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MACROMOLECULAR CHEMISTRY AND PHYSICS · 2022 ·Vol. 223 ·期 9 ·2200022 · IF 2.996

Multiregulation of Aggregation-Induced Emission (AIE) via a Competitive Host–Guest Recognition and α-Amylase Hydrolyzing

Lili Cai,Jiawei Lin,Mingyu Qiao,Jianwei Guo,Huatang Zhang,Sa Liu,Yong-Guang Jia

The multiregulation of aggregation-induced emission (AIE) that responds to external stimuli to finish multifunctions has become a focus of interest in biodiagnosis. Host–guest- recognition is an efficient strategy to introduce switchable, reversible, and other functional properties into AIE molecules. Herein, an amphiphilic tetraphenylethylene (TPE) derivative TPE-PEG is prepared via the simple amidation reaction and chosen as an AIE-based guest polymer. The aggregated state of TPE-PEG is altered and the fluorescence of TPE-PEG can be turned off in the presence of γ -cyclodextrins ( γ -CDs) due to the formation of host–guest complex between TPE units and γ -CDs. TPE units in the cavities of γ -CDs are released free and an aggregated state of TPE-PEG is restored via the guest competition epistasis of bile acid. Meanwhile, α -amylase can hydrolyze the host molecules of γ -CDs, resulting in an aggregated state of TPE-PEG again and turning the fluorescence on subtly. This reversible multiregulation of fluorescence may meet the multirequirements for the diagnosis in vivo due to the biological nature of α -amylase and bile acid.

研究领域: 生物化学 · 分子生物学 · 材料科学
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Materials Research Express · 2017 ·Vol. 4 ·期 3 ·035035 · IF 1.068

Effect of particle size on gamma radiation shielding property of gadolinium oxide dispersed epoxy resin matrix composite

Ran Li,Yizhuo Gu,Yidong Wang,Zhongjia Yang,Min Li,Zuoguang Zhang

Epoxy resin matrix composites filled with dispersed micro and nano gadolinium oxide (Gd2O3) particles of different contents were fabricated in this study. The γ radiation shielding and mechanical properties of these micro and nano composites were evaluated by measuring mass attenuation coefficients at photon energies from 31 keV to 356 keV and flexural performances. Adding Gd2O3 obviously increases mass attenuation coefficients of composites, and the enhancement is stronger at low photon energy because of dominating photoelectric effect and k-edge of element gadolinium. Effect of Gd2O3 particle size on shielding property of composite was also discussed. The results show that nano-Gd2O3 composites have better ability to shield X and γ ray than micro-Gd2O3 composites, and an enhanced effect of ~28% is obtained with Gd2O3 content of around 5 wt.% at 59.5 keV. The reason is attributed to higher probability of interaction between γ-ray and nano particles. Especially, this effect is prominent in low particle concentration. For flexural property, nano-Gd2O3/epoxy composite show equivalent flexural strength and up to15% higher flexural modulus compared with micro-Gd2O3/epoxy composite. Based on these experimental results, nano-Gd2O3 reinforced epoxy composite is believed to be a promising novel radiation shielding material.

研究领域: 材料科学 · 辐射防护
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CERAMICS INTERNATIONAL · 2024 · IF 5.1

Synthesis and application study of α-Al2O3 with large specific surface area at high-temperature by hydrothermal-assisted freeze-drying

Siyi Li,Pinyi Wang,Jianyun Hu,Guangcan Yang,Youjun Lu,Zhenxia Yuan,Xiao Zhang,Sen Liang

