Hierarchical covalent organic framework-foam for multi-enzyme tandem catalysis

Paul, Satyadip; Gupta, Mrinal; Dey, Kaushik; Mahato, Ashok Kumar; Bag, Saikat; Torris, Arun; Gowd, Bhoje; Sajid, Hasnain; Addicoat, Matthew A.; Datta, Supratim; Banerjee, Rahul

doi:10.1039/d3sc01367g

Cited by 16 publications

(8 citation statements)

References 67 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…In recent times, there has been a notable surge in interest in the immobilization of enzymes within porous materials . While there have been a few reports detailing the immobilization of enzymes in materials like COFs, MOFs, and HOFs, these procedures typically entail arduous steps involving enzyme purification, separation, and subsequent loading into the porous matrix .…”

Section: Resultsmentioning

confidence: 99%

Covalent Organic Frameworks for the Purification of Recombinant Enzymes and Heterogeneous Biocatalysis

Paul,

Gupta,

Kumar Mahato

et al. 2023

J. Am. Chem. Soc.

Self Cite

View full text Add to dashboard Cite

Recombinant enzymes have gained prominence due to their diverse functionalities and specificity and are often a greener alternative in biocatalysis. This context makes purifying recombinant enzymes from host cells and other impurities crucial. The primary goal is to isolate the pure enzyme of interest and ensure its stability under ambient conditions. Covalent organic frameworks (COFs), renowned for their well-ordered structure and permeability, offer a promising approach for purifying histidinetagged (His-tagged) enzymes. Furthermore, immobilizing enzymes within COFs represents a growing field in heterogeneous biocatalysis. In this study, we have developed a flow-based technology utilizing a nickel-infused covalent organic framework (Ni-TpBpy COF) to combine two distinct processes: the purification of His-tagged enzymes and the immobilization of enzymes simultaneously. Our work primarily focuses on the purification of three Histagged enzymes β-glucosidase, cellobiohydrolase, and endoglucanase as well as two proteins with varying molecular weights, namely, green fluorescent protein (27 kDa) and BG Rho (88 kDa). We employed Ni-TpBpy as a column matrix to showcase the versatility of our system. Additionally, we successfully obtained a Ni-TpBpy COF immobilized with enzymes, which can serve as a heterogeneous catalyst for the hydrolysis of p-nitrophenyl-β-D-glucopyranoside and carboxymethylcellulose. These immobilized enzymes demonstrated catalytic activity comparable to that of their free counterparts, with the added advantages of recyclability and enhanced stability under ambient conditions for an extended period, ranging from 60 to 90 days. This contrasts with the free enzymes, which do not maintain their activity as effectively over time.

show abstract

Section: Resultsmentioning

confidence: 99%

Covalent Organic Frameworks for the Purification of Recombinant Enzymes and Heterogeneous Biocatalysis

Paul,

Gupta,

Kumar Mahato

et al. 2023

J. Am. Chem. Soc.

Self Cite

View full text Add to dashboard Cite

show abstract

“…Solvothermal synthesis has been the preferred synthetic method for these materials because it favors the formation of the thermodynamic product after a trial-and-error optimization, where the synthetic conditions (e.g., temperature, concentration, and time), the preassembly of the precursors, and the reversibility of the covalent bond employed in their synthesis have proven to be critical factors to yield the most stable thermodynamic structure. − However, solvothermal synthesis typically involves a long preparation time, and the COF powders obtained through this method are often challenging to process, further impeding their practical application. , These drawbacks are especially critical when considering 3D COFs. The absence of effective preassembly mechanisms among the 3D COF precursors during synthesis (such as π–π interactions) and the limited number of 3D COF building blocks have probably prevented the development of a rapid one-pot processing approach specifically tailored for synthesizing and processing 3D COFs. − In stark contrast, several methods are available to process 2D COFs, providing a wide landscape of nanomorphologies, spanning from zero up to three-dimensional ones, i.e., from particles to the obtention of fibers, films, and foams. − …”

Section: Introductionmentioning

confidence: 99%

Large-Scale and Rapid Processing of 3D COFs via 3D-Controlled Reaction–Diffusion Zones

Mattera,

Ngo,

Vale

et al. 2024

Chem. Mater.

