Hollow zeolite microspheres as a nest for enzymes: a new route to hybrid heterogeneous catalysts

Smeets, Valentin; Baaziz, Walid; Ersen, Ovidiu; Gaigneaux, Éric M.; Boissière, Cédric; Sánchez, Clément; Debecker, Damien P.

doi:10.1039/c9sc04615a

Cited by 55 publications

(53 citation statements)

References 69 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…the epoxidation of allyl alcohol carried out in the absence of externally-added hydrogen peroxide, using the H 2 O 2 produced in situ by the enzyme trapped in the hybrid catalyst ( Figure 6A). In the conditions used for the cascade reaction, a purely inorganic catalyst is totally inactive (27). Here, the detection of glycidol proved that the chemoenzymatic epoxidation was indeed catalyzed by the hybrid catalyst.…”

Section: Study Of Hybrid Catalysts (Hybrid_gox and Hybrid_epcs)mentioning

confidence: 78%

“…Zooming in, the TS-1 nanocrystals are clearly visible (Figure S2 B). Their size is equal to the size of the starting TS-1 nanocrystals (27). Interparticle voids are also observable between the aggregated nanocrystals with a size ranging from 40 to 65 nm.…”

Section: Study Of the Inorganic Catalyst (Ts-1 And Aer_ts-1)mentioning

confidence: 96%

“…The titanosilicalite-1 suspension was prepared via hydrothermal synthesis according to a protocol adapted from the literature (27,37,76). Solution A was prepared by solubilizing 0.55 g titanium isopropoxide in 5 g propyl alcohol.…”

Section: Ts-1 Synthesismentioning

confidence: 99%

“…To overcome these drawbacks, we have recently proposed a two-step strategy for the preparation of an efficient GOx/TS-1 hybrid catalyst (27). First, leveraging on a spray drying technique (38), hollow zeolite microspheres were designed, starting from a suspension of TS-1 nanocrystals.…”

Section: Introductionmentioning

confidence: 99%

“…The GOx loading could be easily adapted and the enzyme also gained in stability. This original design allowed reaching relatively high levels of epoxide yield in the one-pot chemoenzymatic reaction (27).…”

Section: Introductionmentioning

confidence: 99%

See 4 more Smart Citations

Hybrid Chemo-Biocatalysts Prepared in One Step from Zeolite Nanocrystals and Enzyme-Polyelectrolyte Complexes

Verren¹,

Smeets²,

Straeten³

et al. 2020

Preprint

Self Cite

View full text Add to dashboard Cite

The combination of heterogeneous catalysts and enzymes, in so-called hybrid catalysts, is an attractive strategy to effectively run chemoenzymatic reactions. Yet, the preparation of such bifunctional materials remains challenging because both the inorganic and the biological moieties must be integrated in the same solid, while preserving their intrinsic activity. Combining an enzyme and a zeolite, for example, is complicated because the pores of the zeolite are too small to accommodate the enzyme and a covalent anchorage on the surface is often ineffective. Herein, we developed a new pathway to prepare a hybrid catalyst built from glucose oxidase and TS-1 zeolite. Such hybrid material can catalyze the in situ formation of H2O2, which is subsequently used by the zeolite to trigger the epoxidation of allylic alcohol. Starting from an enzymatic solution and a suspension of zeolite nanocrystals, the hybrid catalyst is obtained in one step, using a continuous spray drying method. While enzymes are expectedly unable to resist the conditions used in spray drying (temperature, shear stress, etc.), we leverage on the preparation of “enzyme-polyelectrolyte complexes” (EPCs) to increase the enzyme stability. Importantly, the use of EPCs also appears to prevent enzyme leaching and to stabilize the enzyme against pH changes. We show that the one-pot preparation by spray drying gives access to hybrid catalysts with unprecedented performance in the targeted chemoenzymatic reaction. Interestingly, the hybrid catalyst performs much better than the two catalysts operating as separate entities. We anticipate that this strategy could be used as an adaptable method to prepare other types of multifunctional materials.<br>

show abstract

Section: Study Of Hybrid Catalysts (Hybrid_gox and Hybrid_epcs)mentioning

confidence: 78%

Section: Study Of the Inorganic Catalyst (Ts-1 And Aer_ts-1)mentioning

confidence: 96%

Section: Ts-1 Synthesismentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 3 more Smart Citations

