Nature Communications
·
2023
·Vol. 14
·期 1
·1-11
·
IF 16.6
Xiao Mengjun,Wu Qianbao,Ku Ruiqi,Zhou Liujiang,Long Chang,Liang Junwu,Mavrič Andraž,Li Lei,Zhu Jing,Valant Matjaz,Li Jiong,Zeng Zhenhua,Cui Chunhua
Electrochemical chlorine evolution reaction is of central importance in the chlor-alkali industry, but the chlorine evolution anode is largely limited by water oxidation side reaction and corrosion-induced performance decay in strong acids. Here we present an amorphous CoO x Cl y catalyst that has been deposited in situ in an acidic saline electrolyte containing Co 2+ and Cl - ions to adapt to the given electrochemical condition and exhibits ~100% chlorine evolution selectivity with an overpotential of ~0.1 V at 10 mA cm −2 and high stability over 500 h. In situ spectroscopic studies and theoretical calculations reveal that the electrochemical introduction of Cl - prevents the Co sites from charging to a higher oxidation state thus suppressing the O-O bond formation for oxygen evolution. Consequently, the chlorine evolution selectivity has been enhanced on the Cl-constrained Co-O * sites via the Volmer-Heyrovsky pathway. This study provides fundamental insights into how the reactant Cl - itself can work as a promoter toward enhancing chlorine evolution in acidic brine.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2023
·Vol. 34
·期 26
·1-19
·
IF 2.8
Lu Zan,Yuan Li,Liang Guozheng,Gu Aijuan
An effective strategy is developed to improve the energy density for poly(vinylidene fluoride-hexafluoropropylene) (P(VDF-HFP)) composites through building novel multi-layered structure with gradient distribution of a low content of SiO 2 -coated potassium sodium niobate (KNN@SiO 2 ), and the resultant composites were coded as G-K@S/P. To discuss the mechanism behind the unique strategy, the P(VDF-HFP) composites with randomly distributed potassium sodium niobate (KNN) or gradient-distributed KNN, designed as K/P or G-K/P, were prepared; moreover, the structures and integrated properties of the three kinds of composites were systematically studied using experimental method and finite element simulations to declare the influence of both layered structure with gradient distribution and core–shell structure of fillers. Results show that compared to K/P and G-K/P composites, with the same total loading of fillers, G-K@S/P has a greater breakdown strength and energy density. When the filler content is as low as 1 wt%, the energy density of G-K@S/P is about 1.35 and 2.37 times of that of G-K/P and K/P, respectively, the improvement degrees are obviously higher than those of multi-layered polymer composites (SCI database), proving the effectiveness of the strategy. The mechanism behind is that combining the multi-layered structure with gradient distribution of a small content of KNN@SiO 2 plays a synergistic role to simultaneously improve the dielectric properties and breakdown strength and thus enhancing the energy storage performance of the composites.
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JOURNAL OF MATERIALS SCIENCE
·
2023
·Vol. 58
·期 36
·14299-14314
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IF 4.5
Xu Chenzhe,Qiu Yue,Wang Zheng,Gao Zifei,Liu Cai,Sun Yanran,Zhang Haitao,Ma Juanjuan,Liu Lin,Liu Chao,Tong Zhiwei
A facile one-step hydrothermal approach was proposed to fabricate Pd nanoparticles decorated Mg–Al layered double hydroxide nanosheets (denoted as Pd NPs/Mg–Al LDH composite), wherein polyvinylpyrrolidone (PVP) functioned as both a reductant and stabilizer. The resulting samples were characterized by XRD, SEM, TEM, XPS and BET techniques. The effect of synthetic parameters during the hydrothermal reaction including PVP dosage and temperature on the size and distribution of Pd NPs was investigated in details. Pd nanoparticles with an average particle size of 3.6 nm were uniformly supported onto Mg–Al LDH nanosheets under the optimal conditions. The obtained Pd NPs/Mg–Al LDH composite could serve as an efficient heterogeneous catalyst for the Heck reaction between iodobenzene and methyl acrylate, achieving a high yield of 95.8% within 60 min at 100 °C. Furthermore, Pd NPs/Mg–Al LDH was highly stable and reused 6 times without significant loss of its catalytic activity.
