NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 16
·7810-7818
·
IF 3.3
Yanke Guo,Qiaoyun Qin,Jing Zhu,Baohe Wang
Propylene glycol methyl ether was directly synthesized from propylene and hydrogen peroxide under mild conditions via aluminum modified titanium silicalite-1 as a bifunctional catalyst. It has both active sites capable of epoxidation and active sites capable of ring opening reactions, thus realizing the one-pot preparation of propylene glycol methyl ether by propylene. The synergistic effect of Ti–Al on the catalytic performance and the distribution of propylene glycol methyl ether isomer were investigated in detail, and the synergistic catalysis between the two active sites was characterized. The gradual introduction of aluminum reduced the activation ability for hydrogen peroxide, but gradually increased the selectivity for propylene glycol methyl ether. Under the optimum conditions, the selectivity for propylene glycol methyl ether reached 91.53%. Combined with Density Functional Theory (DFT) calculations, the synergistic catalytic effect of doped Al and framework Ti in titanium silicalite-1 is discussed in detail from a microscopic perspective. Al increases the Lewis acid strength of Ti active sites and promotes the conversion of propylene to propylene oxide (PO), and simultaneously Ti increases the Brønsted acid strength of Al active sites and promotes the conversion of propylene oxide to propylene glycol ether.
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JOURNAL OF ORGANIC CHEMISTRY
·
2020
·
IF 4.335
Nian Zheng,Ce Liu,Ya-Nan Ding,Wei-Yu Shi,Bo-Sheng Zhang,Yong-Min Liang
Copper-catalyzed three-component redox-neutral ring opening of benzothiazoles with aryl iodides and O-benzoyl hydroxylamines for the synthesis of 1-amino-N-(2-(phenylthio)phenyl)methanimine has been developed. This one-pot reaction undergoes C–S and N–O bond cleavage and new C–S and C–N bond construction. Several control experiments excluded a free radical procedure and also demonstrated the secondary amine as a possible intermediate, which was vital to the catalytic reaction. Meanwhile, the deuteration experiment got rid of the C–H activation dehydroisomerization of the benzothiazole mechanism.
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APPLIED AND ENVIRONMENTAL MICROBIOLOGY
·
2022
·Vol. 88
·期 6
·
IF 5.005
Ke Huang,Wei Liu,Yuanhe Li,Sha Zeng,Fang-Jie Zhao
Methylarsenate (MAs(V)) is a product of microbial arsenic (As) biomethylation and has also been widely used as an herbicide. Some microbes are able to reduce nontoxic MAs(V) to highly toxic methylarsenite (MAs(III)) possibly as an antibiotic. The mechanism of MAs(V) reduction in microbes has not been elucidated. Here, we found that the bacterium Enterobacter sp. CZ-1 isolated from an As-contaminated paddy soil has a strong ability to reduce MAs(V) to MAs(III). Using a MAs(III)-responsive biosensor to detect MAs(V) reduction in E. coli Trans5α transformants of a genomic library of Enterobacter sp. CZ-1, we identified gshA, encoding a glutamate-cysteine ligase, as a key gene involved in MAs(V) reduction. Heterologous expression of gshA increased the biosynthesis of glutathione (GSH) and MAs(V) reduction in E. coli Trans5α. Deletion of gshA in Enterobacter sp. CZ-1 abolished its ability to synthesize GSH and decreased its MAs(V) reduction ability markedly, which could be restored by supplementation of exogenous GSH. In the presence of MAs(V), Enterobacter sp. CZ-1 was able to inhibit the growth of Bacillus subtilis 168; this ability was lost in the gshA-deleted mutant. In addition, deletion of gshA greatly decreased the reduction of arsenate to arsenite. These results indicate that GSH plays an important role in MAs(V) reduction to generate MAs(III) as an antibiotic.IMPORTANCE Arsenic is a ubiquitous environmental toxin. Some microbes detoxify inorganic arsenic through biomethylation, generating relatively nontoxic pentavalent methylated arsenicals, such as methylarsenate. Methylarsenate has also been widely used as an herbicide. Surprisingly, some microbes reduce methylarsenate to highly toxic methylarsenite possibly to use the latter as an antibiotic. How microbes reduce methylarsenate to methylarsenite is unknown. Here, we show that gshA encoding a glutamate-cysteine ligase in the glutathione biosynthesis pathway is involved in methylarsenate reduction in Enterobacter sp. CZ-1. Our study provides new insights into the crucial role of glutathione in the transformation of a common arsenic compound to a natural antibiotic.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Aonan Qiao,Yu Liu,Fei Li,Haixia Pan,Yanan Guo,Yang Liu,Xianliang Yi,Hao Zhou
