ChemistrySelect
·
2023
·Vol. 8
·期 16
·e202300233
·
IF 2.1
Yang Ling,Yan Peng,Shiyou Guan
Graphical Herein, a series of SiO x /C composites with uniform carbon distribution were prepared by sol-gel method and subsequent pyrolysis process, the carbon content can be easily adjusted just by selecting different organosilanes. Particularly, when BTEB was used as the raw materials, due to the uniformly dispersed of carbon at nanoscale and the appropriate carbon content, the SiO x /C−B exhibited excellent electrochemical performance in LIBs. SiO x /C composites with uniform distribution of silicon oxide (SiO x ) and carbon are promising anodes for lithium-ion batteries. However, designing the SiO x /C composites with uniformly dispersed of carbon at nanoscale and controllable carbon content is still a challenge. Herein, a series of SiO x /C composites with uniform carbon distribution were prepared by sol-gel method and subsequent pyrolysis process, the carbon content can be easily adjusted just by selecting different organosilanes. Due to the uniformly dispersed of carbon at nanoscale, the obtained products showed the excellent energy storage performance. Particularly, when Bis(triethoxysilyl)benzene (BTEB) was used as the raw materials, due to the appropriate carbon content, the SiO x /C−B exhibited a high reversible capacity of 535 mAh g −1 at 0.1 A g −1 over 100 cycles. The cycle stability is preserved even after 300 cycles at a high current density of 1.0 A g −1 , where the electrodes still supply a specific capacity of 389.7 mAh g −1 .
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JOURNAL OF CATALYSIS
·
2023
·
IF 7.3
Jin Yuan,Zhiwei He,Hongbo Zhang
Selective C–H bond oxidation of cyclohexane into KA oil (ketone-alcohol) is of vital importance in both fundamental research and industrial applications while limited by complex reaction network and suffering from low efficiency. In this study, Ce(OH)SO 4 · x H 2 O was chosen as a probe to systematically investigate the C–H bond activation and C–C bond rupture as a function of various reaction parameters, including the reactant/product concentrations, catalyst applied, reaction temperatures, acidic concentrations etc, and found that bi-molecule of C 6 H 12 was probably involved in both C–H bond rupture and C–C bond cleavage and both were controlled by one deprotonation elementary step with ·O 2 – and h + as the key active components, which were supported by parity fittings and primary KIEs determined. In addition, the C–C bond rupture was found to be mainly following C 6 H 10 O to ε-caprolactone and further to linear acids reaction path. Hopefully, this study could help people find/optimize reaction systems in selective hydrocarbon upgradings.
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ANALYTICA CHIMICA ACTA
·
2023
·
IF 6.2
Mengjie Su,Xiaoqing Cao,Hui Gao,Cailing Zhu,Wenjing Peng,Qiyu Jiang,Chunmei Yu
Highly sensitive and specific detection and monitoring of trace norepinephrine (NE) in biological fluids and neuronal cell lines is essential for the investigation of pathogenesis of certain neurological diseases. Herein, we constructed a novel electrochemical sensor for real-time monitoring of NE released by PC12 cells based on glassy carbon electrode (GCE) modified with honeycomb-like nickel oxide (NiO)-reduced graphene oxide (RGO) nanocomposite. The synthesized NiO, RGO and the NiO-RGO nanocomposite were characterized using X-ray diffraction spectrogram (XRD), Raman spectroscopy and scanning electron microscopy (SEM). The porous three-dimensional honeycomb-like structure of NiO and high charge transfer kinetics of RGO endowed the nanocomposite with excellent electrocatalytic activity , large surface area and good conductivity. The developed sensor exhibited superior sensitivity and specificity towards NE in a wide linear range from 20 nM to 14 μM and 14 μM–80 μM, with a low detection limit of 5 nM. The performances of the sensor in terms of excellent biocompatibility and high sensitivity allow it to be successfully employed in the tracking of NE release from PC12 cells under the stimulation of K + , providing an effective strategy for the real-time monitoring of cellular NE.
