Selective hydrogenolysis of the Csp-O bond in the furan ring using hydride-proton pairs derived from hydrogen spillover.

Selective hydrogenolysis of biomass-derived furanic compounds is a promising approach for synthesizing aliphatic polyols by opening the furan ring. However, there remains a significant need for highly efficient catalysts that selectively target the Csp-O bond in the furan ring, as well as for a deeper understanding of the fundamental atomistic mechanisms behind these reactions. In this study, we present the use of Pt-Fe bimetallic catalysts supported on layered double hydroxides [PtFe /LDH] for the hydrogenolysis of furanic compounds into aliphatic alcohols, achieving over 90% selectivity toward diols and triols.

Atomically dispersed cobalt catalysts for tandem synthesis of primary benzylamines from oxidized β-O-4 segments.

This work presents an innovative approach focusing on fine-tuning the coordination environment of atomically dispersed cobalt catalysts for tandem synthesis of primary benzylamines from oxidized lignin model compounds. By meticulously regulating the Co-N coordination environment, the activity of these catalysts in the hydrogenolysis and reductive amination reactions was effectively controlled. Notably, our study demonstrates that, in contrast to cobalt nanoparticle catalysts, atomically dispersed cobalt catalysts exhibit precise control of the sequence of hydrogenolysis and reductive amination reactions.

Electrocatalysis in deep eutectic solvents: from fundamental properties to applications.

Electrocatalysis stands out as a promising avenue for synthesizing high-value products with minimal environmental footprint, aligning with the imperative for sustainable energy solutions. Deep eutectic solvents (DESs), renowned for their eco-friendly, safe, and cost-effective nature, present myriad advantages, including extensive opportunities for material innovation and utilization as reaction media in electrocatalysis. This review initiates with an exposition on the distinctive features of DESs, progressing to explore their applications as solvents in electrocatalyst synthesis and electrocatalysis.

Enhancing C product selectivity in CO electroreduction by enriching intermediates over carbon-based nanoreactors.

Electrochemical CO reduction reaction (CORR) to multicarbon (C) products faces challenges of unsatisfactory selectivity and stability. Guided by finite element method (FEM) simulation, a nanoreactor with cavity structure can facilitate C-C coupling by enriching *CO intermediates, thus enhancing the selectivity of C products. We designed a stable carbon-based nanoreactor with cavity structure and Cu active sites.

Electrocatalytic functional group conversion-based carbon resource upgrading.

The conversions of carbon resources, such as alcohols, aldehydes/ketones, and ethers, have been being one of the hottest topics most recently for the goal of carbon neutralization. The emerging electrocatalytic upgrading has been regarded as a promising strategy aiming to convert carbon resources into value-added chemicals. Although exciting progress has been made and reviewed recently in this area by mostly focusing on the explorations of valuable anodic oxidation or cathodic reduction reactions individually, however, the reaction rules of these reactions are still missing, and how to purposely find or rationally design novel but efficient reactions in batches is still challenging.

Efficient C-N coupling for urea electrosynthesis on defective CoO with dual-functional sites.

Urea electrosynthesis under ambient conditions is emerging as a promising alternative to conventional synthetic protocols. However, the weak binding of reactants/intermediates on the catalyst surface induces multiple competing pathways, hindering efficient urea production. Herein, we report the synthesis of defective CoO catalysts that integrate dual-functional sites for urea production from CO and nitrite.

Optimizing copper nanoparticles with a carbon shell for enhanced electrochemical CO reduction to ethanol.

The electrochemical reduction of carbon dioxide (CORR) holds great promise for sustainable energy utilization and combating global warming. However, progress has been impeded by challenges in developing stable electrocatalysts that can steer the reaction toward specific products. This study proposes a carbon shell coating protection strategy by an efficient and straightforward approach to prevent electrocatalyst reconstruction during the CORR.

Integration of plasma and electrocatalysis to synthesize cyclohexanone oxime under ambient conditions using air as a nitrogen source.

