A study investigated the synergetic catalytic effect in heterogeneous nanocomposite catalysts, focusing on aspects such as the synthesis of nanocomposite catalysts and the advantages of ...mesostructured composites. More research is needed in order to better understand this topic.
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Hollow‐structured mesoporous materials (HMMs), as a kind of mesoporous material with unique morphology, have been of great interest in the past decade because of the subtle combination of the hollow ...architecture with the mesoporous nanostructure. Benefitting from the merits of low density, large void space, large specific surface area, and, especially, the good biocompatibility, HMMs present promising application prospects in various fields, such as adsorption and storage, confined catalysis when catalytically active species are incorporated in the core and/or shell, controlled drug release, targeted drug delivery, and simultaneous diagnosis and therapy of cancers when the surface and/or core of the HMMs are functionalized with functional ligands and/or nanoparticles, and so on. In this review, recent progress in the design, synthesis, functionalization, and applications of hollow mesoporous materials are discussed. Two main synthetic strategies, soft‐templating and hard‐templating routes, are broadly sorted and described in detail. Progress in the main application aspects of HMMs, such as adsorption and storage, catalysis, and biomedicine, are also discussed in detail in this article, in terms of the unique features of the combined large void space in the core and the mesoporous network in the shell. Functionalization of the core and pore/outer surfaces with functional organic groups and/or nanoparticles, and their performance, are summarized in this article. Finally, an outlook of their prospects and challenges in terms of their controlled synthesis and scaled application is presented.
Hollow‐structured mesoporous materials (HMMs), a type of mesoporous material with a unique morphology, present promising application prospects in the fields of storage, adsorption and separation, confined catalysis, controlled drug release, and simultaneous diagnosis and therapy of cancers, owing to the subtle combination of the hollow architecture with the mesoporous nanostructure.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
3.
Electrocatalytic Hydrogen Production Trilogy Li, Yan; Wei, Xinfa; Chen, Lisong ...
Angewandte Chemie International Edition,
September 1, 2021, Volume:
60, Issue:
36
Journal Article
Peer reviewed
H2 production via water electrolysis is of great significance in clean energy production, which, however, suffers from the sluggish kinetics of the anodic oxygen evolution reaction (OER). Moreover, ...the anode product, O2, which is of rather low value, may lead to dangerous explosions and the generation of membrane‐degrading reactive oxygen species. Herein, to address these issues of electrocatalytic H2 production, we summarize the most recent advances in three stages based on the benefit increments and various electron donation routes, which are: 1) electron donation by traditional OER: developing efficient catalysts for water oxidation to promote H2 production; 2) electron donation by the oxidation of sacrificial agents: using sacrificial agents to assist H2 production; 3) electron donation by electrosynthesis reaction: achieving electrosynthesis in parallel with cathodic H2 production. Present challenges and related prospects will also be discussed, hopefully to benefit the further progress of electrocatalytic H2 generation.
Three stages of high‐efficient, low‐cost, and energy‐saving electrochemical hydrogen production are described in this Review based on the benefits and electron donation routes (donators) for hydrogen evolution. Future developments in electrocatalytic hydrogen production should benefit from these insights.
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Tumor cells metabolize in distinct pathways compared with most normal tissue cells. The resulting tumor microenvironment would provide characteristic physiochemical conditions for selective tumor ...modalities. Here we introduce a concept of sequential catalytic nanomedicine for efficient tumor therapy by designing and delivering biocompatible nanocatalysts into tumor sites. Natural glucose oxidase (GOD, enzyme catalyst) and ultrasmall Fe
O
nanoparticles (inorganic nanozyme, Fenton reaction catalyst) have been integrated into the large pore-sized and biodegradable dendritic silica nanoparticles to fabricate the sequential nanocatalyst. GOD in sequential nanocatalyst could effectively deplete glucose in tumor cells, and meanwhile produce a considerable amount of H
O
for subsequent Fenton-like reaction catalyzed by Fe
O
nanoparticles in response to mild acidic tumor microenvironment. Highly toxic hydroxyl radicals are generated through these sequential catalytic reactions to trigger the apoptosis and death of tumor cells. The current work manifests a proof of concept of catalytic nanomedicine by approaching selectivity and efficiency concurrently for tumor therapeutics.The specific metabolism of cancer cells may allow for selective tumor therapeutics. Here, the authors show that a suitable combination of an enzyme and iron nanoparticles loaded on dendritic silica induces apoptosis of cancer cells in response to the glucose-reliant and mild acidic microenvironment.
