"Nanozyme" is used to describe various catalysts from immobilized inorganic metal complexes, immobilized enzymes to inorganic nanoparticles. Here, the history of nanozymes is dvescribed in detail, and they can be largely separated into two types. Type 1 nanozymes refer to immobilized catalysts or enzymes on nanomaterials, which were dominant in the first decade since 2004. Type 2 nanozymes, which rely on the surface catalytic properties of inorganic nanomaterials, are the dominating type in the past decade. The definition of nanozymes is evolving, and a definition based on the same substrates and products as enzymes are able to cover most currently claimed nanozymes, although they may have different mechanisms compared to their enzyme counterparts. A broader definition can inspire application-based research to replace enzymes with nanomaterials for analytical, environmental, and biomedical applications. Comparison with enzymes also requires a clear definition of a nanozyme unit. Four ways of defining a nanozyme unit are described, with iron oxide and horseradish peroxidase activity comparison as examples in each definition. Growing work is devoted to understanding the catalytic mechanism of nanozymes, which provides a basis for further rational engineering of active sites. Finally, future perspective of the nanozyme field is discussed.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/adma.202211041

Nanozymes: Definition, Activity, and Mechanisms.

Abstract Smart nanoparticles, which can respond to biological cues or be guided by them, are emerging as a promising drug delivery platform for precise cancer treatment. The field of oncology, nanotechnology, and biomedicine has witnessed rapid progress, leading to innovative developments in smart nanoparticles for safer and more effective cancer therapy. In this review, we will highlight recent advancements in smart nanoparticles, including polymeric nanoparticles, dendrimers, micelles, liposomes, protein nanoparticles, cell membrane nanoparticles, mesoporous silica nanoparticles, gold nanoparticles, iron oxide nanoparticles, quantum dots, carbon nanotubes, black phosphorus, MOF nanoparticles, and others. We will focus on their classification, structures, synthesis, and intelligent features. These smart nanoparticles possess the ability to respond to various external and internal stimuli, such as enzymes, pH, temperature, optics, and magnetism, making them intelligent systems. Additionally, this review will explore the latest studies on tumor targeting by functionalizing the surfaces of smart nanoparticles with tumor-specific ligands like antibodies, peptides, transferrin, and folic acid. We will also summarize different types of drug delivery options, including small molecules, peptides, proteins, nucleic acids, and even living cells, for their potential use in cancer therapy. While the potential of smart nanoparticles is promising, we will also acknowledge the challenges and clinical prospects associated with their use. Finally, we will propose a blueprint that involves the use of artificial intelligence-powered nanoparticles in cancer treatment applications. By harnessing the potential of smart nanoparticles, this review aims to usher in a new era of precise and personalized cancer therapy, providing patients with individualized treatment options. 

Smart nanoparticles for cancer therapy

Nanomaterials with more than one enzyme-like activity are termed multi-enzymic nanozymes, which have received increasing attention in recent years and hold huge potential to be applied in diverse fields, especially for biosensing and therapeutics. Compared to single enzyme-like nanozymes, multi-enzymic nanozymes offer various unique advantages, including synergistic effects, cascaded reactions, and environmentally-responsive selectivity. Nevertheless, along with these merits, the catalytic mechanism and rational design of multi-enzymic nanozymes are more complicated and elusive as compared to single-enzymic nanozymes. In this review, we systematically discussed the multi-enzymic nanozymes classification scheme based on the numbers/types of activities, the internal and external factors regulating the multi-enzymatic activities, the rational design based on chemical, biomimetic, and computer-aided strategies, and recent progress in applications attributed to the advantages of multi-catalytic activities. Finally, current challenges and future perspectives regarding the development and application of multi-enzymatic nanozymes are suggested. This review aims to deepen the understanding and inspire the research in multi-enzymic nanozymes to a greater extent. This article is protected by copyright. All rights reserved.

Multienzyme-like Nanozymes: Regulation, Rational Design, and Application.

Nanozymes constitute an emerging class of nanomaterials with enzyme-like characteristics. Over the past 15 years, more than 1200 nanozymes have been developed, and they have demonstrated promising potentials in broad applications. With the diversification and complexity of its applications, traditional empirical and trial-and-error design strategies no longer meet the requirements for efficient nanozyme design. Thanks to the rapid development of computational chemistry and artificial intelligence technologies, first-principles methods and machine-learning algorithms are gradually being adopted as a more efficient and easier means to assist nanozyme design. This review focuses on the potential elementary reaction mechanisms in the rational design of nanozymes, including peroxidase (POD)-, oxidase (OXD)-, catalase (CAT)-, superoxide dismutase (SOD)-, and hydrolase (HYL)-like nanozymes. The activity descriptors are introduced, with the aim of providing further guidelines for nanozyme active material screening. The computing- and data-driven approaches are thoroughly reviewed to give a proposal on how to proceed with the next-generation paradigm rational design. At the end of this review, personal perspectives on the prospects and challenges of the rational design of nanozymes are put forward, hoping to promote the further development of nanozymes toward superior application performance in the future.

Rational Design Strategies for Nanozymes.