Direct fixation of N to N-containing value-added chemicals is a promising pathway for sustainable chemical manufacturing. There is extensive demand for cyclohexanone oxime because it is the essential feedstock of Nylon 6. Currently, cyclohexanone oxime is synthesized under harsh conditions that consume a considerable amount of energy.

Nickel-catalysed asymmetric hydromonofluoromethylation of 1,3-enynes for enantioselective construction of monofluoromethyl-tethered chiral allenes.

An unprecedented nickel-catalysed enantioselective hydromonofluoromethylation of 1,3-enynes is developed, allowing the diverse access to monofluoromethyl-tethered axially chiral allenes, including the challenging deuterated monofluoromethyl (CDF)-tethered ones that are otherwise inaccessible. It represents the first asymmetric 1,4-hydrofunctionalization of 1,3-enynes using low-cost asymmetric nickel catalysis, thus opening a new avenue for the activation of 1,3-enynes in reaction development. The utility is further verified by its broad substrate scope, good functionality tolerance, mild conditions, and diversified product elaborations toward other valuable fluorinated structures.

Ultra-fast synthesis of three-dimensional porous Cu/Zn heterostructures for enhanced carbon dioxide electroreduction.

The construction of metal hetero-interfaces has great potential in the application of electro-catalytic carbon dioxide reduction (ECR). Herein, we report a fast, efficient, and simple electrodeposition strategy for synthesizing three-dimensional (3D) porous Cu/Zn heterostructures using the hydrogen bubble template method. When the deposition was carried out at -1.

The construction of a biomass component interaction model based on research into the hydrothermal liquefaction of sewage sludge.

Sewage sludge (SS), a hazardous solid waste with a high water and pollutant content, should be disposed of correctly. Hydrothermal liquefaction (HTL) shows tremendous potential to treat organic matter with substantial water content like SS. In this paper, we examined the impact of key factors on the characteristics and yield of bio-oil during HTL of SS.

Composite polymer electrolytes with ionic liquid grafted-Laponite for dendrite-free all-solid-state lithium metal batteries.

Composite polymer electrolytes (CPEs) with high ionic conductivity and favorable electrolyte/electrode interfacial compatibility are promising alternatives to liquid electrolytes. However, severe parasitic reactions in the Li/electrolyte interface and the air-unstable inorganic fillers have hindered their industrial applications. Herein, surface-edge opposite charged Laponite (LAP) multilayer particles with high air stability were grafted with imidazole ionic liquid (IL-TFSI) to enhance the thermal, mechanical, and electrochemical performances of polyethylene oxide (PEO)-based CPEs.

Enantioselective total syntheses of six natural and two proposed meroterpenoids from .

The first enantioselective total syntheses of six natural and two proposed meroterpenoids isolated from have been achieved in 7-9 steps from 2-methylcyclohexanone. The current synthetic approaches feature a high level of synthetic flexibility, stereodivergent fashion and short synthetic route, thereby providing a potential platform for the preparation of numerous this-type meroterpenoids and their -natural products.

Machine learning based implicit solvent model for aqueous-solution alanine dipeptide molecular dynamics simulations.

Inspired by the recent work from Noé and coworkers on the development of machine learning based implicit solvent model for the simulation of solvated peptides [Chen , , 2021, , 084101], here we report another investigation of the possibility of using machine learning (ML) techniques to "derive" an implicit solvent model directly from explicit solvent molecular dynamics (MD) simulations. For alanine dipeptide, a machine learning potential (MLP) based on the DeepPot-SE representation of the molecule was trained to capture its interactions with its average solvent environment configuration (ASEC). The predicted forces on the solute deviated only by an RMSD of 0.

Nickel-catalyzed regio- and enantio-selective Markovnikov hydromonofluoroalkylation of 1,3-dienes.

A highly enantio- and regio-selective Markovnikov hydromonofluoro(methyl)alkylation of 1,3-dienes was developed using redox-neutral nickel catalysis. It provided a facile strategy to construct diverse monofluoromethyl- or monofluoroalkyl-containing chiral allylic molecules. Notably, this represents the first catalytic asymmetric Markovnikov hydrofluoroalkylation of olefins.

