Two-dimensional Cu-phenylalanine nanoflakes for efficient and robust CO electroreduction to C products.

The electrocatalytic reduction of CO to multicarbon (C) products is of great importance but still faces challenges. The moderate oxidation state of Cu (Cu) plays a critical role in promoting the C-C coupling, thereby enhancing the Faraday efficiency (FE) for C products. However, Cu active species are unstable during the reaction.

Recycling Sulfur-Poisoned Pd Catalysts via Thermal Atomization for Semi-Hydrogenation of Acetylene.

Palladium catalysts are highly efficient for a variety of chemical industrial processes but are prone to being affected by poisons during practical application. Sulfur is one of the major poisons in Pd-based catalysts. The recycling of deeply poisoned Pd species like Pd sulfides is challenging due to the strong Pd-S bond.

Synergetic Modulation of Electronic Properties of Cobalt Oxide via "Tb" Single Atom for Uphill Urea and Water Electrolysis.

Exploring single-atom (SA) catalysts in hybrid urea-assisted water electrolysis offers a viable alternative to both Hydrogen (H) generation and polluted water treatment. However, the unfavorable electronic stabilization, low SA content, intrinsically slow kinetics, and imbalanced adsorption-desorption steps are the bottleneck for its scale-up implementation. Herein, a rare-earth Terbium single atom (Tb) is topologically stabilized on defect-rich CoO (Tb@d-CoO) by Tb─O co-ordination for urea oxidation reaction (UOR) and H evolution reaction (HER).

Enhanced Magnetic Heating for Efficient Oxygen Evolution Reaction by Pinning Effect of Ferromagnetic/Antiferromagnetic Coupling.

The magnetic heating effect under alternating magnetic fields (AMFs) has recently gained attention in catalysis due to its potential to greatly boost catalytic activities by providing localized heating around magnetic nanoparticles. However, nanoparticles still suffer from low magnetic heating efficiency due to their low magnetic anisotropy and thermal fluctuation, which is a key barrier in the wide application of AMF-assisted catalysis. Herein, by introducing the pinning effect of ferromagnetic/antiferromagnetic (FM/AFM) coupling, NiO/NiOOH (AFM/FM) core-shell nanoparticles exhibit significantly enhanced oxygen evolution reaction activity and resistance to thermal fluctuations under AMF, compared to NiOOH nanoparticles.

Highly Selective CO Electroreduction to Multi-Carbon Alcohols via Amine Modified Copper Nanoparticles at Acidic Conditions.

Electroreduction of CO into multi-carbon (C2+) products (e.g. C2+ alcohols) offers a promising way for CO utilization.

Carbon-Boosted and Nitrogen-Stabilized Isolated Single-Atom Sites for Direct Dehydrogenation of Lower Alkanes.

Lower olefins are widely used in the chemical industry as basic carbon-based feedstocks. Here, we report the catalytic system featuring isolated single-atom sites of iridium (Ir) that can function within the entire temperature range of 300-600 °C and transform alkanes with conversions close to thermodynamics-dictated levels. The high turnover frequency values of the Ir system are comparable to those of homogeneous catalytic reactions.

Defect engineering of a TiO anatase/rutile homojunction accelerating sulfur redox kinetics for high-performance Na-S batteries.

Room-temperature sodium-sulfur (RT Na-S) batteries have the drawbacks of the poor shuttle effect of soluble sodium polysulfides (NaPSs) as well as slow sulfur redox kinetics, which result in poor cycling stability and low capacity, seriously affecting their extensive application. Herein, defect engineering is applied to construct rich oxygen vacancies at the interface of a TiO anatase/rutile homojunction (O-TRA) to enhance sulfur affinity and redox reaction kinetics. Combining structural characterizations with electrochemical analysis reveals that O-TRA well alleviates the shuttle effect of NaPSs and precipitates the deposition and diffusion kinetics of NaS.

Oxygen Coordination Promotes Single-Atom Cu(II)-Catalyzed Azide-Alkyne Click Chemistry without Reducing Agents.

Unique active sites make single-atom (SA) catalysts promising to overcome obstacles in homogeneous catalysis but challenging due to their fixed coordination environment. Click chemistry is restricted by the low activity of more available Cu(II) catalysts without reducing agents. Herein, we develop efficient, O-coordinated SA Cu(II) directly catalyzed click chemistry.

Ruthenium Single Atomic Sites Surrounding the Support Pit with Exceptional Photocatalytic Activity.

Single-metal atomic sites and vacancies can accelerate the transfer of photogenerated electrons and enhance photocatalytic performance in photocatalysis. In this study, a series of nickel hydroxide nanoboards (Ni(OH) NBs) with different loadings of single-atomic Ru sites (w-SA-Ru/Ni(OH)) were synthesized via a photoreduction strategy. In such catalysts, single-atomic Ru sites are anchored to the vacancies surrounding the pits.

