MOLECULAR PHARMACEUTICS
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2025
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IF 4.5
Xin Yue,Qian Lin,Xiaohang Liu,Zhaoyi Yu,Jiafeng Xu,Xuan Zhu,Jinyan Lin,Aijie Liu
The high intracellular glutathione (GSH) level, naturally hypoxic conditions within the tumor microenvironment, and limited reactive oxygen species (ROS) generation pose significant obstacles to the effectiveness of sonodynamic therapy (SDT). Overcoming these barriers through depletion of GSH and relieving hypoxia offer a promising strategy to enhance SDT effectiveness. Herein, we developed a dendritic tetra-sulfide-bridged mesoporous silica (DTSMO) that encapsulated both chlorin e6 (Ce6) and cerium via channel-limited in situ coordination and is subsequently cloaked with the macrophage cell membrane (MCM) to facilitate efficient reactive oxygen species (ROS)-based therapy via multispecies enzymatic activities. First, this nanosystem exhibited Ce(IV) ions to mimic catalase (CAT)-like activity, converting H2O2 into O2, thereby effectively alleviating tumor hypoxia. Meanwhile, the nanosystem possessed Ce (III)-based peroxidase (POD)-like activity, enabling the conversion of H2O2 into hydroxyl radicals (•OH) while simultaneously depleting GSH. Both in vitro and in vivo experiments demonstrated that GSH depletion exerted a powerful supplementary effect on CDT and SDT, achieving a tumor inhibition rate of up to 96%, without affecting normal tissues during treatment.
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PubMed
高影响因子
INORGANIC CHEMISTRY
·
2021
·
IF 5.165
Shizhu Song,Tian Qin,Qi Li,Yanqing Wang,Yanfeng Tang,Lifang Zhang,Xiaojuan Liu
Facile synthesis of cost-effective carbon-supported Co single atoms (Co-SAs) exhibits huge potential applications in energy storage and conversion devices. We here report the implantation of Co-SAs into hollow carbon spheres (Co-SAs-HCS) via a facile wet-chemistry strategy followed by controlled pyrolysis. Electron-rich histidine acted as a Lewis base effectively immobilizing Co2+ (Lewis acid) via the electrostatic effect and hydrogen bonds, thus achieving the scalable synthesis of Co-SAs-HCS. We constructed a series of histidine-Co2+ structure models to elucidate the formation of histidine-Co2+ complexes by analyzing their binding energy. X-ray absorption fine-structure results verify that central Co atoms with four N coordination atoms possess a non-planar Co-N4 structure. Electrochemical results indicate that the as-prepared Co-SAs-HCS catalyst shows a low potential difference (0.809 V) between the oxygen evolution reaction potential at 10 mA cm–2 and the oxygen reduction reaction half-wave potential, outperforming the commercial Pt/C catalysts (0.996 V). Moreover, an assembled Zn-air battery based on Co-SAs-HCS exhibits an unexpected long-term durability. We have demonstrated that non-planar Co-N4-1-O2 sites are the source for highly efficient adsorption and dissociation of O2 molecules and then reduction of the free energy of desorption of the intermediates by density functional theory. Our findings provide a new design insight into the exploration of advanced electrocatalysts, which will be applied in the design of green energy devices in the future.
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高影响因子
JOURNAL OF POWER SOURCES
·
2020
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IF 8.247
Hongying Tang,Kang Geng,Jinkai Hao,Xiaojuan Zhang,Zhigang Shao,Nanwen Li
Quaternized poly(sulfone)s based on trimethylamine (PSf-TMA-x) and triethylamine (PSf-TEA-x) are developed to form quaternary ammonium (QA)-biphosphate ion pairs as promising high temperature proton exchange membrane (HT-PEM) in H 2 /O 2 fuel cells. The strong QA-biphosphate ion-pair interaction results in high acid absorption and thus high proton conductivity of 78.1 mS cm −1 for PSf-TEA-110/PA membrane at 160 °C in spite of its lower degree of functionalization. Thus, the peak power density of more than 400 mW cm −2 is achieved at 160 °C for the quaternized PSf membranes in H 2 /O 2 fuel cell, which is higher than that of the poly(benzeimidazole) ( m -PBI) membrane (370 mW cm −2 ). Subsequently, the degradation mechanism of the PSf membranes is demonstrated using NMR technique to be occurred in both the polymer backbone and the QA groups. The stability investigation of model compounds further confirms that the degradation of the membranes resulted from the scission of ether linkage and isopropylidene group and the SN2 nucleophilic substitution of QA at operating conditions. Therefore, the significant performance decrease is observed and the lifetime is only less than 30 h at 200 mA cm −2 which is much lower than that of m -PBI membrane (>40 h).
