A highly active, robust photocatalyst heterogenized in discrete cages of metal–organic polyhedra for CO<sub>2</sub> reduction

Lee, Hyeon Shin; Jee, Seohyeon; Kim, Raekyung; Bui, Hoang Tran; Kim, Bupmo; Kim, Jung‐Keun; Park, Kyo Sung; Choi, Wonyong; Kim, Wooyul; Choi, Kyung Min

doi:10.1039/c9ee02619c

Cited by 73 publications

(51 citation statements)

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“…MOT-1 could be constructed using ditopic Zr-based SBU, although the identical SBU was often utilized as a tritopic node producing well-known tetrahedral structures of MOPs ( Fig. 3) [22][23][24][25][26][56][57][58]. One coordination site in a ditopic SBU of MOT-1 is occupied by formate.…”

Section: Resultsmentioning

confidence: 99%

Discovery of Zr-based metal-organic polygon: Unveiling new design opportunities in reticular chemistry

et al. 2020

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Metal-based secondary building unit and the shape of organic ligands are the two crucial factors for determining the final topology of metal-organic materials. A careful choice of organic and inorganic structural building units occasionally produces unexpected structures, facilitating deeper fundamental understanding of coordination-driven self-assembly behind metal-organic materials. Here, we have synthesized a triangular metal-organic polygon (MOT-1), assembled from bulky tetramethyl terephthalate and Zr-based secondary building unit. Surprisingly, the Zr-based secondary building unit serves as an unusual ditopic Zr-connector, to form metal-organic polygon MOT-1, proven to be a good candidate for water adsorption with recyclability. This study highlights the interplay of the geometrically frustrated ligand and secondary building unit in controlling the connectivity of metal-organic polygon. Such a strategy can be further used to unveil a new class of metal-organic materials.

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Section: Resultsmentioning

confidence: 99%

Discovery of Zr-based metal-organic polygon: Unveiling new design opportunities in reticular chemistry

et al. 2020

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“…X‐ray diffraction (XRD) analyses (Figure S3) indicate that the MOP‐NH 2 solids are crystal with high purity. When dissolved in methanol, the crystalline structure is disassembled into discrete molecular cage [15] …”

Section: Resultsmentioning

confidence: 99%

Enzyme‐Mimetic Molecular Selective Catalysis via Single Zr Atom Catalysis in Chelated Cage Embedded in a Flexible Piezoelectrical Matrix

Liu

Chen

Teng

et al. 2022

Chemistry A European J

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The molecularly selective catalysis in enzyme is central to life. However, their functioning mechanism remains elusive. We propose here that the synergistic effects from (i) effective orbital hybridizing and energy gap decreasing via chelating on single Zr atom as the catalytic center, (ii) selective supramolecular encapsulation in the cage, and (iii) piezoelectrical field motivation are able to achieve the enzyme‐mimetic molecular selective high performance catalysis. Metal–organic polyhedra (MOPs) are added into a piezoelectrical polymer matrix to achieve the composite structure where ultrasonic treatment motivates redox reactions in the MOP‐guest complex. Encapsulated and chelated guest such as Rhodamine B (RhB) is effectively converted with ratios higher than 90 % after 100 min. In comparison, molecules inefficient in either cage encapsulation or chelating with the Zr center can not be converted. This study first proposes a synergistic plot for enzyme‐mimetic catalyst realization and is expected to inspire new mentality in efficient catalyst designing.

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“…Recently, photocatalytic CO 2 reduction as a promising strategy has attracted more and more attentions. [ 97–106 ] A detailed discussion and summary about the thermodynamics and kinetics of CO 2 photoreduction has been reviewed by Chen and co‐workers. [ 107 ] Whether from the perspective of thermodynamics or kinetics, photocatalytic reduction of CO 2 is a more complicated reduction reaction involving multi‐electron and ‐proton interactions and a number of different surface intermediates compared with HER.…”

Section: Photocatalytic Applications Of 2d Cofmentioning

confidence: 99%

Two‐Dimensional Covalent‐Organic Frameworks for Photocatalysis: The Critical Roles of Building Block and Linkage

et al. 2020

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Covalent organic frameworks (COFs) are a class of crystalline porous materials which contain organic build blocks linked via covalent bonds to form ordered and periodic structures. In recent years, 2D COFs have been developed as promising heterogeneous photocatalysts due to their extended π‐conjugated skeletons, high surface area, tunable structure, regular pore structure, and high crystallinity. Herein, recent advances in the design and synthesis of 2D COFs for photocatalysts are surveyed, the illustration of the structural features and synthetic strategy is focused on, and the relationship between the construction and property of 2D COFs for photocatalytic water splitting, CO2 reduction, organic transformation, and degradation of organic pollutants is elucidated. This overview is expected to provide clues to rational design and synthesis of ultra‐stable, high crystalline, and high‐performance 2D COFs for photocatalytic applications.

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A highly active, robust photocatalyst heterogenized in discrete cages of metal–organic polyhedra for CO₂ reduction

Abstract: A photocatalyst heterogenized in discrete cages of metal–organic polyhedra provides highly active and robust conversion of carbon dioxide.

Cited by 73 publications

References 50 publications

Discovery of Zr-based metal-organic polygon: Unveiling new design opportunities in reticular chemistry

Discovery of Zr-based metal-organic polygon: Unveiling new design opportunities in reticular chemistry

Enzyme‐Mimetic Molecular Selective Catalysis via Single Zr Atom Catalysis in Chelated Cage Embedded in a Flexible Piezoelectrical Matrix

Two‐Dimensional Covalent‐Organic Frameworks for Photocatalysis: The Critical Roles of Building Block and Linkage

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A highly active, robust photocatalyst heterogenized in discrete cages of metal–organic polyhedra for CO2 reduction

Abstract: A photocatalyst heterogenized in discrete cages of metal–organic polyhedra provides highly active and robust conversion of carbon dioxide.

Cited by 73 publications

References 50 publications

Discovery of Zr-based metal-organic polygon: Unveiling new design opportunities in reticular chemistry

Discovery of Zr-based metal-organic polygon: Unveiling new design opportunities in reticular chemistry

Enzyme‐Mimetic Molecular Selective Catalysis via Single Zr Atom Catalysis in Chelated Cage Embedded in a Flexible Piezoelectrical Matrix

Two‐Dimensional Covalent‐Organic Frameworks for Photocatalysis: The Critical Roles of Building Block and Linkage

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A highly active, robust photocatalyst heterogenized in discrete cages of metal–organic polyhedra for CO₂ reduction