Chemoenzymatic Cascade Conversion of Methyl Parathion to 4-Aminophenol with Immobilized Organophosphate Hydrolase Onto Cu-MOF-loaded Mesoporous Silica
Journal of environmental chemical engineering(2024)
Abstract
Organophosphates (OPs), essential pesticide ingredients, are highly toxic and environmentally problematic. OPs can be efficiently hydrolyzed by the enzyme organophosphorus hydrolase (OPH). However, the resulting p-nitrophenol (4-NP) is still toxic, and its chemical reduction to p-aminophenol (4-AP) can be environmentally friendly and increase economic value. We constructed a chemical-enzymatic cascade catalyst system for methyl parathion (MP) using OPH and a copper-based metal-organic framework (HKUST-1) with 4-NP reduction catalytic activity. The nano-HKUST-1 was first loaded into aminated mesoporous silica nanospheres (MSN-NH2) to construct HKUST-1@MSN-NH2, and then OPH was immobilized into the HKUST-1@MSN-NH2 pores by a covalent method to obtain OPH@HKUST-1@MSN-NH2. The resulting composite catalyst, OPH@HKUST-1@MSN-NH2, achieved chemoenzymatic cascade catalysis of MP hydrolysis to 4-NP and subsequent reduction to 4-AP. The composite nano-biocatalyst has good catalytic performance and reusability, which can rapidly convert entirely 50μM MP to 4-AP in 8min at a dosage of 30mM NaBH4. Still, it has 77% activity after 10 cycles and a stable material structure. The present study provides a strategy for constructing a chemoenzymatic cascade catalytic system, and the obtained composite nano catalysts achieve the continuous degradation and resourceful conversion of organophosphorus pollutants, which has specific practical application value.
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Key words
Metal -organic frameworks,Organophosphorus hydrolase,Cascade reaction
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