Ascorbate, a kind of polyhydroxy compound with a long history, has been extensively considered as an efficient antioxidant. However, only in the past several decades its pro-oxidation characteristic ...in the presence of transition metal catalysts has been gradually uncovered, attracting broad attention from researchers in chemistry and biology for benefiting various practical applications, such as anticancer therapy. In this work, we report catalytic ascorbate oxidation and reactive oxygen species generation for efficient tumor chemotherapy by an iron-engineered and ascorbate-loaded hollow mesoporous silica nanomedicine. The −Si–O–Fe– hybrid framework of nanomedicine not only enables acidity-triggered degradability and ascorbate release capability but also provides an abundant Fe ion source for catalyzing ascorbate oxidation, hydrogen peroxide formation, and subsequent Fenton reactions. The detailed chemical mechanism of Fe3+-catalyzed ascorbate oxidation has been explored in detail as two one-electron reaction processes, between which the first one involves the sequential Fe3+ and O2 captures by ascorbate to form a metal–ascorbate–oxygen ternary complex favoring hydrogen peroxide generation. Both in vitro and in vivo results demonstrate the significantly enhanced anticancer efficacy of ascorbate oxidation catalyzed by the composite nanomedicine, demonstrating high feasibility of this synergistic therapeutic concept. It is expected that such a nanomedicine design would be beneficial to future advances in the field of ascorbate.
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Ultrasound (US)-triggered sonodynamic therapy (SDT) can solve the critical issue of low tissue-penetrating depth of traditional phototriggered therapies, but the SDT efficacy is still not ...satisfactorily high in combating cancer at the current stage. Here we report on augmenting the SDT efficacy based on catalytic nanomedicine, which takes the efficient catalytic features of nanoenzymes to modulate the tumor microenvironment (TME). The multifunctional nanosonosensitizers have been successfully constructed by the integration of a MnO x component with biocompatible/biodegradable hollow mesoporous organosilica nanoparticles, followed by conjugation with protoporphyrin (as the sonosensitizer) and cyclic arginine-glycine-aspartic pentapeptide (as the targeting peptide). The MnO x component in the composite nanosonosensitizer acts as an inorganic nanoenzyme for converting the tumor-overexpressed hydrogen peroxide (H2O2) molecules into oxygen and enhancing the tumor oxygen level subsequently, which has been demonstrated to facilitate SDT-induced reactive oxygen species production and enhance SDT efficacy subsequently. The targeted accumulation of these composite nanosonosensitizers efficiently suppressed the growth of U87 tumor xenograft on nude mice after US-triggered SDT treatment. The high in vivo biocompatibility and easy excretion of these multifunctional nanosonosensitizers from the body have also been evaluated and demonstrated to guarantee their future clinical translation, and their TME-responsive T 1-weighted magnetic resonance imaging capability provides the potential for therapeutic guidance and monitoring during SDT.
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Recent marked technological advances in the field of exosome nanotechnology have provided unprecedented opportunities to bloom the developments of exosome‐related biology, chemistry, pathology, and ...therapeutics, which have laid a solid basis for scientific community to design exosome‐based nanotheranostic platforms. The unique structural/compositional/morphological characteristics of exosomes as natural nanocarriers, as well as their fascinating physicochemical/biochemical properties, which underpin their special physiopathological roles, have triggered the concept that these cell‐derived nanovesicles with intrinsic biological functions can be highly competent for the establishment of next‐generation nanomedicine. Herein, efforts are made to give a comprehensive overview on the recent advances of exosome nanotechnology based on the representative examples of the current state of the art of exosome‐based research, ranging from their formation, biological function, preparation, and characterization to their extensive nanomedical applications. It is highly expected that the better and clearer elucidation of the fundamental principles for advanced nanotechnology in constructing exosome‐based theranostic nanoplatforms, as well as integrating the intrinsic advantages of exosomes as endogenous cell‐derived nanocarriers with the advanced design methodology of traditional nanomedicine, will help to unlock the innate powers of exosomes for the establishment of next‐generation theranostic nanoplatforms.
