Electrocatalytic Reduction of Carbon Dioxide to High-Value Multicarbon Products with Metal–Organic Frameworks and Their Derived Materials

Abstract

The electrocatalytic carbon dioxide reduction reaction (CO 2 RR) holds great potential in promoting carbon neutral through effectively converting CO 2 molecules to useful chemicals and fuels. The high-efficiency electrochemical conversion of CO 2 to single-carbon products has been well realized, while more efforts are needed for the generation of high-value multicarbon products. Metal−organic frameworks (MOFs), featuring porous structures, high chemical tunability, and ultralarge surface area, have attracted increasing attention in the electrochemical CO 2 RR. Herein, we review the recent progress of electrocatalytic CO 2 RR on MOF-based materials toward multicarbon products. First, the structure of MOFs is briefly introduced. Then, the electrocatalytic CO 2 RR performance and the corresponding catalytic mechanism of pristine MOFs (classified according to the kind of organic ligands/linkers) and MOF-derived materials (including metal nanomaterials, single-atom catalysts and nanocomposites) toward the multicarbon product generation are systematically discussed. Finally, critical challenges and potential opportunities are highlighted to inspire the rational design and targeted synthesis of advanced MOF-based materials for high-performance electrocatalytic CO 2 reduction toward multicarbon products.

Defect engineering of two-dimensional materials for advanced energy conversion and storage

“…Recently, 2D metal-organic frameworks (MOFs) have been considered as ideal multifunctional sulfur carriers for advanced Li-S batteries due to their diverse pore structure, rich active metal sites, and large surface area. [426][427][428] Compared to 1D and 3D MOFs, 2D MOFs possess distinct flexible channels and adjustable interfaces for fast electron/ion transfer. [429][430][431] Nevertheless, the organic ligands around the metal sites lead to poor electrocatalytic activities of MOFs.…”

Metal functionalization of two-dimensional nanomaterials for electrochemical carbon dioxide reduction

“…MOFs are a series of crystalline materials with a large surface area, high surface-to-volume ratio, high porosity, tunable structures, and abundant metal active sites. 26,112,113 Here, the metal active sites could be metal ions or clusters. The tunable structures result from the various organic ligands, which usually contain aromatic rings.…”

MOF-derived transition metal-based catalysts for the electrochemical reduction of CO2to CO: a mini review

“…30 Fortunately, the MOF derivatives well inherit the porous structure of MOFs, exhibit the superiorities of higher stability, conductivity, and catalytic activity, and have been widely applied in electrocatalysis including the CO 2 RR. 31,32 Thus, MOF-derived transition metal-based catalysts become a hot spot. For instance, Cu-based MOFs were used as a precursor to synthesize Cu nanoparticles (NPs) for the CO 2 RR.…”