Quasi-One-Dimensional Zigzag Covalent Organic Frameworks for Photocatalytic Hydrogen Evolution from Water.

Covalent organic frameworks (COFs) have potential applications in a wide range of fields. However, it remains a critical challenge to constrain their covalent expansions in the one-dimensional (1D) direction. Here, we developed a general approach to fabricate 15 different highly crystalline COFs with zigzag-packed 1D porous organic chains through the condensation of V-shaped ditopic linkers and X-shaped tetratopic knots.

Accelerating Oxygen Electrocatalysis Kinetics on Metal-Organic Frameworks via Bond Length Optimization.

Metal-organic frameworks (MOFs) have been developed as an ideal platform for exploration of the relationship between intrinsic structure and catalytic activity, but the limited catalytic activity and stability has hampered their practical use in water splitting. Herein, we develop a bond length adjustment strategy for optimizing naphthalene-based MOFs that synthesized by acid etching Co-naphthalenedicarboxylic acid-based MOFs (donated as AE-CoNDA) to serve as efficient catalyst for water splitting. AE-CoNDA exhibits a low overpotential of 260 mV to reach 10 mA cm and a small Tafel slope of 62 mV dec with excellent stability over 100 h.

Particle-Based Photoelectrodes for PEC Water Splitting: Concepts and Perspectives.

This comprehensive review delves into the intricacies of the photoelectrochemical (PEC) water splitting process, specifically focusing on the design, fabrication, and optimization of particle-based photoelectrodes for efficient green hydrogen production. These photoelectrodes, composed of semiconductor materials, potentially harness light energy and generate charge carriers, driving water oxidation and reduction reactions. The versatility of particle-based photoelectrodes as a platform for investigating and enhancing various semiconductor candidates is explored, particularly the emerging complex oxides with compelling charge transfer properties.

Stabilizing BiVO Photoanode in Bicarbonate Electrolyte for Efficient Photoelectrocatalytic Alcohol Oxidation.

In order to expand the application of bismuth vanadate (BiVO) to the field of photoelectrochemistry, researchers have explored the potential of BiVO in catalyzing or degrading organic substances, potentially presenting a green and eco-friendly solution. A study was conducted to investigate the impact of electrolytes on the photocatalysis of benzyl alcohol by BiVO. The research discovered that, in an acetonitrile electrolyte (pH 9) with sodium bicarbonate, BiVO catalyzed benzyl alcohol by introducing saturated V.

Multifunctional Multigate One-Transistor with Thin Advanced Materials, Logic-in-Memory, and Artificial Synaptic Behaviors.

The high device density and fabrication complexity have hampered the development of the electronics. The advanced designs, which could implement the functions of the circuits with higher device density but less fabrication complexity, are hence required. Meanwhile, the MoS-based devices have recently attracted considerable attention owing to their advantages such as the ultrathin thickness.

Molecular understanding of cation effects on double layers and their significance to CO-CO dimerization.

Cation effects have been shown in numerous experiments to play a significant role in electrocatalysis. To understand these effects at the molecular level, we systematically investigate the structures and capacitances of electric double layers with a variety of cations as counter charges at Pt(111)-CO/water interfaces with molecular dynamics. It is encouraging to find that the computed Helmholtz capacitances for different cations are in quantitative agreement with experiments, and that the trend of cation effects on capacitances shows clear correlation with the structures of interface cations of differing sizes and hydration energies.

Understanding the Effects of Electrode Material, Single Crystal Facet, and Electrolyte Ion on the Helmholtz Capacitance of Metal/Aqueous Solution Interfaces.

The comprehensive interpretation of the measured differential Helmholtz capacitance curve is vital for advancing our understanding of the interfacial structure. While several possible physical effects contributing to the Helmholtz capacitance have been proposed theoretically, combining those factors to explain the experimentally observed potential-dependent capacitance profile remains a significant challenge. In this study, we employ ab initio molecular dynamics simulations to model various metal/solution interfaces.

Spin-State Modulation on Metal-Organic Frameworks for Electrocatalytic Oxygen Evolution.

Electrochemical oxygen evolution reaction (OER) kinetics are heavily correlated with hybridization of the transition metal d-orbital and oxygen intermediate p-orbital, which dictates the barriers of intermediate adsorption/desorption on the active sites of catalysts. Herein, a strategy is developed involving strain engineering and coordination regulation to enhance the hybridization of Ni 3d and O 2p orbitals, and the as-synthesized Ni-2,6-naphthalenedicarboxylic acid metal-organic framework (DD-Ni-NDA) nanosheets deliver a low OER overpotential of 260 mV to reach 10 mA cm . By integrating an alkaline anion exchange membrane electrolyzer and Pt/C electrode, 200 and 500 mA cm current densities are reached with cell voltages of 1.

