Methanol-Enhanced Low-Cell-Voltage Hydrogen Generation at Industrial-Grade Current Density by Triadic Active Sites of Pt-Pd-(Ni,Co)(OH).

Methanol (ME) is a liquid hydrogen carrier, ideal for on-site-on-demand H generation, avoiding its costly and risky distribution issues, but this "ME-to-H" electric conversion suffers from high voltage (energy consumption) and competitive oxygen evolution reaction. Herein, we demonstrate that a synergistic cofunctional PtPd/(Ni,Co)(OH) catalyst with Pt single atoms (Pt) and Pd nanoclusters (Pd) anchored on OH-vacancy(V)-rich (Ni,Co)(OH) nanoparticles create synergistic triadic active sites, allowing for methanol-enhanced low-voltage H generation. For MOR, OH* is preferentially adsorbed on Pd and then interacts with the intermediates (such as *CHO or *CHOOH) adsorbed favorably on neighboring Pt with the assistance of hydrogen bonding from the surface hydrogen of (Ni,Co)(OH).

3D Crystal Construction by Single-Crystal 2D Material Supercell Multiplying.

2D stacking presents a promising avenue for creating periodic superstructures that unveil novel physical phenomena. While extensive research has focused on lateral 2D material superstructures formed through composition modulation and twisted moiré structures, the exploration of vertical periodicity in 2D material superstructures remains limited. Although weak van der Waals interfaces enable layer-by-layer vertical stacking, traditional methods struggle to control in-plane crystal orientation over large areas, and the vertical dimension is constrained by unscalable, low-throughput processes, preventing the achievement of global order structures.

Near-Neighbor Electron Orbital Coupling Effect of Single-Atomic-Layer Au Cluster Intercalated Bilayer 2H-TaS for Surface Enhanced Raman Scattering Sensing.

It is difficult to perfectly analyze the enhancement mechanism of two-dimensional (2D) materials and their combination with precious metals as surface enhanced Raman scattering (SERS) substrates using chemical enhancement mechanisms. Here, we propose a new mentality based on the coupling effect of neighboring electron orbitals to elucidate the electromagnetic field enhancement mechanism of single-atom-layer Au clusters embedded in double-layer 2H-TaS for SRES sensing. The insertion of Au atoms into the 2H-TaS interlayer was verified by XRD, AFM, and HRTEM, and a SERS signal enhancement of 2 orders of magnitude was obtained compared to the pure 2H-TaS.

Activated FeS @NiS Core-Shell Structure Boosting Cascade Reaction for Superior Electrocatalytic Oxygen Evolution.

Unlike single-step reactions, multi-step reactions can be greatly facilitated only if all the intermediate reactions can be catalyzed simultaneously and progressively. Herein, the theoretical analysis and experiments to illustrate the superiority of the cascade oxygen evolution reaction (OER) are conducted. As different OER intermediate reactions demand Fe Ni OOH with altered Fe/Ni ratios, gradient Fe-doped NiOOH can be an ideal electrocatalyst for the efficient cascade OER in line.

Medium/High-Entropy Amalgamated Core/Shell Nanoplate Achieves Efficient Formic Acid Catalysis for Direct Formic Acid Fuel Cell.

High-entropy alloys (HEAs) have been attracting extensive research interests in designing advanced nanomaterials, while their precise control is still in the infancy stage. Herein, we have reported a well-defined PtBiPbNiCo hexagonal nanoplates (HEA HPs) as high-performance electrocatalysts. Structure analysis decodes that the HEA HP is constructed with PtBiPb medium-entropy core and PtBiNiCo high-entropy shell.

Photocatalytic Overall Water Splitting over PbTiO Modulated by Oxygen Vacancy and Ferroelectric Polarization.

Ferroelectric materials hold great promise in the field of photocatalytic water splitting due to their spontaneous polarization that sets up an inherent internal field for the spatial separation of photogenerated charges. The ferroelectric polarization, however, is generally accompanied by some intrinsic defects, particularly oxygen vacancies, whose impact upon photocatalysis is far from being fully understood and modulated. Here, we have studied the role of oxygen vacancies over the photocatalytic behavior of single-domain PbTiO through a combination of theoretical and experimental viewpoints.

Constructing porous carbon nitride nanosheets for efficient visible-light-responsive photocatalytic hydrogen evolution.

The photocatalytic performance of polymeric carbon nitride (CN) is mainly restricted by the poor mass charge separation efficiency and poor light absorption due to its polymeric nature. The conventional strategies to address these problems involved constructing a nanosheets structure would result in a blue shifted light absorption and increased exciton binding energy. Here, with combination of ammonia etching and selectively hydrogen-bond breaking, holey carbon nitride nanosheets (hCNNS) were constructed, thus widening the light absorption range, and spontaneously shortening the migration distance of electrons and holes in the lateral and vertical directions, respectively.

