Nanoscale
·
2023
·
IF 6.7
Yingyi Zhang,Lin Zhang,Yuhan Zhang,Rong Ju,Guoqing Wei
Antimicrobial sonodynamic therapy (SDT) has broad application potential in the eradication of multidrug-resistant (MDR) bacterial infections due to its non-invasiveness, absence of resistance concern, and high cytotoxicity. However, the hypoxic infection microenvironment and the rapid depletion of O2 during SDT severely limit the therapeutic efficacy of SDT. Herein, an ultrasound-controllable ROS-responsive nanoplatform (FOT/Fe3O4@Lipo-ICG) was constructed and prepared by encapsulating FOT and Fe3O4 nanoparticles (Fe3O4 NPs) within sonosensitiser ICG-modified liposomes. Both in vitro and in vivo, we observed that the ICG conjugation on the surface of liposomes could effectively maintain a good dispersion and prevent ICG aggregates in complex biological matrices. In addition, the liposomes could significantly block the catalytic activity of the Fe3O4 NPs, as well as the release of FOT, whereas upon US irradiation, the catalytic activity of Fe3O4 NPs was recovered to catalyse the decomposition of endogenous H2O2 into O2 and •OH. Meanwhile, the FOT was successfully released to react with endogenous glutathione to sequentially produce NO. Based on the aforementioned advantages, the FOT/Fe3O4@Lipo-ICG demonstrated potent efficacy in eradicating methicillin-resistant Staphylococcus aureus-induced local infection and sepsis resulting from local infection. Thus, the developed US-controllable nanoplatform offers a promising strategy for enhancing SDT for eradicating MDR bacterial infections.
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高影响因子
Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Liu Yang,Jing Li,Guoqiang Cao,Yiyan Yang,Wen Luo,Zhiqi Zhang,Lizhi Feng,Xinglai Zhang,Baodan Liu
This study reports on the development of highly-efficient Pt/CuO-Fe 2 O 3 /TiO 2 monolithic catalysts for the low-temperature conversion of NO to N 2 via CO-SCR. In this case, ultrathin TiO 2 nanosheet arrays are designed to in situ grow on flexible Ti mesh to provide more spaces/areas for the loading of highly-dispersed Fe 2 O 3 and CuO active components. Furthermore, Pt nanoparticles with an average size of 1.30 nm are effectively decorated on the surface of CuO-Fe 2 O 3 /TiO 2 . The H 2 -TPR and NO-TPD results demonstrate that the excellent synergistic effect between TiO 2 , CuO, Fe 2 O 3 and trace amounts of Pt is conducive to enhance the adsorption of NO and finally promote the CO-SCR. The obtained Pt/CuO-Fe 2 O 3 /TiO 2 catalysts exhibit excellent CO-SCR performance with 100 % NO conversion, and 100 % N 2 selectivity at 250 °C, showing great potential of de-NO x application by using toxic CO as reductant in industry.
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ACS Applied Nano Materials
·
2023
·
IF 5.9
Hao Fan,Yiming Yang,Xueting Yang,Xuefeng He,Jian Sun,Liu Yang,Jiao Li,Zhenxing Shen
Although the surface acidity of CeO2 has been increased by H2SO4 to increase its acid sites, the low-temperature (<250 °C) activity of sulfated CeO2 catalysts still needs to be improved. In this study, a Pt-modified CeO2 catalyst was prepared by impregnation or reduction methods to increase its catalytic activity. The results showed the Pt-modified CeO2 catalyst significantly widened its low-temperature catalytic window. The NO conversion and N2 selectivity of the Pt1.0%/SCe-I sample were both more than 90% at 200–350 °C because of its numerous acid sites, excellent redox ability, and higher Pt2+ content. NH3, NH4+, –NH2, and bridging nitrates and monodentate nitrates on the Pt1.0%/SCe-I catalyst surface acted as the active substances. Among them, coordinated NH3 at the Lewis acid sites reacted first. This study highlights the interactions among metals, sulfates, and carriers and supplies a useful method to improve the low-temperature activity of sulfated CeO2.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2023
·
IF 4.3
Li-Zhi Zhang,Hong-Bin Ju,Tao Geng,De-Bao Li,Ya-Jie Jiang,Ya-Kui Wang
Graphical A novel phase transfer catalyst comprising phosphotungstic acid and biquaternary ammonium cation salt is synthesized for the epoxidation of long carbon chain olefins under solvent-free conditions, which exhibits high selectivity for epoxides. Different methods are used to characterize the fundamental structure and catalytic mechanism of this catalyst. In this study, we have developed a novel catalyst synthesized by phosphotungstic acid and a gemini quaternary ammonium cation salt. This quaternary ammonium salt not only reduces the interfacial tension between olefins and hydrogen peroxide but also forms a notably stable structure with phosphotungstic acid. Dodecene was successfully epoxidized to epoxy dodecane with a selectivity of 82.9 %. The impact of initial conditions was systematically investigated such as molar ratio, temperature, reaction time, and catalyst dosage on the catalytic performance. Characterization of the catalyst morphology was performed by SEM, TEM and SAXS. Raman spectra, FT-IR and XPS spectra were employed to perform the catalyst transformation during the epoxidation reaction. This catalytic mechanism study could provide the industrial application in the epoxidation of long-chain olefins.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Xiangsen Xu,Fengye Lyu,Jiahao Chen,Yiqing Zeng,Zhaoxiang Zhong,Feng Zhang,Weihong Xing
