Pushing the Limit of Ordered Mesoporous Materials via 2D Self‐Assembly for Energy Conversion and Storage

Abstract

Material and energy efficiencies are two key parameters that benchmark the electrochemical energy conversion and storage devices (EECSDs). Maximizing both requires researchers to grasp the limits of the physiochemical properties of core electrode materials. Ordered mesoporous materials (OMMs) have been regarded as promising electrode materials; however, their intrinsic deficiencies (e.g., plugs, inaccessible pores, and surfaces) impose limits for wide applications. 2D ordered mesoporous materials (2DOMMs) featured with an extended lateral dimension and a nanometer thickness not only inherit the structure advantages of mesoporous materials, but also have a unique 2D ultrathin feature that can fully address the imperfections of conventional OMMs. Herein, recent achievements on the preparation of 2DOMMs by combining single micelle assembly strategy with 2D bottom‐up patterning techniques including the molecular/space confined, interfacial orientated, and surface limited assembly are focused. Special focus is devoted to the newly developed synthetic strategies and their fundamental mechanisms for accurate control of some key structural parameters. Recent advances of 2DOMMs in EECSDs are also highlighted, which suggest that 2DOMMs are excellent material platforms for developing new battery chemistry as well as targeting performance optimization and cost reduction. Finally, the challenges and prospects are proposed based on current development.

Facile Synthesis of Two‐Dimensional Iron/Cobalt Metal–Organic Framework for Efficient Oxygen Evolution Electrocatalysis

“…Meanwhile,t he metal ions supported and protected by the organic framework can ensure along-term stability.However,bulk MOF with nanopores still suffer from poor conductivity and low mass permeability,w hich hamper their application in electrocatalysis.C ompared with bulk MOFs,t he two-dimensional (2D) MOF nanosheets with nanometer layers could possess ahigh electrocatalytic activity owing to many unsaturated coordination sites of metal ions on the surface,a sw ell as the rapid mass transport and charge transfer. [5][6][7][8][9][10] Especially,t he vacancies in the 2D ultrathin MOF nanosheets can increase the carrier concentration, thus leading to improved electrical conductivity. [11][12][13] Usually,the bottom-up method, via restricting the growth along the layer normal direction, is considered as an important means to produce 2D MOF nanosheets with ahigh yield and auniform thickness,ascompared to the top-bottom physical or chemical delamination of bulk crystals.…”

Facile Synthesis of Two‐Dimensional Iron/Cobalt Metal–Organic Framework for Efficient Oxygen Evolution Electrocatalysis

“…However, bulk MOF with nano‐pores still suffer from poor conductivity and low mass permeability, which hamper their application in electrocatalysis. Compared with bulk MOFs, the two‐dimensional (2D) MOF nanosheets with nanometer layers could possess a high electrocatalytic activity owing to many unsaturated coordination sites of metal ions on the surface, as well as the rapid mass transport and charge transfer [5–10] . Especially, the vacancies in the 2D ultrathin MOF nanosheets can increase the carrier concentration, thus leading to improved electrical conductivity [11–13] …”

Mesoporous Zeolitic Imidazolate Frameworks

“…29 Superior to the random porosity that is frequently met in the nanomaterials, the ordered meso/macropore structures contribute to the effective utilization of the smooth diffusion pathways, high surface area, and evenly dispersed active sites. [30][31][32][33] Recently, the ordered macroporous ZIFs were designed and successfully synthesized using the polystyrene-sphere monolith template. 15,34 Strikingly, the introduction of ordered macropores facilitates to prepare the hierarchically porous ZIFs, which exhibit much better overall performances in the diffusion-limited catalytic reactions as compared with conventional ZIFs.…”