Nanolaminated Ternary Transition Metal Carbide (MAX Phase)-Derived Core-Shell Structure Electrocatalysts for Hydrogen Evolution and Oxygen Evolution Reactions in Alkaline Electrolytes.

The development of abundant, cheap, and highly active catalysts for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is important for hydrogen production. Nanolaminate ternary transition metal carbides (MAX phases) and their derived two-dimensional transition metal carbides (MXenes) have attracted considerable interest for electrocatalyst applications. Herein, four new MAX@MXene core-shell structures (TaCoC@TaCT, TaNiC@TaCT, NbCoC@NbCT, and NbNiC@NbCT), in which the core region is Co/Ni-MAX phases while the edge region is MXenes, have been prepared.

Pt Nanoparticle Assisted Homogeneous Surface Engineering of Polymer-Based Bulk-Heterojunction Photocathodes for Efficient Charge Extraction and Catalytic Hydrogen Evolution.

To fabricate a high-efficiency bulk-heterojunction (BHJ)-based photocathode, introducing suitable interfacial modification layer(s) is a crucial strategy. Surface engineering is especially important for achieving high-performance photocathodes because the photoelectrochemical (PEC) reactions at the photocathode/electrolyte interface are the rate-limiting process. Despite its importance, the influence of interfacial layer morphology regulation on PEC activity has attracted insufficient attention.

Modeling stepped Pt/water interfaces at potential of zero charge with ab initio molecular dynamics.

It is worth understanding the potentials of zero charge (PZCs) and structures of stepped metal/water interfaces, because for many electrocatalytic reactions, stepped surfaces are more active than atomically flat surfaces. Herein, a series of stepped Pt/water interfaces are modeled at different step densities with ab initio molecular dynamics. It is found that the structures of Pt/water interfaces are significantly influenced by the step density, particularly in regard to the distribution of chemisorbed water.

Direct Construction of Isomeric Benzobisoxazole-Vinylene-Linked Covalent Organic Frameworks with Distinct Photocatalytic Properties.

Vinylene/olefin-linked two-dimensional covalent organic frameworks (v-2D-COFs) have emerged as advanced semiconducting materials with excellent in-plane conjugation, high chemical stabilities, and precisely tunable electronic structures. Exploring new linkage chemistry for the reticular construction of v-2D-COFs remains in infancy and challenging. Herein, we present a solid-state benzobisoxazole-mediated aldol polycondensation reaction for the construction of two novel isomeric benzobisoxazole-bridged v-2D-COFs (v-2D-COF-NO1 and v-2D-COF-NO2) with and configurations of benzobisoxazole.

Strengthen Synergistic Effect of Soft Carbon and Hard Carbon Toward High-Performance Anode for K-Ion Battery.

Synergistic effect of soft carbon and hard carbon has been proven to be useful for obtaining excellent anode materials for potassium ion battery, which is determined by the mixing degree of precursors. Inspired by the formation of proteins in biology, peptide bonds are used to connect the precursors of the two sort of carbon to prepare soft-hard hybrid carbons with stronger synergistic effects. The hard carbon domain with nanometer size is so highly distributed in the soft carbon that the synergistic effect between two sorts of carbon is significantly enhanced.

Metal-Organic Frameworks with Assembled Bifunctional Microreactor for Charge Modulation and Strain Generation toward Enhanced Oxygen Electrocatalysis.

Two-dimensional metal-organic frameworks (MOFs) have served as favorable prototypes for electrocatalytic oxygen evolution reaction (OER). Despite promising catalytic activity, their OER reaction kinetics are still limited by the sluggish four-electron transfer process. Herein, we develop a ferrocene carboxylic acid (FcCA) partially substituted cobalt-terephthalic acid (CoBDC) catalyst with a bifunctional microreactor composed of two species of Co active sites and ligand FcCA (CoBDC FcCA).

Room Temperature Electrodeposition of Ready-to-Use TiO for Uniform p-n Heterojunction Over Nanoarchitecture.

The photocathodes are essential in photoelectrochemical systems for harvesting solar energy as green fuels. However, the light-absorbing p-type semiconductor in them usually suffers from carrier recombination issues. An effective strategy to address it is fabricating the p-n heterojunction to create an interfacial electric field.

General In Situ Photoactivation Route with IPCE over 80% toward CdS Photoanodes for Photoelectrochemical Applications.

Cost-effective photoanodes with remarkable electronic properties are highly demanded for practical photoelectrochemical (PEC) water splitting. The ability to manipulate the surface carrier separation and recombination is pivotal for achieving high PEC performance for water splitting. Here, a facile and economical approach is reported for substantially improving the surface charge separation property of CdS photoanodes through in situ photoactivation, which significantly reduces surface charge recombination through the formation of thiosulfate ion which is favorable to the transfer of photogenerated holes and a uniform nanoporous morphology via the dissolving Cd with phosphate ions on the surface of CdS.

