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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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JOURNAL OF POWER SOURCES · 2020 · IF 8.247

Heterostructured Mo2C–MoO2 as highly efficient catalyst for rechargeable Li–O2 battery

Chang Wu,Yuyang Hou,Jicheng Jiang,Haipeng Guo,Hua-Kun Liu,Jun Chen,Jiazhao Wang

Li–O 2 batteries has been widely investigated for its ultra-high capacity as next generation batteries. Nevertheless, some problems like sluggish kinetic reaction and instability hugely impede the practical use of Li–O 2 batteries. In this work, Mo 2 C/MoO 2 @RGO heterostructures was fabricated by in-situ growth of Mo 2 C between MoO 2 and RGO during calcination and being employed as cathode to explore the synergistic effect in Li–O 2 batteries. As a result, Mo 2 C/MoO 2 @RGO exhibits good specific capacity with 2365 mAh g −1 , high round-trip efficiency (89% at first cycle) and improved cycling performance. Density functional theory calculations indicated that the Mo 2 C/MoO 2 @RGO heterostructures have better capability of oxygen adsorption than sole constituent (Mo 2 C@RGO or MoO 2 @RGO), which triggers the formation of film-like amorphous discharge products, leading to lower overpotential and stable performance. Our study reveals the important role of heterostructures in Li–O 2 batteries system and demonstrates a promising design strategy for heterostructured catalyst.

CAS / MDL: 7782-42-5
研究领域: 材料科学 · 电化学 · 能源存储
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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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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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Journal of Materials Chemistry A · 2021 ·Vol. 9 ·期 14 ·9354-9363 · IF 12.732

Titanium and fluorine synergetic modification improves the electrochemical performance of Li(Ni0.8Co0.1Mn0.1)O2

Zheng Si,Baozhao Shi,Jin Huang,Ye Yu,You Han,Jinli Zhang,Wei Li

Nickel-rich layered oxides (LiNixCoyMn1−x−yO2) (x ≥ 0.8, NCM) are intensively developed cathode materials for lithium-ion batteries owing to their high energy and low price, however, their application is impeded by poor cycle stability. Herein we explored a Ti and F co-doped Li(Ni0.8Co0.1Mn0.1)O2 cathode through a solid phase reaction using the precursors of TiO2 and NH4F. Combining the characterization results of XRD, Ar sputtering assisted XPS, HRTEM, in situ XRD, etc, it is illustrated that Ti4+ and F− co-modification can synergistically modulate the lattice parameter and the Ni2+/Li+ mixing degree for the Li(Ni0.8Co0.1Mn0.1)O2 cathode material. Particularly, density functional theory (DFT) calculations demonstrate that Ti and F co-doping is beneficial to form stable crystal structures with a layered phase and rock-salt phase. Ti4+ and F− co-dopants induce the formation of an ultra-thin rock-salt phase on the cathode surface, which provides a protective layer on the nickel-rich cathode surface, so as to enhance the electrochemical performance. The optimal Ti4+ and F− co-doped sample 0.5Ti@0.5F-NCM shows a superior discharge capacity of 202.2 mA h g−1 at 1C and 45 °C, and a capacity retention of 88.1% after 200 cycles, much higher than the retention of 45.2% for NCM. For 0.5Ti@0.5F-NCM, the lithium-ion diffusion coefficients after the 1st and 100th cycles are 2.67 × 10−11 cm2 s−1 and 7.14 × 10−12 cm2 s−1 respectively, larger than those of the pristine NCM (1.37 × 10−11 cm2 s−1 and 4.52 × 10−12 cm2 s−1). The Ti4+ and F− co-doping can suppress the H2–H3 phase change of the cathode during the charge and discharge process and reduce the charge transfer resistance. The results provide a simple and feasible design strategy via cation@anion dopants to boost the electrochemical performance of nickel-rich cathodes for lithium-ion batteries.

研究领域: 材料科学 · 能源科学
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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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NEW JOURNAL OF CHEMISTRY · 2018 ·Vol. 42 ·期 21 ·17311-17316 · IF 3.201

Bifunctional electrolyte additive KI to improve the cycling performance of Li–O2 batteries

Changjin Li,Zhengyi Qian,Yulin Ma,Pengjian Zuo,Chunyu Du,Hua Huo,Geping Yin

Non-aqueous rechargeable Li–O2 batteries have attracted great attention owing to their ultra-high specific energy densities. However, the high charge overpotential and the interfacial instability of lithium anodes still need to be overcome before the practical application of Li–O2 batteries. Here, we use KI as a bifunctional electrolyte additive for Li–O2 batteries. The results demonstrate that I− could act as a redox mediator to effectively reduce the charge overpotential by 0.7 V. On the other hand, the introduction of K+ contributes to decreasing the polarization, optimizing the morphology, reducing the surface by-products of the lithium anode and dramatically improving the uniform distribution of discharge products on the cathode surface. The dual functions of KI additive thus successfully boost the electrochemical performances of Li–O2 batteries.

研究领域: 电化学 · 能源材料 · 锂离子电池 · 界面化学 · 储能技术
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY · 2026 · IF 14.3

Atomically dispersed bimetallic Pd-Fe clusters for boosting catalytic antibacterial performance with O2

Tao Li,Wan Wang,Jiawei Chen,Yue Wang,Xiangbin Cai,Lini Yang,Xin Liu,Jiangyong Diao,Zarrin Es'haghi,Lixin Xia,Li Jin,Guoqing Wang,Hongyang Liu

The development of highly efficient nanozymes faces challenges of insufficient catalytic activity and low atom utilization. Atomically dispersed metal nanozymes have received widespread attention due to their high atomic utilization efficiency and exceptional catalytic activity. Bimetallic catalysts demonstrated enhanced catalytic performance owing to synergistic geometric and electronic effects arising from heterometallic interactions. Herein, we report an atomically dispersed palladium-iron bimetallic cluster nanozyme, in which fully exposed Pd clusters bonded to adjacent Fe atomic clusters are anchored onto defect-rich nanodiamond-graphene supports (PdFe/ND@G). The Pd-Fe interfacial sites fabricated in atomically dispersed bimetallic clusters deliver abundant oxygen activation sites for high-efficiency catalytic reactions and exhibit enhanced oxidase-like catalytic activity, demonstrating superior enzymatic activity and antibacterial performance compared to monometallic Pd and Fe clusters, while surpassing those of previously reported nanozymes. DFT calculations reveal that, compared to monometallic Pd clusters, atomically dispersed Pd-Fe clusters synergistically catalyze O 2 cleavage into OO* intermediates via Pd-Fe interfacial sites while exhibiting lower energy barriers, which is the critical factor for their enhanced enzyme-like activity. This study provides novel insights into constructing highly efficient atomically dispersed bimetallic cluster nanozymes.

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