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Acta Pharmaceutica Sinica B · 2021 · IF 11.614

A smart O2-generating nanocarrier optimizes drug transportation comprehensively for chemotherapy improving

Xiaojuan Zhang,Chuanchuan He,Yun Sun,Xiaoguang Liu,Yan Chen,Chen Chen,Ruicong Yan,Ting Fan,Tan Yang,Yao Lu,Jun Luo,Xiang Ma,Guangya Xiang

Drug transportation is impeded by various barriers in the hypoxic solid tumor, resulting in compromised anticancer efficacy. Herein, a solid lipid monostearin (MS)-coated CaO 2 /MnO 2 nanocarrier was designed to optimize doxorubicin (DOX) transportation comprehensively for chemotherapy enhancement. The MS shell of nanoparticles could be destroyed selectively by highly-expressed lipase within cancer cells, exposing water-sensitive cores to release DOX and produce O 2 . After the cancer cell death, the core-exposed nanoparticles could be further liberated and continue to react with water in the tumor extracellular matrix (ECM) and thoroughly release O 2 and DOX, which exhibited cytotoxicity to neighboring cells. Small DOX molecules could readily diffuse through ECM, in which the collagen deposition was decreased by O 2 -mediated hypoxia-inducible factor-1 inhibition, leading to synergistically improved drug penetration. Concurrently, DOX-efflux-associated P-glycoprotein was also inhibited by O 2 , prolonging drug retention in cancer cells. Overall, the DOX transporting processes from nanoparticles to deep tumor cells including drug release, penetration, and retention were optimized comprehensively, which significantly boosted antitumor benefits.

CAS / MDL: 31566-31-1
研究领域: 药学 · 纳米技术 · 癌症研究 · 化疗 · 药物递送系统
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY · 2019 · IF 3.218

RuO2-particle-decorated graphene-nanoribbon cathodes for long-cycle Li–O2 batteries

Peng Xu,Congdi Chen,Jiajia Zhu,Jian Xie,Pei Zhao,Miao Wang

In this work, we report a novel cathode composed of three-dimensional intersected graphene nanoribbons skeleton decorated with RuO 2 catalyst, where graphene nanoribbons are obtained by unzipping multi-walled carbon nanotubes . The graphene nanoribbons framework exhibits a three-dimensional intersected structure and a large specific surface area, leading to a higher capacity than multi-walled carbon nanotubes. The RuO 2 introduced via a facile dropping method enhances the oxygen evolution reaction kinetics and obviously reduces the charge overpotential. More importantly, the Li–O 2 battery with RuO 2 decorated graphene nanoribbons cathode presents an excellent cycling stability of 424   cycles at a curtailed capacity of 1000 mAh g −1 , which can be attributed to the synergistic effect between the intersected band-like graphene and highly effective RuO 2 particles. The Li 2 O 2 deposited on graphene nanoribbons shows a totally different surface morphology compared with that on multi-walled carbon nanotubes due to the different structures of carbon substrates. This work provides a promising design of highly efficient air electrodes for high-performance Li–O 2 batteries.

CAS / MDL: 14898-67-0
研究领域: 材料科学 · 能源化学
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ACS Applied Materials & Interfaces · 2014 · IF 5.9

A Li–O2/Air Battery Using an Inorganic Solid-State Air Cathode

Xiaofei Wang,Ding Zhu,Ming Song,Shengrong Cai,Lei Zhang,Yungui Chen

The “(−) lithium (Li) anode|organic anolyte + inorganic catholyte|solid-state cathode (+)” Li–O2/air battery based on an inorganic solid-state air cathode was fabricated with a simple method. The electrochemical performance and reaction products of the Li–O2/air batteries under pure O2 and ambient air were investigated, respectively. The inorganic Li-ion conductive solid-state electrolyte Li1.3Al0.3Ti1.7(PO4)3 was stable during cycling and avoided the decomposition and volatilization problems that conventional organic electrolytes faced. Moreover, the porous air cathode provided a sufficient gas-phase O2-transport channel, facilitating the achievement of a high capacity of 14192 or 7869 mA h g–1 under pure O2 or ambient air, respectively. Our results demonstrate that the Li–O2/air battery using an inorganic porous air cathode has a great potential for practical application.

