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Electrochemical reduction reaction of carbon monoxide (CORR) offers a promising way to manufacture acetic acid directly from gaseous CO and water at mild condition. Herein, we discovered that the graphitic carbon nitride (g‐C3N4) supported Cu nanoparticles (Cu−CN) with the appropriate size showed a high acetate faradaic efficiency of 62.8 % with a partial current density of 188 mA cm−2 in CORR. In situ experimental and density functional theory calculation studies revealed that the Cu/C3N4 interface and metallic Cu surface synergistically promoted CORR into acetic acid. The generation of pivotal intermediate −*CHO is advantage around the Cu/C3N4 interface and migrated *CHO facilitates acetic acid generation on metallic Cu surface with promoted *CHO coverage. Moreover, continuous production of acetic acid aqueous solution was achieved in a porous solid electrolyte reactor, indicating the great potential of Cu−CN catalyst in the industrial application. [ABSTRACT FROM AUTHOR]

Developing electrocatalytic reactions with high‐efficiency can make important contributions to carbon neutrality. However, poor long‐term stability of catalysts is a bottleneck for its practical application. Herein, an "in situ periodic regeneration of catalyst (PR‐C)" strategy is proposed to give long‐term high efficiency of CO2 electroreduction to generate C2+ products over Cu catalyst by applying a positive potential pulse for a short time periodically in the halide‐containing electrolyte. The high Faradaic efficiency (81.2 %) and current density (22.6 mA cm−2) could be maintained completely at least 36 h, while the activity and selectivity decreased continuously without using the PR‐C method. Control experiments and operando characterization demonstrated that the surface structure and oxidation state of Cu could be recovered periodically by the PR‐C method, which was beneficial for CO2 activation and C−C coupling. [ABSTRACT FROM AUTHOR]

Electroreduction of CO2 into valuable fuels and feedstocks offers a promising way for CO2 utilization. However, the commercialization is limited by the low productivity. Here, we report a strategy to enhance the productivity of CO2 electroreduction by improving diffusion of CO2 to the surface of catalysts using porous organic cages (POCs) as an additive. It was noted that the Faradaic efficiency (FE) of C2+ products could reach 76.1 % with a current density of 1.7 A cm−2 when Cu‐nanorod(nr)/CC3 (one of the POCs) was used, which were much higher than that using Cu‐nr. Detailed studies demonstrated that the hydrophobic pores of CC3 can adsorb a large amount of CO2 for the reaction, and the diffusion of CO2 in the CC3 to the nanocatalyst surface is easier than that in the liquid electrolyte. Thus, more CO2 molecules make contact with the nanocatalysts in the presence of CC3, enhancing CO2 reduction and inhibiting generation of H2. [ABSTRACT FROM AUTHOR]

Using renewable electricity to drive CO2 electroreduction is an attractive way to achieve carbon‐neutral energy cycle and produce value‐added chemicals and fuels. As an important platform molecule and clean fuel, methanol requires 6‐electron transfer in the process of CO2 reduction. Currently, CO2 electroreduction to methanol suffers from poor efficiency and low selectivity. Herein, we report the first work to design atomically dispersed Sn site anchored on defective CuO catalysts for CO2 electroreduction to methanol. It exhibits high methanol Faradaic efficiency (FE) of 88.6 % with a current density of 67.0 mA cm−2 and remarkable stability in a H‐cell, which is the highest FE(methanol) with such high current density compared with the results reported to date. The atomic Sn site, adjacent oxygen vacancy and CuO support cooperate very well, leading to higher double‐layer capacitance, larger CO2 adsorption capacity and lower interfacial charge transfer resistance. Operando experiments and density functional theory calculations demonstrate that the catalyst is beneficial for CO2 activation via decreasing the energy barrier of *COOH dissociation to form *CO. The obtained key intermediate *CO is then bound to the Cu species for further reduction, leading to high selectivity toward methanol. [ABSTRACT FROM AUTHOR]

Guided by first‐principles calculations, it was found that Cd single‐atom catalysts (SACs) have excellent performance in activating CO2, and the introduction of axial coordination structure to Cd SACs cannot only further decrease the free energy barrier of CO2 reduction, but also suppress the hydrogen evolution reaction (HER). Based on the above discovery, we designed and synthesized a novel Cd SAC that comprises an optimized CdN4S1 moiety incorporated in a carbon matrix. It was shown that the catalyst exhibited outstanding performance in CO2 electroreduction to CO. The faradaic efficiency (FE) of CO could reach up to 99.7 % with a current density of 182.2 mA cm−2 in a H‐type electrolysis cell, and the turnover frequency (TOF) value could achieve 73000 h−1, which was much higher than that reported to date. This work shows a successful example of how to design highly efficient catalysts guided by theoretical calculations. [ABSTRACT FROM AUTHOR]