Clinical treatment of pathogenic infection has emerged as a growing challenge in global public health. Such treatment is currently limited to antibiotics, but abuse of antibiotics have induced ...multidrug resistance and high fatality rates in anti‐infection therapies. Thus, it is vital to develop alternative bactericidal agents to open novel disinfection pathways. Drawing inspiration from elements of the human immune system that show great potential for controlling pathogens or regulating cell apoptosis, the design of biocatalytic nanomaterials (BCNs) have provided unrivaled opportunities for future antibacterial therapies. More significantly, BCNs exhibit various superior properties to immune cells and natural enzymes, such as higher biocatalytic performance, extraordinary stability against harsh conditions, and scalable production. In this review, the most recent efforts toward developing BCN‐based biomedical applications in combating bacterial infections are focused upon. BCNs’ antibacterial mechanisms, the classification of BCNs, antibacterial activities that can be triggered or augmented by energy conversion, and the eradication of biofilms with BCNs are systematically introduced and discussed. The current challenges and prospects of BCNs for biocatalytic disinfection are also summarized. It is anticipated this review will provide new therapeutic insights into combating bacteria and biofilms and offer significant new inspiration for designing future biocatalytic nanomaterials.
Recent advancements toward developing biocatalytic nanomaterials (BCNs) as a new pathway for bacterial disinfection are systematically reviewed. The antibacterial mechanism, classification of BCNs, energy‐conversion‐triggered or augmented biocatalytic activities, and biofilms’ eradication are thoroughly discussed. Besides, the challenges and prospects for biocatalytic disinfection are summarized. This review may offer abundant inspirations for designing new BCNs for combating bacteria/biofilms.
Abstract
Pathogenic drug-resistant bacteria represent a threat to human health, for instance, the methicillin-resistant
Staphylococcus aureus
(MRSA). There is an ever-growing need to develop ...non-antibiotic strategies to fight bacteria without triggering drug resistance. Here, we design a hedgehog artificial macrophage with atomic-catalytic centers to combat MRSA by mimicking the “capture and killing” process of macrophages. The experimental studies and theoretical calculations reveal that the synthesized materials can efficiently capture and kill MRSA by the hedgehog topography and substantial generation of •O
2
−
and HClO with its Fe
2
N
6
O catalytic centers. The synthesized artificial macrophage exhibits a low minimal inhibition concentration (8 μg/mL Fe-Art M with H
2
O
2
(100 μM)) to combat MRSA and rapidly promote the healing of bacteria-infected wounds on rabbit skin. We suggest that the application of this hedgehog artificial macrophage with “capture and killing” capability and high ROS-catalytic activity will open up a promising pathway to develop antibacterial materials for bionic and non-antibiotic disinfection strategies.
Developing low‐cost electrocatalysts for efficient and robust oxygen evolution reaction (OER) is the key for scalable water electrolysis, for instance, NiFe‐based materials. Decorating NiFe catalysts ...with other transition metals offers a new path to boost their catalytic activities but often suffers from the low controllability of the electronic structures of the NiFe catalytic centers. Here, we report an interfacial atom‐substitution strategy to synthesize an electrocatalytic oxygen‐evolving NiFeV nanofiber to boost the activity of NiFe centers. The electronic structure analyses suggest that the NiFeV nanofiber exhibits abundant high‐valence Fe via a charge transfer from Fe to V. The NiFeV nanofiber supported on a carbon cloth shows a low overpotential of 181 mV at 10 mA cm−2, along with long‐term stability (>20 h) at 100 mA cm−2. The reported substitutional growth strategy offers an effective and new pathway for the design of efficient and durable non‐noble metal‐based OER catalysts.
An electrocatalytic oxygen‐evolving NiFeV nanofiber was synthesized by an interfacial atom‐substitution strategy to boost the activity of the NiFe centers. The electronic structure analyses suggest that the NiFeV nanofiber exhibits abundant high‐valence Fe via a charge transfer from Fe to V. The reported substitutional growth strategy offers an effective and new pathway for the design of efficient and durable non‐noble metal‐based oxygen evolution reaction (OER) catalysts.
