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      Self-assembled single-atom nanozyme for enhanced photodynamic therapy treatment of tumor

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          Abstract

          Hypoxia of solid tumor compromises the therapeutic outcome of photodynamic therapy (PDT) that relies on localized O 2 molecules to produce highly cytotoxic singlet oxygen ( 1O 2) species. Herein, we present a safe and versatile self-assembled PDT nanoagent, i.e., OxgeMCC-r single-atom enzyme (SAE), consisting of single-atom ruthenium as the active catalytic site anchored in a metal-organic framework Mn 3[Co(CN) 6] 2 with encapsulated chlorin e6 (Ce6), which serves as a catalase-like nanozyme for oxygen generation. Coordination-driven self-assembly of organic linkers and metal ions in the presence of a biocompatible polymer generates a nanoscale network that adaptively encapsulates Ce6. The resulted OxgeMCC-r SAE possesses well-defined morphology, uniform size distribution and high loading capacity. When conducting the in situ O 2 generation through the reaction between endogenous H 2O 2 and single-atom Ru species of OxgeMCC-r SAE, the hypoxia in tumor microenvironment is relieved. Our study demonstrates a promising self-assembled nanozyme with highly efficient single-atom catalytic sites for cancer treatment.

          Abstract

          The hypoxic microenvironment in solid tumors limits the efficacy of photodynamic therapy (PDT) since oxygen is necessary to produce high cytotoxic singlet oxygen species. Here, the authors develop an improved self-assembled single-atom nanozyme which allows oxygen generation to enhance PDT efficacy.

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          Most cited references36

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          Tumor-selective catalytic nanomedicine by nanocatalyst delivery

          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 Fe3O4 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 H2O2 for subsequent Fenton-like reaction catalyzed by Fe3O4 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.
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            Low-temperature hydrogen production from water and methanol using Pt/α-MoC catalysts

            Polymer electrolyte membrane fuel cells (PEMFCs) running on hydrogen are attractive alternative power supplies for a range of applications, with in situ release of the required hydrogen from a stable liquid offering one way of ensuring its safe storage and transportation before use. The use of methanol is particularly interesting in this regard, because it is inexpensive and can reform itself with water to release hydrogen with a high gravimetric density of 18.8 per cent by weight. But traditional reforming of methanol steam operates at relatively high temperatures (200–350 degrees Celsius), so the focus for vehicle and portable PEMFC applications has been on aqueous-phase reforming of methanol (APRM). This method requires less energy, and the simpler and more compact device design allows direct integration into PEMFC stacks. There remains, however, the need for an efficient APRM catalyst. Here we report that platinum (Pt) atomically dispersed on α-molybdenum carbide (α-MoC) enables low-temperature (150–190 degrees Celsius), base-free hydrogen production through APRM, with an average turnover frequency reaching 18,046 moles of hydrogen per mole of platinum per hour. We attribute this exceptional hydrogen production—which far exceeds that of previously reported low-temperature APRM catalysts—to the outstanding ability of α-MoC to induce water dissociation, and to the fact that platinum and α-MoC act in synergy to activate methanol and then to reform it.
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              Direct observation of noble metal nanoparticles transforming to thermally stable single atoms

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                Author and article information

                Contributors
                zhenguo@ustc.edu.cn
                zhaoyanli@ntu.edu.sg
                Journal
                Nat Commun
                Nat Commun
                Nature Communications
                Nature Publishing Group UK (London )
                2041-1723
                17 January 2020
                17 January 2020
                2020
                : 11
                : 357
                Affiliations
                [1 ]ISNI 0000 0001 2224 0361, GRID grid.59025.3b, Division of Chemistry and Biological Chemistry, School of Physical and Mathematical Sciences, , Nanyang Technological University, ; 21 Nanyang Link, Singapore, 637371 Singapore
                [2 ]ISNI 0000000121679639, GRID grid.59053.3a, Anhui Key Laboratory for Cellular Dynamics and Chemical Biology, School of Life Sciences, , University of Science and Technology of China, ; Hefei, 230027 P. R. China
                [3 ]ISNI 0000 0004 1771 3402, GRID grid.412679.f, Radiology Department of the First Affiliated Hospital of Anhui Medical University, ; Hefei, 230022 P. R. China
                [4 ]ISNI 0000 0001 2224 0361, GRID grid.59025.3b, School of Materials Science and Engineering, , Nanyang Technological University, ; Singapore, 639798 Singapore
                Author information
                http://orcid.org/0000-0002-6278-0706
                http://orcid.org/0000-0002-9231-8360
                Article
                14199
                10.1038/s41467-019-14199-7
                6969186
                31953423
                0360fa66-892a-4d8a-9ef8-e7c3d894e922
                © The Author(s) 2020

                Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.

                History
                : 11 June 2019
                : 19 December 2019
                Funding
                Funded by: FundRef https://doi.org/10.13039/501100001809, National Natural Science Foundation of China (National Science Foundation of China);
                Award ID: 31471268
                Award Recipient :
                Funded by: FundRef https://doi.org/10.13039/501100001381, National Research Foundation Singapore (National Research Foundation-Prime Minister's office, Republic of Singapore);
                Award ID: NRF-NRFI2018-03
                Award Recipient :
                Categories
                Article
                Custom metadata
                © The Author(s) 2020

                Uncategorized
                metal-organic frameworks,self-assembly,biomedical materials,nanotechnology in cancer

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