Enhancing CO2 Electroreduction to Multicarbon Products by Modulating the Surface Microenvironment of Electrode with Polyethylene Glycol.

Modulating the surface microenvironment of electrodes stands as a pivotal aspect in enhancing the electrocatalytic performance for CO2 electroreduction. Herein, we propose an innovative approach by incorporating a small amount of linear oligomer, polyethylene glycol (PEG), into Cu2O catalysts during the preparation of the CuPEG electrode. The Faradaic efficiency (FE) toward multicarbon products (C2+) increases from 69.

Switching CO-to-Acetate Electroreduction on Cu Atomic Ensembles.

The electrocatalytic reaction pathway is highly dependent on the intrinsic structure of the catalyst. CO/CO electroreduction has recently emerged as a potential approach for obtaining C products, but it is challenging to achieve high selectivity for a single C product. Herein, we develop a Cu atomic ensemble that satisfies the appropriate site distance and coordination environment required for electrocatalytic CO-to-acetate conversion, which shows outstanding overall performance with an acetate Faradaic efficiency of 70.

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.

Upgrading of nitrate to hydrazine through cascading electrocatalytic ammonia production with controllable N-N coupling.

Nitrogen oxides (NO) play important roles in the nitrogen cycle system and serve as renewable nitrogen sources for the synthesis of value-added chemicals driven by clean electricity. However, it is challenging to achieve selective conversion of NO to multi-nitrogen products (e.g.

Bio-based hydrogels induced by salts.

In this study, we introduce a salt-responsive hydrogel system utilizing a sugar-derived surfactant featuring a polyhydroxy spacer in its headgroup. The inclusion of salts enhances and organizes the intermolecular hydrogen bonding within the hydrophilic region of the polyhydroxy spacer, promoting cross-linking among surfactant molecules.

Switching CO Electroreduction Pathways between Ethylene and Ethanol via Tuning Microenvironment of the Coating on Copper Nanofibers.

Engineering the microenvironment of electrode surface is one of the effective means to tune the reaction pathways in CORR. In this work, we prepared copper nanofibers with conductive polypyrrole coating by polymerization of pyrrole using polyvinyl pyrrolidone (PVP) as template. As a result, the obtained copper nanofibers Cu/CuO/SHNC, exhibited a superhydrophobic surface, which demonstrated very high selectivity for ethanol with a Faraday efficiency (FE) of 66.

Manipulation of Oxygen Species on an Antimony-Modified Copper Surface to Tune the Product Selectivity in CO Electroreduction.

Rational regulation of the electrochemical CO reduction reaction (CORR) pathway to produce desired products is particularly interesting, yet designing economical and robust catalysts is crucial. Here, we report an antimony-modified copper (CuSb) catalyst capable of selectively producing both CO and multicarbon (C) products in the CORR. At a current density of 0.

Urea Synthesis via Coelectrolysis of CO and Nitrate over Heterostructured Cu-Bi Catalysts.

Electrocatalytic coupling of CO and NO to urea is a promising way to mitigate greenhouse gas emissions, reduce waste from industrial processes, and store renewable energy. However, the poor selectivity and activity limit its application due to the multistep process involving diverse reactants and reactions. Herein, we report the first work to design heterostructured Cu-Bi bimetallic catalysts for urea electrosynthesis.

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.

Switching Reaction Pathways of CO Electroreduction by Modulating Cations in the Electrochemical Double Layer.

Tuning the selectivity of CO electroreduction reaction (CORR) solely by changing electrolyte is a very attractive topic. In this study, we conducted CORR in different aqueous electrolytes over bulk metal electrodes. It was discovered that controlled CORR could be achieved by modulating cations in the electrochemical double layer.

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.

Lattice Strain Engineering Boosts CO Electroreduction to C Products.

Regulating the binding effect between the surface of an electrode material and reaction intermediates is essential in highly efficient CO electro-reduction to produce high-value multicarbon (C) compounds. Theoretical study reveals that lattice tensile strain in single-component Cu catalysts can reduce the dipole-dipole repulsion between *CO intermediates and promotes *OH adsorption, and the high *CO and *OH coverage decreases the energy barrier for C-C coupling. In this work, Cu catalysts with varying lattice tensile strain were fabricated by electro-reducing CuO precursors with different crystallinity, without adding any extra components.

CO electrolysis to multi-carbon products in strong acid at ampere-current levels on La-Cu spheres with channels.

Achieving satisfactory multi-carbon (C) products selectivity and current density under acidic condition is a key issue for practical application of electrochemical CO reduction reaction (CORR), but is challenging. Herein, we demonstrate that combining microenvironment modulation by porous channel structure and intrinsic catalytic activity enhancement via doping effect could promote efficient CORR toward C products in acidic electrolyte (pH ≤ 1). The La-doped Cu hollow sphere with channels exhibits a C products Faradaic efficiency (FE) of 86.