Manganese-oxidizing bacteria (MnOB) mediate the oxidation of Mn(II) in both natural and engineered environments. Although numerous MnOB have been isolated, the regulatory mechanisms governing their Mn(II)-oxidizing activity in response to nitrogen sources remain poorly understood. This study investigates how nitrogen sources affect the Mn(II)-oxidizing capability of Pseudomonas sp. AN-1. Mn(II) oxidation was completely inhibited in NH 4 + -supplemented cultures, with no detectable BioMnOx production throughout a 10-day incubation period. In contrast, complete oxidation of 100 μM Mn(II) occurred within 27 h when either NO 3 − or NO 2 − as the nitrogen source. Intriguingly, Mn(II) oxidation exhibited a histidine concentration-dependent pattern: no oxidation was observed at 0.5–1.0 mM histidine, whereas complete oxidation occurred at 2.5 mM. Transcriptomics and proteomics revealed NO 3 − -fed cultures exhibited significantly higher expression of manganese oxidation genes, including mnxG and mcoA , compared to histidine-supplemented cultures. Further analysis identified the MnxS/MnxR as essential for initiating the transcription of mnxG and mcoA . Bioinformatic analysis revealed this regulatory system is widely distributed in the genus Pseudomonas and frequently co-occurs with mnxG and mcoA . This study provides insight into nitrogen-source dependent regulation of bacterial Mn(II) oxidation, uncovering concentration-dependent effects and identifying the MnxS/MnxR system as a key regulatory node that integrates nitrogen sensing with Mn(II) oxidation.
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Materials Research Express
·
2020
·Vol. 6
·期 12
·125376
·
IF 1.929
Sainan Wu,Pan Zhang,Zhilong Xu,Zhang Chen,Yanfeng Gao
A series of microencapsulated phase change materials (microPCMs) are synthesized by encapsulating 1-dodecanol into cellulose nanofibers (CNFs) modified melamine-formaldehyde (MF) resin through in situ polymerization. The chemical structure and crystallography of the microcapsules are characterized by Fourier-transform infrared spectroscopy (FT-IR) and x-ray diffraction (XRD). Scanning electronic microscopy (SEM) images show that the obtained microcapsules are regularly spherical with smooth surface and an average diameter about 1∼3 μm. The cracking ratio test indicates that the addition of CNFs largely enhances the mechanical strength of the microcapsules, and the CNFs/MF-microPCMs (with 3.4 wt% CNFs) have a phase change enthalpy of 100.4 J g−1. Furthermore, the simulation result demonstrates that the indoor temperature modulation ability of CNFs/MF-microPCMs model house is 4.2 °C, which is more than that of model house without microPCMs under room temperature. These results indicate that CNFs/MF-microPCMs are potential candidates for thermoregulating applications.
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MOLECULES
·
2024
·Vol. 29
·期 19
·4709
·
IF 4.2
Xinyu Liu,Shu Wang,Mingxia Wang,Lifang Chen,Zhiwen Qi
The esterification of 1-methoxy-2-propanol (PM) and acetic acid (AA) is an important reaction for the production of 1-methoxy-2-propyl acetate (PMA). Herein, we used the macroporous ion-exchange resin Amberlyst-35 as a catalyst to explore the effects of reaction conditions on the reaction rate and equilibrium yield of PMA. Under the optimized conditions of a reaction temperature of 353 K, using the initial reactant PM/AA with a molar ratio of 1:3, and a catalyst loading of 10 wt%, the PMA equilibrium yield reached 78%, which is the highest equilibrium yield so far. The reaction equilibrium constants and activity coefficients were estimated to obtain reaction thermodynamic properties, indicating the exothermicity of the reaction. Furthermore, pseudo-homogeneous (PH), Eley–Rideal (ER), and Langmuir–Hinshelwood–Hougen–Watson (LHHW) kinetic models were fitted based on experimental reaction kinetic data. The results demonstrate that the LHHW model is the most consistent with experimental data, indicating a surface reaction-controlled process and exhibiting an apparent activation energy of 62.0 ± 0.2 kJ/mol. This work represents a valuable example of calculating reaction thermodynamics and kinetics, which are particularly essential for promising industrial reactor designs.