Microdrop-confined synthesis and regulation of porous hollow Ir-based catalysts for the mass transfer-enhanced electrolysis of pure water.

Maximally exploiting the active sites of iridium catalysts is essential for building low-cost proton exchange membrane (PEM) electrolyzers for green H production. Herein, we report a novel microdrop-confined fusion/blasting (MCFB) strategy for fabricating porous hollow IrO microspheres (IrO-PHM) by introducing explosive gas mediators from a NaNO/glucose mixture. Moreover, the developed MCFB strategy is demonstrated to be general for synthesizing a series of Ir-based composites, including Ir-Cu, Ir-Ru, Ir-Pt, Ir-Rh, Ir-Pd, and Ir-Cu-Pd and other noble metals such as Rh, Ru, and Pt.

Ligand-assisted formation of mesoporous Zn-N-C to realize superior catalytic activity in solvent-free CO cycloaddition reactions.

Mesoporous nitrogen-doped carbon-anchored single atom Zn was synthesized through etching of ZIF-8 with 1,10-phenanthroline and subsequent pyrolysis based on the Kirkendall effect. The abundant pores and increased surface area promote CO adsorption and mass transfer, thus significantly improving the catalytic activity in solvent-free cycloaddition of epoxides with CO.

Mixed-Dimensional Partial Dealloyed PtCuBi/C as High-Performance Electrocatalysts for Methanol Oxidation with Enhanced CO Tolerance.

Developing efficient electrocatalysts for methanol oxidation reaction (MOR) is crucial in advancing the commercialization of direct methanol fuel cells (DMFCs). Herein, carbon-supported 0D/2D PtCuBi/C (0D/2D PtCuBi/C) catalysts are fabricated through a solvothermal method, followed by a partial electrochemical dealloying process to form a novel mixed-dimensional electrochemically dealloyed PtCuBi/C (0D/2D D-PtCuBi/C) catalysts. Benefiting from distinctive mixed-dimensional structure and composition, the as-obtained 0D/2D D-PtCuBi/C catalysts possess abundant accessible active sites.

Single Atom Iridium Decorated Nickel Alloys Supported on Segregated MoO for Alkaline Water Electrolysis.

Hetero-interface engineering has been widely employed to develop supported multicomponent catalysts for water electrolysis, but it still remains a substantial challenge for supported single atom alloys. Herein a conductive oxide MoO supported Ir Ni single atom alloys (Ir Ni@MoO SAAs) bifunctional electrocatalysts through surface segregation coupled with galvanic replacement reaction, where the Ir atoms are atomically anchored onto the surface of Ni nanoclusters via the Ir-Ni coordination accompanied with electron transfer from Ni to Ir is reported. Benefiting from the unique structure, the Ir Ni@MoO SAAs not only exhibit low overpotential of 48.

Optimizing the Spatial Density of Single Co Sites Molecular Spacing for Facilitating Sustainable Water Oxidation.

Advances in single-atom (-site) catalysts (SACs) provide a new solution of atomic economy and accuracy for designing efficient electrocatalysts. In addition to a precise local coordination environment, controllable spatial active structure and tolerance under harsh operating conditions remain great challenges in the development of SACs. Here, we show a series of molecule-spaced SACs (msSACs) using different acid anhydrides to regulate the spatial density of discrete metal phthalocyanines with single Co sites, which significantly improve the effective active-site numbers and mass transfer, enabling one of the msSACs connected by pyromellitic dianhydride to exhibit an outstanding mass activity of (1.

Endowing Nanoparticles with High Stability on the Hydrogenation Reaction by the Amino Group-Assisted Strategy.

In the field of a heterogeneous industrial catalysis process, the encapsulated structure plays a crucial role in preventing active sites from leaching during the reaction; however, related studies on the strategy to fabricate encapsulated catalysts under control remain rare. Herein, we develop an amino-assisted strategy to construct a highly stable catalyst with core-shell copper nanoparticles (NPs), namely, Cu@NC (NC represents the nitrogen-doped carbon), presenting not only excellent activity but also high durability on the hydrogenation of quinolines even in the large-scale tests, which is very vital in practical application. In contrast, in the absence of the amino group, the Cu NPs were dispersed out of the carbon surface to form Cu/NC, leading to readily lose activity in the recycling tests due to the leaching occurred during the catalytic process.

Modulating adsorbed hydrogen drives electrochemical CO-to-C products.

Electrocatalytic CO reduction is a typical reaction involving two reactants (CO and HO). However, the role of HO dissociation, which provides active *H species to multiple protonation steps, is usually overlooked. Herein, we construct a dual-active sites catalyst comprising atomic Cu sites and Cu nanoparticles supported on N-doped carbon matrix.

p-Block Bismuth Nanoclusters Sites Activated by Atomically Dispersed Bismuth for Tandem Boosting Electrocatalytic Hydrogen Peroxide Production.