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IONICS
·
2023
·Vol. 29
·期 12
·5073-5084
·
IF 2.8
Zhang Xiangyang,Xin Yu,Shen Qianyun,Wang Feifei,Xiao Wei
A facile and feasible strategy is carried out combined with the subsequent heat treatments to encapsulate SnO 2 /Cu 3 Sn nanoparticles into N-doped carbon nanofibers (CNFs) by electrospinning to fabricate the SnO 2 /Cu 3 Sn@CNFs nanofibers as anode materials for lithium-ion batteries. The one-dimensional composite nanofibers are well interconnected with each other and randomly intertwined to construct the distinctive three-dimensional networks, which not only shorten Li + transfer pathways and accelerate Li + diffusions in the axial direction, but also improve the electronic conductivity of whole composite electrodes. Furthermore, the fully active SnO 2 phases dominate the lithium storage behaviors of composite electrodes to guarantee the excellent lithium storage capacity, and the relatively active Cu 3 Sn phases play the role of buffer matrixes to accommodate the huge volume expansion of SnO 2 phases. When the dosages of SnCl 2 salts are controlled at 5 mmol, the SnO 2 /Cu 3 Sn@CNFs-5 electrode delivers the excellent comprehensive electrochemical properties, whose initial discharge specific capacity is 1279.1 mAh/g at 100 mA/g and maintains to 560.7 mAh/g after 200 cycles. Moreover, the SnO 2 /Cu 3 Sn@CNFs-5 electrode is endowed with the high-specific capacity of 359.2 mAh/g at 500 mA/g after 1000 cycles and the satisfactory pseudocapacitive contribution of 49.60% at 1.0 mV/s. The new insights into the electrospinning strategy of encapsulating SnO 2 and Cu 3 Sn nanoparticles into CNFs matrixes can contribute to offer a guide for the application of next-generation SnO 2 -based anodes for energy storage devices.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-15
·
IF 16.6
Huang Ting,Lin Ruyi,Su Yuanqin,Sun Hao,Zheng Xixi,Zhang Jinsong,Lu Xiaoyan,Zhao Baiqin,Jiang Xinchi,Huang Lingling,Li Ni,Shi Jing,Fan Xiaohui,Xu Donghang,Zhang Tianyuan,Gao Jianqing
The use of exogenous mitochondria to replenish damaged mitochondria has been proposed as a strategy for the treatment of pulmonary fibrosis. However, the success of this strategy is partially restricted by the difficulty of supplying sufficient mitochondria to diseased cells. Herein, we report the generation of high-powered mesenchymal stem cells with promoted mitochondrial biogenesis and facilitated mitochondrial transfer to injured lung cells by the sequential treatment of pioglitazone and iron oxide nanoparticles. This highly efficient mitochondrial transfer is shown to not only restore mitochondrial homeostasis but also reactivate inhibited mitophagy, consequently recovering impaired cellular functions. We perform studies in mouse to show that these high-powered mesenchymal stem cells successfully mitigate fibrotic progression in a progressive fibrosis model, which was further verified in a humanized multicellular lung spheroid model. The present findings provide a potential strategy to overcome the current limitations in mitochondrial replenishment therapy, thereby promoting therapeutic applications for fibrotic intervention.
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Nano Research
·
2023
·
IF 9.9
Chen Yan,Yang Zhenrui,Wang Juan,Yang Yun,He Xuedong,Wang Yang,Chen Jiadong,Guo Yaqing,Wang Xin,Wang Shun,Jin Huile
Enhancing catalytic activity through modulating the interaction between N-doped carbon and metal phosphides clusters is an effective approach. Herein, the electronic structure modulation of CoP 2 supported N-modified carbon (CoP 2 /NC) has been designed and prepared as efficient electrocatalysts for oxygen reduction reaction (ORR), oxygen evolution reaction (OER), and hydrogen evolution reaction (HER). Notably, CoP 2 /NC-1 catalyst exhibits impressive performance in alkaline media, with an ORR half-wave potential of 0.84 V, as well as OER and HER overpotentials of 290 and 129 mV (at 10 mA·cm −2 ), respectively. In addition, CoP 2 /NC-1 produces a power density as high as 172.9 mW·cm −2 , and excellent reversibility of 100 h at 20 mA·cm −2 in home-made Zn-air batteries. The experimental results demonstrate that the synergistic interactions between N modified carbon substrate and CoP 2 material significantly enhance the kinetics of ORR, OER, and HER. Density functional theory (DFT) calculations reveal the strong electrons redistribution of CoP 2 induced by high-density N atoms at the interface, thus optimizing the key intermediates and significantly lower the energy barrier of reactions. These electronic adjustments of CoP 2 greatly enhance its kinetics of ORR/OER/HER, leading to faster reactions. This study provides profound insights into the specific modification of CoP 2 by N-doped carbon, enabling the construction of efficient catalysts.