The fascinating physicochemical/biochemical properties of exosomes have triggered the concept that these cell‐derived nanovesicles with intrinsic biological functions can be highly competent for the establishment of next‐generation nanomedicine. A comprehensive overview is given on the recent advances of exosome biochemistry and nanotechnology, ranging from their formation, biological function, preparation, and characterization to their extensive nanomedical applications.
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Hydrogen production by electrocatalytic water splitting is an efficient and economical technology, however, is severely impeded by the kinetic-sluggish and low value-added anodic oxygen evolution ...reaction. Here we report the nickel-molybdenum-nitride nanoplates loaded on carbon fiber cloth (Ni-Mo-N/CFC), for the concurrent electrolytic productions of high-purity hydrogen at the cathode and value-added formate at the anode in low-cost alkaline glycerol solutions. Especially, when equipped with Ni-Mo-N/CFC at both anode and cathode, the established electrolyzer requires as low as 1.36 V of cell voltage to achieve 10 mA cm
, which is 260 mV lower than that in alkaline aqueous solution. Moreover, high Faraday efficiencies of 99.7% for H
evolution and 95.0% for formate production have been obtained. Based on the excellent electrochemical performances of Ni-Mo-N/CFC, electrolytic H
and formate productions from the alkaline glycerol solutions are an energy-efficient and promising technology for the renewable and clean energy supply in the future.
Ceramic biomaterials have been investigated for several decades, but their potential biomedical applications in cancer therapy have been paid much less attentions, mainly due to their lack of related ...material functionality for combating the cancer. In this work, we report, for the first time, that MAX ceramic biomaterials exhibit the unique functionality for the photothermal ablation of cancer upon being exfoliated into ultrathin nanosheets within atomic thickness (MXene). As a paradigm, biocompatible Ti3C2 nanosheets (MXenes) were successfully synthesized based on a two-step exfoliation strategy of MAX phase Ti3AlC2 by the combined HF etching and TPAOH intercalation. Especially, the high photothermal-conversion efficiency and in vitro/in vivo photothermal ablation of tumor of Ti3C2 nanosheets (MXenes) were revealed and demonstrated, not only in the intravenous administration of soybean phospholipid modified Ti3C2 nanosheets but also in the localized intratumoral implantation of a phase-changeable PLGA/Ti3C2 organic–inorganic hybrid. This work promises the great potential of Ti3C2 nanosheets (MXenes) as a novel ceramic photothermal agent used for cancer therapy and may arouse much interest in exploring MXene-based ceramic biomaterials to benefit the biomedical applications.
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Hypoxia development in tumor is closely associated with its increased aggressiveness and strong resistance to therapy, leading to the poor prognosis in several cancer types. Clinically, invasive ...oxygen microelectrode and high dosage radiotherapy are often utilized to accurately detect and effectively fight hypoxia. Recently, however, there has been a surge of interdisciplinary research aiming at developing functional molecules and nanomaterials that can be used to noninvasively image and efficiently treat hypoxic tumors. In this review, we will provide an overview of the reports published to date on the imaging and therapy of hypoxic tumors. First, we will present the design concepts and engineering of various hypoxia-responsive probes that can be applied to image hypoxia noninvasively, in an order of fluorescent imaging, positron emission tomography, magnetic resonance imaging, and photoacoustic imaging. Then, we will summarize the up-to-date functional nanomaterials which can be used for the effective treatments of tumor hypoxia. The well-established chemical functions of these elaborately designed nanostructures will enable clinicians to adopt specific treatment concepts by overcoming or even utilizing hypoxia. Finally, challenges and future perspectives facing the researchers in the field will be discussed.
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