Journal of Advanced Ceramics
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2022
·Vol. 11
·期 11
·1801-1814
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IF 11.534
Cheng Fuhao,Zhang Fengnian,Liu Yufeng,Guo Meng,Cheng Chufei,Hou Jiadong,Miao Yang,Gao Feng,Wang Xiaomin
Environmental barrier coatings (EBCs) with excellent chemical resistance and good high-temperature stability are of great significance for their applications in next-generation turbine engines. In this work, a new type of high-entropy fluorite-structured oxide (Ce 0.2 Hf 0.2 Y 0.2 Pr 0.2 Gd 0.2 )O 2− δ (HEFO-1) with different Ti 4+ contents were successfully synthesized. Minor addition of Ti 4+ could be dissolved into a high-entropy lattice to maintain the structure stable, effectively reducing the phase formation temperature and promoting the shrinkage of bulk samples. Heat treatment experiments showed that all the samples remained a single phase after annealing at 1200–1600 °C for 6 h. In addition, high-entropy (Ce 0.2 Hf 0.2 Y 0.2 Pr 0.2 Gd 0.2 Ti 0.2 x )O 2− δ demonstrated great resistance to calcium—magnesium—alumina—silicate (CMAS) thermochemical corrosion. When the content of Ti was increased to x = 0.5, the average thickness of the reaction layer was about 10.5 after being corroded at 1300 °C for 10 h. This study reveals that high-entropy (Ce 0.2 Hf 0.2 Y 0.2 Pr 0.2 Gd 0.2 Ti 0.2 x )O 2− δ is expected to be a candidate for the next-generation EBC materials with graceful resistance to CMAS corrosion.
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MOLECULES
·
2022
·Vol. 27
·期 17
·5576
·
IF 4.927
Songtao Liu,Rui Yan,Muhammad Humayun,Huanli Zhang,Yang Qu,Yingxue Jin
It is highly desired to enhance charge separation and O2adsorption of the pyropheophorbide-a (Ppa) to promote visible-light activity and stability. Herein, Ppa modified 001-facet-exposed TiO2nanosheets (Ppa/001T) nanocomposites with different weight ratios were fabricated via the self-assembly approach by OH induced. Compared with the bare Ppa, the 8% amount optimized 8Ppa/001T sample displayed 41-fold enhanced activity for degradation of Ametryn (AME) under visible-light irradiation. The promoted photoactivities could be attributed to the accelerated charge carrier’s separation by coupling TiO2as thermodynamic platform for accepting the photoelectrons with high energy from Ppa and the promoted O2adsorption because of the residual fluoride on TiO2. As for this, a distinctive two radicals (•O2−and •OH) involved pathway of AME degradation is carried out, which is different from the radical pathway dominated by •O2−for the bare Ppa. This work is of utmost importance since it gives us detailed information regarding the charge carrier’s separation and the impact of the radical pathway that will pave a new approach toward the design of high activity visible-light driven photocatalysts.Keywords:Ppa;001-facet-exposed TiO2;charge separation;visible-light photocatalysis;Ametryn
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高影响因子
COMPOSITES PART B-ENGINEERING
·
2022
·
IF 11.322
Xinbin Wu,Wei Yu,Wei Xu,Yujun Zhang,Shundong Guan,Zheng Zhang,Shuwei Li,Huanchun Wang,Xuanjun Wang,Liang Zhang,Ce-Wen Nan,Liangliang Li
Lithium-oxygen (Li–O 2 ) batteries are promising next-generation energy storage devices due to their ultrahigh theoretical specific energy. Oxide electrocatalysts such as RuO 2 are often used to improve the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) processes in Li–O 2 batteries, but the relation between the structural parameters and their catalytic properties is unclear so far. In this work, we synthesize RuO 2 nanoparticles at different annealing temperatures and investigate the influence of the Ru–O bond distances of RuO 2 on the OER and ORR processes in Li–O 2 batteries. The results of X-ray absorption fine structure show that the bond distances decrease with the increase of the annealing temperature. The RuO 2 with longer Ru–O bond distances renders a lower charge plateau to Li–O 2 batteries, showing a better OER performance, while that with shorter bond distances gives a larger discharge capacity and is more friendly to the ORR process. The cycle life of Li–O 2 batteries with a carbon nanotube-RuO 2 composite cathode is improved to 287 cycles (1148 h) under an extreme testing condition (the voltage range is 2.3–4.2 V), when the Ru–O bond distances are optimized. In addition, the influence of the Ru–O bond distances on the catalytic properties of RuO 2 is analyzed by density functional theory calculations. The findings in this work provide a guidance to enhance the ORR and OER efficiency of RuO 2 and other oxide catalysts.
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CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
·
2021
·Vol. 38
·期 1
·200-208
·
IF 1.307
Wang Yue,Wang Xiaoxue,She Ping,Guan Dehui,Song Lina,Xu Jijing
D esign and fabrication of functional porous air cathode materials with superior catalytic activity is still the key point for non-aqueous lithium-oxygen(Li-O 2 ) batteries. Herein, inspired by the self-standing three-dimensional(3D) structure of the natural spinach leaves, a unique binder-free and self-standing porous Au/spinach cathode for high-performance Li-O 2 batteries has been developed. The carbonized spinach leaves serve as a superconductive current collector and an ideal porous host for accommodating catalysts. The Au/spinach cathode could offer enough spaces for accommodating the discharge products, shorten the distance of the oxygen and electrolyte diffusion, and promote the oxygen reduction reaction(ORR) and oxygen evolution reaction (OER) processes. This optimized Au/spinach cathode achieved a high specific area capacity of 7.23 mA·h/cm 2 at a current density of 0.05 mA/cm 2 and exhibited excellent stability(280 cycles at 0.05 mA/cm 2 with a fixed capacity of 0.2 mA·h/cm 2 ). The superior performance encourages the construction of more advanced cathode architectures by the use of bio-composites for Li-O 2 batteries.
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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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JOURNAL OF HAZARDOUS MATERIALS
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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
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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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