ACS Applied Bio Materials
·
2023
·
IF 4.7
Wen-Xing Zhang,Ze-Lei Zhou,Qi-Yan Lv,Xiejie Song,Junyang Chen,Chang-Bin Niu,Hui-Fang Cui
Cancer starvation/photothermal combined tumor therapy (CST/PTT) has attracted great interest attributed to their mutual compensation and synergistically enhanced effect. However, the very low O2 supply in the tumor microenvironment (TME) greatly limits the CST efficiency of glucose oxidase (GOx). Additionally, the easy degradation in blood circulation and significant off-target effects are big challenges for clinical applications of the GOx-based CST. In this study, a drug delivery system (DDS) with specific tumor-targeted GOx delivery, near-infrared (NIR) light and TME responsive O2 generation, NIR-responsive glucose consumption, high GOx loading, and efficient NIR photothermia was developed. Positively charged AuNRs@MnO2@SiO2 nanoparticles (named AMS+ NPs) were synthesized. GOx was covalently loaded with a high loading ratio of 36.0%. Finally, a thermosensitive biomimetic hybrid membrane composed of a thermosensitive lipid (TSL) membrane, red blood cell membrane (RBCM), and 4T1 cancer cell membrane (CCM) was coated on the NPs through a double-layer strategy. The AMS+-G@TSL@[RBC-CC-TSL]M NPs consumed 32.7 times glucose at 50 °C as that at 37 °C and generated 4.9 times O2 upon NIR laser irradiation. The thermosensitive biomimetic NPs showed an efficient targeting capability to the homotypic 4T1 cancer cells/tumors accompanied by good biocompatibility, macrophage evading capability, high cancer cell cytotoxicity, and excellent antitumor efficacy. The tumor growth inhibition ratio with NIR laser irradiation reached 92.8%. The AMS+-GOx@TSL@[RBC-CC-TSL]M NPs provide a smart, efficient, safe, PTT/CST combined DDS for highly efficient tumor therapy.
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ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Zhengyi Qian,Xudong Li,Liguang Wang,Tianpin Wu,Baoyu Sun,Lei Du,Yulin Ma,Chunyu Du,Pengjian Zuo,Geping Yin
Rechargeable aprotic Li–O2 batteries have drawn much attention in light of their ultrahigh theoretical energy density. However, the sluggish kinetics of oxygen cathode reactions lead to huge energy loss, while the unfavorable side reactions associated with the widely used carbon and binder account for fast battery decay during cycles. Herein, hierarchically holey IrNi alloy nanosheets are facilely designed on Ni foam substrate as a freestanding, binder- and carbon-free cathode to address these challenges. The IrNi nanosheets consist of numerous interconnected nanoparticles, forming abundant nanoholes, benefiting active-site exposure. Moreover, the meso-/macropores pave channels for the transfer of oxygen and lithium ions and provide enough accommodation for the insoluble Li2O2 product. The corresponding Li–O2 batteries demonstrate low polarization and excellent cycle stability with full discharge/charge capability (up to 292 cycles at a current density of 0.2 mA cm–2 within a voltage range from 2.3 to 4.3 V). The long-term cycling performance is principally attributed to the exclusive catalytic stability of the holey IrNi nanosheets and its good compatibility with dimethyl sulfoxide-based electrolyte. Our research provides novel insights into the design of robust and freestanding porous cathodes for high energy density Li–O2 batteries.
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ACS Applied Energy Materials
·
2020
·
IF 4.473
Jia Liu,Ying Wang,Dan Zhou,Dan Li,Ziye Kang,Haiming Xie
Although a redox mediator (RM) strategy can lower the overpotential of Li–O2 batteries (LOBs), the redox shuttling results in an undesired RM consumption and a continued decomposition of lithium metal anode, leading to a poor cycling stability. In this work, a hybrid inorganic–organic composite separator based on polyethylene oxide/TiO2/polypropylene (PEO/TiO2/PE) in LOBs has been reported for the first time, which aims to suppress the RM shuttling. The influences of TiO2 nanoparticles and PEO on battery performance are systematically investigated. Benefiting from the synergistic advantages, a LOB with PEO/TiO2/PE separator displays stable cyclability, considerable rate performance, and good reversibility. Additionally, the mechanism of inhibiting shuttling effect by this composite separator is proposed. We hope that this work can give an insight into the development of multiple functional separators for Li anode protection in LOBs.
