Facile Synthesis of Enzyme-Embedded Metal–Organic Frameworks for Size-Selective Biocatalysis in Organic Solvent

Wang, Yangxin; Zhang, Ningning; Tan, Deming; Qi, Zhenhui; Wu, Changzhu

doi:10.3389/fbioe.2020.00714

Cited by 15 publications

(5 citation statements)

References 72 publications

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“…Curiously, ZIF growth has never been shown to degrade any biomacromolecules, even with such high concentrations of Lewis acids and alkaline ligands. To the contrary, ZIF shells grow and protect even very delicate systems like protein-embedded liposomes, enzymes, , whole yeast, , and bacteria. , To confirm that the CpG was not damaged during the encapsulation, the ZIF shells of CpG@μZIF and CpG@nZIF were removed by treatment with 0.5 M EDTA to pull Zn 2+ from the coating and recover the DNA. Using a 5% agarose gel stained with ethidium bromide, we found that the CpG was unaltered (Figure F).…”

Section: Resultsmentioning

confidence: 99%

Zeolitic Imidazolate Framework Nanoencapsulation of CpG for Stabilization and Enhancement of Immunoadjuvancy

Brohlin

Ehrman

Herbert

et al. 2022

ACS Appl. Nano Mater.

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Metal–organic frameworks (MOFs) have been used to improve vaccine formulations by stabilizing proteins and protecting them against thermal degradation. This has led to increased immunogenicity of these proteinaceous therapeutics. In this work, we show that MOFs can also be used to protect the single-stranded DNA oligomer CpG to increase its immunoadjuvancy. By encapsulation of the phosphodiester CpG in the zinc-based MOF, zeolitic imidazolate framework-8, the DNA oligomer is protected from nuclease degradation and exhibits improved cellular uptake. As a result, we have been able to achieve drastically enhanced B-cell activation in splenocyte cultures comparable to the current state-of-the-art phosphorothioate CpG. Furthermore, we have made a direct comparison of micro- and nanosized MOFs for optimization of the particulate delivery of immunoadjuvants to maximize immune activation.

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Section: Resultsmentioning

confidence: 99%

Zeolitic Imidazolate Framework Nanoencapsulation of CpG for Stabilization and Enhancement of Immunoadjuvancy

Brohlin

Ehrman

Herbert

et al. 2022

ACS Appl. Nano Mater.

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“…[4][5][6] To date, more than fifty types of nanomaterials have been found with diverse enzyme-like activities (peroxidases (PODs), oxidases (OXDs), glucose oxidases (GOxs), and so on), [7][8][9] such as the noble metals, [10][11][12] metal oxides, [13][14][15] carbon nanostructures, [16][17][18][19][20] and metal-organic frameworks (MOFs). [21][22][23][24] However, the high cost of noble metals, the low operational stability and high cytotoxicity of metal oxides, the poor accuracy of carbon-based materials due to their high absorbabilities to substrates, severally hindering their applications as sensors for detecting biomarkers. To meet the ever-increasing demands of sensors in biological applications, it is still urgent to explore new nanomaterials with satisfied detecting activity and physicochemical properties.…”

Section: Introductionmentioning

confidence: 99%

π‐Conjugated Copper Phthalocyanine Nanoparticles as Highly Sensitive Sensor for Colorimetric Detection of Biomarkers

Chen

Zhu

et al. 2022

Chemistry A European J

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Though numerous nanomaterials with enzyme-like activities have been utilized as probes and sensors for detecting biological molecules, it is still challenging to construct highly sensitive detectors for biomarkers using polymeric materials. Benefiting from the π-d delocalization effect of electrons, excellent metal-chelating property, high electron transferability, and good chemical stability of πconjugated phthalocyanine, the design of the copper phthalocyanine-based conjugated polymer nanoparticles (Cu-PcCP NPs) as a colorimetric sensor for a variety of biomarkers is reported. The Cu-PcCP NPs are synthesized through a simple microwave-assisted polymerization, and their chemical structures are thoroughly characterized. The colorimetric results of Cu-PcCP NPs demonstrate excellent peroxidase-like detecting activity and also great substrate selectivity than most of the reported Cu-based nanomaterials. The Cu-PcCP NPs can achieve a detection limit of 4.88 μM for the H 2 O 2 , 4.27 μM for the L-cysteine, and 21.10 μM for the glucose via a cascade catalytic system, which shows comparable detecting sensitivity as that of many earlier reported enzyme-like nanomaterials. Moreover, Cu-PcCP NPs present remarkable resistance to harsh conditions, including high temperature, low pH, and excessive salts. These highly specific π-conjugated copper-phthalocyanine nanoparticles not only overcome the current limitation of polymeric material-based sensors but also provide a new direction for designing next-generation enzyme-like nanomaterial-based colorimetric biosensors.

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“…Polymers are holding breakthrough advantages for customizing protein catalysts. , Unlike time-consuming genetic evolution, , polymer catalysts can be modularly designed with a high degree of specificity and tunability in a short period of time. − The development of various polymerization methods allows for the fine-tuning of structures and density of catalytic species based on structure–property relations. − Combined with an in-depth understanding of catalytic reaction mechanisms, tailored catalysts can be easily developed to have improved catalytic reactivity and beneficial macromolecular effects. − Despite these merits, the application of polymer catalysts in modular design of artificial enzymes is still limited.…”

Section: Introductionmentioning

confidence: 99%

Tailoring Protein–Polymer Conjugates as Efficient Artificial Enzymes for Aqueous Asymmetric Aldol Reactions

Zhang

2022

ACS Synth. Biol.

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Artificial enzymes are becoming a powerful toolbox for selective organic syntheses. Herein, we first propose an advanced artificial enzyme by polymeric modularity as an efficient aldolase mimic for aqueous asymmetric aldol reactions. Based on an in-depth understanding of the aldolase reaction mechanism and our previous work, we demonstrate the modular design of protein−polymer conjugates by co-incorporating L-proline and styrene onto a noncatalytic protein scaffold with a high degree of controllability. The tailored conjugates exhibited remarkable catalytic performance toward the aqueous asymmetric aldol reaction of p-nitrobenzaldehyde and cyclohexanone, achieving 94% conversion and excellent selectivity (95/5 diastereoselectivity, 98% enantiomeric excess). In addition, this artificial enzyme showed high tolerance against extreme conditions (e.g., wide pH range, high temperature) and could be reused for more than four times without significant loss of reactivity. Experiments have shown that the artificial enzyme displayed broad specificity for various aldehydes.

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Facile Synthesis of Enzyme-Embedded Metal–Organic Frameworks for Size-Selective Biocatalysis in Organic Solvent

Cited by 15 publications

References 72 publications

Zeolitic Imidazolate Framework Nanoencapsulation of CpG for Stabilization and Enhancement of Immunoadjuvancy

Zeolitic Imidazolate Framework Nanoencapsulation of CpG for Stabilization and Enhancement of Immunoadjuvancy

π‐Conjugated Copper Phthalocyanine Nanoparticles as Highly Sensitive Sensor for Colorimetric Detection of Biomarkers

Tailoring Protein–Polymer Conjugates as Efficient Artificial Enzymes for Aqueous Asymmetric Aldol Reactions

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