In this work, TiO 2 nanocones grown on SiC membrane was used as the support of V 2 O 5 -WO 3 species to prepare V 2 O 5 -WO 3 /TiO 2 @SiC (VWTi(C-X)@SiC) catalytic membrane for dust filtration and NH 3 -SCR denitration. On account of the large specific surface area, abundant surface acid sites and prominent redox property, the optimized VWTi(C-550)@SiC catalytic membrane shows >90% NO removal efficiency at the temperature of 280–360 °C, which are much higher than VWTi(P-550)/SiC catalytic membrane (TiO 2 nanoparticles prepared by traditional vacuum coating titanium sol method was used as the support of V 2 O 5 -WO 3 species, NO conversion <80% at whole tested temperature). Additionally, VWTi(C-550)@SiC displays superior stability during the SO 2 + H 2 O resistance and 300 h long-term test at 300 °C, and exhibits an excellent dust filtration performance (2.5 μm SiO 2 particles interception rate exceeded 99.99%) under all test conditions. More importantly, the structure of nanocones decrease the influence of tensile stresses due to the different thermal expansion coefficients of TiO 2 and SiC membranes, which significantly suppress the fall of VWTi catalyst layer from the surface of SiC during pulse-jet cleaning. Among above results, it can be concluded that the optimized VWTi(C-550)@SiC catalytic membrane shows a prosperous application prospect for the simultaneously dust filtration and NH 3 -SCR denitration of medium–high temperature flue gas .
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Zhihui Hu,Huanmin Liu,Ningxin Kang,Kangle Lv,Qin Li
Using solvothermal methods to in situ oxidize two-dimensional titanium carbide (Ti 3 C 2 T x ) MXene into TiO 2 nanocrystals offered an effective strategy to construct highly efficient TiO 2 /Ti 3 C 2 T x heterojunctions for photocatalytic applications. Nevertheless, the effect of the chosen solvent on the Ti 3 C 2 T x oxidation and the product's performance was often neglected. Herein, isopropanol (ISO), ethanol (EtOH), ethylene glycol (EG), dimethyl sulphoxide (DMSO) and deionized water (Water) were taken as the representative solvents to prepare TiO 2 /Ti 3 C 2 T x composites by one-step solvothermal method for photocatalytic NO emission. It was the large polarity, dielectric constant and surface tension of the solvents that offered Ti 3 C 2 T x with good dispersibility and high oxidation degree during the solvothermal process. More importantly, the solvothermal treatment of Ti 3 C 2 T x in DMSO could promote the formation of TiO 2 nanoparticles with obviously higher crystallinity and more surface oxygen vacancies than those in EG, EtOH and ISO. Therefore, the photocatalytic NO oxidation efficiency of the samples within 30-min irradiation showed a descending order of TT-DMSO (46.9%), TT-Water (42.2%), TT-EG (32.3%), TT-EtOH (26.7%), and TT-ISO (19.9%). This work highlighted the significance of oxidation environment for Ti 3 C 2 T x , which could bring about some new but necessary consideration on the processing technique of MXene families for their future practical applications.
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ENERGY & FUELS
·
2019
·
IF 3.021
Zhitao Han,Tian Lan,Zhiwei Han,Shaolong Yang,Jingming Dong,Deping Sun,Zhijun Yan,Xinxiang Pan,Liguo Song
Experiments were conducted to simultaneously remove NO and SO2 from simulated exhaust gas by cyclic scrubbing and online supplementing pH-buffered NaClO2 solutions in a bench-scale reactor. The effects of key operating parameters on pollutant removal performance had been investigated. The results suggested that an extremely high oxidant utilization rate could be obtained when the oxidant supplementing molar rate approached the oxidant consumption molar rate. Though co-existing SO2 in flue gas would consume a certain amount of the oxidant during the absorption process, the intermediate products of SO32– ions generated from SO2 hydrolysis might be in favor of NO2 absorption to some extent. The introduction of ethanol in scrubbing solution could enhance NOx removal performance largely, which was possibly because of its inhibition effect on SO32– oxidation. The reaction mechanism and reaction products in scrubbing solutions were also discussed roughly through theoretical calculations and ion chromatography analysis.