Inflammation-associated diseases encompass a range of infectious diseases and non-infectious inflammatory diseases, which continuously pose one of the most serious threats to human health, attributed to factors such as the emergence of new pathogens, increasing drug resistance, changes in living environments and lifestyles, and the aging population. Despite rapid advancements in mechanistic research and drug development for these diseases, current treatments often have limited efficacy and notable side effects, necessitating the development of more effective and targeted anti-inflammatory therapies. In recent years, the rapid development of nanotechnology has provided crucial technological support for the prevention, treatment, and detection of inflammation-associated diseases. Various types of nanoparticles (NPs) play significant roles, serving as vaccine vehicles to enhance immunogenicity and as drug carriers to improve targeting and bioavailability. NPs can also directly combat pathogens and inflammation. In addition, nanotechnology has facilitated the development of biosensors for pathogen detection and imaging techniques for inflammatory diseases. This review categorizes and characterizes different types of NPs, summarizes their applications in the prevention, treatment, and detection of infectious and inflammatory diseases. It also discusses the challenges associated with clinical translation in this field and explores the latest developments and prospects. In conclusion, nanotechnology opens up new possibilities for the comprehensive management of infectious and inflammatory diseases. 

Nanotechnology’s frontier in combatting infectious and inflammatory diseases: prevention and treatment

An abundant number of nanomaterials have been discovered to possess enzyme‐like catalytic activity, termed nanozymes. It is identified that a variety of internal and external factors influence the catalytic activity of nanozymes. However, there is a lack of essential methodologies to uncover the hidden mechanisms between nanozyme features and enzyme‐like activity. Here, a data‐driven approach is demonstrated that utilizes machine‐learning algorithms to understand particle–property relationships, allowing for classification and quantitative predictions of enzyme‐like activity exhibited by nanozymes. High consistency between predicted outputs and the observations is confirmed by accuracy (90.6%) and R2 (up to 0.80). Furthermore, sensitive analysis of the models reveals the central roles of transition metals in determining nanozyme activity. As an example, the models are successfully applied to predict or design desirable nanozymes by uncovering the hidden relationship between different periods of transition metals and their enzyme‐like performance. This study offers a promising strategy to develop nanozymes with desirable catalytic activity and demonstrates the potential of machine learning within the field of material science.

Prediction and Design of Nanozymes using Explainable Machine Learning

The central dogma that nanoparticle delivery to tumours requires enhanced leakiness of vasculatures is a topic of debate. To address this, we propose a single-vessel quantitative analysis method by taking advantage of protein-based nanoprobes and image-segmentation-based machine learning (nano-ISML). Using nano-ISML, >67,000 individual blood vessels from 32 tumour models were quantified, revealing highly heterogenous vascular permeability of protein-based nanoparticles. There was a >13-fold difference in the percentage of high-permeability vessels in different tumours and >100-fold penetration ability in vessels with the highest permeability compared with vessels with the lowest permeability. Our data suggest passive extravasation and transendothelial transport were the dominant mechanisms for high- and low-permeability tumour vessels, respectively. To exemplify the nano-ISML-assisted rational design of nanomedicines, genetically tailored protein nanoparticles with improved transendothelial transport in low-permeability tumours were developed. Our study delineates the heterogeneity of tumour vascular permeability and defines a direction for the rational design of next-generation anticancer nanomedicines. Using genetically tailored protein-based nanoprobes and taking advantage of image-segmentation-based machine learning, a high-throughput assessment of vascular permeability of individual blood vessels in 32 different tumours is quantified. These insights are valuable in developing personalized anticancer nanomedicine therapeutics and strategies modulating vascular permeability to treat tumours. 

/pdf/machine-learning-assisted-single-vessel-analysis-of-20yqzsl4.pdf

Machine-learning-assisted single-vessel analysis of nanoparticle permeability in tumour vasculatures

The emergence of nanomedicine has provided a promising strategy to greatly enhance the therapeutic efficacy of O2‐dependent photodynamic therapy (PDT). However, plasma‐derived protein corona and/or discontinuous O2 supply substantially limit their tumor delivery efficiency and therapeutic outcomes. Herein, protein corona cloaking‐based cascade nanozymes are developed using genetically engineered human ferritin heavy chain nanocages (FTn) as unique pre‐coated protein corona and cascade nanozymes as steady O2 suppliers. Specifically, FTn is coated onto mesoporous silica nanoparticles (MSNs) to form FTn‐based protein corona, providing active targeting of tumor cells by binding with its receptor. In situ synthesis of ultra‐small Au nanoparticles in MSNs, and biomimetic incorporation of Ru nanoclusters into FTn inner cavity showed glucose oxidase‐like activity and catalase‐like activity, respectively. The two nanozymes are incorporated into MSNs nanoplatform to induce cascade and circular catalytic reactions by consuming glucose and H2O2 within the tumor microenvironment. Compared to MSNs alone, the FTn‐based protein corona is capable of efficiently diminishing plasma‐derived protein corona formation to prolong blood circulation time and improving in vitro tumor cell uptake and in vivo tumor accumulation, thereby providing significantly enhanced therapeutic benefits of PDT by combining with the continuously produced O2 of cascade nanozymes.

Genetically Engineered Protein Corona‐based Cascade Nanozymes for Enhanced Tumor Therapy

Correction to "Rational Design of Genetically Engineered Mitochondrial-Targeting Nanozymes for Alleviating Myocardial Ischemic-Reperfusion Injury".

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Prediction and Design of Nanozymes using Explainable Machine Learning

Machine-learning-assisted single-vessel analysis of nanoparticle permeability in tumour vasculatures

Genetically Engineered Protein Corona‐based Cascade Nanozymes for Enhanced Tumor Therapy

Correction to "Rational Design of Genetically Engineered Mitochondrial-Targeting Nanozymes for Alleviating Myocardial Ischemic-Reperfusion Injury".