A Biocatalytic Cascade in an Ultrastable Mesoporous Hydrogen‐Bonded Organic Framework for Point‐of‐Care Biosensing

Tang, Zhuopeng; Li, Xinyi; Tong, Linjing; Yang, Huangsheng; Wu, Jiayi; Zhang, Xiliu; Song, Ting; Huang, Siming; Zhu, Fang; Chen, Guosheng; Ouyang, Gangfeng

doi:10.1002/anie.202110351

Cited by 86 publications

(91 citation statements)

References 46 publications

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“… [41] This idea is in good agreement with examples of HOF composites that report superior Y P for amino‐modified model proteins (i. e., BSA and GFP), compared with pristine and carboxyl‐modified proteins. [ 41 , 67 ] The structures of the DAAO biocomposites were examined by X‐ray diffraction (XRD), which revealed that the diffraction patterns of DAAO@BioHOF‐1 and Z‐DAAO@BioHOF‐1 were analogous to that of as‐synthesized BioHOF‐1 (see Figure S9 and Figure 3 a). [40] …”

Section: Resultsmentioning

confidence: 99%

Combining a Genetically Engineered Oxidase with Hydrogen‐Bonded Organic Frameworks (HOFs) for Highly Efficient Biocomposites

et al. 2022

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Enzymes incorporated into hydrogen‐bonded organic frameworks (HOFs) via bottom‐up synthesis are promising biocomposites for applications in catalysis and sensing. Here, we explored synthetic incorporation of d‐amino acid oxidase (DAAO) with the metal‐free tetraamidine/tetracarboxylate‐based BioHOF‐1 in water. N‐terminal enzyme fusion with the positively charged module Zbasic2 strongly boosted the loading (2.5‐fold; ≈500 mg enzyme gmaterial−1) and the specific activity (6.5‐fold; 23 U mg−1). The DAAO@BioHOF‐1 composites showed superior activity with respect to every reported carrier for the same enzyme and excellent stability during catalyst recycling. Further, extension to other enzymes, including cytochrome P450 BM3 (used in the production of high‐value oxyfunctionalized compounds), points to the versatility of genetic engineering as a strategy for the preparation of biohybrid systems with unprecedented properties.

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Section: Resultsmentioning

confidence: 99%

Combining a Genetically Engineered Oxidase with Hydrogen‐Bonded Organic Frameworks (HOFs) for Highly Efficient Biocomposites

et al. 2022

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Section: Multienzyme Immobilization Utilizing Pofs Hostmentioning

confidence: 99%

“…1D). Since the well‐arranged mesoporous channels of HOFs enabled the accessibility of the guests that have a wide range of molecular dimensions, the HOFs‐MBCS allowed operating versatile cascade process that had previously not been explored in micropore ZIFs counterparts [5c] …”

Section: Multienzyme Immobilization Utilizing Pofs Hostmentioning

confidence: 99%

“…In addition to ABTS, chromogenic substrates including 3,3,5,5‐tetramethylbenzidine (TMB), o‐phenylenediamine (OPD) and 1,2,3‐trihydroxybenzene (THB) have been extensively used for the colorimetric glucose sensing [5b,21,27] . As well as for multienzyme@MOFs, the robust enzymes@COFs and enzymes@HOFs biocomposites were also fabricated for colorimetric determination of glucose [5c,12] …”

Section: Biosensingmentioning

confidence: 99%

“…Besides, the inherent mesoporous microenvironment of HOFs also can favor the diffusion of the substrates, thus a HOF‐MBCS bioreactor for point‐of‐care biosensing was conducted. For lactose, the dynamic linear range is 1–200×10 −5 M. Most importantly, the sensitivity was greatly improved compared with the diffusion‐limited ZIF‐8 bioreactor [5c] . Another three‐step cascade reaction, aryloxyphenoxypropionate (AOPP), herbicide hydrolase (QpeH), and alcohol oxidase (AOx) were wrapped into a magnetic ZIF‐8 by Ma et al [35] .…”

Section: Biosensingmentioning

confidence: 99%

See 2 more Smart Citations

Multienzyme Biocatalytic Cascade Systems in Porous Organic Frameworks for Biosensing

Gao

Zhong

Huang

et al. 2022

Chemistry A European J

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Multienzyme biocatalytic cascade systems (MBCS)have attracted widespread research in the field of biosensing due to selective substrate transformations and signal amplification function. However, the poor stability of enzymes significantly restricts their effectiveness in practical applications. The spatial organization of MBCS within porous organic frameworks (POFs), such as metal-organic frameworks, covalent organic frameworks, and hydrogen-bonded organic frameworks, is regarded as a promising strategy to overcome these challenges. This advanced biotechnology sets up a POFs microenvironment for enzymes immobilization, and thus make it possible to shield the enzyme from the external stimulus by POFs-guided structural confinement. Simultaneously, the tailorable porous structure of POFs shell allows for the selective transport of substrates into interior enzymes, thereby accelerating the sensing process. Herein, we present the concept of this POFs-confined MBCS, wherein enzymes were completely encapsulated into, rather than adsorption onto, the POFs. We highlight the new strategies for MBCS spatial organization through rational POFs support, and describe how this new bio-nanosystem that integrates framework and enzymes functions can be designed as a versatile biosensing platform. In addition, the challenges and outlooks are also discussed.

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Metal–Organic Frameworks Nanoarchitectures Boost Catalytic Activity for the Construction of Sensitive Immunosensor

Wang

et al. 2022

Adv Funct Materials

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Benefiting from the distinct structural features, metal-organic frameworks (MOFs) open new significant opportunities for biomacromolecule encapsulation to design biofunctional composites, whereas their biological activity and utilization efficiency remain challenging for the construction of advanced immunosensor. Herein, biomacromolecules are spatially encapsulated integration on the cavity of peptide-mediated MOFs with controllable nanoarchitectures, which amplifies the immunosensor signals via boosting bioactivity and utilization efficiency. Notably, the morphological evolution of MOFs composite including dodecahedrons, nanostars and flower-shaped nanostructures is achieved by introducing peptide surface modifier to trigger the coordination defects procedure. Nanostars are evidenced with the enhanced catalytic activity of biomacromolecules, which amplifies the recognition signal via regulating the pore channel and particle size of biomacromolecules@ MOFs composite, shortening the diffusion path of substrate molecules and promoting the interfacial contact. As proof-of-principle, imidacloprid is chosen as a model target to demonstrate the superiority of biomacromolecules@MOFs-based immunosensor. Combining the enhanced activity of biomacromolecules with size tunability of biomacromolecules@MOFs composite, 160-fold improvement in the sensitivity is obtained in comparison with the conventional enzyme-based immunoassay, paving the way for the employment of controllable nanostructures for high-sensitive biosensors.

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A Biocatalytic Cascade in an Ultrastable Mesoporous Hydrogen‐Bonded Organic Framework for Point‐of‐Care Biosensing

Cited by 86 publications

References 46 publications

Combining a Genetically Engineered Oxidase with Hydrogen‐Bonded Organic Frameworks (HOFs) for Highly Efficient Biocomposites

Combining a Genetically Engineered Oxidase with Hydrogen‐Bonded Organic Frameworks (HOFs) for Highly Efficient Biocomposites

Multienzyme Biocatalytic Cascade Systems in Porous Organic Frameworks for Biosensing

Metal–Organic Frameworks Nanoarchitectures Boost Catalytic Activity for the Construction of Sensitive Immunosensor

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