Catalytically Active Site Mapping Realized through Energy Transfer Modeling DOI
W. Jake Thompson, Buddhima K. P. Maldeni Kankanamalage, Grace C. Thaggard

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 64(4)

Published: Oct. 4, 2024

The demands of a sustainable chemical industry are driving force for the development heterogeneous catalytic platforms exhibiting facile catalyst recovery, recycling, and resilience to diverse reaction conditions. Homogeneous-to-heterogeneous transitions can be realized through integration efficient homogeneous catalysts within porous matrices. Herein, we offer versatile approach understanding how guest distribution evolution impact performance host-guest by implementing resonance energy transfer (RET) concept using fluorescent model systems mimicking steric constraints targeted catalysts. Using RET-based methodology, mapped condition-dependent (re)distribution support on example modular matrices such as metal-organic frameworks (MOFs). Furthermore, correlate RET results performed with two MOF-encapsulated used promote CO2 hydrogenation ring-closing metathesis. Guests incorporated aperture-opening encapsulation, redistribution is not observed under practical conditions, showcasing pathway advance recyclability in case platforms. These studies represent first generalizable mapping systems, providing foundation predicting tailoring integrated into various supports.

Language: Английский

Zirconium-based metal−organic frameworks and their roles in electrocatalysis DOI

Meng‐Dian Tsai,

Kuan-Chu Wu,

Chung‐Wei Kung

et al.

Chemical Communications, Journal Year: 2024, Volume and Issue: 60(64), P. 8360 - 8374

Published: Jan. 1, 2024

Due to their exceptional chemical stability in water and high structural tunability, zirconium(IV)-based MOFs (Zr-MOFs) have been considered attractive materials the broad fields of electrocatalysis. Numerous studies published since 2015 attempted utilise Zr-MOFs electrocatalysis, with porous framework serving as either active electrocatalyst or scaffold surface coating further enhance performance actual electrocatalyst. Herein, roles electrocatalytic processes are discussed, some selected examples reporting applications various reactions, including several from our group, overviewed. Challenges, limitations opportunities using electrocatalysis future discussed.

Language: Английский

Citations

4
Optimizing iodine adsorption in functionalized metal-organic frameworks via an unprecedented positional isomerism strategy DOI
Zi‐Jian Li, Juejing Liu, Guangtao Zhang

et al.

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 499, P. 156586 - 156586

Published: Oct. 10, 2024

Language: Английский

Citations

4
Pioneering radiation dosimetry and photothermal conversion in a photochromic and radiochromic thorium cluster DOI
Jingqi Ma, Junpu Yang, Huangjie Lu

et al.

Science China Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 7, 2025

Language: Английский

Citations

0
Mining for Metal–Organic Systems: Chemistry Frontiers of Th-, U-, and Zr-Materials DOI

Kyoung Chul Park,

Jaewoong Lim, Grace C. Thaggard

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(27), P. 18189 - 18204

Published: June 29, 2024

The conceptual framework presented in this Perspective overviews the design principles of innovative thorium-based materials that could address urgent needs medicinal, nuclear energy, and waste remediation sectors from lens zirconium uranium analogs. We survey intersections Zr, Th, U chemistry with a focus on how intrinsic behavior each metal translates to broader material properties, including, but not limited to, structural topological diversity, preferential metal–ligand binding, reactivity. On example several classes materials, including organometallic complexes, polyoxometalates, primary Perspective, metal–organic frameworks (MOFs), govern preparation Zr-, Th-, U-compounds, oxophilicity, variation oxidation states, stable coordination environments have been considered. Further, we highlight impact mentioned variables may shift throughout progression discrete molecular systems extended structures. discuss common assumption zirconium-organic are typically considered close analog congeners areas such as preparation. Through consideration fundamental principles, shed light relationships between U-based critical analysis their distinct properties can be used target desired performance. As result, provide detailed understanding Th-based by anchoring two well-studied reference points, zirconium- uranium-containing

Language: Английский

Citations

3
Switching from Molecules to Functional Materials: Breakthroughs in Photochromism With MOFs DOI
Grace C. Thaggard, Buddhima K. P. Maldeni Kankanamalage,

Kyoung Chul Park

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 7, 2024

Abstract Photochromic materials with properties that can be dynamically tailored as a function of external stimuli are rapidly expanding field driven by applications in areas ranging from molecular computing, nanotechnology, or photopharmacology to programable heterogeneous catalysis. Challenges arise, however, when translating the rapid, solution‐like response stimuli‐responsive moieties solid‐state due intermolecular interactions imposed through close packing bulk solids. As result, integration photochromic compounds into synthetically porous matrices, such metal‐organic frameworks (MOFs), has come forefront an emerging strategy for material development. This review highlights how core principles reticular chemistry (on example MOFs) play critical role performance, surpassing limitations previously observed solution solid state. The symbiotic relationship between photoresponsive and focus on synthesis creates avenues toward tailorable photoisomerization kinetics, directional energy charge transfer, switchable gas sorption, synergistic chromophore communication is discussed. not only focuses recent cutting‐edge advancements development, but also novel, vital‐to‐pursue pathways multifaceted functional realms energy, technology, biomedicine.

Language: Английский

Citations

3
Catalytically Active Site Mapping Realized through Energy Transfer Modeling DOI
W. Jake Thompson, Buddhima K. P. Maldeni Kankanamalage, Grace C. Thaggard

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 64(4)

Published: Oct. 4, 2024

The demands of a sustainable chemical industry are driving force for the development heterogeneous catalytic platforms exhibiting facile catalyst recovery, recycling, and resilience to diverse reaction conditions. Homogeneous-to-heterogeneous transitions can be realized through integration efficient homogeneous catalysts within porous matrices. Herein, we offer versatile approach understanding how guest distribution evolution impact performance host-guest by implementing resonance energy transfer (RET) concept using fluorescent model systems mimicking steric constraints targeted catalysts. Using RET-based methodology, mapped condition-dependent (re)distribution support on example modular matrices such as metal-organic frameworks (MOFs). Furthermore, correlate RET results performed with two MOF-encapsulated used promote CO2 hydrogenation ring-closing metathesis. Guests incorporated aperture-opening encapsulation, redistribution is not observed under practical conditions, showcasing pathway advance recyclability in case platforms. These studies represent first generalizable mapping systems, providing foundation predicting tailoring integrated into various supports.

Language: Английский

Citations

0