Rapidly increasing atmospheric CO2 concentrations threaten human society, the natural environment, and the synergy between the two. In order to ameliorate the CO2 problem, carbon capture and conversion techniques have been proposed. Metal–organic framework (MOF)-based materials, a relatively new class of porous materials with unique structural features, high surface areas, chemical tunability and stability, have been extensively studied with respect to their applicability to such techniques. Recently, it has become apparent that the CO2 capture capabilities of MOF-based materials significantly boost their potential toward CO2 conversion. Furthermore, MOF-based materials’ well-defined structures greatly facilitate the understanding of structure–property relationships and their roles in CO2 capture and conversion. In this review, we provide a comprehensive account of significant progress in the design and synthesis of MOF-based materials, including MOFs, MOF composites and MOF derivatives, and their application to carbon capture and conversion. Special emphases on the relationships between CO2 capture capacities of MOF-based materials and their catalytic CO2 conversion performances are discussed.

Carbon capture and conversion using metal–organic frameworks and MOF-based materials

Solar energy is an alternative, sustainable energy source for mankind. Finding a convenient way to convert sunlight energy into chemical energy is a key step towards realizing large-scale solar energy utilization. Owing to their structural regularity and synthetic tunability, metal–organic frameworks (MOFs) provide an interesting platform to hierarchically organize light-harvesting antennae and catalytic centers to achieve solar energy conversion. Such photo-driven catalytic processes not only play a critical role in the solar to chemical energy conversion scheme, but also provide a novel methodology for the synthesis of fine chemicals. In this review, we summarize the fundamental principles of energy transfer and photocatalysis and provide an overview of the latest progress in energy transfer, light-harvesting, photocatalytic proton and CO2 reduction, and water oxidation using MOFs. The applications of MOFs in organic photocatalysis and degradation of model organic pollutants are also discussed.

Metal–organic frameworks for artificial photosynthesis and photocatalysis

Photoreduction of CO2 into sustainable and green solar fuels is generally believed to be an appealing solution to simultaneously overcome both environmental problems and energy crisis. The low selectivity of challenging multi-electron CO2 photoreduction reactions makes it one of the holy grails in heterogeneous photocatalysis. This Review highlights the important roles of cocatalysts in selective photocatalytic CO2 reduction into solar fuels using semiconductor catalysts. A special emphasis in this review is placed on the key role, design considerations and modification strategies of cocatalysts for CO2 photoreduction. Various cocatalysts, such as the biomimetic, metal-based, metal-free, and multifunctional ones, and their selectivity for CO2 photoreduction are summarized and discussed, along with the recent advances in this area. This Review provides useful information for the design of highly selective cocatalysts for photo(electro)reduction and electroreduction of CO2 and complements the existing reviews on various semiconductor photocatalysts.

Cocatalysts for Selective Photoreduction of CO2 into Solar Fuels.

Metal–organic frameworks (MOFs) are porous crystalline materials constructed from metal ions or clusters and multidentate organic ligands. Recently, the use of MOFs or MOF composites as catalysts for synergistic catalysis and tandem reactions has attracted increasing attention due to their tunable open metal centres, functional organic linkers, and active guest species in their pores. In this review, the applications of MOFs with multiple active sites in synergistic organic catalysis, photocatalysis and tandem reactions are discussed. These multifunctional MOFs can be categorized by the type of active centre as follows: (i) open metal centres and functional organic linkers in the MOF structure, (ii) active guest sites in the pores and active sites in the MOF structure, and (iii) bimetallic nanoparticles (NPs) on MOF supports. The types of synergistic catalysis and tandem reactions promoted by multifunctional MOFs and their proposed mechanisms are presented in detail. Here, catalytic MOFs with a single type of active site and MOFs that only serve as supports to enhance substrate adsorption are not discussed.

Multifunctional metal–organic framework catalysts: synergistic catalysis and tandem reactions

Large amounts of anthropogenic CO2 emissions associated with increased fossil fuel consumption have led to global warming and an energy crisis. The photocatalytic reduction of CO2 into solar fuels such as methane or methanol is believed to be one of the best methods to address these two problems. In addition to light harvesting and charge separation, the adsorption/activation and reduction of CO2 on the surface of heterogeneous catalysts remain a scientifically critical challenge, which greatly limits the overall photoconversion efficiency and selectivity of CO2 reduction. This review describes recent advances in the fundamental understanding of CO2 photoreduction on the surface of heterogeneous catalysts and particularly provides an overview of enhancing the adsorption/activation of CO2 molecules. The reaction mechanism and pathways of CO2 reduction as well as their dependent factors are also analyzed and discussed, which is expected to enable an increase in the overall efficiency of CO2 reduction through minimizing the reaction barriers and controlling the selectivity towards the desired products. The challenges and perspectives of CO2 photoreduction over heterogeneous catalysts are presented as well.

CO2 photo-reduction: insights into CO2 activation and reaction on surfaces of photocatalysts

Metal-organic frameworks (MOFs) have shown great promise for CO2 capture and storage. However, the operation of chemical redox functions of framework substan- ces and organic CO2-trapping entities which are spatially linked together to catalyze CO2 conversion has had much less attention. Reported herein is a cobalt-containing zeolitic imidazolate framework (Co-ZIF-9) which serves as a robust MOF cocatalyst to reduce CO2 by cooperating with a ruthe- nium-based photosensitizer. The catalytic turnover number of Co-ZIF-9 was about 450 within 2.5 hours under mild reaction conditions, while still keeping its original reactivity during prolonged operation. The conversion of CO2 into chemical feedstocks has attracted enormous attention owing to the increasing concern with global energy and environmental problems. (1) The light- stimulated CO2 conversion promises the utilization of solar energy to fulfill a vital mission of artificial photosynthesis, which usually exploits dyes, semiconductors, electron medi- ators, and desirable coupling to CO2 activators. (2) A great deal of effort has therefore been devoted to developing light harvesters, electron-transport carriers, CO2 activators, and their integration into a chemical system for CO2 reduction. (3) Transition-metal ions of multiple redox states and organic ligands are indispensable for creating electron-transport chains, which cooperate with light harvesters and CO2 activators, to accelerate the multielectron reduction of CO2 coupled to a proton flux so as to avoid the formation of high- energy intermediates. Cobalt, nickel, and copper ions/com- plexes have been demonstrated to act as cocatalysts by promoting the kinetics of both charge-separation and surface reaction for CO2 photoreduction. (4)

Cobalt Imidazolate Metal–Organic Frameworks Photosplit CO 2 under Mild Reaction Conditions

Innenrücktitelbild: Cobalt Imidazolate Metal-Organic Frameworks Photosplit CO2under Mild Reaction Conditions (Angew. Chem. 4/2014)

https://www.onlinelibrary.wiley.com/doi/pdf/10.1002/anie.201310957

Inside Back Cover: Cobalt Imidazolate Metal–Organic Frameworks Photosplit CO2 under Mild Reaction Conditions (Angew. Chem. Int. Ed. 4/2014)

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Cobalt Imidazolate Metal–Organic Frameworks Photosplit CO 2 under Mild Reaction Conditions

Innenrücktitelbild: Cobalt Imidazolate Metal-Organic Frameworks Photosplit CO2under Mild Reaction Conditions (Angew. Chem. 4/2014)

Inside Back Cover: Cobalt Imidazolate Metal–Organic Frameworks Photosplit CO2 under Mild Reaction Conditions (Angew. Chem. Int. Ed. 4/2014)