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Advanced Healthcare Materials
·
2018
·Vol. 7
·期 24
·1801094
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IF 5.609
Guoqing Wei,Yi Wang,Xuehui Huang,Guang Yang,Jingya Zhao,Shaobing Zhou
The accumulation of nanoparticles in tumors by the enhanced permeability and retention (EPR) effect is effective and well known. However, how to maximize accumulation is still a bottleneck in the development of nanomedicine. Herein, a tumor vascular-targeted hybrid polymeric micelle, which has a great capacity to selectively augment the EPR effect of nanoparticles by dilating tumor blood vessels via the activity of nitric oxide (NO), is presented. Under neutral conditions, the micelle is stable, with a long blood circulation half-life due to the carboxylated poly(ethylene glycol) (PEG) layer; in mildly acidic tumor tissues, the micelle can selectively target the tumor blood vessels by the exposed cyclic Arg-Gly-Asp peptide (cRGD) peptides, which is realized with a pH-dependent hydrolysis of the monomethoxy PEG layer. Simultaneously, exposed copper ions catalyze the decomposition of endogenous NO donors, which generates NO in situ, leading to vasodilation and increased tumor vascular permeability. As a result, the accumulation of nanoparticles is significantly enhanced, and a high accumulation of doxorubicin in tumors is achieved at 48 h after injection. This high dose of therapeutic agent produces a large inhibition of tumor growth (94%) in cancer treatment, and shows no general toxicity, with 100% of the mice surviving the treatment regimen.
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高影响因子
APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Fawei Lin,Jiaming Shao,Hairong Tang,Yan Li,Zhihua Wang,Guanyi Chen,Dingkun Yuan,Kefa Cen
NO x control by catalytic oxidation combined with wet absorption has been a promising technology for the flue gas treatment of industrial boiler and furnace. LaMnO 3+δ perovskites were investigated as catalysts for NO oxidation. The comparison between metal substitution of La and Mn cations was researched. The activity results indicated that La site substitution was more favorable for NO oxidation than Mn site substitution. LaCoMnO exhibited the highest activity in NO oxidation with maximum value of 83.74% at 250 °C. That value further increased to 89.96% after acid etching (LaCoMnO-A), and closely, such high value of 89.78% was achieved at 220 °C. The surface area was significantly improved by acid etching, i.e., from 47.0 m 2 /g to 212.0 m 2 /g, Tremendous changes in crystalline structure and morphology were taken place, i.e., perovskites phase disappeared and MnO 2 was detected instead; compact amorphous particle morphology was replaced by multiple layer structure. Even more, Mn 4+ ions and oxygen vacancies accumulated on the surface were improved. Deservedly, the redox property was enhanced enormously, especially at low temperature. Subsequently, SO 2 poisoning tests were conducted at 250 °C under 20 ppm SO 2 . Interestingly, no decrease was observed for LaCoMnO-A within 480-min SO 2 poisoning test, which was totally contrasted with the nearly complete deactivation results of LaCoMnO. In-situ DRIFTS measurements validated nitrate disappeared and replaced by sulfate formation on the catalyst surface. Merely, under low-concentration SO 2 atmosphere, the monodentate nitrate and bidentate nitrate were destroyed, while the free nitrates exhibited higher resistance. Overall, the acid etching improved the catalyst resistance to SO 2 , which may have the potential to apply in the flue gas treatment of low-sulfur and sulfur-free fuel fired boiler and furnace.