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2020
·
IF 9.038
Yong Liu,Ni Tan,Jinrui Guo,Jianlong Wang
In this study, a novel Al°-CNTs-Cu 2 O composite, capable of activating O 2 to generate H 2 O 2 and further to reactive oxygen species (ROSs) at a wide pH range, was synthetized, characterized and applied for the degradation of sulfamerazine. In the activation of O 2 by Al°-CNTs-Cu 2 O composite, H 2 O 2 was generated from the reaction of O 2 with Al°-CNTs, which could be catalytically decomposed into O 2 − and OH by Cu 2 O, the formed Cu(II) could be rapidly reduced to Cu 2 O by Al°-CNTs in composite, which made Al°-CNTs-Cu 2 O composite reusable and decreased the leaching of copper ions into solution. The removal efficiency of SMR and TOC was 73.91 % and 56.80 %, respectively at initial pH = 5.8, T = 20 °C, O 2 flow rate = 100 mL/min, Al°-CNTs-Cu 2 O dosage = 2 g/L, SMR = 50 mg/L, and reaction time = 60 min. The removal efficiency of SMR kept almost unchanged and the concentration of copper ions in solution was below 0.5 mg/L. The Al°-CNTs-Cu 2 O/O 2 process could be used as a novel catalyst for the degradation of refractory organic contaminants in water and wastewater by Fenton-like process at a wide pH range through the in situ generation of H 2 O 2 .
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Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 19
·9813-9824
·
IF 11.301
Yue Li,Jian Song,Mengting Jiang,Mbage Bawa,Xiaohong Wang,Yuyang Tian,Guangshan Zhu
Na5[IMo6O24]·3H2O and a porous aromatic framework (iPAF-1) were used to build an off-the-shelf building material (IMo6@iPAF-1) to realize the highly efficient oxidation of organic sulfurs like oxygenase. The synergy between IMo6 and iPAF-1 resulted in a higher BET surface area, hydrophobic microenvironment, and redox sites to show higher activity in aerobic oxidative desulfurization with almost 100% removal of model organic sulfurs under atmospheric pressure with almost 246 times higher TOFs compared to IMo6. It also showed efficiency in the desulfurization of gasoline and diesel to give very low S contents of 7.1 and 7.6 ppm with 99.3% and 99.4% removal, respectively, at 100 °C for 6 h. More importantly, IMo6@iPAF-1 could also catalyze desulfurization using concentrated O2 mixed with N2 or air instead of pure O2 with better safety and economics, while as low as 4.9 and 6.9 ppm S contents were achieved for gasoline and diesel, respectively. The special surroundings of IMo6@iPAF-1 repelled the sulfone product and allowed it to perform with the same efficiency when recycled without any treatment of the used catalyst.
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NEW JOURNAL OF CHEMISTRY
·
2020
·Vol. 44
·期 27
·11808-11816
·
IF 3.288
Shi-Yuan Zhang,Jing-Jing Ma,Hong-Lin Zhu,Yue-Qing Zheng
Syngas, as a necessary feedstock dependent on non-renewable fossil fuels, is a mixture of CO and H2, which could be prepared by a renewable strategy via electrochemical CO2 reduction in water electrolyte solutions. Herein, beaded Au@Co3O4 nanowire arrays (denoted as Au@Co3O4 NAs) were obtained by immersion in HAuCl4 solution with Co3O4 nanowire arrays. The Au@Co3O4 NAs exhibited outstanding electrochemical performance of producing syngas via tuning from 1 : 1 to 4 : 1 with controlling voltage. In addition, the Au@Co3O4 NAs showed better catalytic performance for the oxygen evolution reaction with an overpotential of 320 mV at a current density of 50 mA cm−2, along with a small Tafel slope of 75 mV dec−1 in 1 M KOH solution. The electrochemical performance of Au@Co3O4 NAs is obviously superior to Co3O4 NAs, which will open up a viable strategy for the design and fabrication of a bi-functional electrocatalyst for the overall reaction (CO2 + H2O → CO + H2 + O2).