Exploring highly active, stable electrocatalysts with earth‐abundant metal centers for the oxygen reduction reaction (ORR) is essential for sustainable energy conversion. Due to the high cost and ...scarcity of platinum, it is a general trend to develop metal–N–C (M–N–C) electrocatalysts, especially those prepared from the zeolite imidazolate framework (ZIF) to replace/minimize usage of noble metals in ORR electrocatalysis for their amazingly high catalytic efficiency, great stability, and readily‐tuned electronic structure. In this review, the most pivotal advances in mechanisms leading to declined catalytic performance, synthetic strategies, and design principles in engineering ZIF‐derived M–N–C for efficient ORR catalysis, are presented. Notably, this review focuses on how to improve intrinsic ORR activity, such as M–Nx–Cy coordination structures, doping metal‐free heteroatoms in M–N–C, dual/multi‐metal sites, hydrogen passivation, and edge‐hosted M–Nx. Meanwhile, how to increase active sites density, including formation of M–N complex, spatial confinement effects, and porous structure design, are discussed. Thereafter, challenges and future perspectives of M–N–C are also proposed. The authors believe this instructive review will provide experimental and theoretical guidance for designing future, highly active ORR electrocatalysts, and facilitate their applications in diverse ORR‐related energy technologies.
Recent advances in designing ZIF‐derived atomic metal–N–C electrocatalysts for the oxygen reduction reaction are presented. The authors present the most pivotal advances, synthetic strategies, and performance decline mechanisms; design principles for improving the intrinsic ORR activity and increasing the number of active sites are systematically discussed. The challenges and future perspectives of metal–N–C electrocatalysts are also highlighted.
The diversity, complexity, and heterogeneity of malignant tumor seriously undermine the efficiency of mono‐modal treatment. Recently, multi‐modal therapeutics with enhanced antitumor efficiencies ...have attracted increasing attention. However, designing a nanotherapeutic platform with uniform morphology in nanoscale that integrates with efficient chem‐/sono‐/photo‐trimodal tumor therapies is still a great challenge. Here, new and facile Pd‐single‐atom coordinated porphyrin‐based polymeric networks as biocatalysts, namely, Pd‐Pta/Por, for chem‐/sono‐/photo‐trimodal tumor therapies are designed. The atomic morphology and chemical structure analysis prove that the biocatalyst consists of atomic Pd‐N coordination networks with a Pd‐N2‐Cl2 catalytic center. The characterization of peroxidase‐like catalytic activities displays that the Pd‐Pta/Por can generate abundant •OH radicals for chemodynamic therapies. The ultrasound irradiation or laser excitation can significantly boost the catalytic production of 1O2 by the porphyrin‐based sono‐/photosensitizers to achieve combined sono‐/photodynamic therapies. The superior catalytic production of •OH is further verified by density functional theory calculation. Finally, the corresponding in vitro and in vivo experiments have demonstrated their synergistic chem‐/sono‐/photo‐trimodal antitumor efficacies. It is believed that this study provides new promising single‐atom‐coordinated polymeric networks with highly efficient biocatalytic sites and synergistic trimodal therapeutic effects, which may inspire many new findings in reactive oxygen species‐related biological applications across broad therapeutics and biomedical fields.
A precisely designed Pd single‐atom coordinated biocatalyst (Pd‐Pta/Por) is synthesized for achieving chem‐/sono‐/photo‐trimodal dynamic tumor therapies. Experimental results and theoretical calculations demonstrate that the Pd‐Pta/Por biocatalyst consists of atomic Pd‐N coordination active sites and has efficient catalytic yield of reactive oxygen species (ROS) for highly synergistic antitumor therapies, which takes an essential step toward developing ROS‐related therapeutic and biological applications.