γ-AlOOH nanopowder synthesized using hydrothermal-assisted freeze-drying was employed as a precursor, with AlF₃ as a sintering aid, to explore the preparation of α-Al₂O₃ with a high specific surface area at elevated temperatures. The γ-AlOOH nanopowder produced in this study exhibited superior dispersion, achieving a specific surface area of 198.06 m 2 /g and a zeta potential of 45.8 mV. At a calcination temperature of 1200 °C, the resulting α-Al₂O₃, synthesized from γ-AlOOH and AlF₃, maintained a specific surface area of 27.72 m 2 /g, significantly higher than the typical values reported in the literature (generally below 10 m 2 /g). The α-phase purity exceeded 99 %, and the [AlO₆] proportion was 95.07 %. Furthermore, at a calcination temperature of 1150 °C, the specific surface area of the α-Al₂O₃ reached 50.48 m 2 /g. Using this α-Al₂O₃ as a carrier, a composite TiO₂ catalyst was prepared via a sol-gel and hydrothermal method. This catalyst demonstrated a photocatalytic degradation rate of over 98 % for rhodamine B (10 mg/L) within 30 min of irradiation, under the illumination of a 300 W mercury lamp in proximity to the light source.

研究领域: 材料科学 · 环境科学
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International Journal of Applied Ceramic Technology · 2018 ·Vol. 15 ·期 6 ·1490-1501 · IF 1.165

Influence of alumina binders on adhesion and cohesion during preparation of Cu-SAPO-34/monolith catalysts

Xiangli Kong,Minghui Qiu,Anran Wang,Lu Yang,Rongfei Zhou,Yiqun Fan,Deshuang Kong,Changjun Gu

The adhesion and cohesion between the coating layers and the ceramic honeycombs are usually one of the key issues in the preparation of high-performance zeolite-based/Monolith catalysts. In this work, we investigate the deposition of high-efficiency Cu-SAPO-34 catalyst on a cordierite monolith with special focus on the impact of alumina binders on the structure, mechanical adhesion and cohesion, and catalytic performance of the monolithic catalyst. Two kinds of alumina nanoparticles, α-alumina and γ-alumina, have no significant impacts on the Cu-SAPO-34 crystal structure, micropore morphology and catalytic activity. But washcoating experiments showed that the mass loss rate of the coating was less and the loading of the catalyst was higher when α-alumina was used as the binder. The reason of improving the adhesion and cohesion strength is the suitable thermal shrinkage, the uniform distribution and densification structure of α-alumina. Furthermore, optimization of the coating formulation with α-alumina as the binder has been performed. Finally, the catalyst prepared under the optimal conditions was tested by SCR and a maximum conversion rate of 97.4% was obtained. It was concluded that the use of the washcoating method with α-alumina does not affect catalytic performance while it increases bonding strength between substrate and catalysts.

研究领域: 化学工程 · 催化材料科学
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Small · 2024 · IF 13

Cluster–Cluster Co-Nucleation Induced Defective Polyoxometalate-Based Metal–Organic Frameworks for Efficient Tandem Catalysis

Songzhu Xing,Xujiao Ma,Qingqing Gu,Nana Ma,Zhong Zhang,Guoying Han,Rui Huang,Xiao Feng,Bing Yang,Chunying Duan,Yiwei Liu

The construction of defective sites is one of the effective strategies to create high-activity Metal–Organic frameworks (MOFs) catalysts. However, traditional synthesis methods usually suffer from cumbersome synthesis steps and disordered defect structures. Herein, a cluster–cluster co-nucleation (CCCN) strategy is presented that involves the in situ introduction of size-matched functional polyoxometalates (H 6 P 2 W 18 O 62 , {P 2 W 18 }) to intervene the nucleation process of cluster-based MOFs (UiO-66), achieving one-step inducement of exposed defective sites without redundant post-processing. POM-induced UiO-66 ({P 2 W 18 }-0.1@UiO-66) exhibits a classical reo topology for well-defined cluster defects. Moreover, the defective sites and the interaction between POM and skeletal cluster nodes are directly observed by Integrated Differential Phase Contrast in Scanning Transmission Electron Microscopy (iDPC-STEM). Owing to the molecular-level proximity between defective sites and POM in the same nano-reaction space, {P 2 W 18 }-0.1@UiO-66 exhibits efficient tandem catalysis in the preparation of γ-valerolactone (γ-GVL) from laevulinic acid (LA) by the combination of Lewis and Brønsted acids with 11 times higher performance than defective UiO-66 formed by conventional coordination modulation strategy. The CCCN strategy is applicable to different POM and has the potential to be extended to other cluster-based MOFs, which will pave a new way for the construction of functional MOFs with multi-centered synergistic catalysis.

