Encapsulation of a Nerve Agent Detoxifying Enzyme by a Mesoporous Zirconium Metal-Organic Framework Engenders Thermal and Long-Term Stability.

Immobilized enzymes typically have greater thermal and operational stability than their soluble form. Here we report that for the first time, a nerve agent detoxifying enzyme, organophosphorus acid anhydrolase (OPAA), has been successfully encapsulated into a water-stable zirconium metal-organic framework (MOF). This MOF features a hierarchical mesoporous channel structure and exhibits a 12 wt % loading capacity of OPAA. The thermal and long-term stabilities of OPAA are both significantly enhanced after immobilization.

[1]  Peyman Z. Moghadam,et al.  Toward Design Rules for Enzyme Immobilization in Hierarchical Mesoporous Metal-Organic Frameworks , 2016 .

[2]  S. Harvey,et al.  Engineering the Organophosphorus Acid Anhydrolase Enzyme for Increased Catalytic Efficiency and Broadened Stereospecificity on Russian VX. , 2015, Biochemistry.

[3]  Jie Su,et al.  Piezofluorochromic Metal-Organic Framework: A Microscissor Lift. , 2015, Journal of the American Chemical Society.

[4]  J. Hupp,et al.  Synthesis of nanocrystals of Zr-based metal-organic frameworks with csq-net: significant enhancement in the degradation of a nerve agent simulant. , 2015, Chemical communications.

[5]  Michael J. Katz,et al.  Destruction of chemical warfare agents using metal-organic frameworks. , 2015, Nature materials.

[6]  Jie Su,et al.  Stable metal-organic frameworks containing single-molecule traps for enzyme encapsulation , 2015, Nature Communications.

[7]  Krista S. Walton,et al.  Water stability and adsorption in metal-organic frameworks. , 2014, Chemical reviews.

[8]  Diego A. Gómez-Gualdrón,et al.  Computational Design of Metal–Organic Frameworks Based on Stable Zirconium Building Units for Storage and Delivery of Methane , 2014 .

[9]  H. Furukawa,et al.  Water adsorption in porous metal-organic frameworks and related materials. , 2014, Journal of the American Chemical Society.

[10]  P. Masson,et al.  Progress in the development of enzyme-based nerve agent bioscavengers. , 2013, Chemico-biological interactions.

[11]  Michael O’Keeffe,et al.  The Chemistry and Applications of Metal-Organic Frameworks , 2013, Science.

[12]  S. Nguyen,et al.  Vapor-phase metalation by atomic layer deposition in a metal-organic framework. , 2013, Journal of the American Chemical Society.

[13]  M. Fröba,et al.  Designing Inorganic Porous Materials for Enzyme Adsorption and Applications in Biocatalysis , 2013 .

[14]  Zhangwen Wei,et al.  Zirconium-metalloporphyrin PCN-222: mesoporous metal-organic frameworks with ultrahigh stability as biomimetic catalysts. , 2012, Angewandte Chemie.

[15]  Shengqian Ma,et al.  Size-selective biocatalysis of myoglobin immobilized into a mesoporous metal-organic framework with hierarchical pore sizes. , 2012, Inorganic chemistry.

[16]  Kheireddine El-Boubbou,et al.  Enhanced Enzymatic Activity of OPH in Ammonium-Functionalized Mesoporous Silica: Surface Modification and Pore Effects , 2012 .

[17]  F. Raushel,et al.  Enzymes for the homeland defense: optimizing phosphotriesterase for the hydrolysis of organophosphate nerve agents. , 2012, Biochemistry.

[18]  D. Cascio,et al.  Synthesis, structure, and metalation of two new highly porous zirconium metal-organic frameworks. , 2012, Inorganic chemistry.

[19]  J. F. Stoddart,et al.  Large-Pore Apertures in a Series of Metal-Organic Frameworks , 2012, Science.

[20]  Saumil S. Shah,et al.  In vitro release of organophosphorus acid anhydrolase from functionalized mesoporous silica against nerve agents. , 2012, Analytical biochemistry.

[21]  Shengqian Ma,et al.  Immobilization of MP-11 into a mesoporous metal-organic framework, MP-11@mesoMOF: a new platform for enzymatic catalysis. , 2011, Journal of the American Chemical Society.

[22]  F. Raushel,et al.  Chemical biology: Catalytic detoxification , 2011, Nature.

[23]  Bernd J Pichler,et al.  A hyperspectral fluorescence system for 3D in vivo optical imaging , 2006, Physics in medicine and biology.

[24]  F. Raushel,et al.  Detoxification of organophosphate nerve agents by bacterial phosphotriesterase. , 2005, Toxicology and applied pharmacology.

[25]  V. Rastogi,et al.  Hydrolysis of acetylcholinesterase inhibitors--organophosphorus acid anhydrolase enzyme immobilization on photoluminescent porous silicon platforms. , 2005, Chemical communications.

[26]  Michael O'Keeffe,et al.  Reticular chemistry: occurrence and taxonomy of nets and grammar for the design of frameworks. , 2005, Accounts of chemical research.

[27]  J. Newmark Therapy for nerve agent poisoning. , 2004, Archives of neurology.

[28]  Joseph S. Schoeniger,et al.  Enzyme-based biosensor for the direct detection of fluorine-containing organophosphates , 2001 .

[29]  Yu-Chu Yang Chemical Detoxification of Nerve Agent VX , 1999 .

[30]  S. Harvey,et al.  Cloning and expression of a gene encoding a bacterial enzyme for decontamination of organophosphorus nerve agents and nucleotide sequence of the enzyme , 1996, Applied and environmental microbiology.

[31]  F. C. Hoskin,et al.  Hydrolysis of nerve gas by squid-type diisopropyl phosphorofluoridate hydrolyzing enzyme on agarose resin. , 1982, Science.

[32]  J. Bajgar Organophosphates/nerve agent poisoning: mechanism of action, diagnosis, prophylaxis, and treatment. , 2004, Advances in clinical chemistry.