Nanomaterial‐based enzyme‐mimetic catalysts (Enz‐Cats) have received considerable attention because of their optimized and enhanced catalytic performances and selectivities in diverse physiological ...environments compared with natural enzymes. Recently, owing to their molecular/atomic‐level catalytic centers, high porosity, large surface area, high loading capacity, and homogeneous structure, metal–organic frameworks (MOFs) have emerged as one of the most promising materials in engineering Enz‐Cats. Here, the recent advances in the design of MOF‐engineered Enz‐Cats, including their preparation methods, composite constructions, structural characterizations, and biomedical applications, are highlighted and commented upon. In particular, the performance, selectivities, essential mechanisms, and potential structure–property relations of these MOF‐engineered Enz‐Cats in accelerating catalytic reactions are discussed. Some potential biomedical applications of these MOF‐engineered Enz‐Cats are also breifly proposed. These applications include, for example, tumor therapies, bacterial disinfection, tissue regeneration, and biosensors. Finally, the future opportunities and challenges in emerging research frontiers are thoroughly discussed. Thereby, potential pathways and perspectives for designing future state‐of‐the‐art Enz‐Cats in biomedical sciences are offered.
Recent advancements in metal–organic‐framework‐engineered enzyme‐mimetic catalysts (Enz‐Cats) are highlighted. The catalytic activities, essential mechanisms, and potential structure–property relations of these Enz‐Cats in accelerating biological reactions are discussed. In addition, the potential biomedical applications and challenges are summarized. Thus, promising avenues for designing future state‐of‐the‐art Enz‐Cats in biomedical applications are provided.
Severe infectious diseases caused by pathogenic bacteria have become urgent threats to global public health. Antibacterial materials with combined chemo‐photothermal therapeutic capabilities possess ...distinct advantages when compared with many other antibacterial approaches. However, developing simplified and chemically tunable precursors to synthesize such antibacterial nanoagents for rapidly, safely, and synergistically combating pathogenic bacteria remains a huge challenge. Herein, metal–organic framework (MOF)‐derived nanocarbons with near‐infrared (NIR)‐responsive and size‐transformable capabilities are designed to overcome this challenge. The MOF‐derived nanocarbons with chemo‐photothermal bactericidal capabilities are first synthesized, and then coated with a thermoresponsive gel layer to obtain ON–OFF switching capability for bacterial trapping. The fabricated nanocarbons exhibit high photo‐to‐thermal conversion efficiency and fast size transformation from nanodispersions to micrometer aggregations upon NIR irradiation, thus enabling nanocarbons to generate localized massive heat and abundant Zn2+ ions for directly disrupting bacterial membrane and intracellular proteins. Furthermore, these nanocarbons not only exhibit a nearly 100% bactericidal ratio at very low dosage, but also possess highly efficient and safe wound disinfection activities, which are comparable to vancomycin. Overall, these proposed novel nanocarbons display robust and localized chemo‐photothermal bactericidal capability and possess great potential to be used as alternative to antibiotics for broad‐spectrum eradication of pathogenic bacteria.
Size‐transformable metal–organic framework–derived nanocarbons with ON–OFF near‐infrared switching capability for chemo‐photothermal disinfection are demonstrated. The unique transformation from nanodispersions to micrometer aggregations enables nanocarbons to generate localized massive heat and abundant Zn2+ ions for directly disrupting bacterial membrane and intracellular substances. Such novel nanocarbons provide great potential to be used as alternative to antibiotics for broad‐spectrum eradication of pathogenic bacteria.
Recent emerged antibacterial agents provide enormous new possibilities to replace antibiotics in fighting bacterial infectious diseases. Although abundant types of nanoagents are developed for ...preventing pathogen colonization, however, rationally design of nonchemotherapic, robust, and clinical‐adaptable nanoagents with tunable bacterial trap and killing activities remains a major challenge. Here, a demonstration of controlling the trap, ablation, and release activities of pathogenic bacteria via stimulus‐responsive regulatory mechanism is reported. First, temperature‐sensitive polymer brush is chemically grown onto carbon nanotube–Fe3O4, whereby the synthesized nanoagents can transfer from hydrophilic dispersion to hydrophobic aggregation upon near‐infrared light irradiation, which thus controls the bacterial trap, killing, and detaching. In turn, the formed aggregations will serve as localized heating sources to enhance photothermal ablation of bacteria. Systematically antibacterial experiments and mouse wound disinfection demonstrate the ultrarobust and recyclable disinfection capability of nanoagents with nearly 100% killing ratio to Staphylococcus aureus. Overall, for the first time, we represent a pioneering study on designing nonchemotherapic and robust dual‐responsive nanoagents that can sensitively and reversibly trap, inactivate, and detach bacteria. We envision that such nanoagents will not only have potential applications in pathogenic bacteria prevention but also provide a new pathway for wound disinfection, implant sterilization, and also live bacteria transportation.
