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

Self-activated energy release cascade from anthracene-based solid-state molecular solar thermal energy storage systems DOI
Subhayan Chakraborty, Han Nguyen, Junichi Usuba

et al.

Chem, Journal Year: 2024, Volume and Issue: 10(11), P. 3309 - 3322

Published: July 22, 2024

Language: Английский

Citations

9
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

4
Photochromic Ln-MOFs: A Platform for Metal-Photoswitch Cooperativity DOI
Corey R. Martin, Grace C. Thaggard, Ingrid Lehman-Andino

et al.

Inorganic Chemistry, Journal Year: 2024, Volume and Issue: 63(28), P. 12810 - 12817

Published: June 27, 2024

Optoelectronic devices based on lanthanide-containing materials are an emergent area of research due to imminent interest in a new generation diode materials, optical and magnetic sensors, ratiometric thermometers. Tailoring material properties through the employment photo- or thermochromic moieties is powerful approach that requires deep fundamental understanding possible cooperativity between lanthanide-based metal centers integrated switchable units. In this work, we probe concept synthesis, structural analysis, spectroscopic characterization novel photochromic metal-organic containing noncoordinatively photoresponsive 4,4'-azopyridine centers. As result, photophysical response tailored demand incorporation compounds within rigid matrix was investigated. The comprehensive analysis includes single-crystal X-ray diffraction diffuse reflectance studies provide guiding principles necessary for unit-lanthanide-based framework (MOF) cooperativity. Furthermore, steady-state time-resolved revealed rapid rate moiety attenuation upon its integration MOFs comparison with solution, highlighting unique role synergy occurred stimuli-responsive MOF platform, allowing tunability control photoisomerization kinetics.

Language: Английский

Citations

3
A Change of Pace: Record Photoresponse through Spirooxazine Confinement in a Metal–Organic Matrix DOI
Grace C. Thaggard,

Gina R. Wilson,

Mamata Naik

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(46), P. 31746 - 31756

Published: Nov. 6, 2024

Modern and upcoming high-speed optoelectronics as well secure data storage or solar energy harvesting technologies integrating stimuli-responsive materials fully rely on the fundamental concept of rapid transitions between discrete states possessing different properties. Relatively slow transition kinetics those for commonly used classes photochromic compounds in solution bulk solids severely restrict applicability device development. Herein, we report a multivariate strategy based spirooxazine derivative, coordinatively integrated solvent-free confined space solid-state matrix, such metal-organic framework (MOF), first time, resulting fastest photoresponse reported any material to date. The photoisomerization rate developed was estimated be 126 s

Language: Английский

Citations

2
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