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高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2025
·
IF 11.3
Hao Liu,Siqing Cheng,Jianjun Chen,Xiaoping Chen,Shangchao Xiong,Fang Huang,Houfeng Liu,Junhua Li,Chuanzhi Sun
Mitigating industrial nitrous oxide (N2O) emissions is critical for climate action, yet developing efficient low-temperature N2O decomposition catalysts under O2-containing conditions remains challenging. The weak oxygen–support interaction leads to unsatisfactory N2O decomposition performance in the supported Co3O4/CeO2 catalyst. This study aims to enhance the electronic oxide–support interaction in the Co3O4/CeO2 catalyst through Zn doping, thereby improving its catalytic performance for N2O decomposition under O2-rich conditions. The results demonstrate that, in the presence of 5% O2, the activation energy of the catalyst sharply decreases from 117.5 to 60.4 kJ·mol–1 after Zn doping (Co2.4Zn0.6O4/CeO2). Additionally, the doped catalyst exhibits strong durability to the O2 + H2O + NOx impurity gas components. Advanced spectral characterization and density functional theory calculations reveal that Zn doping modulates the geometry and electronic structure of active cobalt sites, optimizing the adsorption and activation capabilities of N2O molecules. This study elucidates the mechanism of N2O decomposition over the catalysts and establishes a clear structure–activity relationship between the atomic-scale configuration of active sites and their performance. These findings provide critical insights for designing efficient supported oxide catalysts through targeted doping strategies and offer new perspectives for developing highly efficient and low-energy N2O decomposition catalysts.
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高影响因子
Molecular Catalysis
·
2020
·
IF 3.687
Hai-Min Shen,Lei Liu,Bei Qi,Meng-Yun Hu,Hong-Liang Ye,Yuan-Bin She
Non-solvent and non-additive oxidation of secondary benzylic C–H bonds to aromatic ketones utilizing simple metalloporphyrins as catalysts and O 2 was investigated systematically. Based on systematical studies on reaction parameters, such as the structures of porphyrins, the types of central metals, the amount of catalyst, the pressure of oxygen, and the temperature, most aromatics with secondary benzylic C–H had been converted efficiently and selectively to their corresponding aromatic ketones catalyzed by the optimized metalloporphyrin catalyst T(2,3,6-triCl)PPCo. And the selectivity towards aromatic ketones reached up to 80 %–95 % with acceptable conversions in lower catalyst-loading (2.4 × 10 −3 %, mol/mol). The highest selectivity was achieved for substrate 1,2,3,4-tetrahydronaphthalene with the selectivity of 95.0 % in the conversion of 46.3 %. The superior catalytic performance of T(2,3,6-triCl)PPCo could be mainly ascribed to its excellent plane structure, superior ability for electron transfer and low positive charge around the central metal. All of above properties promoted the formation of catalytic active species high-valence cobalt-oxo complexes, and facilitated the approach of substrates to the catalytic active centers. This work presented an optimized balance among higher selectivity, milder conditions, lower catalyst-loading, and simpler catalysts compared with current documents, which was not only an efficient, practical and significant strategy to functionalize the widely available aromatics possessing secondary benzylic C H with high efficiency and selectivity under milder conditions, but also an important instance in the effective functionalization and utilization of other C H bonds employing optimized catalytic systems based on metalloporphyrins.
