Promises of MOF-Based and MOF-Derived Materials for Electrocatalytic CO2 Reduction

Electrocatalytic CO2 reduction (ECR) powered by renewable electricity is a promising technology to mitigate carbon emissions and lessen the dependence on fossil fuels toward a carbon-neutral energy cycle. Metal-organic frameworks (MOFs) and their derivatives, due to their excellent intrinsic activity, have emerged as promising materials for the ECR to high-demand products. However, challenges such as unsatisfactory energy efficiency, selectivity, and relatively low production rates hinder their industrial scalability. Here, a comprehensive and critical review is presented that summarizes the state-of-the-art progress in MOF-based and MOF-derived CO2 electroreduction catalysts from design and functionality perspectives. The fundamentals of CO2 reduction reaction (CO2RR) over heterogeneous catalysts, reaction mechanisms, and key challenges faced by ECR are described first to establish a solid foundation for forthcoming in-depth analyses. MOF's building blocks, properties, and shortcomings pertinent to ECR including low conductivity and stability, are systematically discussed. Moreover, comprehensive discussions are provided on MOF-based and MOF-derived catalysts design, fabrication, characterization, and CO2RR activity to pinpoint the intricate structure-property-performance relationship. Finally, promising recommendations are put forward for enhancing MOF electrocatalysts activity, selectivity, and durability. This work may serve as a guideline for developing high-performance MOF-related catalysts for CO2RR, benefiting researchers working in this growing and potentially game-changing area.<br />