Direct Synthesis, Structural Features, and Enhanced Catalytic Activity of the Basolite F300-like Semiamorphous Fe-BTC Framework

Sánchez‐Sánchez, Manuel; Asúa, Íñigo de; Ruano, Daniel; Díaz, Kenya

doi:10.1021/acs.cgd.5b00755

Cited by 113 publications

(120 citation statements)

References 40 publications

(102 reference statements)

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“…Between 230–500 °C, the decomposition of the enzymes occurs with mass losses of 7.3 % and 11.4 % for AK@ZIF‐8 LR and RM@ZIF‐8 LR , respectively. The diversity in shape in Figure C–D are due to the different synthesis conditions …”

Section: Resultsmentioning

confidence: 99%

Lipase Encapsulation onto ZIF‐8: A Comparison between Biocatalysts Obtained at Low and High Zinc/2‐Methylimidazole Molar Ratio in Aqueous Medium

et al. 2018

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Lipase AK from Pseudomonas fluorescens and Lipase RM from Rhizomucor miehei were encapsulated into a zeolite imidazolate framework (ZIF‐8) by a “one‐pot” synthesis to obtain AK@ZIF‐8 and RM@ZIF‐8 biocatalysts. The effect of a high (1:40) and low (1:4) Zn/2‐methylimidazole molar ratio on the biocatalysts synthesis was investigated. The different Zn/ligand (L) ratios affected both the surface area, the loading, and the specific activity of the biocatalysts. Samples synthesized by using a high Zn/L ratio had high values of surface area whereas those obtained by using a low Zn/L ratio had higher loadings and specific activities. The decrease of pH (from 11.6 to 9.4) during the synthesis at high Zn/L ratio produced ZIF‐8 samples with features similar to those observed for low Zn/L ratio samples. The low Zn/L (1:4) ratio AK@ZIF‐8 biocatalyst retained 99 % activity after storage for 15 days at 5 °C and 40 % activity after five reaction cycles.

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Section: Resultsmentioning

confidence: 99%

Lipase Encapsulation onto ZIF‐8: A Comparison between Biocatalysts Obtained at Low and High Zinc/2‐Methylimidazole Molar Ratio in Aqueous Medium

et al. 2018

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“…This indicates that the synthesized material indeed has the MTN‐zeotype architecture. On the other hand, Basolite® F300 presents a smooth pattern, in contrast to previous literature, characteristic of non‐crystalline solid, thus preventing the assignment to a given crystalline structure. To further understand MIL‐100(Fe) and Basolite® F300 structure at the short and intermediate range, X‐ray Pair Distribution Function (XPDF) analysis was conducted on both materials.…”

Section: Resultsmentioning

confidence: 99%

Metal‐Organic Frameworks as Catalyst Supports: Influence of Lattice Disorder on Metal Nanoparticle Formation

Rivera‐Torrente

Filez

Hardian

et al. 2018

Chemistry A European J

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Because of their high tunability and surface area, metal-organic frameworks (MOFs) show great promise as supports for metal nanoparticles. Depending on the synthesis route, MOFs may contain defects. Here, we show that highly crystalline MIL-100(Fe) and disordered Basolite® F300, with identical iron 1,3,5-benzenetricarboxylate composition, exhibit very divergent properties when used as a support for Pd nanoparticle deposition. While MIL-100(Fe) shows a regular MTN-zeotype crystal structure with two types of cages, Basolite® F300 lacks long-range order beyond 8 Å and has a single-pore system. The medium-range configurational linker-node disorder in Basolite® F300 results in a reduced number of Lewis acid sites, yielding more hydrophobic surface properties compared to hydrophilic MIL-100(Fe). The hydrophilic/hydrophobic nature of MIL-100(Fe) and Basolite® F300 impacts the amount of Pd and particle size distribution of Pd nanoparticles deposited during colloidal synthesis and dry impregnation methods, respectively. It is suggested that polar (apolar) solvents/precursors attractively interact with hydrophilic (hydrophobic) MOF surfaces, allowing tools at hand to increase the level of control over, for example, the nanoparticle size distribution.

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“…Firstly, it presents a semi-crystalline/semiamorphous nature. Despite it is not purely crystalline, its powder X-ray diffraction pattern (PXRD) suggests a close structural relationship with the crystalline mesocages-containing Fe-BTC MOF material known as MIL-100(Fe) [49][50][51]. Indeed, this material contains only one type of the two mesocavities found in MIL-100(Fe) [51,52].…”

Section: Introductionmentioning

confidence: 99%

Semi-crystalline Fe-BTC MOF material as an efficient support for enzyme immobilization

et al. 2018

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Graphical abstractResearch Highlights: Semi-crystalline Fe-BTC MOF material is an efficient support for enzymes  It can be used by either in-situ or post-synthesis approaches  The in-situ (one-step) biocatalysts are more active and have lower enzyme leaching  This enzyme support improves the benefits given by some other MOF-based supports ABSTRACT. Metal-organic frameworks (MOFs) have revolutionized the potential applications of nanoporous materials. One of the most recent and promising applications of these materials is their use as supports for enzyme immobilization. In this context, the in-situ (one-step) methodologies, which do not require the use of MOFs with pores larger than the enzyme to be immobilized, seem to be particularly encouraging. This work presents a systematic study of the semi-crystalline Fe-BTC MOF material (commercialized as Basolite F300) employed as support of the enzymes laccase and lipase through either in-situ or postsynthesis methodology. The presence of the enzyme in the resultant solid biocatalysts was proved by CHNS chemical analysis, thermogravimetric analysis, Bradford assays and by SDS-PAGE electrophoresis. The enzymatic activity of the resultant Fe-BTC-based biocatalysts was also tested. The in-situ approach is particularly relevant due to various reasons: (i) the enzyme immobilization is given in one step; (ii) it is rapid (10 minutes); (iii) it is very efficient in terms of encapsulation capacity (≥ 98 % for laccase and ≥ 87 % for lipase); (iv) the enzymes are fully retained and no leaching is observed after an initial release of only around 10% of the enzyme molecules weakly immobilized; and (v) the activity of the retained enzyme can be substantially maintained (97 % with respect to the free enzyme in the case of lipase). Any of these parameters systematically improves these given by the post-synthesis (two-step) approach. Moreover, Fe-BTC widely surpasses the benefits given by other MOF-based supports either by in-situ or postsynthesis approaches.

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Direct Synthesis, Structural Features, and Enhanced Catalytic Activity of the Basolite F300-like Semiamorphous Fe-BTC Framework

Cited by 113 publications

References 40 publications

Lipase Encapsulation onto ZIF‐8: A Comparison between Biocatalysts Obtained at Low and High Zinc/2‐Methylimidazole Molar Ratio in Aqueous Medium

Lipase Encapsulation onto ZIF‐8: A Comparison between Biocatalysts Obtained at Low and High Zinc/2‐Methylimidazole Molar Ratio in Aqueous Medium

Metal‐Organic Frameworks as Catalyst Supports: Influence of Lattice Disorder on Metal Nanoparticle Formation

Semi-crystalline Fe-BTC MOF material as an efficient support for enzyme immobilization

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