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ACS Applied Materials & Interfaces · 2019 · IF 8.456

Cell Membrane-Coated Porphyrin Metal–Organic Frameworks for Cancer Cell Targeting and O2-Evolving Photodynamic Therapy

Di Zhang,Zhongju Ye,Lin Wei,Haibin Luo,Lehui Xiao

Photodynamic therapy (PDT) has attracted great attention as an alternative tumor treatment method. Unfortunately, it suffers from some limitations like poor targeting capability and insufficient therapeutic efficiency caused by tumor hypoxia. In this work, we introduce a novel O2-evolving PDT nanoparticle for homologous cancer cell targeting as well as dual-mode imaging [i.e., magnetic resonance imaging (MRI) and fluorescence imaging]. Specifically, the nanostructure consists of a MnO2 nanosheet-coated metal–organic framework core and cancer cell membrane shell (defined as CM-MMNPs). The MnO2 layer displays H+ and H2O2 responsiveness, which can produce O2 to enhance O2-mediated singlet oxygen (1O2) generation for PDT. Moreover, the resulted Mn2+ can also be used as an optimal MRI contrast agent. The introduction of cell membrane and membrane proteins endow the CM-MMNPs with good stability and integrity in the process of cellular endocytosis, as well as strong homologous cell-targeting ability. This multifunctional nanoparticle has the potential to overcome the hypoxia of cancer cells in PDT, and provides a new paradigm for tumor targeting, detection, and therapy, which is promising for biomedical applications in the future.

研究领域: 生物医学工程 · 癌症研究 · 纳米技术 · 诊疗学
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WATER ENVIRONMENT RESEARCH · 2019 ·Vol. 91 ·期 8 ·770-779 · IF 1.24

Degradation of 4-chlorophenol by BM Fe/Cu-O2 system: The symbiosis of and ·OH radicals

Jinhong Fan,Hehe Qin,Yunfei Zhang,Simin Jiang

In this study, Fe/Cu bimetal composite was prepared by high-energy ball milling (BM) method for the removal of refractory organics. The BM Fe/Cu bimetal was characterized by SEM-EDS, XRD, and XPS. Evenly distributed Fe and Cu was observed in the EDS mapping. In contrasting experiments, the removal rate of 4-chlorophenol (4-CP) by BM Fe/Cu materials was about 10-fold faster than that by chemical substitution deposition (CSD) of Fe/Cu material. Complete 4-CP removal and 66.7% of total organic carbon (TOC) mineralization in the BM Fe/Cu–O 2 system were achieved. Dissolved oxygen plays a crucial role for 4-CP degradation through the in situ generation of reactive oxygen species (ROS) such as H 2 O 2 , ·OH, and via oxygen activation reactions. The predominant reactive radicals were identified to be and ·OH through ESR technique and inhibition experiments. The coexistence of oxidation and reduction of 4-CP in the BM Fe/Cu-O 2 system was proposed. Practitioner points 4-CP removal rate by BM Fe/Cu is 10-fold faster than that by CSD Fe/Cu at the same conditions. Complete 4-CP removal and 66.7% of TOC reduction were achieved. All three ROS including ·OH, , and H 2 O 2 coexisted in the BM Fe/Cu-O 2 system. A harmonious coexistence of oxidation and reduction mechanism was proposed.

研究领域: 环境科学 · 化学工程
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Nanoscale · 2019 ·Vol. 11 ·期 24 ·11513-11520 · IF 6.97

Stabilizing electrochemical Li–O2 batteries with a metal-based cathode of PdNi on Ni nonwoven fabric

Huan-Feng Wang,Jun-Feng Li,Xue-Xi Sun,Ji-Jing Xu

The design of a nanoporous cathode for Li–O2 batteries that can achieve high chemical stability and superior electrochemical performance remains a formidable challenge. A novel approach for the fabrication of nanoengineered PdNi alloys directly coated onto Ni nonwoven fabric (PdNi/NiNF) obtained through electrospinning has been proposed. On the basis of the contributions of the porous structure, the prepared metal-based cathodes can exhibit high chemical and mechanical stabilities, high catalytic activity, and high conductivity. In this design, the major side reactions were excluded when compared with popularly used carbon cathodes, and excellent cycling stability (266 cycles) could be achieved. The proposed cathode exhibited a high discharge capacity of 15 700 mA h g−1 at 500 mA g−1, which was 5 times higher than those reported for carbon-free cathodes.