Constructing electrocatalysts with p-block elements is generally considered rather challenging owing to their closed d shells. Here for the first time, we present a p-block-element bismuth-based (Bi-based) catalyst with the co-existence of single-atomic Bi sites coordinated with oxygen (O) and sulfur (S) atoms and Bi nanoclusters (Bi ) (collectively denoted as BiOS /Bi ) for the highly selective oxygen reduction reaction (ORR) into hydrogen peroxide (H O ). As a result, BiOS /Bi gives a high H O selectivity of 95 % in rotating ring-disk electrode, and a large current density of 36 mA cm at 0.

Directional and Ultrafast Charge Transfer in Oxygen-Vacancy-Rich ZnO@Single-Atom Cobalt Core-Shell Junction for Photo-Fenton-Like Reaction.

In photosynthesis, solar energy is harvested by photosensitizers, and then, the excited electrons transfer via a Z-Scheme mode to enzymatic catalytic centers to trigger redox reactions. Herein, we constructed a core-shell Z-scheme heterojunction of semiconductor@single-atom catalysts (SACs). The oxygen-vacancy-rich ZnO core and single-atom Co-N sites supported on nitrogen-rich carbon shell (SA-Co-CN) act as the photosensitizer and the enzyme-mimicking active centers, respectively.

Improving CO-to-C Product Electroreduction Efficiency Atomic Lanthanide Dopant-Induced Tensile-Strained CuO Catalysts.

Cu is a promising electrocatalyst in CO reduction reaction (CORR) to high-value C products. However, as important C-C coupling active sites, the Cu species is usually unstable under reduction conditions. How atomic dopants affect the performance of Cu-based catalysts is interesting to be studied.

Oxidation of metallic Cu by supercritical CO and control synthesis of amorphous nano-metal catalysts for CO electroreduction.

Amorphous nano-metal catalysts often exhibit appealing catalytic properties, because the intrinsic linear scaling relationship can be broken. However, accurate control synthesis of amorphous nano-metal catalysts with desired size and morphology is a challenge. In this work, we discover that Cu(0) could be oxidized to amorphous CuO species by supercritical CO.

Modulating the Asymmetric Atomic Interface of Copper Single Atoms for Efficient CO Electroreduction.

Cu single-atom catalysts (Cu SACs) have been considered as promising catalysts for efficient electrocatalytic CO reduction reactions (ECRRs). However, the reports on Cu SACs with an asymmetric atomic interface to obtain CO are few. Herein, we rationally designed two Cu SACs with different asymmetric atomic interfaces to explore their catalytic performance.

Atomically Dispersed Ni-Cu Catalysts for pH-Universal CO Electroreduction.

CO electroreduction is of great significance to reduce CO emissions and complete the carbon cycle. However, the unavoidable carbonate formation and low CO utilization efficiency in neutral or alkaline electrolytes hinder its application at commercial scale. The development of CO reduction under acidic conditions provides a promising strategy, but the inhibition of the hydrogen evolution reaction is difficult.

A Sn-stabilized Cu electrocatalyst toward highly selective CO-to-CO in a wide potential range.

Current techno-economic evaluation manifests that the electrochemical CO reduction reaction (eCORR) to CO is very promising considering its simple two-electron transfer process, minimum cost of electricity, and low separation cost. Herein, we report a Sn-modification strategy that can tune the local electronic structure of Cu with an appropriate valence. The as-prepared catalysts can alter the broad product distribution of Cu-based eCORR to predominantly generate CO.

Interfacial water engineering boosts neutral water reduction.

Hydrogen evolution reaction (HER) in neutral media is of great practical importance for sustainable hydrogen production, but generally suffers from low activities, the cause of which has been a puzzle yet to be solved. Herein, by investigating the synergy between Ru single atoms (RuNC) and RuSe cluster compounds (RuSe) for HER using ab initio molecular dynamics, operando X-ray absorption spectroscopy, and operando surface-enhanced infrared absorption spectroscopy, we establish that the interfacial water governs neutral HER. The rigid interfacial water layer in neutral media would inhibit the transport of HO*/OH* at the electrode/electrolyte interface of RuNC, but the RuSe can promote HO*/OH* transport to increase the number of available HO* on RuNC by disordering the interfacial water network.

Constraining the formation and transport of lunar impact glasses using the ages and chemical compositions of Chang'e-5 glass beads.

Impact glasses found in lunar soils provide a possible window into the impact history of the inner solar system. However, their use for precise reconstruction of this history is limited by an incomplete understanding of the physical mechanisms responsible for their origin and distribution and possible relationships to local and regional geology. Here, we report U-Pb isotopic dates and chemical compositions of impact glasses from the Chang'e-5 soil and quantitative models of impact melt formation and ejection that account for the compositions of these glasses.