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Nanoscale
·
2019
·Vol. 11
·期 31
·14654-14667
·
IF 6.97
Binbin Ding,Shuai Shao,Haihua Xiao,Chunqiang Sun,Xuechao Cai,Fan Jiang,Xueyan Zhao,Ping'an Ma,Jun Lin
The limited light penetration depth and tumor hypoxia are two natural shortcomings of photodynamic therapy (PDT). Overcoming these two issues within a single system is still a great challenge. Herein, photosensitizer (PS)-loaded and PEG-modified MnFe2O4-decorated large-pore mesoporous silica-coated β-NaYF4:20%Yb,2%Er@β-NaYF4 upconversion nanoparticles (UCMnFe-PS-PEG) as excellent PDT agents are successfully prepared for NIR light-mediated and O2 self-sufficient PDT. The large mesoporous structure observably increases PS loading efficiency (11.33 wt%) and the green luminescence from upconversion nanoparticles activated by NIR is able to activate PSs to generate ROS effectively. In addition, sub-10 nm MnFe2O4 nanoparticles work as a Fenton catalyst to generate O2in situ. In vivo experiments further prove that UCMnFe-PS-PEG not only provides magnetic guidance to the tumor, but also overcomes tumor hypoxia and dramatically enhances PDT efficiency. Furthermore, in vivo MR and UCL imaging are performed for accurate cancer therapy. We believe that the successful construction of the multifunctional UCMnFe-PS-PEG provides more revelations for developing advanced nano-drug systems for cancer therapy.
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Journal of Materials Chemistry A
·
2015
·Vol. 4
·期 4
·1399-1407
·
IF 7.443
Guangyu Zhao,Li Zhang,Jixian Lv,Changle Li,Kening Sun
Hydrothermal self-assembly is a highly efficient and low cost method to prepare graphitic foam from graphene oxides; however, the self-assembly frameworks usually do not have controllable pore structures because of the spontaneous process. In this paper, a hydrothermal synthesis assisted by ammonium peroxo-polymolybdate [(NH4)2Mo2O11] tailoring to fabricate graphitic foam is presented. The foam possesses pore structures which can be controlled by adjusting the rate of charge in the hydrothermal experiments. Furthermore, the foam obtained from a definite rate of charge [(NH4)2Mo2O11 : graphene oxide is 1 : 2 in weight] has a hierarchical pore structure and a through-hole net. In electrochemical energy storage, such unique features are beneficial for providing efficient mass transport as well as abundant, accessible active sites. The graphitic foam was tested for use as self-supported electrodes of Li–O2 batteries (LOBs) and Li ion batteries (LIBs) without any metallic current collectors or organic binders, and the foam frameworks exhibited remarkable lithium ion storage properties in both of the two batteries (e.g., 5500 mA h g−1 at 0.2 A g−1 as LOB cathodes and 250 mA h g−1 at 50 A g−1 as LIB anodes).
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Catalysts
·
2025
·Vol. 15
·期 6
·545
·
IF 4
Xiaohong Yao,Jian Zhang,Chao Long
This study explored how pore size engineering in Nb-Mn/MCM-41 catalysts affects plasma-catalytic toluene oxidation. Adjusting the pore diameter (2.49–3.98 nm) modulated metal-support interactions and oxygen dynamics, with pore expansion to 3.73 nm (M3) optimizing the Mn4+/(Mn2++ Mn3+) ratio (XPS: 36.8%), the amount of lattice oxygen species (O2-TPD: 0.222 mmol/g), and crystallite size control (1.5 ± 0.2 nm, TEM). Smaller pores (M1: 2.49 nm) enhanced toluene adsorption but limited active site accessibility, while oversized pores (M4: 3.98 nm) reduced oxygen storage capacity (0.600→0.412 mmol/g). The Nb-Mn/M3 catalyst achieved superior performance with 96.8% toluene conversion, 55.0% CO2selectivity, and 85.4% carbon balance, while minimizing organic byproducts (GC-MS). Mechanistic studies revealed pore-mediated oxygen storage-transport cycles as critical for decoupling adsorption and oxidation steps. This study reveals fundamental mechanisms linking pore architecture to plasma-catalytic synergy in toluene oxidation, offering critical insights for the systematic design of energy-efficient, plasma-catalytic systems targeting industrial VOCs remediation.
研究领域:
催化化学
·
环境化学
·
材料科学
·
等离子体化学
·
纳米技术
·
表面科学
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高影响因子
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Tong Zhou,Guohui Dong,Jiahao Geng,Kai Han,Chenyang Xiao
In this study, a novel Z-scheme + II-type ternary heterojunction nanocomposite was prepared by one-step solvothermal method using g-C 3 N 4 , FeS 2 and Fe 2 O 3 as raw materials. The successful preparation of this ternary heterojunction was confirmed by the structural analysis and the surface morphology study. Compared with g-C 3 N 4 , the ternary photocatalyst showed excellent photocatalytic performance for the degradation of tetracycline (TC). The enhancement of photocatalytic activity is mainly due to the increase of light absorption capacity, effective separation of carrier in space, and increase of electron transfer channels in this Z-Scheme + II-type composite system. The scavenger test and electron spin resonance spectroscopy show that O 2 − is the main oxidizing free radical in the photocatalytic system. Based on liquid chromatograph-mass spectrometer, a possible degradation pathway of TC was proposed. This study opens up a new idea for the design and synthesis of efficient Z-Scheme + II-type photocatalysts for environmental purification.