研究领域: 材料科学 · 电化学
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JOURNAL OF SOLID STATE ELECTROCHEMISTRY · 2015 ·Vol. 19 ·期 8 ·2421-2429 · IF 2.446

The investigation of water vapor on the Li–O2 battery using a solid-state air cathode

Wang Xiaofei,Cai Shengrong,Zhu Ding,Mu Shijia,Chen Yungui

A lithium (Li)–oxygen (O 2 ) battery based on an inorganic solid-state air cathode was fabricated, and the influence of water vapor (key component in the air) on the electrochemical behavior of the proposed Li–O 2 battery was deeply investigated. Excluding the negative influence of the corrosion of Li anode that existed in organic-based electrolyte Li–O 2 battery when operated in wet environment, our results showed that water vapor has a positive effect on the discharge and cycling performances of the Li–O 2 battery using a solid-state air cathode. The discharge capacity reached 11734 mA h g −1 (7.8 mA h cm −2 ) in wet O 2 , which was not markedly different with that in dry O 2 (11956 mA h g −1 (8.0 mA h cm −2 )). However, the discharge voltage in wet O 2 was about 110 mV higher than that in dry O 2 . Although the formation of LiOH increased the charge overpotential, the formed LiOH in turn minimized the decomposition of carbon to form Li 2 CO 3 , and enhanced the cycling performance to a certain extent. In addition, we showed that the polarization involved by water vapor could also be largely decreased by slightly increasing the operating temperature; the charge voltage plateau decreased from 4.04 to 3.3 V when the temperature increased from 25 to 50 °C. These results suggest that the Li–O 2 battery using a solid-state air cathode is promising for practical application, especially in wet environment.

CAS / MDL: 90076-65-6 143-24-8
研究领域: 材料科学 · 电化学
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CHEMICAL ENGINEERING JOURNAL · 2017 · IF 6.216

Synergistic effects of nitrogen-doped graphene and Fe2O3 nanocomposites in catalytic oxidization of aldehyde with O2

Fan Yang,Tian Qiu,Cheng Chi,Shuang Liang,Lei Deng,Xuyang Wang,Chunxia Wang,Jingyi Fu,Ying Wang,Yongfeng Li

Promotion of nitrogen-doped graphene (NG) by incorporation of ferric oxide (NG-Fe 2 O 3 ) is found to strongly enhance the activity in the catalytic oxidization of aldehyde to synthesize carboxylic acid with O 2 . The composite NG-Fe 2 O 3 catalysts can be fabricated by a facile one-pot hydrothermal method. The characterization results of the composite catalysts have revealed that the Fe 2 O 3 nanoparticles (NPs) with sizes of 40–90   nm are not only on both sides of NG sheets but also tightly enwrapped by the graphene layers. In comparison to NG and Fe 2 O 3 NPs, synergistic adsorption that confirmed by DFT studies has been created on the NG-Fe 2 O 3 composites, where both NG and Fe 2 O 3 are proposed to be involved in the adsorptive interaction. The synergistic adsorption can lead to strengthen O 2 molecule adsorption of NG and weaken O 2 molecule adsorption of Fe 2 O 3 NPs. More importantly, the NG-Fe 2 O 3 composite is found to considerably facilitate the longest elongation of O-O bonds and contribute to the striking enhancement of the catalytic performance. The highly active NG-Fe 2 O 3 composite shows wide scope for catalysis of oxidation of aldehydes to carboxylic acids and good stability for recycle six times.

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JOURNAL OF NANOBIOTECHNOLOGY · 2021 ·Vol. 19 ·期 1 ·1-14 · IF 10.435

α-Fe2O3@Pt heterostructure particles to enable sonodynamic therapy with self-supplied O2 and imaging-guidance

Zhang Tian,Zheng Qiang,Fu Yike,Xie Congkun,Fan Gonglin,Wang Yifan,Wu Yongjun,Cai Xiujun,Han Gaorong,Li Xiang

Sonodynamic therapy (SDT), presenting spatial and temporal control of ROS generation triggered by ultrasound field, has attracted considerable attention in tumor treatment. However, its therapeutic efficacy is severely hindered by the intrinsic hypoxia of solid tumor and the lack of smart design in material band structure. Here in study, fine α-Fe 2 O 3 nanoparticles armored with Pt nanocrystals (α-Fe 2 O 3 @Pt) was investigated as an alternative SDT agent with ingenious bandgap and structural design. The Schottky barrier, due to its unique heterostructure, suppresses the recombination of sono-induced electrons and holes, enabling superior ROS generation. More importantly, the composite nanoparticles may effectively trigger a reoxygenation phenomenon to supply sufficient content of oxygen, favoring the ROS induction under the hypoxic condition and its extra role played for ultrasound imaging. In consequence, α-Fe 2 O 3 @Pt appears to enable effective tumor inhibition with imaging guidance, both in vitro and in vivo. This study has therefore demonstrated a highly potential platform for ultrasound-driven tumor theranostic, which may spark a series of further explorations in therapeutic systems with more rational material design. Graphical Abstract