Subnanometer high-entropy alloy nanowires enable remarkable hydrogen oxidation catalysis.

High-entropy alloys (HEAs) with unique physicochemical properties have attracted tremendous attention in many fields, yet the precise control on dimension and morphology at atomic level remains formidable challenges. Herein, we synthesize unique PtRuNiCoFeMo HEA subnanometer nanowires (SNWs) for alkaline hydrogen oxidation reaction (HOR). The mass and specific activities of HEA SNWs/C reach 6.

Iron-doped NiS microcrystals with exposed {001} facets for electrocatalytic water oxidation.

Developing high-performance electrocatalysts with favorable phase, surface structure and electronic structure for oxygen evolution reaction (OER) is crucial for efficient electrocatalytic water splitting. With Fe ions as both dopant and morphology-controlling agent, Fe-doped NiS microcrystals with the exposed chemically stable {001} facets were synthesized hydrothermally for electrocatalytic OER. The initial electrocatalytic OER activation processes led to the conversion of iron-rich surface layers of the NiS microcrystals into Fe-doped Ni (oxy)hydroxide as the shell and the residual inner of the NiS microcrystals as the core.

Perovskite Oxynitride Solid Solutions of LaTaON-CaTaON with Greatly Enhanced Photogenerated Charge Separation for Solar-Driven Overall Water Splitting.

The search for solar-driven photocatalysts for overall water splitting has been actively pursued. Although metal oxynitrides with metal d/d-closed shell configuration are very promising candidates in terms of their visible light absorption, they usually suffer from serious photo-generated charge recombination and thus, little photoactivity. Here, by forming their solid solutions of LaTaON and CaTaON, which are traditionally considered to be inorganic yellow-red pigments but have poor photocatalytic activity, a class of promising solar-driven photocatalysts La Ca TaON (0 ≤ , ≤ 1) are explored.

Gradient Sn-Doped Heteroepitaxial Film of Faceted Rutile TiO as an Electron Selective Layer for Efficient Perovskite Solar Cells.

The high-efficiency photocarrier collection at the interfaces plays an important role in improving the performance of perovskite solar cells (PSCs) because the photocarrier effective diffusion lengths in the lead halide perovskite absorbers usually surpass the incident depths of light. Developing the electron selective layer (ESL) that has good interfaces with photoactive perovskite and current collector layer-like fluorine-doped tin oxide (FTO) is actively pursued. Here, an unusual dense film of faceted rutile TiO single crystals with a gradient of the Sn dopant grown heteroepitaxially on the FTO layer is obtained by a hydrothermal route and subsequent thermal treatment.

Control of Spatially Homogeneous Distribution of Heteroatoms to Produce Red TiO Photocatalyst for Visible-Light Photocatalytic Water Splitting.

The strong band-to-band absorption of photocatalysts spanning the whole visible-light region (400-700 nm) is critically important for solar-driven photocatalysis. Although it has been actively and widely used as a photocatalyst for various reactions in the past four decades, TiO has a very poor ability to capture the whole spectrum of visible light. In this work, by controlling the spatially homogeneous distribution of boron and nitrogen heteroatoms in anatase TiO microspheres with a predominance of high-energy {001} facets, a strong visible-light absorption spectrum with a sharp edge beyond 680 nm has been achieved.

Insights into the role of nanoalloy surface compositions toward catalytic acetone hydrogenation.

A significant composition-dependent catalysis behavior was observed in catalytic acetone hydrogenation. Carbon supported PtRu alloy nanoparticles (NPs) with optimal surface composition achieved ultra-efficient and highly selective production of isopropyl alcohol.

Noninvasively Modifying Band Structures of Wide-Bandgap Metal Oxides to Boost Photocatalytic Activity.

Although doping with appropriate heteroatoms is a powerful way of increasing visible light absorption of wide-bandgap metal oxide photocatalysts, the incorporation of heteroatoms into the photocatalysts usually leads to the increase of deleterious recombination centers of photogenerated charge carriers. Here, a conceptual strategy of increasing visible light absorption without causing additional recombination centers by constructing an ultrathin insulating heterolayer of amorphous boron oxynitride on wide-bandgap photocatalysts is shown. The nature of this strategy is that the active composition nitrogen in the heterolayer can noninvasively modify the electronic structure of metal oxides for visible light absorption through the interface contact between the heterolayer and metal oxides.

A Langmuir and AFM study on interfacial behavior of binary monolayer of hexadecanol/DPPE at the air-water interface.

Hexadecanol is chemically stable and can be used as an effective addition in synthetic clinical lung surfactant preparations to improve their spreading properties. In this work, a detailed thermodynamic and structural characterization of a simple model system, which based on a hexadecanol-phospholipid mixture is reported. Langmuir monolayers of binary mixtures of hexadecanol/1,2-dipalmitoyl-sn-glycero-3-phosphoethanolamine (DPPE) have been studied with thermodynamic parameters and monolayer structure.