Surface passivation for highly active, selective, stable, and scalable CO electroreduction.

Electrochemical conversion of CO to formic acid using Bismuth catalysts is one the most promising pathways for industrialization. However, it is still difficult to achieve high formic acid production at wide voltage intervals and industrial current densities because the Bi catalysts are often poisoned by oxygenated species. Herein, we report a BiS nanowire-ascorbic acid hybrid catalyst that simultaneously improves formic acid selectivity, activity, and stability at high applied voltages.

Fast and Durable Alkaline Hydrogen Oxidation Reaction at the Electron-Deficient Ruthenium-Ruthenium Oxide Interface.

The slow hydrogen oxidation reaction (HOR) kinetics under alkaline conditions remain a critical challenge for the practical application of alkaline exchange membrane fuel cells. Herein, Ru/RuO in-plane heterostructures are designed with abundant active Ru-RuO interface domains as efficient electrocatalysts for the HOR in alkaline media. The experimental and theoretical results demonstrate that interfacial Ru and RuO domains at Ru-RuO interfaces are the optimal H and OH adsorption sites, respectively, endowing the well-defined Ru(100)/RuO (200) interface as the preferential region for fast alkaline hydrogen electrocatalysis.

Continuous Modulation of Electrocatalytic Oxygen Reduction Activities of Single-Atom Catalysts through p-n Junction Rectification.

Fine-tuning single-atom catalysts (SACs) to surpass their activity limit remains challenging at their atomic scale. Herein, we exploit p-type semiconducting character of SACs having a metal center coordinated to nitrogen donors (MeN ) and rectify their local charge density by an n-type semiconductor support. With iron phthalocyanine (FePc) as a model SAC, introducing an n-type gallium monosulfide that features a low work function generates a space-charged region across the junction interface, and causes distortion of the FeN moiety and spin-state transition in the Fe center.

Atomically dispersed chromium coordinated with hydroxyl clusters enabling efficient hydrogen oxidation on ruthenium.

Overcoming the sluggish kinetics of alkaline hydrogen oxidation reaction (HOR) is challenging but is of critical importance for practical anion exchange membrane fuel cells. Herein, abundant and efficient interfacial active sites are created on ruthenium (Ru) nanoparticles by anchoring atomically isolated chromium coordinated with hydroxyl clusters (Cr(OH)) for accelerated alkaline HOR. This catalyst system delivers 50-fold enhanced HOR activity with excellent durability and CO anti-poisoning ability via switching the active sites from Ru surface to Cr(OH)-Ru interface.

Ultrahigh Stable Methanol Oxidation Enabled by a High Hydroxyl Concentration on Pt Clusters/MXene Interfaces.

Anchoring platinum catalysts on appropriate supports, e.g., MXenes, is a feasible pathway to achieve a desirable anode for direct methanol fuel cells.

Novel Two-Dimensional Metal-Based π-d Conjugated Nanosheets as Photocatalyst for Nitrogen Reduction Reaction: The First-Principle Investigation.

Photocatalytic nitrogen reduction reaction (NRR) is becoming a promising route for producing green and sustainable ammonia under ambient conditions. However, the development of highly efficient photocatalysts for NRR still remains a grand challenge as a result of the sluggish activation of inert N, the competitive hydrogen evolution reaction (HER), and inadequate photogenerated external potential, which usually cause extremely poor NRR performance and low light utilization efficiency. Herein, on the basis of density functional theory (DFT) computations, we rationally designed a series of two-dimensional (2D) π-d conjugated metal-BN (MBNS) semiconductors.

Lattice-Confined Ir Clusters on Pd Nanosheets with Charge Redistribution for the Hydrogen Oxidation Reaction under Alkaline Conditions.

Electrocatalysts with high activity and long-term stability for the hydrogen oxidation reaction (HOR) under alkaline conditions is still a major challenge for anion exchange membrane fuel cells (AEMFCs). Herein, a heterostructured Ir@Pd electrocatalyst with ultrasmall Ir nanoclusters (NCs) epitaxially confined on Pd nanosheets (NSs) for catalyzing the sluggish alkaline HOR is reported. Apparent charge redistribution occurs across the heterointerface, and both experimental and theoretical results suggest that the electrons transfer from Pd to Ir, which consequently greatly weakens the hydrogen binding on Pd.

Atomic-Level Modulation of the Interface Chemistry of Platinum-Nickel Oxide toward Enhanced Hydrogen Electrocatalysis Kinetics.