研究领域:
有机化学
·
催化化学
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Yingying Zhang,Qiang Huang,Ruoting Wang,Xinjie Du,Yu Yu,Zhe Chen
Modulating the coordination environment of single-atom catalysts (SACs) and designing architectures to maximize the exposure of active sites are pivotal strategies for enhancing peroxymonosulfate (PMS) activation. The fabrication of single-atom‑iron catalysts on support with particular coordination is essential but still remains challenge. Herein, we proposed the construction of single-atom‑iron embedded in graphitic carbon nitride nanosheets (SA-Fe@C 3 N 4 ) catalyst. The layer-confined synthesis strategy realized the loading of single-atom irons and ultrathin C 3 N 4 nanosheet formation in the interlayer of layered template RUB-15. XANES analysis corroborated that the isolated iron atoms are coordinated with three nitrogen and one oxygen atoms (Fe-N 3 O 1 ). Notably, the single iron atoms within the SA-Fe@C 3 N 4 matrix serve as the predominant active sites for PMS activation. The catalyst exhibited exceptional activity for the degradation of sulfamethoxazole (SMX), achieving a mass-normalized rate constant ( k Fe ) of 1.54 × 10 5 min −1 mol −1 with high selectivity toward 1 O 2 /•O 2 − .Theoretical calculations revealed that the Fe-N 3 O 1 moiety accelerated the PMS adsorption and reduced energy barriers for the activation of PMS, thus produce key *O intermediate SO 5 •- and form 1 O 2 /•O 2 − with nearly 100% selectivity. This study supplied a simple avenue to fabricate single-atom‑iron on C 3 N 4 with regulated coordination for wastewater treatment.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Xingyu Zhan,Yunxiong Zeng,Jingcai Xu,Yingchun Xia,Xinqing Wang,Fang Tao,Jie Ouyang,Hongliang Li,Liming Yang,Shenglian Luo,Bo Hong
The reactive oxygen species (ROS) contribute to photodegrading tetracycline (TC), which determines the overall efficiency of photocatalysts. Superoxide radical (·O 2 – ) is one of the excellent ROS for photodegrading TC by carbon nitride. However, achieving hierarchical carbon nitride with efficient, stabile, and selective production of ·O 2 – via O 2 photoreduction is a great challenge. Herein, a carbon nitride oxide nest (CNON 6 ) with carbon/nitrogen vacancies (C-v, N-v) and oxygen substitution (O-s) was prepared via tailoring surface microenvironment. The CNON 6 can photodegrade 82% of TC within 2 min under visible light, and the pseudo-first-order kinetic constant is 1.22 min −1 , 24-fold higher than that of CN. The superior photoactivity is attributed to a unique surface microenvironment, which N-v increased photoelectric conversion efficiency, C-v enhanced O 2 adsorption and O-s induced ·O 2 – evolution with ∼ 100% selectivity. Moreover, PVDF membrane-supported CNON 6 (11.33 cm 2 , 0.88 mg/cm 2 ) can completely remove TC from wastewater at a rate of 2.62 mg/h in a simulated industrial continuous flow cell. The cost-effectiveness assessment was $6.36/kg/h, implying the CNON 6 /PVDF has a bright application prospect in wastewater treatment. This work developed a surface microenvironment tailor strategy to design photocatalysts for efficient degradation of TC.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Hanbang Liu,Liping Yang,Danhua Yuan,Guangye Liu,Jiacheng Xing,Yunpeng Xu,Zhongmin Liu
For air separation, the separation method relying on adsorbents has attracted wide attention as a low energy consumption process, and the development of O 2 -selective adsorbents is of great significance. Metal-organic frameworks with coordinatively unsaturated transition metal sites have great potential in O 2 -selective adsorption, but most of them cannot be completely regenerated at ambient temperature or can only be effective at very low temperatures. Herein, we report two mixed-ligand metal–organic framework adsorbents [M(AIP)(BPY) 0.5 ·H 2 O] n ·2nH 2 O with coordinatively unsaturated cobalt(II) and nickel(II) sites, which can preferentially adsorb O 2 versus N 2 , and their IAST O 2 /N 2 selectivities are both significantly greater than 1 at 25 °C. These materials exhibited excellent stability and had no loss of adsorption capacities even after immersion in water for 7 days. More importantly, O 2 adsorption–desorption cycle experiments showed that these adsorbents can be completely regenerated at ambient temperature after adsorbing O 2 , and the breakthrough experiments further confirmed their dynamic O 2 /N 2 separation potential and regeneration ability. The results of theoretical calculations suggested that the interactions between adsorbents and O 2 are stronger than those of N 2 , and they have relatively obvious differences in the N 2 and O 2 interaction energies. This work provides inspirations for searching for metal–organic frameworks that can selectively adsorb O 2 at ambient temperature.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Yuran Li,Zhicheng Xu,Jian Wang,Bin Wang,Tingyu Zhu
