co Alloying Nanoparticles.

Among renewable energy technologies, particular attention is paid to electrochemically transforming methanol into valuable formate and storing energy into supercapacitors. In this study, we detailed a simple colloidal-based protocol for synthesizing a series of alloy nanoparticles with tuned Ni/Co atomic ratios, thereby optimizing their electrochemical performance. With the addition of 1 M methanol in 1 M KOH, the optimized composition was able to electrochemically produce formate at 0.

Coupling Photocatalytic Hydrogen Production with Key Oxidation Reactions.

Hydrogen represents a clean and sustainable energy source with wide applications in fuel cells and hydrogen energy storage systems. Photocatalytic strategies emerge as a green and promising solution for hydrogen production, which still reveals several critical challenges in enhancing the efficiency and stability and improving the whole value. This review systematically elaborates on various coupling approaches for photocatalytic hydrogen production, aiming to improve both efficiency and value through different oxidation half-reactions.

Steering the Site Distance of Atomic Cu-Cu Pairs by First-Shell Halogen Coordination Boosts CO-to-C Selectivity.

Electrocatalytic reduction of CO into C products of high economic value provides a promising strategy to realize resourceful CO utilization. Rational design and construct dual sites to realize the CO protonation and C-C coupling to unravel their structure-performance correlation is of great significance in catalysing electrochemical CO reduction reactions. Herein, Cu-Cu dual sites with different site distance coordinated by halogen at the first-shell are constructed and shows a higher intramolecular electron redispersion and coordination symmetry configurations.

Regulating Local Electron Density of Cyano Sites in Graphitic Nitride Carbon by Giant Internal Electric Field for Efficient CO Photoreduction to Hydrocarbons.

Selective photocatalytic CO reduction to high-value hydrocarbons using graphitic carbon nitride (g-CN) polymer holds great practical significance. Herein, the cyano-functionalized g-CN (CN-g-CN) with a high local electron density site is successfully constructed for selective CO photoreduction to CH and CH. Wherein the potent electron-withdrawing cyano group induces a giant internal electric field in CN-g-CN, significantly boosting the directional migration of photogenerated electrons and concentrating them nearby.

Enhanced water decontamination via photogenerated electron delocalization of π → π* and D-π-A synergistically.

Mixed-dimensional van der Waals heterojunctions (MD-vdWhs), known for exceptional electron transfer and charge separation capabilities, remain underexplored in photocatalysis. In this study, we leveraged the synergistic effect of intermolecular π → π* and D-π-A dual channels to fabricate novel MD-vdWhs. Owing to the synergistic effect, it exhibits superior electron transfer and delocalization ability, thereby enhancing its photocatalytic performance.

A photocatalytic redox cycle over a polyimide catalyst drives efficient solar-to-HO conversion.

Circumventing the conventional two-electron oxygen reduction pathway remains a great problem in enhancing the efficiency of HO photosynthesis. A promising approach to achieve outstanding photocatalytic activity involves the utilization of redox intermediates. Here, we engineer a polyimide aerogel photocatalyst with photoreductive carbonyl groups for non-sacrificial HO production.

Activating Inert Perovskite Oxides for CO Electroreduction via Slight Cu Doping in B-Sites.

Perovskite oxides are proven as a striking platform for developing high-performance electrocatalysts. Nonetheless, a significant portion of them show CO electroreduction (CORR) inertness. Here a simple but effective strategy is reported to activate inert perovskite oxides (e.

Enhancing Built-in Electric Fields via Molecular Symmetry Modulation in Supramolecular Photocatalysts for Highly Efficient Photocatalytic Hydrogen Evolution.

Nature-inspired supramolecular self-assemblies are attractive photocatalysts, but their quantum yields are limited by poor charge separation and transportation. A promising strategy for efficient charge transfer is to enhance the built-in electric field by symmetry breaking. Herein, an unsymmetric protonation, N-heterocyclic π-conjugated anthrazoline-based supramolecular photocatalyst SA-DADK-H was developed.

Dual Function of Naphthalenediimide Supramolecular Photocatalyst with Giant Internal Electric Field for Efficient Hydrogen and Oxygen Evolution.

Organic supramolecular photocatalysts have garnered widespread attention due to their adjustable structure and exceptional photocatalytic activity. Herein, a novel bis-dicarboxyphenyl-substituent naphthalenediimide self-assembly supramolecular photocatalyst (SA-NDI-BCOOH) with efficient dual-functional photocatalytic performance is successfully constructed. The large molecular dipole moment and short-range ordered stacking structure of SA-NDI-BCOOH synergistically create a giant internal electric field (IEF), resulting in a remarkable 6.

