Nitrogen-Bridged S-N-Cu Sites for CO2 Photoreduction to Ethanol with 99.5% Selectivity in Pure Water.

Solar-driven CO2 reduction to ethanol is extremely challenging due to the limited efficiency of charge separation, sluggish kinetics of C-C coupling, and unfavorable formation of oxygenate intermediates. Here, we elaborately design a red polymer carbon nitride (RPCN) consisting of S-N and Cu-N4 dual active sites (Cu/S-RPCN) to address this challenge, which achieves an impressive ethanol evolution rate of 50.4 µmol g-1 h-1 with 99.

Modulating the properties of g-C3N4 through two-step annealing and ionic-liquid gating.

We reported a novel strategy by the combination of two-step annealing treatment and ionic-liquid gating technology for effectively regulating the properties of g-C3N4, especially largely reducing the recombination rate of the electron-hole pairs, with evidenced by the remarkable reduction of photoluminescence (PL) intensity. Firstly, graphitic carbon nitrides with typical layered structure were obtained by annealing melamine with temperature above 500°C. Further annealing at 600°C with much longer time (from 2 hours to 12 hours) were found to effectively reduce the imperfections or defects, and thus the PL intensity (49% reduction).

Flash Joule Heating Synthesis of Layer-Stacked Vanadium Oxide/Graphene Hybrids within Seconds for High-Performance Aqueous Zinc-Ion Batteries.

Vanadium oxides have been regarded as highly promising cathodes for aqueous zinc-ion batteries (ZIBs). However, obtaining high-performance vanadium oxide-based cathodes suitable for industrial application remains a significant challenge due to the need for cost-effective, straightforward, and efficient preparation methods. Herein, we present a facile and rapid synthesis of a composite cathode, consisting of layer-stacked VO/VO and graphene-like carbon nanosheets, in just 2.

Structural Ni-Ni Pair Sites for Highly Active Hydrogenation of Nitriles to Primary Amines.

Supported metal pair sites have sparked interest due to their tremendous potential as bifunctional catalysts. Here, we report the structural Ni-Ni pair sites constructed in a well-defined nanocrystal phase of NiP. These Ni-Ni pair sites exhibited a remarkable product formation rate of 123 mol/mol/h for the hydrogenation of benzonitrile (BN) to benzylamine (BA).

Design Principle of Molybdenum-Based Metal Nitrides for Lattice Nitrogen-Mediated Ammonia Production.

Chemical looping ammonia synthesis (CLAS) is a promising technology for reducing the high energy consumption of the conventional ammonia synthesis process. However, the comprehensive understanding of reaction mechanisms and rational design of novel nitrogen carriers has not been achieved due to the high complexity of catalyst structures and the unrevealed relationship between electronic structure and intrinsic activity. Herein, we propose a multistage strategy to establish the connection between catalyst intrinsic activity and microscopic electronic structure fingerprints using density functional theory computational energetics as bridges and apply it to the rational design of metal nitride catalysts for lattice nitrogen-mediated ammonia production.

Unlocking Spin Gates of Transition Metal Oxides via Strain Stimuli to Augment Potassium Ion Storage.

Transition metal oxides (TMOs) are key in electrochemical energy storage, offering cost-effectiveness and a broad potential window. However, their full potential is limited by poor understanding of their slow reaction kinetics and stability issues. This study diverges from conventional complex nano-structuring, concentrating instead on spin-related charge transfer and orbital interactions to enhance the reaction dynamics and stability of TMOs during energy storage processes.

Cu-Modified Palladium Catalysts: Boosting Formate Electrooxidation via Interfacially OH-Driven H Removal.

Direct formate fuel cells have gained traction due to their eco-friendly credentials and inherent safety. However, their potential is hampered by the kinetic challenges of the formate oxidation reaction (FOR) on Pd-based catalysts, chiefly due to the unfavorable adsorption of hydrogen species (H). These species clog the active sites, hindering efficient catalysis.

Significant hydrogen generation photo-mechanical coupling in flexible methylammonium lead iodide nanowires.

The flexoelectric effect, which refers to the mechanical-electric coupling between strain gradient and charge polarization, should be considered for use in charge production for catalytically driving chemical reactions. We have previously revealed that halide perovskites can generate orders of higher magnitude flexoelectricity under the illumination of light than in the dark. In this study, we report the catalytic hydrogen production by photo-mechanical coupling involving the photoflexoelectric effect of flexible methylammonium lead iodide (MAPbI) nanowires (NWs) in hydrogen iodide solution.

Revealing the Role of the Tetragonal Distortion in the Metal-Insulator Transition of Co- and Fe-Doped NiS.

Although the NiS exhibits the most widely adjustable metal-to-insulator (MIT) properties among the chalcogenides, the mechanisms, with respect to the regulations in their critical temperatures (), are yet unclear. Herein, we demonstrate the overlooked role associated with the structurally tetragonal distortion in elevating the of NiS; this is in distinct contrast to the previously expected hybridization and bandwidth regulations that usually reduces . Compared to the perspective of structure distortions, the orbital hybridization and band regulation of NiS are ∼19 times more effective adjustment in .

Surface Self-Transforming FeTi-LDH Overlayer in Fe O /Fe TiO Photoanode for Improved Water Oxidation.

