Biomimetic single Al-OH site with high acetylcholinesterase-like activity and self-defense ability for neuroprotection

Abstract

Neurotoxicity of organophosphate compounds (OPs) can catastrophically cause nervous system injury by inhibiting acetylcholinesterase (AChE) expression. Although artificial systems have been developed for indirect neuroprotection, they are limited to dissociating P-O bonds for eliminating OPs. However, these systems have failed to overcome the deactivation of AChE. Herein, we report our finding that Al3+ is engineered onto the nodes of metal–organic framework to synthesize MOF-808-Al with enhanced Lewis acidity. The resultant MOF-808-Al efficiently mimics the catalytic behavior of AChE and has a self-defense ability to break the activity inhibition by OPs. Mechanism investigations elucidate that Al3+ Lewis acid sites with a strong polarization effect unite the highly electronegative –OH groups to form the enzyme-like catalytic center, resulting in superior substrate activation and nucleophilic attack ability with a 2.7-fold activity improvement. The multifunctional MOF-808-Al, which has satisfactory biosafety, is efficient in reducing neurotoxic effects and preventing neuronal tissue damage.

Atomic-level design of metalloenzyme-like active pockets in metal–organic frameworks for bioinspired catalysis

“…23a). 199 Highly toxic OPs can irreversibly inhibit the bioactivity of AChE, causing fatal nerve injury. In this regard, the mononuclear Al III –OH species were incorporated into the node of MOF-808 to obtain MOF-808-Al for recapitulating the catalytic behaviour of AChE.…”

Programmable Lanthanide Metal–Organic Framework for Ultra-Efficient Nucleic Acids Extraction and Interaction Analysis

“…Biochemical research based on metal–organic frameworks (MOFs) is a very attractive topic in the field of modern chemistry, given its extensive potential for application in fields such as medicine and pharmacy. − Due to their diverse and adjustable structures, MOFs provide a powerful platform for the design of multifunctional nanomaterials. , They often have advantages over other nanomaterials in terms of flexibility and adjustability, such as MXene , or polymers . The research on nanozymes based on MOFs has made significant progress and has been widely applied in multidisciplinary fields, such as artificial photosynthesis, − carbon dioxide storage, methane oxidation, catalytic degradation of organic pollutants, biosensing, , disease treatment, − etc. However, so far, few studies have focused on the enormous potential of MOFs as affinity nanomaterials, which limits the possibility of MOFs performing more practical functions, especially in nucleic acids analysis.…”

Improvement in ORR Durability of Fe Single-Atom Carbon Catalysts Hybridized with CeO2 Nanozyme

“…However, the high cost of natural enzymes and their harsh living conditions render their use in electrocatalysis impractical. Fortunately, the emergence of nanozymes with multienzyme properties overcomes the limitations of natural enzymes. − Specifically, nanozymes with SOD-like and CAT-like activities have been widely explored in many fields including tumor therapy, − environment protection, , and analysis sensing , because of their antioxidant capabilities. Therefore, the rational design of nanozymes with SOD-like and CAT-like activities presents a potential alternative to natural enzymes as ROS scavengers, actively mitigating the destructive effects of ROS during the ORR procedure for FeNC catalysts.…”