Strategic design of Fe and N co-doped hierarchically porous carbon as superior ORR catalyst: from the perspective of nanoarchitectonics.

In this study, we present microporous carbon (MPC), hollow microporous carbon (HMC) and hierarchically porous carbon (HPC) to demonstrate the importance of strategical designing of nanoarchitectures in achieving advanced catalyst (or electrode) materials, especially in the context of oxygen reduction reaction (ORR). Based on the electrochemical impedance spectroscopy and ORR studies, we identify a marked structural effect depending on the porosity. Specifically, mesopores are found to have the most profound influence by significantly improving electrochemical wettability and accessibility.

Selective desaturation of amides: a direct approach to enamides.

C(sp)-H bond desaturation has been an attractive strategy in organic synthesis. Enamides are important structural fragments in pharmaceuticals and versatile synthons in organic synthesis. However, the dehydrogenation of amides usually occurs on the acyl side benefitting from enolate chemistry like the desaturation of ketones and esters.

Nanoparticles and single atoms of cobalt synergistically enabled low-temperature reductive amination of carbonyl compounds.

Low-temperature and selective reductive amination of carbonyl compounds is a highly promising approach to access primary amines. However, it remains a great challenge to conduct this attractive route efficiently over earth-abundant metal-based catalysts. Herein, we designed several Co-based catalysts (denoted as Co@C-N(), where represents the pyrolysis temperature) by the pyrolysis of the metal-organic framework ZIF-67 at different temperatures.

Enhancing CO electroreduction to CH over Cu nanoparticles supported on N-doped carbon.

The electroreduction of CO to CH has attracted extensive attention. However, it is still a challenge to achieve high current density and faradaic efficiency (FE) for producing CH because the reaction involves eight electrons and four protons. In this work, we designed Cu nanoparticles supported on N-doped carbon (Cu-np/NC).

Preparation of trimetallic electrocatalysts by one-step co-electrodeposition and efficient CO reduction to ethylene.

Use of multi-metallic catalysts to enhance reactions is an interesting research area, which has attracted much attention. In this work, we carried out the first work to prepare trimetallic electrocatalysts by a one-step co-electrodeposition process. A series of Cu-X-Y (X and Y denote different metals) catalysts were fabricated using this method.

Understanding of chiral site-dependent enantioselective identification on a plasmon-free semiconductor based SERS substrate.

Chiral differentiation is an important topic in diverse fields ranging from pharmaceutics to chiral synthesis. The improvement of sensitivity and the elucidation of the mechanism of chiral recognition are still the two main challenges. Herein, a plasmon-free semiconductive surface-enhanced Raman spectroscopy (SERS) substrate with sensitive chiral recognition ability is proposed for the discrimination of enantiomers.

Selective photocatalytic aerobic oxidation of methane into carbon monoxide over Ag/AgCl@SiO.

Design of active catalysts for chemical utilization of methane under mild conditions is of great importance, but remains a challenging task. Here, we prepared a Ag/AgCl with SiO coating (Ag/AgCl@SiO) photocatalyst for methane oxidation to carbon monoxide. High carbon monoxide production (2.

The construction of a two-dimensional organic-inorganic hybrid double perovskite ferroelastic with a high and narrow band gap.

Two-dimensional (2D) hybrid double perovskites have attracted extensive research interest for their fascinating physical properties, such as ferroelectricity, X-ray detection, light response and so on. In addition, ferroelastics, as an important branch of ferroic materials, exhibits wide prospects in mechanical switches, shape memory and templating electronic nanostructures. Here, we designed a 2D phase-transition double perovskite ferroelastic through a structurally progressive strategy.

Nitrogen-doped mesoporous carbon supported CuSb for electroreduction of CO.

The construction of an efficient catalyst for electrocatalytic reduction of CO to high value-added fuels has received extensive attention. Herein, nitrogen-doped mesoporous carbon (NMC) was used to support CuSb to prepare a series of materials for electrocatalytic reduction of CO to CH. The catalytic activity of the composites was significantly improved compared with that of Cu/NMC.