研究领域: 材料科学 · 催化化学
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Frontiers of Chemical Science and Engineering · 2020 ·Vol. 15 ·期 5 ·1088-1098 · IF 3.552

Synthesis of boron modified CoMo/Al2O3 catalyst under different heating methods and its gasoline hydrodesulfurization performance

Shang Hui,Guo Chong,Ye Pengfei,Zhang Wenhui

Catalytic hydrodesulfurization (HDS) technique is widely used for clean gasoline production. However, traditional HDS catalyst (CoMo/γ-Al 2 O 3 ) exhibits high hydrogenation performance of olefins (HYDO), resulting in the loss of gasoline octane number. To achieve high HDS/HYDO ratio, the key issue is to reduce the interaction between active metals and the support, therefore, in this research, the modified CoMo/γ-Al 2 O 3 catalysts with various boron amounts were investigated under traditional or microwave heating. The effects of preparing methods as well as boron amounts on the active phase, acidic properties and HDS catalytic activities were examined. Results show that the modification, especially under microwave treatment, can significantly weaken the interaction between the active component and the support by enlarging the surface area and pore diameter, and reducing the acidity of the support. As a result, the stacking numbers of MoS 2 slabs were obviously improved by the modification and microwave treatment, contributing to higher edge/ rim ratio, and resulting in higher HDS performance and selectivity to olefin.

研究领域: 催化化学 · 能源化工
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LANGMUIR · 2018 · IF 3.789

Controllable Synthesis of Monolayer Poly(acrylic acid) on the Channel Surface of Mesoporous Alumina for Pb(II) Adsorption

Ya-Ping Wang,Peng Zhou,Shi-Zhong Luo,Xue-Pin Liao,Bin Wang,Qian Shao,Xingkui Guo,Zhanhu Guo

Polymer/inorganic nanocomposites exhibit special properties due to highly intimate interactions between organic and inorganic phases and thus have been deployed for various applications. Among them, nanocomposites with monolayer polymer coverage on the inorganic surface demonstrate the highest efficiency for applications. However, the controllable synthesis of the polymer monolayer in mesopores of inorganic substrates remains a challenge. In this study, poly(acrylic acid)/γ-alumina nanocomposites (PAA/alumina) were synthesized via the in situ polymerization of acrylic acid impregnated in mesopores of alumina. By applying the preneutralization of monomers, the polymerization was found to be highly controllable in generating monolayer PAA coverage. The formation of monolayers was verified by thermogravimetry, semiquantitative Fourier transform infrared spectroscopy, N2 adsorption–desorption, and Pb(II) adsorption. Alternatively, the organic loadings of PAA/alumina composite samples could be controlled in the range of 0.2 to 1.0 equiv of monolayer, together with the linearly correlated metal ion adsorption capacity. As calculated by the complexation model, one Pb(II) is combined with two carboxylate groups of PAA. The formation of the monolayer polymer inside mesoporous oxide channels represents a method for the development of highly promising functional nanocomposites.