CAS / MDL: 18497-13-7 5471-63-6
研究领域: 纳米技术 · 生物医学工程 · 癌症治疗 · 材料科学
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ACS Applied Energy Materials · 2022 · IF 6.959

Ethyl Viologen as a Superoxide Quencher to Enhance the Oxygen Reduction Reaction in Li–O2 Batteries

Sisi Wu,Jing Yang,Ning Qin,Yingzhi Li,Haiou Wang,Yong-Wei Zhang,Qing Wang,Zhouguang Lu

LiO2 is a critical intermediate of oxygen reduction reaction in nonaqueous Li–O2 batteries that largely determines the discharge capacity and cycling stability. Currently, functional redox mediators that can promote the solution reaction route by enhancing the solvation of LiO2 have attracted tremendous interest to increase the attainable capacity. Conversely, redox mediators that quench LiO2 and facilitate the surface reaction route receive little attention. Here, we provide an in-depth exploration of the catalytic pathway and effect of a superoxide quencher that modulates the surface growth of Li2O2. Surprisingly, the predomination of the surface reaction route by ethyl viologen helps deliver a capacity as much as that promoted by the solution reaction route. The findings of this work provide a new direction of screening and evaluating functioning redox mediators for Li–O2 batteries.

研究领域: 材料科学 · 电化学 · 能源存储
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NEW JOURNAL OF CHEMISTRY · 2022 ·Vol. 46 ·期 30 ·14510-14516 · IF 3.925

Regulable pyrrolic-N-doped carbon materials as an efficient electrocatalyst for selective O2 reduction to H2O2

Yunxian Zhang,Yongyu Pang,Dong Xia,Guoliang Chai

As a successful alternative to the complex and dangerous anthraquinone process, a simple and safe method for the efficient preparation of hydrogen peroxide is to use the electrochemical two-electron oxygen reduction reaction (2e− ORR) process. Herein, we report a facile approach to achieving metal-free nitrogen-doped carbon material electrocatalysts (N-CMCs) using cheap and easily available raw materials, which also have an excellent electrochemical 2e− ORR catalytic performance and selectivity for hydrogen peroxide (H2O2). The as-fabricated nitrogen-doped carbon material electrocatalysts (named as N-CMC-1 : 5) deliver the high H2O2 selectivity of over 80% in a wide potential range from 0.30 to 0.70 V vs. RHE, where the highest H2O2 selectivity can reach 81.4% at 0.42 V vs. RHE. X-ray photoelectron spectroscopy and electrochemical analyses reveal that the content of pyrrolic-N in the catalysts has a positive effect on the 2e− ORR activity. When the catalyst contains more pyrrolic-N, the catalyst demonstrates a better 2e− ORR performance and H2O2 selectivity in alkaline medium, as well as the long-term stability of the catalyst.

CAS / MDL: 1310-58-3
研究领域: 材料科学 · 电化学
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY · 2022 · IF 4.598

Non-woven fabrics derived binder-free gas diffusion catalyst cathode for long cycle Li-O2 batteries

Deyu Mao,Shenglong Yi,Zirui He,Qiancheng Zhu

Lithium-oxygen (Li-O 2 ) batteries with high theoretical energy density are well developed over the past decade, as the cycle performance and round-trip efficiency had enhanced prominently. However, there are still several obstacles that need to be tackled before commercial application. Among them, proper cathode structure design with low cost stands as a core problem. A Typical type of gas diffusion layer cathode are usually carbon paper, which is valuableness, meanwhile, cannot fit the application of flexible devices. In this work, non-woven fabrics were applied as basis materials to synthesis Fe 3 C/N-doped carbon tubes gas diffusion layer by a simple carbonization method. The resulting carbon cloth can be used directly as binder-free and current collector-free cathode for Li-O 2 batteries. More than 130 stable cycles were achieved. The composite synthesized in this paper has the possibility for future application in flexible lithium-oxygen batteries and provide a new strategy for the recovery of non-woven fabrics.