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RSC Advances
·
2019
·Vol. 9
·期 9
·4682-4692
·
IF 3.049
Yang Yang,Zhun Hu,Rongli Mi,Dan Li,Xiang Yong,Huie Yang,Kunfeng Liu
A series of manganese-based catalysts supported by 5–10 nm, 10–25 nm, 40 nm and 60 nm anatase TiO2 particles was synthesized via an impregnation method to investigate the effect of the initial support particle size on the selective catalytic reduction (SCR) of NO with NH3. All catalysts were characterized by transmission electron microscopy (TEM), N2 physisorption/desorption, X-ray diffraction (XRD), temperature programmed techniques, X-ray photoelectron spectroscopy (XPS) and in situ diffuse reflectance infrared transform spectroscopy (DRIFTS). TEM results indicated that the particle sizes of the MnOx/TiO2 catalysts were similar after the calcination process, although the initial TiO2 support particle sizes were different. However, the initial TiO2 support particle sizes were found to have a significant influence on the SCR catalytic performance. XPS and NH3-TPD results of the MnOx/TiO2 catalysts illustrated that the surface Mn4+/Mn molar ratio and acid amount could be influenced by the initial TiO2 support particle sizes. The order of surface Mn4+/Mn molar ratio and acid amount over the MnOx/TiO2 catalysts was as follows: MnOx/TiO2(10–25) > MnOx/TiO2(40) > MnOx/TiO2(60) > MnOx/TiO2(5–10), which agreed well with the order of SCR performance. In situ DRIFTS results revealed that the NH3-SCR reactions over MnOx/TiO2 at low temperature occurred via a Langmuir–Hinshelwood mechanism. More importantly, it was found that the bridge and bidentate nitrates were the main active substances for the low-temperature SCR reaction, and bridge nitrate adsorbed on Mn4+ showed superior SCR activity among all the adsorbed NOx species. The variation of the initial TiO2 support particle size over MnOx/TiO2 could change the surface Mn4+/Mn molar ratio, which could influence the adsorption of NOx species, thus bringing about the diversity of the SCR catalytic performance.
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高影响因子
CHEMOSPHERE
·
2019
·
IF 5.108
Rongji Cui,Suxia Ma,Jie Wang,Shujun Sun
The catalytic gas-phase H 2 O 2 oxidation of NO was achieved over Fe-based catalysts supported on montmorillonite K10, γ-alumina and ZSM-5. ESR tests illustrate that the three catalysts can catalyze decomposition of H 2 O 2 yielding highly reactive hydroxyl radicals , of which Fe/K10 has the fastest rate, followed by Fe/γ-alumina. Fe 3+ in Fe/K10 and Fe/γ-alumina show lower density of electron cloud due to a strong interaction between Fe 3+ and the support, which benefits the electron transfer from the H 2 O 2 to Fe 3+ , thus favoring the production of hydroxyl radicals. Fe species exist on the surface of Fe/K10 mainly in the form of Fe 2 O 3 , whereas Fe species of Fe/γ-alumina and Fe/ZSM-5 exist mainly in the form of Fe 3 O 4 , and it is found that Fe 2 O 3 is more active than Fe 3 O 4 in catalytic gas-phase H 2 O 2 oxidation of NO. Interestingly, Fe/ZSM-5 has the lowest efficiency in generating hydroxyl radicals, its NO removal efficiency is 90%, which is much higher than 47.5% for Fe/γ-alumina and 62.3% for Fe/K10. In-situ IR results suggested that Fe/ZSM-5 are dual functional in oxidation of NO, that is, whether both Fe ion sites and Brønsted acid sites collectively provide the catalytic functionality. In the meantime, a possible reaction mechanism on catalytic gas-phase H 2 O 2 oxidation of NO over Brønsted acid sites is proposed.
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高影响因子
APPLIED SURFACE SCIENCE
·
2018
·
IF 4.439
Weiyuan Yao,Xiaoqiang Wang,Yue Liu,Zhongbiao Wu
In this paper, Ce O P material (mainly consisted of CePO 4 ) and TiO 2 supported CeO 2 catalysts were prepared by wet impregnation route for the selective catalytic reduction (SCR) of NO with NH 3 . The SCR activity results had revealed that CeO 2 /Ce O P-0.4 catalyst yielded over than 90% NO conversion within the temperature range of 200–300 °C, whereas the deNO x efficiency of CeO 2 /TiO 2 -0.4 catalyst was less than 30% at 200 °C. After a series of characterization tests, it was found that CeO 2 /Ce O P catalysts were of better dispersion of active phase than CeO 2 /TiO 2 owing to the strong interactions between CeO 2 and surficial Ce O species on Ce O P material. Thus, more active oxygen species could participate in the SCR reaction at low temperature. Furthermore, compared to CeO 2 /TiO 2 sample, the surface acidity was greatly enhanced for CeO 2 /Ce O P catalysts by the introduction of the acidic support, benefiting the adsorption of NH 3 . Both of which were attributed to the main reasons of the promoted SCR performance over CeO 2 /Ce O P catalysts. Moreover, the NO x ad-species on CeO 2 /TiO 2 sample were very stable and could hardly react with adsorbed NH 3 , impeding L-H reaction pathway at low temperature.
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