A nonchemotherapic and robust dual‐responsive antibacterial nanoagent to control the trap, ablation, and release of pathogenic bacteria is established. The unique dispersion–aggregation transformation capability endows nanoagents with ultrarobust and recyclable disinfection activity both in vitro and in vivo. Such nanoagents will provide a new pathway for bacteria and biofilm prevention, wound disinfection, implants sterilization, and also live bacteria transportation.
Besides the pandemic caused by the coronavirus outbreak, many other pathogenic microbes also pose a devastating threat to human health, for instance, pathogenic bacteria. Due to the lack of ...broad‐spectrum antibiotics, it is urgent to develop nonantibiotic strategies to fight bacteria. Herein, inspired by the localized “capture and killing” action of bacteriophages, a virus‐like peroxidase‐mimic (V‐POD‐M) is synthesized for efficient bacterial capture (mesoporous spiky structures) and synergistic catalytic sterilization (metal–organic‐framework‐derived catalytic core). Experimental and theoretical calculations show that the active compound, MoO3, can serve as a peroxo‐complex‐intermediate to reduce the free energy for catalyzing H2O2, which mainly benefits the generation of •OH radicals. The unique virus‐like spikes endow the V‐POD‐M with fast bacterial capture and killing abilities (nearly 100% at 16 µg mL–1). Furthermore, the in vivo experiments show that V‐POD‐M possesses similar disinfection treatment and wound skin recovery efficiencies to vancomycin. It is suggested that this inexpensive, durable, and highly reactive oxygen species (ROS) catalytic active V‐POD‐M provides a promising broad‐spectrum therapy for nonantibiotic disinfection.
A bioinspired, spiky, and highly catalytic‐active virus‐like peroxidase‐mimic (V‐POD‐M) is synthesized for the localized “capture and killing” eradication of pathogenic bacteria. Experimental and theoretical calculations demonstrate that the V‐POD‐M exhibits strong bacterial interactions and efficient capture, synergistic catalytic sterilization, and similar in vivo disinfection efficiency to that of vancomycin, which provides a promising broad‐spectrum therapy for nonantibiotic disinfection.
Novel bionanocatalysts have opened a new era in fighting multidrug‐resistant (MDR) bacteria. They can kill bacteria by elevating the level of reactive oxygen species (ROS) in the presence of ...chemicals like H2O2. However, ROSs’ ultrashort diffusion distance limit their bactericidal activity. We present a nanohook‐equipped bionanocatalyst (Ni@Co‐NC) with bacterial binding ability that shows robust ROS‐generating capacity under physiological H2O2 levels. The Ni@Co‐NC's pH‐dependent performance confines its effects to the biofilm microenvironment, leaving healthy tissue unaffected. Furthermore, it can generate heat upon NIR laser irradiation, enhancing its catalytic performance while achieving heat ablation against bacteria. With the Ni@Co‐NC's synergistic effects, bacterial populations fall by >99.99 %. More surprisingly, the mature biofilm shows no recurrence after treatment with the Ni@Co‐NC, demonstrating its tremendous potential for treating MDR bacterial related infections.
A nanohook‐equipped bionanocatalyst can firstly hook to bacteria and biofilm, then catalyze H2O2 to generate toxic hydroxyl radicals for localized disinfection. Upon the near‐infrared laser irradiation, the bionanocatalyst can generate heat, which simultaneously accelerates the catalytic therapy and enables the heat ablation against bacteria.
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