CAS / MDL: 461-58-5 10025-77-1
研究领域: 材料科学 · 能源技术
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Energy Storage Materials · 2021 · IF 17.789

Two-dimensional Mo-based compounds for the Li-O2 batteries: Catalytic performance and electronic structure studies

Xiaowei Mu,Chao Xia,Bin Gao,Shuyi Guo,Xueping Zhang,Jianping He,Yonggang Wang,Hao Dong,Ping He,Haoshen Zhou

Rechargeable Li-O 2 batteries have captured increasing attention owing to their ultra-high theoretical specific energy. However, this promising system is confronted with the large overpotential, limited discharge capacity and low cyclic life. Herein, three two-dimensional (2D) molybdenum-based compounds of MoN, MoO 3 and MoS 2 are used as cathode catalysts in Li-O 2 batteries . The catalytic performance and electronic structures of these catalysts are compared comprehensively. Electrochemical test results reveal the superior battery performance of MoN cathodes, which deliver the highest specific discharge capacity of approximately 7400 mAh g − 1 and the lowest discharge/charge overpotential of 0.19/0.72 V. Density functional theory (DFT) calculations demonstrate the metallic property of MoN whereas MoO 3 and MoS 2 are poor conductive. Besides, interface properties between MoN and Li 2 O 2 products as well as reaction pathways of the Li-O 2 battery with MoN cathode are also investigated detailedly by DFT calculations, explaining the excellent catalytic properties of MoN at the atomic level. The present work provides intrinsic insights into designing high-performance cathode catalysts for Li-O 2 batteries with fine-tuned morphology and electronic characteristics.

CAS / MDL: 1317-33-5
研究领域: 材料科学 · 电化学 · 电池技术 · 催化 · 理论化学
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY · 2022 ·Vol. 169 ·期 6 ·060507 · IF 4.386

PEGDA-SN as Both Solid-State Electrolyte and Solid-Solid Interface Material for Li-O2 Battery

Zining Man,Hao Tian,Xingbao Zhu,Yu Wang,Yuanguo Wu,Xiangyu Wen,Zhe Lü

The solid-state batteries have received widespread attention due to their excellent stability and safety, however, the low ionic conductivity and weak interface contact always restricted its performance. In this work, we propose an in situ thermally cross-linked and solidified polymer electrolyte with polyethylene glycol diacrylate (PEGDA) as scaffold in which succinonitrile (SN) and lithium bis-trifluoromethanesulfonimide (LiTFSI) were further introduced to improve the ionic conductivity. Herein, the composite gel was served as not only solid-solid interface material but also solid-state electrolyte. Different with conventional polymer gels, the solvent evaporation could not happen for this composite material during the solidification process, and therefore resulting in good interface contact without inside bubbles. We further present the investigation on transport principle of Li+ in the solid-state electrolyte and the effect of molecular chain on ionic conductivity. The conductivity of the solid-state electrolyte can reach 1.76 × 10−4 S cm−1 at room temperature without any assistance of liquid electrolytes, which is attributed to the short molecular chain of PEGDA. Electrochemical window of the solid-state electrolyte can reach 5.2 V after cross-linking treatment. And the lithium-oxygen battery using this solid-state electrolyte can stably cycle for more than 1100 cycles with a current density of 200 mA g−1 and a limit capacity of 200 mAh g−1 at room temperature.

CAS / MDL: 90076-65-6
研究领域: 材料科学 · 电化学
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Nanomaterials · 2022 ·Vol. 12 ·期 11 ·1931 · IF 5.719

Tunable Carrier Transfer of Polymeric Carbon Nitride with Charge-Conducting CoV2O6∙2H2O for Photocatalytic O2 Evolution

Shaohong Zang,Xiaorong Cai,Mengshan Chen,Dehong Teng,Fei Jing,Zhe Leng,Yingtang Zhou,Feng Lin

Photocatalytic water splitting is one of the promising approaches to solving environmental problems and energy crises. However, the sluggish 4e−transfer kinetics in water oxidation half-reaction restricts the 2e−reduction efficiency in photocatalytic water splitting. Herein, cobalt vanadate-decorated polymeric carbon nitride (named CoVO/PCN) was constructed to mediate the carrier kinetic process in a photocatalytic water oxidation reaction (WOR). The photocatalysts were well-characterized by various physicochemical techniques such as XRD, FT-IR, TEM, and XPS. Under UV and visible light irradiation, the O2evolution rate of optimized 3wt% CoVO/PCN reached 467 and 200 μmol h−1g−1, which were about 6.5 and 5.9 times higher than that of PCN, respectively. Electrochemical tests and PL results reveal that the recombination of photogenerated carriers on PCN is effectively suppressed and the kinetics of WOR is significantly enhanced after CoVO introduction. This work highlights key features of the tuning carrier kinetics of PCN using charge-conducting materials, which should be the basis for the further development of photocatalytic O2reactions.Keywords:photocatalysis;water oxidation;cobalt vanadates;polymeric carbon nitride

CAS / MDL: 57-13-6
研究领域: 材料科学 · 环境科学
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