CAS / MDL: 90076-65-6 143-24-8
研究领域: 材料科学 · 能源技术
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PARTICLE & PARTICLE SYSTEMS CHARACTERIZATION · 2020 ·Vol. 37 ·期 3 ·1900496 · IF 3.099

Tumor Microenvironment Adaptable Nanoplatform for O2 Self-Sufficient Chemo/Photodynamic Combination Therapy

Shi-Ying Li,Lin-Ping Zhao,Rong-Rong Zheng,Gui-Ling Fan,Ling-Shan Liu,Xiang Zhou,Xian-Tong Chen,Xiao-Zhong Qiu,Xi-Yong Yu,Hong Cheng

Malignant proliferation of tumor cells induces abnormal tissue microenvironments, leading to therapeutic resistance and poor therapeutic outcome. In this paper, manganese dioxide (MnO 2 ) nanoshells are coated on a porphyrinic metal–organic framework of porous coordination network (PCN)-224 for doxorubicin (DOX) loading and hyaluronic acid (HA) modification to obtain an intelligent nanoplatform of PCN@MnO 2 @DOX@HA (PMDH). Benefiting from the HA functionalization, PMDH prefers to accumulate in tumor sites and enhance the cellular uptake by CD44-overexpressed tumor cells. Subsequently, the internalized PMDH could catalyze the abundant H 2 O 2 in cells into O 2 to relieve tumor hypoxia. Further, the MnO 2 nanoshells of PMDH could be degraded into Mn 2+ for magnetic resonance imaging with glutathione reduction and the release of DOX. By integrating the O 2 self-sufficiency with glutathione reduction abilities, PMDH possesses highly potent chemo/photodynamic combination therapeutic effects against hypoxic tumors. Significantly, PMDH exhibits a good biocompatibility with a low cardiotoxicity and negligible systemic side effects, which provides a new insight in developing tumor microenvironment adaptable nanoplatforms for synergistic tumor theranostics.

研究领域: 癌症治疗 · 纳米医学 · 材料科学 · 生物医学工程
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ChemSusChem · 2022 ·Vol. 15 ·期 16 ·e202200769 · IF 9.14

Suppressing Redox Shuttling with Lithiated Nafion-Modified Separators for Li-O2 Batteries

Yuqing Zhang,Shuyuan Xie,Dan Li,Yulong Liu,Chao Li,Jia Liu,Haiming Xie

Graphical Everyday I'm shuttling : A functional lithiated Nafion-decorated separator (Li-Nafion@PE) exhibits a good inhibition for redox shuttling in LiI-containing Li-O 2 batteries. The fabrication combines the wide universality, easy operation, and suitability for mass production. A cell with as-prepared Li-Nafion@PE exhibits considerable cycling stability and good reversibility associated with desired Li 2 O 2 generation and degradation. Although the employment of redox mediator (RM) is an effective strategy to reduce the overpotential by avoiding the direct electrochemical oxidization of Li 2 O 2 during charging, an unexpected redox shuttling in Li-O 2 system leads to RM degradation and continuous deterioration of Li anode, finally resulting in a limited cycling stability. Here, a functional lithiated Nafion-modified separator was firstly introduced to inhibit the shuttle effect by coulombic/electrostatic interactions in RM-involved Li-O 2 batteries. The fabrication of the separator involved easily accessible raw materials and an easy-to-operate process, which made it suitable for large-scale production. The enhancement of lithiated process on electrochemical properties was systematically investigated. In addition, the influence of decorated amount on cycling stability was also studied. Furthermore, the functional contribution of lithiated Nafion on inhibition of redox shuttling and the working mechanism for cells with and without as-prepared separators were proposed. This work can give an insight into the development of functional separator ( i . e ., activity issue) and the suppression of parasitic reactions ( i . e ., selectivity issue) in Li-O 2 batteries.

研究领域: 电化学 · 材料科学 · 能源存储技术
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ACS Nano · 2023 · IF 17.1

“Closed-Loop” O2-Economizer Induced In Situ Therapeutic Vaccine against Hypoxic Tumors

Yifan Zhao,Min Zhang,Bai Lv,Guanghe Xue,Huimei Jiang,Gang Chen,Yi Ma,Yong Sun,Jie Cao

Therapeutic tumor vaccines, which use tumor antigens to stimulate a cancer patient’s immune system to eventually kill the tumor tissues, have emerged as one of the most attractive strategies in anticancer research. Especially, exploring in situ vaccines has become a potential field in cancer immunotherapy. However, due to the hypoxic tumor microenvironment, the generation of tumor antigens is always mild and not sufficient. Hence, in this study, we designed a closed-loop mitochondrial oxygen-economizer (TPCA) to induce enhanced phototherapy-driven in situ vaccines. The O2-economizer was developed by the integration of the photosensitizer CyI and the mitochondrial inhibitor atovaquone into the PAMAM dendrimer. In vitro and in vivo studies showed that TPCA could enter the mitochondria through (3-propylcarboxyl) triphenylphosphine bromide (TPP) and effectively restrict the respiration of tumor cells to reduce tumor hypoxia, thus providing continuous oxygen for enhanced iodinated cyanine dye mediated photodynamic therapy, which could further induce in situ vaccines for ablating the primary tumor directly and inhibiting the tumor metastasis and recurrence. Furthermore, the antitumor mechanism revealed that O2-economizer-based oxygen-boosted PDT elicited immunogenic cancer cell death with enhanced exposure and release of DAMPs and altered the immunosuppressive tumor microenvironment with increased recruitment of T cells in tumors, thereby inducing in situ vaccines and provoking the systematic antitumor responses against CT26 tumors. This study will provide innovative approaches for local, abscopal, and metastatic tumor treatment.