Hybrid Chemo-Biocatalysts Prepared in One Step from Zeolite Nanocrystals and Enzyme-Polyelectrolyte Complexes

Verren¹,

Smeets²,

Straeten³

et al. 2020

Preprint

Self Cite

View full text Add to dashboard Cite

show abstract

Multifunctional, Hybrid Materials Design via Spray‐Drying: Much more than Just Drying

Wintzheimer,

Luthardt,

Cao

et al. 2023

Advanced Materials

Self Cite

View full text Add to dashboard Cite

Spray‐drying is a popular and well‐known “drying tool” for engineers. This perspective highlights that, beyond this application, spray‐drying is a very interesting and powerful tool for materials chemists to enable the design of multifunctional and hybrid materials. Upon spray‐drying, the confined space of a liquid droplet is narrowed down, and its ingredients are forced together upon “falling dry.” As detailed in this article, this enables the following material formation strategies either individually or even in combination: nanoparticles and/or molecules can be assembled; precipitation reactions as well as chemical syntheses can be performed; and templated materials can be designed. Beyond this, fragile moieties can be processed, or “precursor materials” be prepared. Post‐treatment of spray‐dried objects eventually enables the next level in the design of complex materials. Using spray‐drying to design (particulate) materials comes with many advantages—but also with many challenges—all of which are outlined here. It is believed that multifunctional, hybrid materials, made via spray‐drying, enable very unique property combinations that are particularly highly promising in myriad applications—of which catalysis, diagnostics, purification, storage, and information are highlighted.

show abstract

Synthesis of hierarchical ZSM‐5 microspheres with superior performance for catalytic methanol‐to‐olefin conversion

Zhang

Shang

et al. 2022

AIChE Journal

View full text Add to dashboard Cite

Methanol-to-olefin (MTO) conversion on zeolites has encountered severe coke deposition and rapid deactivation. Creating different levels of porosity is essential to mitigate such issues. Herein, we demonstrate a facile and green strategy to synthesize uniform and hierarchically macro/mesoporous ZSM-5 microspheres by combining spray-freeze drying and steaming-assisted crystallization (SAC). The structure, crystallinity, and porosity of the zeolite microspheres are controlled by adjusting the water/gel mass ratio and time in the SAC process. The structure evolution during the SAC process is revealed. In the catalytic MTO reaction, the representative hierarchically porous ZSM-5 catalyst exhibits superior catalytic performance. At a very high weight hourly space velocity of 18 h À1 , it shows a dramatically prolonged lifetime (47 h at >99% conversion) and much-improved selectivity to ethylene and propylene compared with the conventional microporous ZSM-5 and nano-sized ZSM-5. The enhanced performance is originated from the hierarchical structure and suitable acidity of the ZSM-5 microspheres.

show abstract

Hollow zeolite microspheres as a nest for enzymes: a new route to hybrid heterogeneous catalysts

Abstract: A spray drying technique is used to prepare hollow zeolite microparticles into which an enzyme can be entrapped. Via this “Lego-like” strategy, we create hybrid heterogeneous catalysts that can run multistep chemo-enzymatic cascade reactions.

Cited by 55 publications

References 69 publications

Hybrid Chemo-Biocatalysts Prepared in One Step from Zeolite Nanocrystals and Enzyme-Polyelectrolyte Complexes

Hybrid Chemo-Biocatalysts Prepared in One Step from Zeolite Nanocrystals and Enzyme-Polyelectrolyte Complexes

Multifunctional, Hybrid Materials Design via Spray‐Drying: Much more than Just Drying

Synthesis of hierarchical ZSM‐5 microspheres with superior performance for catalytic methanol‐to‐olefin conversion

Contact Info

Product

Resources

About