研究领域:
环境科学
·
材料科学
·
化学
·
光催化
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Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 8
·4880-4889
·
IF 12.732
Wei Wu,Wang Lin,Hongjiang Chen,Keyan Wei,Zhitong Li,Haitao Yang,Mingxian Liu,Huaicheng Xiang,Libo Deng,Lei Yao
The development of high-performance solid-state batteries (SSBs) that integrate high safety with high energy density has long been pursued. However, conventional lithium-containing anode materials are unable to balance these two requirements, thereby necessitating the exploration of lithium-free anodes for SSBs. In the current study, a core–shell lithium-free α-Fe2O3@TiNb2O7 (TNO) nanofiber composite is synthesized and applied as an SSB anode. The confinement effect from the hollow TNO nanotubes on the encapsulated α-Fe2O3 nanoparticles can buffer the volume-change crushing during charging/discharging, leading to robust structural stability. Moreover, the high rate capability of TNO and high capacity of α-Fe2O3 work synergistically to provide superior electrochemical performances. The prepared α-Fe2O3@TNO composite delivers twice the reversible capacity (625 mA h g−1 at 0.1 A g−1) of pristine TNO as well as a remarkably prolonged cycle life (500 cycles with 79.2% capacity retention) and an improved rate performance (305 mA h g−1 at 3 A g−1) compared with those of α-Fe2O3, making this composite the most efficient TNO-based anode material ever reported. By pairing the composite with the high-energy Li[Ni0.8Co0.1Mn0.1]O2 (NCM811) cathode, the SSB full cell exhibits a high energy density of 400 W h kg−1. These results demonstrate the feasibility and great potential of the proposed lithium-free anode material in SSBs for practical applications.
研究领域:
材料科学
·
电化学
·
能源存储
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高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Liying Hao,Jikui Sun,Qingyin Wang,Haijiao Xie,Xiangui Yang,Qiang Wei
As an atom-economical reaction, the direct generation of dimethyl carbonate (DMC) and ethylene glycol (EG) via the transesterification of CH3OH and ethylene carbonate (EC) has several promising applications, but the exploration of carriers with high specific surface areas and novel heterogeneous catalysts with more basic sites remains a long-standing research challenge. For this purpose, herein, a nitrogen-doped mesoporous carbon (NMC, 439 m2/g) based K–O2 Lewis base catalyst (K–O2/NMC) with well-dispersed strongly basic sites (2.23 mmol/g, 84.5%) was designed and synthesized. The compositions and structures of NMC and K–O2/NMC were comprehensively investigated via Fourier transform infrared spectroscopy, X-ray diffraction, X-ray photoelectron spectroscopy, scanning electron microscopy, transmission electron microscopy, N2 adsorption–desorption, CO2 temperature-programmed desorption, and contact angle measurements. The optimal structural configuration and electron cloud distribution of the K–O2/NMC catalyst were simulated using first-principles calculations. The electron transfer predominantly manifested as a flow from K–O to C–O/C–N, and the interatomic interactions between each atom were enhanced and exhibited a tendency for a more stable state after redistribution. Furthermore, the adsorption energies (Eads) of CH3OH at K–O–O and K–O–N sites were −1.4185 eV and −1.3377 eV, respectively, and the O atom in CH3OH exhibited a stronger adsorption tendency for the K atom at the K–O–O site. Under the optimal conditions, the EC conversion, DMC/EG selectivity, and turnover number/frequency were 80.9%, 98.6%/99.4%, and 40.5/60.8 h–1, respectively, with a reaction rate constant (k) of 0.1005 mol/(L·min). Results showed that the heterogeneous K–O2/NMC catalyst prepared herein greatly reduced the reaction cost while guaranteeing the catalytic effect, and the whole system required a lower reaction temperature (65 °C), a shorter reaction time (40 min), and a lower catalyst amount (2.0 wt % of EC). Therefore, K–O2/NMC can be used as a catalyst in different transesterification reactions.
研究领域:
催化化学
·
材料科学
·
绿色化学
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高影响因子