Integrating hematite nanostructures with efficient layer double hydroxides (LDHs) is highly desirable to improve the photoelectrochemical (PEC) water oxidation performance. Here, an innovative and facile strategy is developed to fabricate the FeTi-LDH overlayer decorated Fe O /Fe TiO photoanode via a surface self-transformation induced by the co-treatment of hydrazine and NaOH at room temperature. Electrochemical measurements find that this favorable structure can not only facilitate the charge transfer/separation at the electrode/electrolyte interface but also accelerate the surface water oxidation kinetics.

Modulating the Interfacial Water Network of Dual-Site Pd/FeO/C Catalyst for Efficient Formate Electrooxidation.

The rational design of electrocatalysts for formate oxidation reaction (FOR) in alkaline media is crucial to promote the practical applications of direct formate fuel cells (DFFCs). The FOR kinetic on palladium (Pd) based electrocatalysts is strongly hindered by unfavorably adsorbed hydrogen (H) as the major intermediate species blocking the active sites. Herein, we report a strategy of modulating the interfacial water network of dual-site Pd/FeO/C catalyst to significantly enhance the desorption kinetics of H during FOR.

CoMoO-modified hematite with oxygen vacancies for high-efficiency solar water splitting.

Hematite is a potential photoelectrode for photoelectrochemical (PEC) water splitting. Nevertheless, its water oxidation efficiency is highly limited by its significant photogenerated carrier recombination, poor conductivity and slow water oxidation kinetics. Herein, under low-vacuum (LV) conditions, we fabricated a CoMoO layer on oxygen-vacancy-modified hematite (CoMo-FeO (LV)) for the first time for efficient solar water splitting.

Growth mechanism study and band structure modulation of a manganese doped two-dimensional BlueP-Au network.

Two-dimensional (2D) materials are a very promising material family. The two-dimensional inorganic metal network called BlueP-Au network is rapidly attracting the attention of researchers due to its customizable architecture, adjustable chemical functions and electronic properties. Herein, manganese (Mn) was successfully doped on a BlueP-Au network for the first time, then the doping mechanism and electronic structure evolution was studied by X-ray photoelectron spectroscopy (XPS) based on synchrotron radiation, X-ray absorption spectroscopy (XAS), Scanning Tunneling Microscopy (STM), Density functional theory (DFT), Low-energy electron diffraction (LEED), Angle resolved photoemission spectroscopy (ARPES), Mn atoms tend to be stably adsorbed on two sites of the BlueP-Au network.

Regulation of the Work Function Difference Promotes In Situ Phase Transition of WO for Efficient Formate Electrooxidation.

Direct formate fuel cells (DFFCs) have drawn tremendous attention because they are environmentally benign and have good safety. However, the lack of advanced catalysts for formate electrooxidation hinders the development and applications of DFFCs. Herein, we report a strategy of regulating the metal-substrate work function difference to effectively promote the transfer of adsorbed hydrogen (H), thus enhancing formate electrooxidation in alkaline solutions.

Promoting nickel oxidation state transitions in single-layer NiFeB hydroxide nanosheets for efficient oxygen evolution.

Promoting the formation of high-oxidation-state transition metal species in a hydroxide catalyst may improve its catalytic activity in the oxygen evolution reaction, which remains difficult to achieve with current synthetic strategies. Herein, we present a synthesis of single-layer NiFeB hydroxide nanosheets and demonstrate the efficacy of electron-deficient boron in promoting the formation of high-oxidation-state Ni for improved oxygen evolution activity. Raman spectroscopy, X-ray absorption spectroscopy, and electrochemical analyses show that incorporation of B into a NiFe hydroxide causes a cathodic shift of the Ni(OH) → NiOOH transition potential.

Construction of Novel Bimetallic Oxyphosphide as Advanced Anode for Potassium Ion Hybrid Capacitor.

Potassium ion hybrid capacitors (PIHCs) have attracted considerable interest due to their low cost, competitive power/energy densities, and ultra-long lifespan. However, the more sluggish insertion kinetics of battery-type anodes than capacitor-type cathodes in PIHCs seriously limits their practical application. Therefore, developing advanced anodes with high capacitor and suitable K intercalation is imperative and significant.

Renal-Clearable Ultrasmall Coordination Polymer Nanodots for Chelator-Free Cu-Labeling and Imaging-Guided Enhanced Radiotherapy of Cancer.

Developing tumor-homing nanoparticles with integrated diagnostic and therapeutic functions, and meanwhile could be rapidly excreted from the body, would be of great interest to realize imaging-guided precision treatment of cancer. In this study, an ultrasmall coordination polymer nanodot (CPN) based on the coordination between tungsten ions (W) and gallic acid (W-GA) was developed via a simple method. After polyethylene glycol (PEG) modification, PEGylated W-GA (W-GA-PEG) CPNs with an ultrasmall hydrodynamic diameter of 5 nm were rather stable in various physiological solutions.

Synergistic Effects in CNTs-PdAu/Pt Trimetallic Nanoparticles with High Electrocatalytic Activity and Stability.

We present a straightforward physical approach for synthesizing multiwalled carbon nanotubes (CNTs)-PdAu/Pt trimetallic nanoparticles (NPs), which allows predesign and control of the metal compositional ratio by simply adjusting the sputtering targets and conditions. The small-sized CNTs-PdAu/Pt NPs (~3 nm, Pd/Au/Pt ratio of 3:1:2) act as nanocatalysts for the methanol oxidation reaction (MOR), showing excellent performance with electrocatalytic peak current of 4.4 A mg and high stability over 7000 s.