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FUEL
·
2023
·
IF 7.4
Wenli Zhao,Linlin Liu,Xiaopo Niu,Xinyue Yang,Jiuyi Sun,Qingfa Wang
Designing a bifunctional catalyst to achieve efficient hydroisomerization of long-chain alkanes is very essential for producing high-performance fuel and lubricant base oils. Herein, a bifunctional catalyst composed of an intimate mixture of ZSM-48 zeolite and alumina binder and with platinum (Pt) metal controllably deposited on zeolite or alumina was fabricated by a strong electrostatic adsorption method. The dependence of reaction pathways of hydroisomerization and hydrocracking of n -hexadecane on the metal-acid sites intimacy was investigated. High Brønsted acid density and suitable metal-acid sites intimacy favored to promote the catalytic activity. The selectivity, hydroisomerization mechanism and hydrocracking mechanism were significantly altered by tailoring the metal-acid sites intimacy. Too large or too small metal-acid sites intimacy was conducive to inhibit the occurrence of pore-mouth mode. A linear decease of the hydroisomerization selectivity with the increase of acid steps ( n as ) was observed. The catalyst with nanoscale intimacy of metal-acid sites (Pt/A-48) showed the highest catalytic activity and isomer selectivity (87%) and the least acid steps ( n as = 1.4). This work provides a promising approach to fabricating highly efficient and shape-selective bifunctional catalysts for selective hydroisomerization of long-chain alkanes. A reaction network was proposed over the catalysts with different metal-acid intimacy.
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MOLECULES
·
2023
·Vol. 28
·期 10
·4214
·
IF 4.6
Tianyun Du,Xiaojie Xue,Xiuxun Han
Rare earth silicate phosphors of high quantum efficiency with a stable performance are promising materials in the fields of display and illumination. The grain sizes of products synthesized via the conventional solid-state reaction method are usually too large to satisfy the requirements of color cast and extraction efficiency in high-resolution light-emitting devices (LEDs). We designed a synthetic route and successfully fabricated rare earth silicate NaGd9Si6O26(NGSO) sub-microcrystals with a size ranging from 550 to 1200 nm. The reaction mechanism and optical properties were systematically investigated. The quantum efficiency of Eu3+-activated NGSO sub-microcrystals was about 36.6%. The LED encapsulated with these sub-microcrystals showed lower color deviation and higher lumen efficiency and lumen flux compared to that with NGSO fabricated using the conventional solid state reaction method.
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ACS Omega
·
2023
·
IF 4.1
Jie Liang,Weiwei Zhang,Jun Wang,Wanzhen Li,Fei Ge,Weihao Jin,Yugui Tao
Recently, the combination of chemotherapy and chemodynamic therapy (CDT) has become a desirable strategy in the treatment of cancer. However, a satisfactory therapeutic outcome is often difficult to achieve due to the deficiency of endogenous H2O2 and O2 in the tumor microenvironment. In this study, a CaO2@DOX@Cu/ZIF-8 nanocomposite was prepared as a novel nanocatalytic platform to enable the combination of chemotherapy and CDT in cancer cells. The anticancer drug doxorubicin hydrochloride (DOX) was loaded onto calcium peroxide (CaO2) nanoparticles (NPs) to form CaO2@DOX, which was then encapsulated in a copper zeolitic imidazole ester MOF (Cu/ZIF-8) to form CaO2@DOX@Cu/ZIF-8 NPs. In the mildly acidic tumor microenvironment, CaO2@DOX@Cu/ZIF-8 NPs rapidly disintegrated, releasing CaO2, which reacted with water to generate H2O2 and O2 in the tumor microenvironment. The ability of CaO2@DOX@Cu/ZIF-8 NPs to combine chemotherapy and CDT was assessed by conducting cytotoxicity, living dead staining, cellular uptakes, H&E staining, and TUNEL assays in vitro and in vivo. The combination of chemotherapy and CDT of CaO2@DOX@Cu/ZIF-8 NPs had a more favorable tumor suppression effect than the nanomaterial precursors, which were not capable of the combined chemotherapy/CDT.