View full text Add to dashboard Cite

Covalent organic frameworks (COFs) are an emerging class of two-dimensional (2D) or three-dimensional (3D) porous structures. Most COFs are typically prepared via solvothermal methods involving long reaction times (>12 h) that generally result in unprocessable powders, significantly hindering their straightforward integration into devices and applications. Current processing methods for 2D COFs have not been implemented for 3D COFs, probably due to the lack of preassembly mechanisms among the 3D COF precursors during synthesis. Here, we report a pioneering synthetic environment that achieves two objectives: precise control over the reaction time of 3D COF precursors through controlled diffusion, ensuring the absence of turbulent mixing, and the ability to fine-tune the specific reaction zone where the reaction and controlled diffusion of the 3D COF precursors will occur. We further demonstrate that controlling these two features in 3D creates an unparalleled synthetic environment, allowing for a rapid one-pot synthesis of 3D COFs, with their formation occurring in less than a minute. Additionally, this approach yields self-standing 3D COF fibers on a centimeter scale, showcasing the versatility and potential of the approach presented for scalable production of 3D COFs as well as for their seamless integration into devices and patterning strategies.

show abstract

“…COFs possess nontrivial structural attributes, such as low density, high crystallinity, large specific surface area, superb chemical stability, adjustable poremetrics, and customizable skeletons. [1][2][3][4][5] Consequently, COFs hold immense promise across a wide spectrum of applications spanning gas storage, [6][7][8] chromatographic separation, [9][10][11][12][13] heterogeneous catalysis, [14][15][16][17][18] chemical sensing, [19][20][21][22][23] optoelectronics, [24][25][26] and energy storage. [27][28][29][30] Among these diverse applications, there has been a growing interest in recent years in the use of COF adsorbents with taskspecific affinity sites for the removal of aqueous pollutants.…”

Section: Introductionmentioning

confidence: 99%

Tuning the Topology of Two‐Dimensional Covalent Organic Frameworks through Site‐Selective Synthetic Strategy

Wu,

Tang,

Zhang

et al. 2024

Chemistry A European J

View full text Add to dashboard Cite

Tuning the topology of two‐dimensional (2D) covalent organic frameworks (COFs) is of paramount scientific interest but remains largely unexplored. Herein, we present a site‐selective synthetic strategy that enables the tuning of 2D COF topology by simply adjusting the molar ratio of an amine‐functionalized dihydrazide monomer (NH2‐Ah) and 4,4',4''‐(1,3,5‐triazine‐2,4,6‐triyl)tribenzaldehyde (Tz). This approach resulted in the formation of two distinct COFs: a clover‐like 2D COF with free amine groups (NH2‐Ah‐Tz) and a honeycomb‐like COF without amine groups (Ah‐Tz). Both COFs exhibited good crystallinity and moderate porosity. Remarkably, the clover‐shaped NH2‐Ah‐Tz COF, with abundant free amine groups, displayed significantly enhanced adsorption capacities toward crystal violet (CV, 261 mg/g) and congo red (CR, 1560 mg/g) compared to the nonfunctionalized honeycomb‐like Ah‐Tz COF (123 mg/g for CV and 1340 mg/g for CR), underscoring the pivotal role of free amine functional groups in enhancing adsorption capacities for organic dyes. This work highlights that the site‐selective synthetic strategy paves a new avenue for manipulating 2D COF topology by adjusting the monomer feeding ratio, thereby modulating their adsorption performances toward organic dyes.

show abstract

Hierarchical covalent organic framework-foam for multi-enzyme tandem catalysis

Abstract: Covalent organic frameworks (COFs) are ideal host matrices for biomolecule immobilization and biocatalysis due to their high porosity, various functionalities, and structural robustness. However, the porosity of COFs is limited...

Cited by 16 publications

References 67 publications

Covalent Organic Frameworks for the Purification of Recombinant Enzymes and Heterogeneous Biocatalysis

Covalent Organic Frameworks for the Purification of Recombinant Enzymes and Heterogeneous Biocatalysis

Large-Scale and Rapid Processing of 3D COFs via 3D-Controlled Reaction–Diffusion Zones

Tuning the Topology of Two‐Dimensional Covalent Organic Frameworks through Site‐Selective Synthetic Strategy

Contact Info

Product

Resources

About