Activated carbon exhibits a high adsorption capacity for chlorinated volatile organic compounds (Cl-VOCs), while the desorption of Cl-VOCs is not desirable in the thermal regeneration progress of activated carbon. Chlorobenzene was selected as the model substance to explore whether Cl-VOCs can be oxidized as expected in the regeneration atmosphere of O 2 -free at the temperature range of 150–450 °C. The modification of activated carbon by Cu or Fe has been shown to considerably improve the decomposition activities. According to the breakthrough curves and detection results from XPS and in situ DRIFTS, the decomposition mechanism of C 6 H 5 Cl on Cu and Fe active sites is illustrated. The adsorbed C 6 H 5 Cl is firstly dechlorinated to form C 6 H 6 and *Cl, and then it was found there are two pathways for the C 6 H 6 oxidation. C 6 H 6 is indirectly oxidized to form C 6 H 5 OH and benzoquinone species, or directly ring-opened to generate ethylene and 1,3-butadiene, and further oxidized to produce CO 2 , CO and H 2 O. The C 6 H 6 oxidation is determined by the decomposition of acetate on Cu/AC, but the decomposition of benzoquinone and maleate on Fe/AC. The Fe 3 O 4 and Fe 2 O 3 active sites have a higher dechlorination activity but accelerate the deposition of FeCl 2 , FeCl 3 and organic Cl-containing components. The CuO active center has a higher oxidation performance with a higher CO 2 selectivity. About 83.0–83.5% of adsorbed chlorobenzene has been oxidized, and the main Cl-containing product is HCl accounting for approximately 77.8–81.0%, a small amount of Cl forms polychlorinated organic compounds or metal chlorides occupying 2.0–5.7%. As the regeneration temperature decreases, the total amount of Cl-containing species is reduced due the lower oxidation and dechlorination activity of catalysts. The decomposition products of Cl-VOCs in the thermal regeneration process of activated carbon were clarified and quantified, which provides a theoretical basis to control Cl-VOCs in regeneration gas.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Dan Li,Ziye Kang,Hao Sun,Ying Wang,Haiming Xie,Jia Liu,Jiefang Zhu
Although redox mediator (RM) strategy can decrease the overpotential in Li-O 2 batteries by tuning the electrochemical formation/degradation of Li 2 O 2 from the circumscribed surface pathway to the solution one, the redox shuttling causes an unexpected RM degradation and a continuous deterioration of Li anode, finally leading to a poor cyclability. This work presents the first report detailing the development of a novel Mn x Co 3-x O 4 -decorated separator for Li-LiI-O 2 batteries. Benefiting from the promotion effect of Mn x Co 3-x O 4 nanocages on I − /I 3 − and I 3 − /I 2 redox coupling, the cell with as-prepared separator maintains a low charge potential of ~3.3 V till the death of cell cycling. In addition, as-prepared separator can efficiently restrain the redox shuttling, leading to an obvious improvement on cycling stability for the cell. Moreover, the contributions of LiI to the battery performance and the operation mechanism are systematically investigated. These results present a promising progress in the development of multi-functional separator materials for RM-involved Li-O 2 batteries and the new design of hybrid energy storage device.
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高影响因子
CHEMISTRY OF MATERIALS
·
2014
·
IF 8.535
Na Lu,Wei Chen,Guoyong Fang,Bi Chen,Keqin Yang,Yun Yang,Zhencai Wang,Shaoming Huang,Yadong Li
We report that 5-fold twinned nanowires and single twinned right bipyramids of Pd with high yields can be selectively synthesized in a hydrophilic system with the assistance of acetonitrile and ethanol, respectively. The controlled synthesis is based on an idea that small organic molecules (SOMs) that can attract halide ions via electrostatic interactions of different strengths could well adjust their activity to tune the etching degree of O2/halides for protecting the twinned Pd crystal nucleus. We consider that relatively stronger interaction between acetonitrile and halide ions for the formation of nanowires is due to the existence of three C–Hδ+ bonds induced by the electron-withdrawing CN group of CH3CN, which is confirmed by an as-called iodine starch test, 1H nuclear magnetic resonance spectra, and theoretical calculations. On the basis of this finding, we then have successfully expanded SOMs to other molecules, including acetone, 1,4-dioxane, and 1,3,5-trioxane, which have a function similar to that of acetonitrile for the production of Pd nanowires, and 2-propanol, which has a function similar to that of ethanol for the fabrication of right bipyramids. Although nanowires and bipyramids are both mainly bound by {001} planes, nanowires show better catalytic performance toward the reduction of 4-nitrophenol, indicating that more twin boundaries could offer more active catalytic sites. This work not only provides new information to decrease the degree of etching of O2/halides for controlling twin structure of noble metals but also supports the idea that creating a twin structure is good for enhancing catalytic activity.
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高影响因子
Inorganic Chemistry Frontiers
·
2017
·Vol. 4
·期 9
·1533-1538
·
IF 4.036
Ming Zhong,Xin Zhang,Dong-Hui Yang,Bei Zhao,Zhaojun Xie,Zhen Zhou,Xian-He Bu
In this work, a composite of 3D network nitrogen-doped porous carbon on reduced graphene oxide (denoted as NPC/rGO) was derived from pyrolysis of zeolitic imidazolate framework-8 and graphene oxide. The as-prepared NPC/rGO possesses high specific surface area, nitrogen doping and mesopores. When evaluated as the cathode catalyst for Li–O2 batteries, NPC/rGO exhibited higher specific capacity, better cyclability, and greater rate capability than either nitrogen doped porous carbon or reduced graphene oxide. The outstanding performances suggest that zeolitic imidazolate framework derived nitrogen doped porous carbon materials are promising for Li–O2 batteries.
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高影响因子
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