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MICROCHIMICA ACTA
·
2023
·Vol. 191
·期 1
·1-9
·
IF 5.7
Huang Xuemin,Chen Haiyan,Huang Rui,Shi Yuande,Ye Ruihong,Qiu Bin
Benefit from the strong coordination property, lanthanide metal ions have been used as competitive reagents to modulate the fluorescence changes of the system. However, lanthanide metal ions as inducers for aggregation-induced emission enhancement in nanosystems is rare. Herein, we report a “turn on–off-on” fluorescent switch for cascade detection of acid phosphatase (ACP) and adenosine triphosphate (ATP) based on the competitive coordination of samarium ions (Sm 3+ ). Novel copper nanoclusters (CuNCs) with long wavelength emission (614 nm) stabilized by glutathione (GSH) and glycylglycine (Gly-Gly) have been confirmed to have AIE property. With the continuous aggregation of GSH/Gly-Gly CuNCs under the induction of Sm 3+ , the fluorescence of the system increased to achieve the “turn-on” process. The coordinated behaviour between Sm 3+ and GSH/Gly-Gly CuNCs is discussed. Due to the strong metal coordination ability of ATP, the Sm 3+ coordinated with the GSH/Gly-Gly CuNCs is competed out, resulting in the fluorescence “turn-off” process of the system. As the substrate of enzymatic hydrolysis of ACP, with the continuous hydrolysis of ATP by ACP, Sm 3+ coordinates with GSH/Gly-Gly CuNCs again, which leads to the AIE effect and realize the fluorescence "turn-on" process of the system. This strategy results in ATP linear range of 0.508 ~ 120.0 μM with a detection limit of 0.508 μM (S/N = 3) and ACP linear range of 0.011 ~ 30.0 U·L −1 with a detection limit of 0.011 U·L −1 (S/N = 3). Application to biologic samples was successful. Graphical Abstract
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Nature Communications
·
2021
·Vol. 12
·期 1
·1-8
·
IF 14.919
Ling Huan,Wu Jianchang,Su Fengyu,Tian Yanqing,Liu Yan Jun
Electrochromic devices can modulate their light absorption under a small driving voltage, but the requirement for external electrical supplies causes response-lag. To address this problem, self-powered electrochromic devices have been studied recently. However, insensitivity to the surrounding light and unsatisfactory stability of electrochromic devices have hindered their critical applications. Herein, novel perovskite solar cell-powered all-in-one gel electrochromic devices have been assembled and studied in order to achieve automatic light adjustment. Two alkynyl-containing viologen derivatives are synthesized as electrochromic materials, the devices with very high stability (up to 70000 cycles) serves as the energy storage and smart window, while the perovskite solar cell with power-conversion-efficiency up to 18.3% serves as the light detector and power harvester. The combined devices can automatically switch between bleached and colored state to adjust light absorption with variable surrounding light intensity in real-time swiftly, which establish significant potentials for applications as modern all-day intelligent windows.
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Nano Research
·
2021
·Vol. 14
·期 11
·4046-4055
·
IF 8.897
Xu Yue,Zhao Chenxi,Zhang Xi,Xu Jingwen,Yang Lingling,Zhang Zhechen,Gao Zhida,Song Yan-Yan
Infectious diseases caused by bacteria are a global threat to the human health. Here, we propose a solvent “irrigation” technique to endow TiO 2 nanotubes (NTs) to precisely modify with functional nanomaterials, and apply them in constructing a near-infrared (NIR) light controlled drug-delivery system for rapid necrosis of bacteria. In this design, the NIR stimuli-responsive functional shell is located on the external tube wall of TiO 2 NT; the internal tube wall offers sufficient binding sites for drug loading. Using kanamycin as a model drug, we demonstrate that the reactive oxygen species generated in photocatalysis not only controllably release the loaded drug by scissoring the linked chains, but also effectively compromise bacteria membrane integrity by damaging the cell wall. Benefiting from the damages, antibiotics rapidly enter the bacteria and reach ≥99.9% reduction in Escherichia coli colony within only 2 h. Importantly, such a covalently conjugation-based delivery system can efficiently relieve radical-induced inflammation and cytotoxicity. This study provides an innovative design strategy for engineering delivery systems with tailorable components, enduring stimuli-response by multiple triggers.