CAS / MDL: 95233-18-4
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ChemistrySelect · 2024 ·Vol. 9 ·期 41 ·e202403137 · IF 1.9

Fluorescent Scandium Microspheres for Highly Efficient White-Light Photocatalysis

Hua-Ying Chen,Jian Lv,Ruo-Can Qian,Da-Wei Li,Bin-Bin Chen

Graphical Fluorescent scandium microspheres for highly efficient white-light photocatalysis. Scandium-based fluorescent microspheres (Sc-FMs) are prepared by a facile one-pot hydrothermal polymerization method, which can be well used for the highly-efficient photodegradation of dye pollutants (rhodamine 6 G) under low power white light without the assistance of any radical generating agents due to the strong generation ability of ⋅O 2 - and h + by Sc-FMs Efficient photocatalysts play an important role in the various fields such as pollutant treatment and the generation of clean energy. Therefore, developing a photocatalyst with high activity is of great significance. Herein, scandium-based fluorescent microspheres (Sc-FMs) are facilely prepared through the one-pot hydrothermal polymerization of scandium ions and tartaric acid. The prepared Sc-FMs show strong blue solid-state fluorescence, with a maximum emission at 412 nm. Meanwhile, Sc-FMs possess a strong white-light photocatalysis ability, which can be used for the photodegradation of dye pollutants (rhodamine 6 G) under low power white light without the assistance of any radical generating agents. In addition, the Sc-FMs display good stability and recyclability. As a result, this new and efficient Sc-FMs photocatalysts hold a promise for potential applications in environmental treatment.

CAS / MDL: 67-63-0
研究领域: 环境科学 · 材料科学 · 化学
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Catalysis Science & Technology · 2023 ·Vol. 13 ·期 7 ·2101-2107 · IF 5

Ligand functionalization on Zr-MOFs enables efficient visible-light-driven H2O2 evolution in pure water

Jianhao Qiu,Lu Zhang,Guanglu Xia,Dingliang Dai,Yong Tang,Jianfeng Yao

Different ligand functionalized UiO-66 (UiO-66-X, X = OH, (OH)2 and NH2) were prepared and then modified by ZnIn2S4 lamellas to form ZnIn2S4/UiO-66-X heterostructures for visible-light-driven H2O2 evolution in pure water. The H2O2 yields using ZnIn2S4/UiO-66-NH2, ZnIn2S4/UiO-66-(OH)2 and ZnIn2S4/UiO-66-OH are 799, 733 and 165 μmol L−1, respectively, which are 9.5, 8.7 and 2.0 times that of ZnIn2S4/UiO-66. The high performance of ZnIn2S4/UiO-66-NH2 and ZnIn2S4/UiO-66-(OH)2 is ascribed to the benign visible-light response and Z-scheme heterostructures, and the H2O2 evolution abides by indirect O2 reduction with ˙O2− as an intermediate species. Additionally, H2O2 yields using ZnIn2S4/UiO-66-NH2 on tap water and Xuanwu Lake (Nanjing, China) water can be comparable to that on the above-deionized water. This study sheds light on the great promise of functionalized MOFs and their applications on green (photo)catalytic energy conversion.

研究领域: 材料科学 · 光化学 · 环境科学
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ACS Applied Polymer Materials · 2022 · IF 4.855

Interfacial Polymerization-Modified Polyetherimide (PEI) Separator for Li–O2 Battery with Boosted Performance

Jiuqing Liu,Lishun Bai,Junying He,Cheng Wang,Qihou Li,Feifei Song,Zikun Hong,Ya Chen,Fanli Zeng,Chen Cheng,Zehao Chen

Lithium–oxygen (Li–O2) batteries, having an ultrahigh theoretical energy density (3500 Wh kg–1), have gained a lot of attention. However, its application is seriously obstructed by pivotal issues like instability of lithium metal anode, low energy efficiency, and electrolyte decomposition. Herein, a separator modification method based on interfacial polymerization (IP) was proposed by us to solve these issues. The obtained interfacial polymerization layer shows good ion-selective permeability on the surface of the polyetherimide (PEI) separator, and the ion transport of the larger EMIM+, TFSI–, and BF4– between the electrodes is greatly inhibited. Consequently, the representative P2-PEI separator presents the best cycle performance and the Li–O2 battery assembled with it can stably operate over 135 cycles, even under a current density of 0.05 mA cm–2 and a limited specific capacity of 1000 mAh g–1.