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Biomaterials Science
·
2023
·
IF 6.6
Yukun Wang,Wenjing Li,Bi Lin,Ying Yuan,Pengbo Ning,Xiaofeng Tao,Ruichan Lv
Photothermal therapy has a remarkable effect on the destruction of tumors. It kills tumor cells by photothermal ablation and induces immunogenic cell death by activating the immune response in tumor tissues. However, inhibition of the tumor immune microenvironment suppresses PTT-induced body-specific anti-tumor immunity. In this study, we designed the GdOF@PDA-HA-R837-hydrogel complex to achieve NIR-II imaging-guided photothermal ablation and enhanced immune response. Due to the doping of Yb and Er elements and the presence of a polydopamine coating, the synthesized nanoparticles enable NIR-II and photoacoustic imaging of tumor tissues, which will help in the integration of multimodal tumor imaging for diagnosis and treatment. Polydopamine is used as a photothermal agent and drug carrier because of its excellent photothermal ability and high drug loading capacity under 808 nm near infrared light. Hyaluronic acid can bind to specific receptors on the surface of cancer cells, allowing nanoparticles to aggregate around the tumor, thus enhancing the targeting ability of nanoparticles. In addition, imiquimod (R837) has been used as an immune response modulator to enhance the immunotherapeutic effect. The presence of a hydrogel enhanced the retention effect of nanoparticles in the tumor. We demonstrate that the combination of photothermal therapy with immune adjuvants effectively induces ICD, which in turn stimulates the activation of specific anti-tumor immunity and enhances the effect of photothermal therapy in vivo.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2023
·
IF 8.2
Boyu Du,Hongwei Zhu,Jingyu Xu,Yating Bai,Qingyu Wang,Xing Wang,Jinghui Zhou
Recently, multifunctional lignin-based materials are gaining more and more attention due to their great potential for low-cost and sustainability. In this work, to obtain both an excellent supercapacitor electrode and an outstanding electromagnetic wave (EMW) absorber, a series of multifunctional nitrogen-sulphur (N-S) co-doped lignin-based carbon magnetic nanoparticles (LCMNPs) had been successfully prepared through Mannich reaction at different carbonization temperature. As compared with the directly carbonized lignin carbon (LC), LCMNPs had more nano-size structure and higher specific surface area. Meanwhile, with the increase of carbonization temperature, the graphitization of the LCMNPs could also be effectively improved. Therefore, LCMNPs-800 displayed the best performance advantages. For the electric double layer capacitor (EDLC), the optimal specific capacitance of LCMNPs-800 reached 154.2 F/g, and the capacitance retention after 5000 cycles was as high as 98.14 %. When the power density was 2204.76 W/kg, the energy density achieved 33.81 Wh/kg. In addition, N-S co-doped LCMNPs also exhibited strong electromagnetic wave absorption (EMWA) ability, whose the minimum reflection loss (RL) value of LCMNPs-800 was realized −46.61 dB at 6.01 GHz with an thickness of 4.0 mm, and the effective absorption bandwidth (EAB) was up to 2.11 GHz ranging from 5.10 to 7.21 GHz, which could cover the C-band. Overall, this green and sustainable approach is a promising strategy for the preparation of high-performance multifunctional lignin-based materials.
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Materials Today Physics
·
2023
·
IF 11.5
Qiqin Liang,Yanling Hao,Xiaosi Qi,Junfei Ding,Yunpeng Qu,Xiu Gong,Yanli Chen,Jing-Liang Yang,Qiong Peng,Wei Zhong
It is well recognized that making best of interfacial engineering and magnetic-dielectric synergistic effect is an effective strategy to improve microwave absorption. Herein, a series of cube-like yolk-shell structured magnetic carbon-based multicomponent nanocomposites (MCNCs) including CoNi@void@C, FeNi@void@C and FeCo@void@C could be selectively and successfully produced in large scale through a simple continuous process of co-precipitation, polymerization and thermal treatment, respectively. The obtained results indicated that the as-prepared cube-like yolk-shell structured magnetic MCNCs were composed of black magnetic nanoparticles acting as core, void spaces as intermediate layer and thin obscure carbon layer serving as shell. Owing to the excellent impedance matching and electromagnetic wave loss characteristics, the obtained CoNi@void@C, FeNi@void@C and FeCo@void@C MCNCs displayed the outstanding comprehensive electromagnetic wave absorption performances including strong absorption capabilities, broad absorption bandwidths and thin matching thicknesses. Especially, the obtained FeCo@void@C presented a minimum reflection loss of −54.32 dB with a matching thickness of 1.90 mm, and the effective bandwidth can reach 5.60 GHz with a matching thickness of 1.96 mm. Therefore, our findings not only provided a universal and alternative approach to produce yolk-shell structured magnetic carbon-based MCNCs, but also presented an effective pathway to take full advantage of interfacial and magnetic-dielectric synergistic effects to develop the tunable, broadband, strong absorption, lightweight high-efficiency microwave absorbers.