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WATER AIR AND SOIL POLLUTION
·
2021
·Vol. 232
·期 2
·1-15
·
IF 2.52
Zhang Hongling,Shi Mingxing,Xia Mingzhu,FengyunWang,Zhao Feng
Previous researches investigated the adsorption properties and mechanism of clay minerals on antibiotic pharmaceuticals and personal care products (PPCPs) via batch adsorption experiments and X-ray diffraction (XRD) and Fourier transform infrared spectroscopy (FTIR) characterization, but many PPCPs exhibit different ionization states under different pH conditions; the research on the microscopic mechanism of different ionized PPCPs species adsorbed by clay minerals is very scarce. In this work, as a typical PPCPs contaminant, the common tetracycline (TC) was chosen as the study target; the adsorption micro mechanism of montmorillonite (MMT) on different TC species in aqueous solution was explored in details. Especially outstanding, for the first time, with the help of Multiwfn wavefunction program, quantitative analysis of molecular surface analysis and basin analysis were applied to quantitatively investigate the electrostatic interaction between MMT and different TC species, the possible positions of lone pair electrons. Independent gradient model (IGM) analysis and Hirshfeld surface analysis including local surface analysis were integrated to visualize the binding sites, interaction types, and relative strength between MMT and TC +/− or TC +/2− species, which can insight into the interaction essence from the microscopic perspective at the atomic level.
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BULLETIN OF ENVIRONMENTAL CONTAMINATION AND TOXICOLOGY
·
2021
·Vol. 107
·期 2
·255-262
·
IF 2.151
Liu Jingliang,An Fengxia,Li Mei,Yang Lu,Wan Jinzhong,Zhang Shengtian
Sulfate radical based-advanced oxidation process has received increasing interest in the remediation of wastewater and contaminated soil. In this study, degradation of 2, 4-dichlorophenol (2, 4-DCP) was investigated over peroxymonosulfate (PMS) activation by MnO 2 , which was prepared by liquid-phase oxidation method. The prepared MnO 2 was characterized by transition electron microscopy, X-ray diffraction, N 2 adsorption–desorption, and X-ray photoelectron spectroscopy. Characterization results showed that α-MnO 2 exhibited the highest surface area and Mn (III) content. The PMS activation by MnO 2 in 2, 4-DCP degradation followed the order of α-MnO 2 > γ-MnO 2 > β-MnO 2 , which is dependent on the properties of MnO 2 including crystal structure, surface area and Mn (III) content. Influences of initial concentration of 2, 4-DCP, PMS and MnO 2 dosage, pH and co-existing inorganic ions on the degradation were examined. Electron paramagnetic resonance (EPR) and quenching experiments with ethanol and tert-butanol suggested that sulfate radicals were the dominant radicals in the process. Findings in this study indicated that α-MnO 2 was an attractive catalyst for activation of PMS to degrade 2, 4-DCP in aqueous solution.
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ACTA PHARMACOLOGICA SINICA
·
2021
·Vol. 43
·期 1
·133-145
·
IF 6.15
Shen Dai-fei,Cheng He,Cai Bo-zhi,Cai Wen-feng,Wang Bin,Zhu Qing,Wu Yue-bin,Liu Man,Chen Run-ji,Gao Fen-fei,Zhang Yan-mei,Niu Yong-dong,Shi Gang-gang
N -n-Butyl haloperidol iodide (F 2 ) is a novel compound that has antiproliferative and antifibrogenic activities. In this study we investigated the therapeutic potential of F 2 against liver fibrosis in mice and the underlying mechanisms. Two widely used mouse models of fibrosis was established in mice by injection of either carbon tetrachloride (CCl 4 ) or thioacetamide (TAA). The mice received F 2 (0.75, 1.5 or 3 mg·kg −1 ·d −1 , ip) for 4 weeks of fibrosis induction. We showed that F 2 administration dose-dependently ameliorated CCl 4 - or TAA-induced liver fibrosis, evidenced by significant decreases in collagen deposition and c-Jun, TGF-β receptor II (TGFBR2), α-smooth muscle actin (α-SMA), and collagen I expression in the liver. In transforming growth factor beta 1 (TGF-β1)-stimulated LX-2 cells (a human hepatic stellate cell line) and primary mouse hepatic stellate cells, treatment with F 2 (0.1, 1, 10 μM) concentration-dependently inhibited the expression of α-SMA, and collagen I. In LX-2 cells, F 2 inhibited TGF-β/Smad signaling through reducing the levels of TGFBR2; pretreatment with LY2109761 (TGF-β signaling inhibitor) or SP600125 (c-Jun signaling inhibitor) markedly inhibited TGF-β1-induced induction of α-SMA and collagen I. Knockdown of c-Jun decreased TGF-β signaling genes, including TGFBR2 levels. We revealed that c-Jun was bound to the TGFBR2 promoter, whereas F 2 suppressed the binding of c-Jun to the TGFBR2 promoter to restrain TGF-β signaling and inhibit α-SMA and collagen I upregulation. In conclusion, the therapeutic benefit of F 2 against liver fibrosis results from inhibition of c-Jun expression to reduce TGFBR2 and concomitant reduction of the responsiveness of hepatic stellate cells to TGF-β1. F 2 may thus be a potentially new effective pharmacotherapy for human liver fibrosis.
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