Suppression of poisoning of photocathode catalysts in photoelectrochemical cells for highly stable sunlight-driven overall water splitting.

A photoelectrochemical (PEC) cell composed of two semiconductor electrodes, a photocathode, and a photoanode is a potentially effective means of obtaining hydrogen through spontaneous overall water splitting under light irradiation. However, the long-term stability (that is, operation for more than one day) of a PEC cell has not yet been demonstrated. In addition to the corrosion of both photoelectrodes, the gradual migration of heavy metal cations from the photoanode into the electrolyte can also result in degradation of the cell by contamination of the photocathode surface.

Boosting photocatalytic overall water splitting by Co doping into MnO nanoparticles as oxygen evolution cocatalysts.

The effect of cobalt doping into a manganese oxide (tetragonal spinel MnO) nanoparticle cocatalyst up to Co/(Co + Mn) = 0.4 (mol/mol) on the activity of photocatalytic water oxidation was studied. Monodisperse ∼10 nm CoMnO (0 ≤y≤ 0.

Ternary Nonfullerene Polymer Solar Cells with 12.16% Efficiency by Introducing One Acceptor with Cascading Energy Level and Complementary Absorption.

A novel small-molecule acceptor, (2,2'-((5E,5'E)-5,5'-((5,5'-(4,4,9,9-tetrakis(5-hexylthiophen-2-yl)-4,9-dihydro-s-indaceno[1,2-b:5,6-b']dithiophene-2,7-diyl)bis(4-(2-ethylhexyl)thiophene-5,2-diyl))bis(methanylylidene)) bis(3-hexyl-4-oxothiazolidine-5,2-diylidene))dimalononitrile (ITCN), end-capped with electron-deficient 2-(3-hexyl-4-oxothiazolidin-2-ylidene)malononitrile groups, is designed, synthesized, and used as the third component in fullerene-free ternary polymer solar cells (PSCs). The cascaded energy-level structure enabled by the newly designed acceptor is beneficial to the carrier transport and separation. Meanwhile, the three materials show a complementary absorption in the visible region, resulting in efficient light harvesting.

Overall water splitting by photoelectrochemical cells consisting of (ZnSe)(CuInGaSe) photocathodes and BiVO photoanodes.

The design of photoelectrochemical (PEC) cell structures that mitigate challenges related to mass transfer is the key to achieving efficient hydrogen production. A PEC cell based on an integrated photoelectrode incorporating (ZnSe)(CuInGaSe) strips and BiVO strips exhibited 1.0% solar-to-hydrogen energy conversion efficiency even without stirring the electrolyte solution.

A CoO-modified SnNbO photoelectrode for highly efficient oxygen evolution from water.

SnNbO has arisen as a candidate for photoanodes for solar water splitting. CoO cocatalyst-loaded SnNbO showed a stable, high anodic photocurrent with an incident photon-to-current conversion efficiency (IPCE) of 18% at 0.6 V and a half-cell solar-to-hydrogen (HC-STH) efficiency of 0.

Visible Light-Driven Z-Scheme Water Splitting Using Oxysulfide H Evolution Photocatalysts.

A SmTiSO (STSO) oxysulfide photocatalyst prepared by a novel flux method showed a higher degree of crystallinity and greater photocatalytic activity than that prepared by conventional polymerized complex and sulfurization processes. Co-loading with both IrO, as an oxidative cocatalyst, and Pt, as a reductive cocatalyst, was found to be essential for promoting the photocatalytic activity of the STSO. Visible light-driven Z-scheme water splitting into H and O was realized by utilizing the STSO photocatalyst for H evolution in conjunction with a WO photocatalyst treated with H and Cs and loaded with PtO for O evolution, and a triiodide/iodide (I/I) redox couple as a shuttle electron mediator.

Pt/In2S3/CdS/Cu2ZnSnS4 Thin Film as an Efficient and Stable Photocathode for Water Reduction under Sunlight Radiation.

An electrodeposited Cu2ZnSnS4 (CZTS) compact thin film modified with an In2S3/CdS double layer and Pt deposits (Pt/In2S3/CdS/CZTS) was used as a photocathode for water splitting of hydrogen production under simulated sunlight (AM 1.5G) radiation. Compared to platinized electrodes based on a bare CZTS film (Pt/CZTS) and a CZTS film modified with a CdS single layer (Pt/CdS/CZTS), the Pt/In2S3/CdS/CZTS electrode exhibited a significantly high cathodic photocurrent.