研究领域: 材料科学 · 环境科学
✓ 已验证 DOI PubMed 高影响因子
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JOURNAL OF BIOMATERIALS SCIENCE-POLYMER EDITION · 2023 · IF 3.6

Physicochemical properties and cytocompatibility of radiation-resistant and anti-washout calcium phosphate cement by introducing artemisia sphaerocephala krasch gum

Chenyu Tang,Teliang Lu,Haishan Shi,Jiandong Ye

The anti-washout ability of calcium phosphate cement (CPC) determines the effectiveness of CPC in clinical application. The γ-ray irradiation method often used in the sterilization process of CPC products is easy to degrade some commonly polymer anti-washout agent, which greatly reduces its anti-washout performance. Artemisia sphaerocephala Krasch gum (ASKG) has the potential of radiation resistance and anti-washout, but no one has considered its performance as anti-washout agent of CPC and mechanism of radiation resistance and anti-washout so far. In this study, we report the effect of γ-ray on ASKG and the effectiveness of ASKG for enhancing of radiation resistance and anti-washout ability of CPC, the physical, chemical properties and in vitro cell behaviors of ASKG-CPCs were also investigated. The results showed that addition of ASKG before and after irradiation could significantly enhanced the anti-washout performance of CPC, which is differ from conventional anti-washout agents. Meanwhile, ASKG-CPCs had an excellent injectable property and biocompatibility, and low content of irradiated ASKG could promote bone differentiation well. We anticipate that the radiation-resistant and anti-washout ASKG-CPCs have potential application prospect in orthopaedic surgery.

研究领域: 生物医学工程 · 材料科学 · 骨科手术
✓ 已验证 DOI PubMed 高影响因子
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Science China-Chemistry · 2021 ·Vol. 64 ·期 5 ·770-777 · IF 9.445

All at once arrangement of both oxygen atoms of dioxygen into aliphatic C(sp3)-C(sp3) bonds for hydroxyketone difunctionalization

Qiao Xiaofeng,Lin Yuhan,Li Jiazhen,Ma Wanhong,Zhao Jincai

Both β- and γ- hydroxyketone structures are important units in biologically active molecules, synthetic drugs and fine chemicals. Although there are some routes available for their manufacture from pre-functionalized groups on one or two matrix molecule(s), the approaches to simply and simultaneously deposit two oxygen atoms from dioxygen into two specific C(sp 3 ) positions of pure saturated hydrocarbons have rarely succeeded because they are involved in the targeted activation of three inert C-H σ bonds all at once. Here, we show that a TiO 2 -CH 3 CN photocatalytic suspension system enables the insertion of dioxygen into one C(sp 3 )-C(sp 3 ) bond of strained cycloparaffin derivatives, by which difunctionalized hydroxyketone products are obtained in a one-pot reaction. With the cleavage event to release strain as the directional driving force, as-designed photocatalytic reaction systems show 21 examples of β-hydroxyketone products with 31%–76% isolated yields for three-membered ring derivatives and 5 examples of γ-hydroxyketone products with 30%–63% isolated yields for four-membered ring substrates. 18 O isotopic labeling experiments using 18 O 2 , Ti 18 O 2 and intentionally added H 2 18 O, respectively, indicated that both oxygen atoms of hydroxyketone products were exclusively from dioxygen, suggesting a previously unknown H + /TiO 2 -e − catalyzed arrangement pathway of the hydroperoxide intermediate to convert dioxygen into hydroxyketone units.

研究领域: 有机化学 · 光催化化学 · 药物化学
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JOURNAL OF CHEMICAL SCIENCES · 2020 ·Vol. 132 ·期 1 ·1-9 · IF 1.406

Influence of sugars in preparing improved FeAl catalyst for carbon dioxide hydrogenation

