Heterogeneous Electrocatalysis of Carbon Dioxide to Methane

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Abstract

Electrocatalytic CO2 reduction to valued products is a promising way to mitigate the greenhouse effect, as this reaction makes use of the excess CO2 in the atmosphere and at the same time forms valued fuels to partially fulfill the energy demand for human beings. Among these valued products, methane is considered a high-value product with a high energy density. This review systematically summarizes the recently studied reaction mechanisms for CO2 electroreduction to CH4. It guides us in designing effective electrocatalysts with an improved electrocatalytic performance. In addition, we briefly summarize the recent progress on CO2 electroreduction into CH4 from the instructive catalyst design, including catalyst structure engineering and catalyst component engineering, and then briefly discuss the electrolyte effect. Furthermore, we also provide a simplified techno-economic analysis of this technology. These summaries are helpful for beginners to rapidly master the contents related to the electroreduction of carbon dioxide to methane and also help to promote the further development of this field.

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The chemistry and applications of metal-organic frameworks.

Hiroyasu Furukawa, Kyle E. Cordova, Michael O'Keeffe … (2013)

Crystalline metal-organic frameworks (MOFs) are formed by reticular synthesis, which creates strong bonds between inorganic and organic units. Careful selection of MOF constituents can yield crystals of ultrahigh porosity and high thermal and chemical stability. These characteristics allow the interior of MOFs to be chemically altered for use in gas separation, gas storage, and catalysis, among other applications. The precision commonly exercised in their chemical modification and the ability to expand their metrics without changing the underlying topology have not been achieved with other solids. MOFs whose chemical composition and shape of building units can be multiply varied within a particular structure already exist and may lead to materials that offer a synergistic combination of properties.

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Single-atom catalysts: a new frontier in heterogeneous catalysis.

Xiao-feng Yang, Aiqin Wang, Botao Qiao … (2013)

Supported metal nanostructures are the most widely used type of heterogeneous catalyst in industrial processes. The size of metal particles is a key factor in determining the performance of such catalysts. In particular, because low-coordinated metal atoms often function as the catalytically active sites, the specific activity per metal atom usually increases with decreasing size of the metal particles. However, the surface free energy of metals increases significantly with decreasing particle size, promoting aggregation of small clusters. Using an appropriate support material that strongly interacts with the metal species prevents this aggregation, creating stable, finely dispersed metal clusters with a high catalytic activity, an approach industry has used for a long time. Nevertheless, practical supported metal catalysts are inhomogeneous and usually consist of a mixture of sizes from nanoparticles to subnanometer clusters. Such heterogeneity not only reduces the metal atom efficiency but also frequently leads to undesired side reactions. It also makes it extremely difficult, if not impossible, to uniquely identify and control the active sites of interest. The ultimate small-size limit for metal particles is the single-atom catalyst (SAC), which contains isolated metal atoms singly dispersed on supports. SACs maximize the efficiency of metal atom use, which is particularly important for supported noble metal catalysts. Moreover, with well-defined and uniform single-atom dispersion, SACs offer great potential for achieving high activity and selectivity. In this Account, we highlight recent advances in preparation, characterization, and catalytic performance of SACs, with a focus on single atoms anchored to metal oxides, metal surfaces, and graphene. We discuss experimental and theoretical studies for a variety of reactions, including oxidation, water gas shift, and hydrogenation. We describe advances in understanding the spatial arrangements and electronic properties of single atoms, as well as their interactions with the support. Single metal atoms on support surfaces provide a unique opportunity to tune active sites and optimize the activity, selectivity, and stability of heterogeneous catalysts, offering the potential for applications in a variety of industrial chemical reactions.