Wen-Jun Xie

Electrochemical CO ₂ reduction to ethylene requires Cu sites that simultaneously enrich carbon intermediates, promote C–C coupling, and suppress hydrogen evolution at high current density. Heteroatom doping is widely used to tune Cu‐based catalysts. However, conventional single‐dopant strategies typically impose either electron donation or electron withdrawal, limiting their ability to balance these coupled interfacial processes. Herein, a Y single‐atom and Cl co‐modified Cu ₂ O catalyst (Y _0.19 ‐Cu ₂ O‐Cl) is developed to create lattice‐confined donor–acceptor pairs for bidirectionally modulating Cu electronic states. Formation energy calculations prove the favorable thermodynamics of Y–Cl co‐doping configuration. HAADF‐STEM, XPS, and XAS support atomically dispersed Y, retained Cl‐containing species, and coupled charge redistribution within the Cu ₂ O‐derived matrix. In situ Raman/ATR‐SEIRAS and density functional theory calculations reveal that Y favors *CO enrichment, whereas Cl modifies hydrogen adsorption; the two dopants synergistically regulate Cu ⁺ active sites and lower the C–C coupling energy barrier from 0.75 to 0.39 eV. Consequently, the catalyst achieves an FE _C2H4 of 62.5% at 656.6 mA cm ⁻² and maintains higher ethylene selectivity than the singly modified controls, establishing donor–acceptor electronic pairing as a strategy for industrial‐grade current densities for CO ₂ electroreduction.

The electrochemical reduction of CO ₂ to ethylene (C ₂ H ₄ ) offers an attractive route for carbon valorization to bulk chemicals by using sustainable energy. However, its practical application is hindered by sluggish C─C coupling kinetics and poor C ₂ H ₄ selectivity at high current densities. While hollow‐structured Cu ₂ O can enrich *CO intermediates, further enhancing C─C coupling on such structures remains challenging. In this context, we developed a ligand modulation strategy to tailor the catalytic properties of double‐shell hollow Cu ₂ O by anchoring π‐conjugated 1,4‐bis(4‐pyridyl)benzene (BPB) onto the Cu ₂ O surface via Cu─N coordination bonds. Concentration‑dependent studies identify 10 mM BPB as the optimal balance between electronic modulation and surface accessibility. In situ ATR‑SEIRAS and density functional theory calculations collectively demonstrate that the electron donation from pyridinic N donors to Cu ⁺ sites promotes CO ₂ activation and *COOH formation, while the strengthened *CO adsorption is expected to facilitate C─C coupling. As a result, the optimized Cu ₂ O‐BPB‐10 catalyst delivered a C ₂ H ₄ Faradaic efficiency (FE) of 61.6% and a total C ₂₊ FE of 85.1% at a current density of 600 mA cm ⁻² . This work provides a facile and versatile ligand engineering strategy for designing high‐performance Cu‐based catalysts for practical electrochemical CO ₂ reduction under industrially relevant conditions.

With H ₂ O ₂ as the oxidant, the bifunctional ionic liquid facilitated a two-step process for the synthesis of cyclic carbonate directly from olefins and CO ₂ in 90% yield obviating the need for transition metals.

An earth-abundant nickel-catalyzed Heck type cyclization/carboxylation of iodoarene-tethered propargyl ethers using CO₂ as the C₁ source was developed herein. This protocol affords a series of exocyclic alkenyl carboxylic acids bearing a dihydrobenzofuran scaffold with exclusive syn-selectivity. Gram-scale experiments demonstrate the scalability of this transformation, and the products undergo further functionalization through aromatization or esterification with eugenol, indicating potential application.

The electrochemical conversion of CO₂ into value-added chemicals represents a promising strategy for sustainable synthesis. Herein, we report a novel electrochemical carboxylative cyclization of propargylamines with CO₂ to access exocyclic iodo-carboxyl-vinylene 2-oxazolidinones bearing two CO₂ moieties by using tetraethylammonium iodide (Et₄NI) as both the electrolyte and the "iodine source", which enables the one-pot construction of C-O, C-C, C-N, and C-I bonds. The protocol proceeds under mild conditions and accommodates a broad range of substrates, providing access to functionalized 2-oxazolidinones with high structural complexity.

Herein, we report an electrochemical protocol for the dicarboxylation of aryl alkynes using CO₂. With a graphite rod as the cathode and Al as the sacrificial anode, a series of valuable butenedioic acids are obtained in moderate to excellent yields with an E/Z ratio up to 50:1. This method features high E-selectivity, high step and atom economy, easy scalability, and a nice substrate scope, which renders it appealing for promising applications in organic synthesis and materials chemistry.

A novel member of the metal porphyrinoids family, cobalt 5,15-diazaporphyrin, as a molecular catalyst immobilized onto carbon nanotubes, was developed for highly efficient ECO ₂ R to CO.

Electroreduction of carbon dioxide (CO ₂ ) or carbon monoxide (CO) toward C ₂₊ hydrocarbons such as ethylene, ethanol, acetate and propanol represents a promising approach toward carbon-negative electrosynthesis of chemicals. Fundamental understanding of the carbon─carbon (C-C) coupling mechanisms in these electrocatalytic processes is the key to the design and development of electrochemical systems at high energy and carbon conversion efficiencies. Here, we report the investigation of CO electreduction on single-atom copper (Cu) electrocatalysts. Atomically dispersed Cu is coordinated on a carbon nitride substrate to form high-density copper─nitrogen moieties. Chemisorption, electrocatalytic, and computational studies are combined to probe the catalytic mechanisms. Unlike the Langmuir-Hinshelwood mechanism known for copper metal surfaces, the confinement of CO adsorption on the single-copper-atom sites enables an Eley-Rideal type of C-C coupling between adsorbed (*CO) and gaseous [CO(g)] carbon moxide molecules. The isolated Cu sites also selectively stabilize the key reaction intermediates determining the bifurcation of reaction pathways toward different C ₂₊ products.