Post-synthetic modulation of the charge distribution in a metal–organic framework for optimal binding of carbon dioxide and sulfur dioxide

Li, Lei; Silva, Iván da; Kolokolov, Daniil I.; Han, Xue; Li, Jiangnan; Smith, Gemma L.; Cheng, Yongqiang; Daemen, Luke L.; Morris, Christopher G.; Godfrey, Harry G. W.; Jacques, Nicholas M.; Zhang, Xinran; Manuel, Pascal; Frogley, Mark D.; Murray, Claire; Ramirez‐Cuesta, Anibal J.; Cinque, Gianfelice; Tang, Chiu C.; Stepanov, Alexander G.; Yang, Sihai; Schröder, Martin

doi:10.1039/c8sc01959b

Cited by 69 publications

(52 citation statements)

References 49 publications

(63 reference statements)

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“…176 Initial results show that trivalent Al 3+ and In 3+ carboxylate frameworks reversibly bind dry SO2 in static adsorption experiments. [177][178][179] The Al 3+ carboxylate MOFs, MFM-305-CH3, MFM-305, and MFM-300 (née NOTT-300) all reversibly adsorb SO2 with high capacities above 5 mmol g -1 . 178,179 In situ powder X-ray diffraction analysis on MFM-300 revealed that SO2 strongly interacts with the bridging hydroxyl groups of the SBU.…”

Section: Mofs For So 2 Adsorptionmentioning

confidence: 99%

“…[177][178][179] The Al 3+ carboxylate MOFs, MFM-305-CH3, MFM-305, and MFM-300 (née NOTT-300) all reversibly adsorb SO2 with high capacities above 5 mmol g -1 . 178,179 In situ powder X-ray diffraction analysis on MFM-300 revealed that SO2 strongly interacts with the bridging hydroxyl groups of the SBU. 178 Moving to the more labile In 3+ , NOTT-202a [In(O2CR)4] (O2CR = biphenyl-3,3,5,5-tetra-(phenyl-4-carboxylate)) reversibly binds SO2 with an adsorption capacity of 10 mmol g -1 at 1 bar and temperatures between 293-303 K. 177 However, low temperature (268-283 K) SO2 adsorption isotherms feature hysteretic adsorption of an additional 2-6 mmol SO2 g -1 as a consequence of an irreversible phase change to form a denser crystalline polymorph.…”

Section: Mofs For So 2 Adsorptionmentioning

confidence: 99%

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Kinetic stability of metal–organic frameworks for corrosive and coordinating gas capture

2019

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Metal-organic frameworks (MOFs) have demonstrated their utility for a variety of applications involving the storage, separation, and sensing of weakly interacting gases of high purity. Exposure to more realistic, impure gas streams and interactions with corrosive and coordinating gases raises the question of chemical robustness, which remains a paramount concern for practical applications of MOFs. However, factors that determine the stability of MOFs remain incompletely understood. Although past researchers attempted to categorize framework materials as either thermodynamically stable or kinetically stable, recent work has elucidated an energetic penalty for porosity for all materials in this class with respect to a dense material. The metastability of porous phases has important implications for the design of materials for gas storage, heterogeneous catalysts, and electronic materials. Here, we focus on two main strategies for stabilization of the porous phase, either by using inert metal ions, or by increasing the heterolytic metal-ligand bond strength, both of which increase the activation barrier for framework collapse. These two strategies have led to exceptionally robust materials for the capture of coordinating and corrosive gases such as water vapor, ammonia, H2S, SO2, NOx, and even elemental halogens, and we review the progress in designing stable materials for these gases. Looking forward, we envision that the continued pursuit of strategies for kinetic stabilization in the synthesis of new MOFs will provide increasing numbers of robust frameworks suited to harsh conditions, and that short-term stability towards these challenging gases will be predictive of long-term stability for applications in less demanding environments.

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Section: Mofs For So 2 Adsorptionmentioning

confidence: 99%

Section: Mofs For So 2 Adsorptionmentioning

confidence: 99%

Kinetic stability of metal–organic frameworks for corrosive and coordinating gas capture

2019

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“…Porous metal-organic frameworks (MOFs) have been studied extensively for uptake and separation of a wide variety of gases, notably CO 2 , H 2 and hydrocarbons, 9-adsorbents ( Table 1, Fig 2), [15][16][17][18][19][20][21][22][23][24][25] but many exhibit limited stability and/or reversibility under near-ambient conditions. Current top-performing MOFs for SO 2 adsorption at 298 K and 1.0 bar include MFM-202a (10.2 mmol g -1 ) 18 and SIFSIX-1-Cu (11.0 mmol g -1 ) 16 .…”

Section: ------------------------------------------------------------mentioning

confidence: 99%

Reversible coordinative binding and separation of sulfur dioxide in a robust metal–organic framework with open copper sites

et al. 2019

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“…Developments in gas-handling systems have also paved the way to probe gate-opening and related network-breathing phenomena arising from the unique elastic properties of MOFs—see entries in Table 1 and Refs. [ 151 , 266 , 267 , 268 , 269 , 270 , 271 , 272 , 273 , 274 , 275 , 276 , 277 , 278 , 279 , 280 , 281 , 282 , 283 , 284 , 285 , 286 , 287 , 288 , 289 , 290 ].…”

Section: From Confined Polymers To Soft Supramolecular Frameworkmentioning

confidence: 99%

Dynamics & Spectroscopy with Neutrons—Recent Developments & Emerging Opportunities

2021

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This work provides an up-to-date overview of recent developments in neutron spectroscopic techniques and associated computational tools to interrogate the structural properties and dynamical behavior of complex and disordered materials, with a focus on those of a soft and polymeric nature. These have and continue to pave the way for new scientific opportunities simply thought unthinkable not so long ago, and have particularly benefited from advances in high-resolution, broadband techniques spanning energy transfers from the meV to the eV. Topical areas include the identification and robust assignment of low-energy modes underpinning functionality in soft solids and supramolecular frameworks, or the quantification in the laboratory of hitherto unexplored nuclear quantum effects dictating thermodynamic properties. In addition to novel classes of materials, we also discuss recent discoveries around water and its phase diagram, which continue to surprise us. All throughout, emphasis is placed on linking these ongoing and exciting experimental and computational developments to specific scientific questions in the context of the discovery of new materials for sustainable technologies.

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Post-synthetic modulation of the charge distribution in a metal–organic framework for optimal binding of carbon dioxide and sulfur dioxide

Abstract: Modulation of pore environment is an effective strategy to optimize guest binding in porous materials.

Cited by 69 publications

References 49 publications

Kinetic stability of metal–organic frameworks for corrosive and coordinating gas capture

Kinetic stability of metal–organic frameworks for corrosive and coordinating gas capture

Reversible coordinative binding and separation of sulfur dioxide in a robust metal–organic framework with open copper sites

Dynamics & Spectroscopy with Neutrons—Recent Developments & Emerging Opportunities

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