Steering the Reaction Pathway of CO Electroreduction by Tuning the Coordination Number of Copper Catalysts.

Cu-based catalysts are optimal for the electroreduction of CO to generate hydrocarbon products. However, controlling product distribution remains a challenging topic. The theoretical investigations have revealed that the coordination number (CN) of Cu considerably influences the adsorption energy of *CO intermediates, thereby affecting the reaction pathway.

Synthesis of Hydroxylamine via Ketone-Mediated Nitrate Electroreduction.

Hydroxylamine (HA, NHOH) is a critical feedstock in the production of various chemicals and materials, and its efficient and sustainable synthesis is of great importance. Electroreduction of nitrate on Cu-based catalysts has emerged as a promising approach for green ammonia (NH) production, but the electrosynthesis of HA remains challenging due to overreduction of HA to NH. Herein, we report the first work on ketone-mediated HA synthesis using nitrate in water.

Highly Efficient Electrosynthesis of Glycine over an Atomically Dispersed Iron Catalyst.

Glycine is a nonessential amino acid that plays a vital role in various biological activities. However, the conventional synthesis of glycine requires sophisticated procedures or toxic feedstocks. Herein, we report an electrochemical pathway for glycine synthesis via the reductive coupling of oxalic acid and nitrate or nitrogen oxides over atomically dispersed Fe-N-C catalysts.

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.

Rare-earth Element-based Electrocatalysts Designed for CO Electro-reduction.

Electrochemical CO reduction presents a promising approach for synthesizing fuels and chemical feedstocks using renewable energy sources. Although significant advancements have been made in the design of catalysts for CO reduction reaction (CORR) in recent years, the linear scaling relationship of key intermediates, selectivity, stability, and economical efficiency are still required to be improved. Rare earth (RE) elements, recognized as pivotal components in various industrial applications, have been widely used in catalysis due to their unique properties such as redox characteristics, orbital structure, oxygen affinity, large ion radius, and electronic configuration.

Selective and Efficient CO Electroreduction to Formate on Copper Electrodes Modified by Cationic Gemini Surfactants.

Electroreduction of CO into valuable chemicals and fuels is a promising strategy to mitigate energy and environmental problems. However, it usually suffers from unsatisfactory selectivity for a single product and inadequate electrochemical stability. Herein, we report the first work to use cationic Gemini surfactants as modifiers to boost CO electroreduction to formate.

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.

Selective Electrochemical Oxidation of Benzylic C-H to Benzylic Alcohols with the Aid of Imidazolium Radical Mediators.

Selective oxidation of benzylic C-H to benzylic alcohols is a well-known challenge in the chemical community since benzylic C-H is more prone to be overoxidized to benzylic ketones. In this work, we report the highly selective electro-oxidation of benzylic C-H to benzylic alcohols in an undivided cell in ionic liquid-based solution. As an example, the selectivity toward xanthydrol could be as high as 95.

Switching between C Products and CH in CO Electrolysis by Tuning the Composition and Structure of Rare-Earth/Copper Catalysts.

Rational regulation of the reaction pathway to produce the desired products is one of the most significant challenges in the electrochemical CO reduction reaction (CORR). Herein, we designed a series of rare-earth Cu catalysts with mixed phases. It was found that the products could be switched from C to CH by tuning the composition and structure of the catalysts.

Oxophilicity-Controlled CO Electroreduction to C Alcohols over Lewis Acid Metal-Doped Cu Catalysts.

Cu-based electrocatalysts have great potential for facilitating CO reduction to produce energy-intensive fuels and chemicals. However, it remains challenging to obtain high product selectivity due to the inevitable strong competition among various pathways. Here, we propose a strategy to regulate the adsorption of oxygen-associated active species on Cu by introducing an oxophilic metal, which can effectively improve the selectivity of C alcohols.

Boosting Electrocatalytic Nitrate-to-Ammonia via Tuning of N-Intermediate Adsorption on a Zn-Cu Catalyst.

The renewable-energy-powered electroreduction of nitrate (NO ) to ammonia (NH ) has garnered significant interest as an eco-friendly and promising substitute for the Haber-Bosch process. However, the sluggish kinetics hinders its application at a large scale. Herein, we first calculated the N-containing species (*NO and *NO ) binding energy and the free energy of the hydrogen evolution reaction over Cu with different metal dopants, and it was shown that Zn was a promising candidate.

Highly efficient zinc electrode prepared by electro-deposition in a salt-induced pre-phase separation region solution.

Efficient electrode design is crucial for the electrochemical reduction of CO to produce valuable chemicals. The solution used for the preparation of electrodes can affect their overall properties, which in turn determine the reaction efficiency. In this work, we report that transition metal salts could induce the change of two-phase ionic liquid/ethanol mixture into miscible one phase.