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PROCESS BIOCHEMISTRY
·
2023
·
IF 4.4
Haidong Teng,Kaitong Chen,Lan Wang,Jianping Wu,Gang Xu
l -syn-3-[4-(methylsulfonyl)] phenylserine is a key industrial intermediate for the synthesis of florfenicol, thiamphenicol , and other products. l -Threonine aldolase can synthesize l -syn-3-[4-(methylsulfonyl)] phenylserine from glycine and 4-methylsulphonyl benzaldehyde directly. However, the selectivity of free l -threonine aldolase was difficult to meet the requirement of industrialization. Here, we selected the suitable site to insert His tag as immobilized site to improve the selectivity of l -threonine aldolase based on the molecular dynamics simulation and prior protein engineering. The phenanthroline was coupled to the surface of magnetic nanoparticles coated with silicon and thus enabled the selective and oriented immobilization of His-tagged l -threonine aldolase. Due to magnetic nanoparticles coated with silicon as supports, it was easy to separate the residual reactant and impurities from the immobilized enzyme by magnetic attraction. Moreover, the immobilization was combined with the purification of free enzymes through directional immobilization, which avoided heterozyme linking supports and improved the utilization efficiency of supports. Our study demonstrates an effective approach: how to analyze and select enzyme-targeted ligation sites in conjunction with previous modifications of engineered bacteria, and the immobilized enzyme obtained also provided a good candidate for the industrial production of l -syn-3-[4-(methylsulfonyl)] phenylserine.
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RSC Advances
·
2023
·Vol. 13
·期 21
·14554-14564
·
IF 3.9
Zhong Xie,Jinpei Hei,Chuan Li,Xiaojie Yin,Fengyi Wu,Lei Cheng,Sugang Meng
An activated carbon-supported Cu/ZnO catalyst (CCZ-AE-ox) was successfully obtained by the ammonia evaporation method for the hydrogenation of carbon dioxide to methanol, and the surface properties of the catalyst post-calcination and reduction were investigated. Activated carbon facilitated the increased dispersion of the loaded metals, which promote the CO2 space-time yield (STY) of methanol and turnover frequency (TOF) on the active sites. Furthermore, the factors affecting the catalyst in the hydrogenation of CO2 to methanol were in-depth investigated. The larger surface area and higher CO2 adsorption capacity are found to make possible the main attributions of the superior activity of the CCZ-AE-ox catalyst.
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SURFACE & COATINGS TECHNOLOGY
·
2023
·
IF 5.4
Yi Huang,Chenyang Zhao,Yue Li,Chen Wang,Tao Shen,Di Cheng,Hui Yang
Zeolitic imidazolate framework-8 (ZIF-8)-based pH-responsive nanocontainers present a new pathway to endowing sol-gel anticorrosion coatings with self-healing ability. The organic nature of the ZIF-8-based nanocontainers, however, makes them less compatible with the inorganic sol-gel coating matrix, thus ineffective in protection against corrosion. In this paper, a novel pH-responsive corrosion inhibitor release system (BTA-ZIF-8@SiO 2 ) based on ZIF-8 for self-healing sol-gel anticorrosion coating was reported. A facile one-step self-assembly procedure was used to create the 1H-benzotriazole (BTA)-encapsulated ZIF-8 core, on which a layer of silica was subsequently coated using a standard sol-gel method. The silica shell can provide better compatibility of the nanocontainers with the sol-gel matrix, thus improving the overall corrosion protection . Characterizations of the BTA-ZIF-8@SiO 2 nanocontainers via X-ray diffraction spectroscopy, Fourier transform infrared spectroscopy , thermogravimetric analysis , Brunauer−Emmett−Teller, scanning electron microscopy/energy-dispersive X-ray spectroscopy, and X-ray photoelectron spectroscopy confirmed the successful synthesis of ZIF-8-based nanocontainers with high loading content of BTA and mesoporous SiO 2 shell. Inhibitor release studies revealed the pH-responsive smart release of inbuilt BTA at both acidic and alkaline media. The anticorrosion performance of sol-gel coating incorporating the nanocontainers was investigated by electrochemical impedance spectroscopy , scanning Kelvin probe , and salt spray test , and the results indicated that BTA-ZIF-8@SiO 2 could effectively enhance the corrosion protection properties of the coating and exhibit excellent self-healing performance, in which the |Z| 0.01Hz was >2 orders of magnitude higher and coating resistance and oxide layer resistance were >3 orders of magnitude higher than these of pure sol-gel coating after 28 d of immersion. This could be attributed to the synergistic effect of enhanced passive protection, improved nanocontainer compatibility with the sol-gel matrix, and corrosion inhibitor film formed on metal surface .
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