Ning Wensheng,Li Bei,Dai Hui,Hu Shiye,Yang Xiazhen,Wang Biao,Zhang Bo

Abstract The influences of sugars (sucrose, fructose and glucose) on the performance of FeAl catalysts were investigated for CO 2 hydrogenation. FeAl catalysts were prepared with two steps. At first, the catalyst precursors were obtained by co-precipitation. During this step, three methods were used to add sucrose into the precursors. Then, promoter K and Cu were impregnated into the precursors. The improved CO 2 conversion and C 5+ hydrocarbon selectivity by sucrose addition were attributed to the formation of γ-Fe 2 O 3 phase in the catalyst precursor, which was different from the popular opinion that sucrose acted as a chelating agent. With the inspiration from sucrose hydrolysis effect, FeAl oxide, mainly in γ-Fe 2 O 3 phase was prepared by adding fructose and glucose (the products of sucrose hydrolysis) into the newly centrifuged precipitate. The formation of γ-Fe 2 O 3 phase was explained based on the results of XRD and XPS. The best catalyst possessed CO 2 conversion of 30.3% and C 5  + selectivity of 52.2% under the reaction conditions of H 2 :CO 2  = 3:1, 6.0 L/(h·g-cat), 1.6 MPa and 235 °C. Graphic abstract Effects of fructose and glucose on FeAl catalyst

研究领域: 化学工程 · 催化科学
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APPLIED CATALYSIS A-GENERAL · 2021 · IF 5.706

One-pot conversion of furfural to gamma-valerolactone in the presence of multifunctional zirconium alizarin red S hybrid

Qingrui Peng,Haijun Wang,Yongmei Xia,Xiang Liu

A multifunctional Zr-containing catalyst (FM-Zr-ARS) was successfully synthesized by a modulated hydrothermal synthesis route. Systematic characterization results supported the presence of robust porous inorganic-organic frameworks stabilized by the strong coordination interaction of Zr 4+ with oxygen-rich functional groups in Alizarin red S (ARS). Moreover, the -O-Zr-O- network in the FM-Zr-ARS structure formed a rich content of acid-base sites. In addition, the inherent sulfonic groups in ARS made the FM-Zr-ARS hybrids possess Brønsted acid sites. Therefore, under the synergistic catalysis of the multiple functional sites, FM-Zr-ARS showed remarkably high catalytic activity for γ-valerolactone (GVL) production from levulinate esters and furfural. Finally, 72.4 % and 97.7 % yields of GVL were obtained in the conversion of furfural and ethyl levulinate, respectively, after 8 h of reaction at 433 K. On the basis of the role of different functional sites, a plausible catalytic mechanism was presented for the conversion of biomass-derived furfural to GVL.

研究领域: 化学工程 · 生物质转化
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Food Bioscience · 2023 · IF 5.2

Poly-γ-glutamic acid-producing Bacillus velezensis fermentation can improve the feed properties of soybean meal

Han Hu,Caiyun Wu,Fanglan Ge,Yao Ren,Wei Li,Jiao Li

Soybean meal (SBM), a high-protein animal feed, contains several anti-nutritional factors, which limit its utilization. Poly-γ-glutamic acid (γ-PGA), a biological macromolecule , can significantly improve the health and growth benefits of animal feed. However, there are rare reports about SBM fermentation with γ-PGA-producing bacteria to improve its nutritional quality . In this study, we isolated a glutamic acid-independent poly γ-glutamic acid (γ-PGA) producing Bacillus velezensis SCP024–S-4 bacterial strain and used it for solid fermentation of SBM. The results showed that the maximum γ-PGA yield in fermented soybean meal (FSBM) reached up to 89.64 g/kg without adding glutamic acid . Meanwhile, the content of proteins, free amino acids and small peptides increased by 12.83%, 347.96 μg/g and 108.11 mg/g, respectively. Soy globulin, β-conglutinin and trypsin inhibitor all decreased below 3 mg/g. Mice were fed with CK (control diet), SBM and FSBM respectively. The average daily food intake in the FSBM, SBM, and CK groups were 7.68, 5.25, and 6.36 g, respectively. Compared with the CK group, the mice weight growth rate was significantly higher in the FSBM group. Mice blood and spleen tests showed no negative effect of FSBM. The high-throughput sequencing of mice intestinal microflora indicated that FSBM increased the richness of intestinal microbiota ; especially, the types and quantities of Lactobacillus were significantly increased. This study provides a feasible strategy to improve the nutritional quality of SBM as an animal feed.

研究领域: 微生物学 · 动物营养 · 发酵技术 · 食品科学
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