Precise manipulation of the interactions between different components represents the frontier of heterostructured electrocatalysts and is crucial to understanding the structure-function relationship. Current studies, however, are quite limited. Here, we report targeted modulation of the atomic-level interface chemistry of Pt/NiO heterostructure via an annealing treatment, which results in substantially enhanced hydrogen electrocatalysis kinetics in alkaline media.

Metal-Organic Framework-Derived Fe-Doped Co Te Embedded in Nitrogen-Doped Carbon Nanotube for Water Splitting.

A rational design is reported of Fe-doped cobalt telluride nanoparticles encapsulated in nitrogen-doped carbon nanotube frameworks (Fe-Co Te @NCNTF) by tellurization of Fe-etched ZIF-67 under a mixed H /Ar atmosphere. Fe-doping was able to effectively modulate the electronic structure of Co Te , increase the reaction activity, and further improve the electrochemical performance. The optimized electrocatalyst exhibited superior hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) performances in an alkaline electrolyte with low overpotentials of 107 and 297 mV with a current density of 10 mA cm , in contrast to the undoped Co Te @NCNTF (165 and 360 mV, respectively).

Three-Dimensional Porous Nitrogen-Doped Carbon Nanosheet with Embedded NiCoS Nanocrystals for Advanced Lithium-Sulfur Batteries.

The shuttle effect of lithium polysulfides (LiS) in electrolyte and the low conductivity of sulfur are the two key hindrances of lithium sulfur (Li-S) batteries. In order to address the two issues, we propose a three-dimensional porous nitrogen-doped carbon nanosheet with embedded NiCoS nanocrystals derived from metal-organic frameworks for the durable-cathode host material in Li-S batteries. Experiments and density functional theory simulations show that the large porosity, robust N-doped carbon framework, and evenly embedded NiCoS nanocrystals with high polarity act as strong "traps" for the immobilization of LiS, which leads to an effective suppressing of the shuttle effect and promotes efficient utilization of sulfur.

In Situ Doping of Nitrogen in <110>-Oriented Bulk 3C-SiC by Halide Laser Chemical Vapour Deposition.

Doping of nitrogen is a promising approach to improve the electrical conductivity of 3C-SiC and allow its application in various fields. N-doped, <110>-oriented 3C-SiC bulks with different doping concentrations were prepared via halide laser chemical vapour deposition (HLCVD) using tetrachlorosilane (SiCl) and methane (CH) as precursors, along with nitrogen (N) as a dopant. We investigated the effect of the volume fraction of nitrogen () on the preferred orientation, microstructure, electrical conductivity (), deposition rate (), and optical transmittance.

MXene Surface Terminations Enable Strong Metal-Support Interactions for Efficient Methanol Oxidation on Palladium.

Efficient catalysis of the methanol oxidation reaction (MOR) greatly determines the widespread implementation of direct methanol fuel cells. Exploring a suitable support for noble metal catalysts with regard to decreasing the mass loading and optimizing the MOR activity remains a key challenge. Herein, we achieve an over 60% activity enhancement of a palladium (Pd) catalyst by introducing a two-dimensional TiCT MXene as the support compared to a commercial Pd/C catalyst.

Extrapolation of high-order correlation energies: the WMS model.

We have developed a new composite model chemistry method called WMS (Wuhan-Minnesota scaling method) with three characteristics: (1) a composite scheme to approximate the complete configuration interaction valence energy with the affordability condition of requiring no calculation more expensive than CCSD(T)/jul-cc-pV(T+d)Z, (2) low-cost methods for the inner-shell correlation contribution and scalar relativistic correction, and (3) accuracy comparable to methods with post-CCSD(T) components. The new method is shown to be accurate for the W4-17 database of 200 atomization energies with an average mean unsigned error (averaged with equal weight over strongly correlated and weakly correlated subsets of the data) of 0.45 kcal mol-1, and the performance/cost ratio of these results compares very favorably to previously available methods.

A 3D Nitrogen-Doped Graphene/TiN Nanowires Composite as a Strong Polysulfide Anchor for Lithium-Sulfur Batteries with Enhanced Rate Performance and High Areal Capacity.

Lithium-sulfur (Li-S) batteries have attracted remarkable attention due to their high theoretical capacity of 1675 mAh g , rich resources, inexpensiveness, and environmental friendliness. However, the practical application of the Li-S battery is hindered by the shuttling of soluble lithium polysulfides (LiPSs) and slow redox reactions. Herein, a 3D nitrogen-doped graphene/titanium nitride nanowires (3DNG/TiN) composite is reported as a freestanding electrode for Li-S batteries.