研究领域: 材料科学 · 电化学 · 能源存储
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JOURNAL OF CATALYSIS · 2018 · IF 6.759

Selective oxidation of amines using O2 catalyzed by cobalt thioporphyrazine under visible light

Juanjuan Jin,Changjun Yang,Bingguang Zhang,Kejian Deng

A highly efficient oxidation of amines including primary and secondary amines into imines using O 2 as the oxidant was realized by cobalt tetra(2-hydroxymethyl-1,4-dithiin)porphyrazine (CoPz(hmdtn) 4 ) under irradiation of visible light ( λ  ≥ 420 nm). Particularly, the photocatalytic selective oxidation of benzylamine into N -benzylidenebenzylamine was thoroughly studied in order to get more insight into the reaction kinetics and mechanism for the oxidation of amine. The photocatalytic oxidation of benzylamine was observed to follow pseudo-first-order reaction kinetics. Moreover, a reasonable linear relationship between the log( k X / k H ) values and the Brown-Okamoto constant ( σ + ) parameters was obtained for oxidation of para - and meta -substituted benzylamines. Besides imine, the presence of other intermediate products such as NH-imine and H 2 O 2 was further evidenced in this photocatalytic system. Additionally, the reactive oxygen species (ROSs) generated in this photocatalytic process were confirmed by electron spin resonance (ESR) technique. The possible photocatalytic transformation pathway of amine into imine was also proposed, involving the dehydrogenation of amine to form NH-imine and the nucleophilic addition of NH-imine by free amine to afford the final imine.

研究领域: 化学 · 催化 · 光化学
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Journal of the American Chemical Society · 2024 · IF 14.4

Second-Shell N Dopants Regulate Acidic O2 Reduction Pathways on Isolated Pt Sites

Baoxin Ni,Peng Shen,Guiru Zhang,Jiajun Zhao,Honghe Ding,Yifan Ye,Zhouying Yue,Hui Yang,Hao Wei,Kun Jiang

Pt is a well-known benchmark catalyst in the acidic oxygen reduction reaction (ORR) that drives electrochemical O2-to-H2O conversion with maximum chemical energy-to-electricity efficiency. Once dispersing bulk Pt into isolated single atoms, however, the preferential ORR pathway remains a long-standing controversy due to their complex local coordination environment and diverse site density over substrates. Herein, using a set of carbon nanotube supported Pt–N–C single-atom catalysts, we demonstrate how the neighboring N dopants regulate the electronic structure of the Pt central atom and thus steer the ORR selectivity; that is, the O2-to-H2O2 conversion selectivity can be tailored from 10% to 85% at 0.3 V versus reversible hydrogen electrode. Moreover, via a comprehensive X-ray-radiated spectroscopy and shell-isolated nanoparticle-enhanced Raman spectroscopy analysis coupled with theoretical modeling, we reveal that a dominant pyridinic- and pyrrolic-N coordination within the first shell of Pt–N–C motifs favors the 4e– ORR, whereas the introduction of a second-shell graphitic-N dopant weakens *OOH binding on neighboring Pt sites and gives rise to a dominant 2e– ORR. These findings underscore the importance of the chemical environment effect for steering the electrochemical performance of single-atom catalysts.

CAS / MDL: 56-40-6
研究领域: 电化学 · 催化科学
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Journal of the American Chemical Society · 2026 · IF 16.6

Spontaneous Chlorine Generation via Interfacial Oxidation of Chloride by O2 on Acidic Microdroplets

Li Shuying,Wang Zhuo,Cao Yiqun,Ma Wei,Li Hao,Chen Tianzeng,Wang Yonghong,Zhang Peng,Liu Pengfei,Chu Biwu,Liu Chang,Liu Yongchun,Mu Yujing,Zhang Xiuhui,Wang Tao,Ma Qingxin,Francisco Joseph S.,He Hong

Reactive chlorine species significantly influence atmospheric chemistry, yet their sources remain inadequately defined. We have discovered a spontaneous formation pathway for substantial molecular chlorine (Cl 2 ) from the oxidation of chloride (Cl – ) through interfacial oxidation by O 2 on acidic microdroplets. This efficient interfacial reaction is facilitated by protons (H + ), which enrich Cl – at the gas–liquid interface and mediate the electron-transfer process, concurrently releasing gaseous Cl 2 and hydroxyl radicals (OH). Given the prevalence of acidic, chloride-containing droplets in marine and polluted urban environments, this formation mechanism constitutes a substantial and previously unaccounted tropospheric chlorine source. Unlike established mechanisms, this pathway generates active halogens without consuming gaseous oxidants like O 3 or OH, instead producing particulate reactive oxygen species (ROS). Consequently, current atmospheric models likely underestimate the contribution of reactive halogens to atmospheric oxidation capacity.

CAS / MDL: 7647-14-5
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