Tuning Lewis acidity of iron-based metal-organic frameworks for enhanced catalytic ozonation

Yu, Deyou; Wang, Liping; Yang, Taoyu; Yang, Guangpeng; Wang, Dong; Ni, Huagang; Wu, Minghua

doi:10.1016/j.cej.2020.127075

Cited by 90 publications

(35 citation statements)

References 64 publications

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“…MOFs are described as crystalline, rigid, highly stable and highly porous materials [ 5 ]. Depending on the ligands and corresponding tridimensional structures, it is possible to control the crystalline framework and the shape of the pores for a wide range of specific, highly directed applications, such as adsorption of gas and pollutants, energy storage, chemical sensing or heterogeneous catalysis [ 4 , 6 , 7 , 8 ].…”

Section: Reticular Chemistry and Mofsmentioning

confidence: 99%

Covalent Organic Frameworks: Synthesis, Properties and Applications—An Overview

et al. 2021

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Covalent Organic Frameworks (COFs) are an exciting new class of microporous polymers with unprecedented properties in organic material chemistry. They are generally built from rigid, geometrically defined organic building blocks resulting in robust, covalently bonded crystalline networks that extend in two or three dimensions. By strategically combining monomers with specific structures and properties, synthesized COF materials can be fine-tuned and controlled at the atomic level, with unparalleled precision on intrapore chemical environment; moreover, the unusually high pore accessibility allows for easy post-synthetic pore wall modification after the COF is synthesized. Overall, COFs combine high, permanent porosity and surface area with high thermal and chemical stability, crystallinity and customizability, making them ideal candidates for a myriad of promising new solutions in a vast number of scientific fields, with widely varying applications such as gas adsorption and storage, pollutant removal, degradation and separation, advanced filtration, heterogeneous catalysis, chemical sensing, biomedical applications, energy storage and production and a vast array of optoelectronic solutions. This review attempts to give a brief insight on COF history, the overall strategies and techniques for rational COF synthesis and post-synthetic functionalization, as well as a glance at the exponentially growing field of COF research, summarizing their main properties and introducing the numerous technological and industrial state of the art applications, with noteworthy examples found in the literature.

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Section: Reticular Chemistry and Mofsmentioning

confidence: 99%

Covalent Organic Frameworks: Synthesis, Properties and Applications—An Overview

et al. 2021

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“…Such exposed metal sites would interact with organic substrates inside the MOFs pores for proceeding catalytic activation. [ 86–89 ] The regular arrangement and tunable chemical environment of the metal centers endow MOFs with regioselectivity and shape‐/size‐selectivity.…”

Section: Designing Mofs For Catalysismentioning

confidence: 99%

Engineering Nanoscale Metal‐Organic Frameworks for Heterogeneous Catalysis

et al. 2021

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Metal‐organic frameworks (MOFs) are porous crystalline materials composed of metal ions (or clusters) and organic ligands. Targeted preparation of nanoscale MOFs has been successfully achieved through numerous synthetic methods and is beneficial to improve the utilization of catalytic sites. On one hand, the dynamic bonds and rich selection of both metal centers and organic molecules enable broadening the types and functions of MOFs, thus offering the basis for rational design of heterogeneous catalysts at the molecular level. On the other hand, the reversible nature of connections between metal centers and organic ligands brings serious challenges about its stability under harsh reaction conditions. To optimize the catalytic performance of MOFs, considerable efforts have been devoted to tune the chemical environment of active sites by introducing electronic or channel confinement effect as well as controlling their size growth at nanoscale for increasing the surface coordination unsaturated sites. In this review, the state‐of‐the‐art development of nanoscale MOFs is summarized and particular focus is placed on regulation strategies of catalytic sites. The authors also propose the current challenges, the problems awaiting to be solved and opportunities in the future.

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“…The volumetric mass transfer coefficient k L a and the gas holdup φ (g) were computed with the empirical equations from Inkeri et al for gassed stirred tank reactors [51], and the ozone gas flow-rate Q (g) was maintained fixed to 2.0 L min −1 . Meanwhile, the ozone concentration at the interphase C * O 3 was a function of the mean logarithmic ozone gas concentration C O 3(g) , according to Equation (29).…”

Section: Mathematical Modelsmentioning

confidence: 99%

“…According to Yu et al, the amount of Lewis active sites (LAS) for a given catalyst significantly influences the degradation and mineralization during the COz [28][29][30]. Furthermore, for PCOz processes, a large amount of LAS could also increase the rate of capture of pairs electron-hole because of the high concentration of adsorbed ozone molecules, consequently increasing its oxidative potential [31].…”

Section: Introductionmentioning

confidence: 99%

Mechanistic Model and Optimization of the Diclofenac Degradation Kinetic for Ozonation Processes Intensification

Acosta-Angulo

Lara-Ramos

Díaz-Angulo

et al. 2021

Water

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This work focused on estimating the rate constants for three ozone-based processes applied in the degradation of diclofenac. The ozonation (Oz) and its intensification with catalysis (COz) and photocatalysis (PCOz) were studied. Three mathematical models were evaluated with a genetic algorithm (GA) to find the optimal values for the kinetics constants. The Theil inequality coefficient (TIC) worked as a criterion to assess the models’ deviation. The diclofenac consumption followed a slow kinetic regime according to the Hatta number (Ha<0.3). However, it strongly contrasted with earlier studies. The obtained values for the volumetric rate of photon absorption (VRPA) corresponding to the PCOz process (1.75×10−6 & 6.54×10−7 Einstein L−1 min−1) were significantly distant from the maximum (2.59×10−5 Einstein L−1 min−1). The computed profiles of chemical species proved that no significant amount of hydroxyl radicals was produced in the Oz, whereas the PCOz achieved the highest production rate. According to this, titanium dioxide significantly contributed to ozone decomposition, especially at low ozone doses. Although the models’ prediction described a good agreement with the experimental data (TIC<0.3), the optimization algorithm was likely to have masked the rate constants as they had highly deviated from already reported values.

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Tuning Lewis acidity of iron-based metal-organic frameworks for enhanced catalytic ozonation

Cited by 90 publications

References 64 publications

Covalent Organic Frameworks: Synthesis, Properties and Applications—An Overview

Covalent Organic Frameworks: Synthesis, Properties and Applications—An Overview

Engineering Nanoscale Metal‐Organic Frameworks for Heterogeneous Catalysis

Mechanistic Model and Optimization of the Diclofenac Degradation Kinetic for Ozonation Processes Intensification

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