The Transfer Dehydrogenation Method Enables a Family of High Crystalline Benzimidazole-linked Cu (II)-phthalocyanine-based Covalent Organic Frameworks Films.

Heterocycle-linked phthalocyanine-based COFs with close-packed π-π conjugated structures are a kind of material with intrinsic electrical conductivity, and they are considered to be candidates for photoelectrical devices. Previous studies have revealed their applications for energy storage, gas sensors, and field-effect transistors. However, their potential application in photodetector is still not fully studied.

Promoting CO Electroreduction Over Nano-Socketed Cu/Perovskite Heterostructures via A-Site-Valence-Controlled Oxygen Vacancies.

Despite the intriguing potential, nano-socketed Cu/perovskite heterostructures for CO electroreduction (CORR) are still in their infancy and rational optimization of their CORR properties is lacking. Here, an effective strategy is reported to promote CO-to-C conversion over nano-socketed Cu/perovskite heterostructures by A-site-valence-controlled oxygen vacancies. For the proof-of-concept catalysts of Cu/LaSrTiO (x from 0 to 0.

Engineering Atomic Ag-N Sites with Enhanced Performance of Eradication Drug-Resistant Bacteria over Visible-Light-Driven Antibacterial Membrane.

Utilizing visible light for water disinfection is a more convenient, safe, and practical alternative to ultraviolet-light sterilization. Herein, we developed silver (Ag) single-atom anchored g-CN (P-CN) nanosheets (Ag/CN) and then utilized a spin-coating method to fabricate the Ag/CN-based-membrane for effective antibacterial performance in natural water and domestic wastewater. The incorporated Ag single atom formed a Ag-N motif, which increased the charge density around the N atoms, resulting in a built-in electric field ∼17.

Superexchange-stabilized long-distance Cu sites in rock-salt-ordered double perovskite oxides for CO electromethanation.

Cu-oxide-based catalysts are promising for CO electroreduction (CORR) to CH, but suffer from inevitable reduction (to metallic Cu) and uncontrollable structural collapse. Here we report Cu-based rock-salt-ordered double perovskite oxides with superexchange-stabilized long-distance Cu sites for efficient and stable CO-to-CH conversion. For the proof-of-concept catalyst of SrCuWO, its corner-linked CuO and WO octahedral motifs alternate in all three crystallographic dimensions, creating sufficiently long Cu-Cu distances (at least 5.

Forked Vein Structure W/WO with Dual Active Sites in W and Oxygen Vacancies to Enhance Methylene Self-Coupling for Efficient Conversion of Methane to Ethylene.

The directional conversion of methane to ethylene is challenging due to the dissociation of the C─H bond and the self-coupling of methyl intermediates. Herein, a novel W/WO catalyst with the fork vein structure consisting of an alternating arrangement of WO and W is developed. Impressively, the catalyst achieves an unprecedented CH yield of 1822.

Progress on mechanism and efficacy of heterogeneous photocatalysis coupled oxidant activation as an advanced oxidation process for water decontamination.

The rising debate on the dilemma of photocatalytic water treatment technologies has driven researchers to revisit its prospects in water decontamination. Nowadays, heterogeneous photocatalysis coupled oxidant activation techniques are intensively studied due to their dual advantages of high mineralization and high oxidation efficiency in pollutant degradation. This paved a new way for the development of solar-driven oxidation technologies.

Dipole-Dipole Tuned Electronic Reconfiguration of Defective Carbon Sites for Efficient Oxygen Reduction into HO.

Metal-free carbon-based materials are one of the most promising electrocatalysts toward 2-electron oxygen reduction reaction (2e-ORR) for on-site production of hydrogen peroxide (HO), which however suffer from uncontrollable carbonizations and inferior 2e-ORR selectivity. To this end, a polydopamine (PDA)-modified carbon catalyst with a dipole-dipole enhancement is developed via a calcination-free method. The HO yield rate outstandingly reaches 1.

Polymer Photocatalysts Containing Segregated π-Conjugation Units with Electron-Trap Activity for Efficient Natural-light-driven Bacterial Inactivation.

Development of highly efficient and metal-free photocatalysts for bacterial inactivation under natural light is a major challenge in photocatalytic antibiosis. Herein, we developed an acidizing solvent-thermal approach for inserting a non-conjugated ethylenediamine segment into the conjugated planes of 3,4,9,10-perylene tetracarboxylic anhydride to generate a photocatalyst containing segregated π-conjugation units (EDA-PTCDA). Under natural light, EDA-PTCDA achieved 99.