Converting CO2 into value-added products by photocatalysis, electrocatalysis, and photoelectrocatalysis is a promising method to alleviate the global environmental problems and energy crisis. Among the semiconductor materials applied in CO2 catalytic reduction, Cu2 O has the advantages of abundant reserves, low price and environmental friendliness. Moreover, Cu2 O has unique adsorption and activation properties for CO2 , which is conducive to the generation of C2+ products through CC coupling. This review introduces the basic principles of CO2 reduction and summarizes the pathways for the generation of C1 , C2 , and C2+ products. The factors affecting CO2 reduction performance are further discussed from the perspective of the reaction environment, medium, and novel reactor design. Then, the properties of Cu2 O-based catalysts in CO2 reduction are summarized and several optimization strategies to enhance their stability and redox capacity are discussed. Subsequently, the application of Cu2 O-based catalysts in photocatalytic, electrocatalytic, and photoelectrocatalytic CO2 reduction is described. Finally, the opportunities, challenges and several research directions of Cu2 O-based catalysts in the field of CO2 catalytic reduction are presented, which is guidance for its wide application in the energy and environmental fields is provided.

Converting CO2 into Value-Added Products by Cu2 O-Based Catalysts: From Photocatalysis, Electrocatalysis to Photoelectrocatalysis.

Photoelectrochemical (PEC) water splitting is an appealing approach for "green" hydrogen generation. The natural p-type semiconductor of Cu2O is one of the most promising photocathode candidates for direct hydrogen generation. However, the Cu2O-based photocathodes still suffer severe self-photo-corrosion and fast surface electron-hole recombination issues. Herein, we propose a facile in-situ encapsulation strategy to protect Cu2O with hydrogen-substituted graphdiyne (HsGDY) and promote water reduction performance. The HsGDY encapsulated Cu2O nanowires (HsGDY@Cu2O NWs) photocathode demonstrates a high photocurrent density of -12.88 mA cm-2 at 0 V versus the reversible hydrogen electrode under 1 sun illumination, approaching to the theoretical value of Cu2O. The HsGDY@Cu2O NWs photocathode as well as presents excellent stability and contributes an impressive hydrogen generation rate of 218.2 ± 11.3 μmol h-1cm-2, which value has been further magnified to 861.1 ± 24.8 μmol h-1cm-2 under illumination of concentrated solar light. The in-situ encapsulation strategy opens an avenue for rational design photocathodes for efficient and stable PEC water reduction. 

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Hydrogen-substituted graphdiyne encapsulated cuprous oxide photocathode for efficient and stable photoelectrochemical water reduction

The electrochemical reduction of carbon dioxide into multi‐carbon products (C2+) using renewably generated electricity provides a promising pathway for energy and environmental sustainability. Various oxide‐derived copper (OD‐Cu) catalysts have been showcased, but still require high overpotential to drive C2+ production owing to sluggish carbon–carbon bond formation and low CO intermediate (*CO) coverage. Here, the dilemma is circumvented by elaborately devising the OD‐Cu morphology. First, computational studies propose a hollow and hierarchical OD‐Cu microstructure that can generate a core–shell microenvironment to inhibit CO evolution and accelerate *CO dimerization via intermediate confinement and electric field enhancement, thereby boosting C2+ generation. Experimentally, the designed nanoarchitectures are synthesized through a heteroseed‐induced approach followed by electrochemical activation. In situ spectroscopic studies further elaborate correlation between *CO dimerization and designed architectures. Remarkably, the hierarchical OD‐Cu manifests morphology‐dependent selectivity of CO2 reduction, giving a C2+ Faradaic efficiency of 75.6% at a considerably positive potential of −0.55 V versus reversible hydrogen electrode.

Hollow Hierarchical Cu2O‐Derived Electrocatalysts Steering CO2 Reduction to Multi‐Carbon Chemicals at Low Overpotentials

Cu-based CO2 electrochemical reduction (CO2ER) is promising for reducing greenhouse gas emission and producing high-value multicarbon (C2+) chemicals and fuels. Unfortunately, the C2+ selectivity is still quite low. In this work, well-defined [email protected]2O core–shell nanospheres with time-dependent evolution of phase composition, crystallinity and morphology were specifically designed by a facile chemically induced self-transformation strategy. A maximum C2+ Faradaic efficiency (FE) exceeding 79%, including FEC2H4 reaching 44%, was achieved using phase-engineered [email protected]2O nanospheres. Based on the temperature-programmed desorption analyses and in-situ Raman spectroscopy, the adsorption behaviors of both CO2 reactant and *CO intermediate can be synergistically tuned by phase engineering of [email protected]2O nanospheres: Cu2O shell enhances *CO2 and *CO adsorption coverage, while porous Cu core concentrate and strengthens *CO intermediates for subsequent CO-CO coupling towards C2+ products. This work will shed new light on the phase engineering of Cu-based tandem electrocatalysts for tuning CO2/CO-catalyst interaction and modulating CO2ER processes and selectivity. 

Phase engineering of Cu@Cu2O core-shell nanospheres for boosting tandem electrochemical CO2 reduction to C2+ products

The electrocatalytic reduction reaction of nitrate (NO 

Cu/CuxO/Graphdiyne Tandem Catalyst for Efficient Electrocatalytic Nitrate Reduction to Ammonia

Electron transfer in Cu/Cu2O generated by disproportionation promoting efficient CO2 photoreduction

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Electron transfer in Cu/Cu2O generated by disproportionation promoting efficient CO2 photoreduction