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2024
·
IF 11.2
Guilin Wei,Junhong Luo,Wenwen Yong,Jiangfeng Song,Yan Shi,Xingwen Feng,Ning Liu
Controllable nuclear fusion is a major breakthrough in the future energy field and an important way for mankind to pursue clean and sustainable energy. However, since the fusion reaction raw material tritium is radioactive (β decay, half-life is 12.43 years), the leakage of these hydrogen isotopes under accident conditions will bring the risk of explosion and cause radiation damage to human. Therefore, efficient removal of hydrogen isotopes leaked due to accidents is crucial to the safe operation of nuclear fusion and human health. This study utilizes the metal-support interaction effect to design a series of Pd catalysts for efficient catalytic oxidation of hydrogen isotopes. Using pure silicon zeolite as a carrier, Pd is confined in the channel structure using a ligand-stabilized in situ encapsulation method. The prepared catalyst has nanoscale dispersed metal clusters and has excellent hydrogen isotope catalytic oxidation performance. This study systematically explored the effects of catalyst post-treatment methods, reaction space velocity, and reaction temperature on the hydrogen isotope catalytic oxidation conversion rate. The results show that the catalyst can be fully reduced at 600 °C and can achieve a hydrogen isotope catalytic oxidation conversion rate of greater than 98 % (24,000 mL g –1 h –1 ) at 100 °C. The conversion rate for hydrogen is higher than 96 % under the same space velocity at 50 °C. After 35,360 min (∼24.5 d) of continuous testing and intermittent operation, the catalyst can also maintain a conversion rate of 99 % (100 °C, 24,000 mL g –1 h –1 ). A lower reduction temperature will leave some organic matter, which will coordinate and bond on the Pd clusters and thus affect the catalytic activity. Under the same conditions, the hydrogen conversion rate of the catalyst directly reduced at 400 °C was 14 % lower than that of reduction at 600 °C, which proves the criticality of the reduction temperature. This work demonstrates a systematic study of utilizing the confinement effect of molecular sieve pores to obtain Pd cluster catalysts and applying them to the oxidative removal of hydrogen isotopes. It focuses on exploring the impact of the direct reduction temperature of the catalyst on its performance, which may be useful for providing a certain reference for designing relevant catalysts in engineering applications.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Weijie Zhang,Xiaofei Wang,Peng Wang,Qingdong Li,Yankun Zhang,Xiaoshuo Meng,Geng Tian,Jianmin Xiao,Guilong Zhang
Cisplatin (CDDP), a first-line chemotherapeutic agent, faces significant challenges in the treatment of non-small-cell lung cancer (NSCLC) due to the rapid emergence of drug resistance. In this study, a glucose transporter protein 1-targeted nanodrug (RCPM) was developed by coordinating rutin with polymetallic ions, including Fe, V , and Pt. RCPM selectively targeted CDDP-resistant A549 (A549R) cells, efficiently accumulating within tumors. Exhibiting exceptional photothermal (PT) properties, RCPM facilitated PT-induced tumor ablation. Within the tumor microenvironment, RCPM underwent degradation, releasing high concentrations of V , Fe, and CDDP. The liberated V and Fe ions catalyzed the Fenton reaction, generating reactive oxygen species (ROS) and inducing ferroptosis. Simultaneously, these metal ions synergistically suppressed the expression of excision repair cross-complementing 1 (ERCC1), glutathione (GSH), and adenosine triphosphate (ATP), effectively disrupting DNA repair pathways, preventing CDDP inactivation, and enhancing its cytotoxicity against A549R tumors. Furthermore, RCPM demonstrated complete and rapid renal clearance, ensuring excellent biosafety and strong clinical translational potential. In vivo studies revealed that a single administration of RCPM, combined with PT therapy, significantly inhibited NSCLC progression. These findings highlight RCPM as a promising nanodrug for overcoming CDDP resistance and enhancing NSCLC treatment efficacy.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Xiaohang Sun,Zhengzuo Liu,Shuairen Qian,Kaiqi Nie,Zhengwen Li,Weiming Wan,Binhang Yan
Designing an active Cu/ZnO interface is crucial for efficient catalytic hydrogenation of CO 2 to methanol. In this study, we introduce a straightforward impregnation method to synthesize HKUST-1-derived inverse ZnO x /Cu catalysts. The resulting ZnO x /Cu interface exhibits outstanding methanol space-time yield and selectivity, surpassing conventional Cu/ZnO catalysts synthesized via the co-precipitation and impregnation methods. In situ characterization reveals that small, well-dispersed ZnO x nanoparticles are located on moderately sized Cu nanoparticles, which is attributed to the high specific surface area and ligand coordination of HKUST-1. The inverse ZnO x /Cu structure promotes the formation of reduced ZnO x nanoparticles, which significantly enhance CO 2 and H 2 activation, resulting in increased methanol production. Additionally, the moderate size of Cu nanoparticles minimizes CO* intermediate formation, further enhancing methanol selectivity. This work not only offers valuable insights for the development of new Cu/ZnO catalysts but also provides guidance for the synthesis of inverse metal oxide/metal catalysts for other catalytic systems.
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APPLIED CATALYSIS A-GENERAL
·
2025
·
IF 4.8
Huimin Li,Bin Wu,Zhimin Zhu,Chenyang Li,Zhihan Liu,Fuweng Zhang,Huidong Zheng,Longfei Yan
Ethylene sulfate (DTD) is a new type of solid electrolyte interphase (SEI) film-forming additive for lithium-ion batteries. DTD was typically synthesized in the industry by oxidation of ethylene sulfite (ES) with NaClO via a RuCl 3 -catalyzed reaction. However, this route generates significant amount of Cl-containing wastes, and the recovery of RuCl 3 is costly and technically challenging. Herein, we present a green and heterogeneous route for synthesizing DTD from ES, utilizing the Titanium Silicalite-1 (TS-1) and H 2 O 2 as catalysts and green oxidants, respectively. Our research reveals that the tetra-coordination framework of Ti in TS-1 serves as the main active site for the oxidation of ES, achieving a remarkable yield of DTD up to 92 % under optimized reaction conditions. Additionally, we developed a continuous green oxidation process for synthesizing DTD from ES, which is the first of its kind and has been successfully operated continuously for over 300 h. This work provides a cost-effective, green, and efficient route for synthesizing DTD from ES.
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CANCER CELL
·
2022
·
IF 38.585
Haixia Long,Qingzhu Jia,Liuyang Wang,Wenfeng Fang,Zhongyu Wang,Tao Jiang,Fei Zhou,Zheng Jin,Jiani Huang,Li Zhou,Chunyan Hu,Xinxin Wang,Jin Zhang,Yujie Ba,Yujie Gong,Xianghua Zeng,Dong Zeng,Xingxing Su,Peter B. Alexander,Li Wang,Limei Wang,Yisong Y. Wan,Xiao-Fan Wang,Li Zhang,Qi-Jing Li,Bo Zhu
Summary Despite the unprecedented success of immune checkpoint inhibitors (ICIs) as anti-cancer therapy, it remains a prevailing clinical need to identify additional mechanisms underlying ICI therapeutic efficacy and potential drug resistance. Here, using lineage tracking in cancer patients and tumor-bearing mice, we demonstrate that erythroid progenitor cells lose their developmental potential and switch to the myeloid lineage. Single-cell transcriptome analyses reveal that, notwithstanding quantitative differences in erythroid gene expression, erythroid differentiated myeloid cells (EDMCs) are transcriptionally indistinguishable from their myeloid-originated counterparts. EDMCs possess multifaceted machinery to curtail T cell-mediated anti-tumor responses. Consequently, EDMC content within tumor tissues is negatively associated with T cell inflammation for the majority of solid cancers; moreover, EDMC enrichment, in accordance with anemia manifestation, is predictive of poor prognosis in various cohorts of patients undergoing ICI therapy. Together, our findings reveal a feedforward mechanism by which tumors exploit anemia-triggered erythropoiesis for myeloid transdifferentiation and immunosuppression.
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DALTON TRANSACTIONS
·
2022
·Vol. 51
·期 31
·11703-11712
·
IF 4.569
Jun Sun,Minghui Zhou,Bei Zhang,Youjie Hua,Feifei Huang,Hongping Ma,Renguang Ye,Shiqing Xu
A series of Rb1−yKyNa3(Li3SiO4)4:Eu2+(0 ≤ y ≤ 1) phosphors were successfully synthesized through a high-temperature solid-state reaction. The introduction of K+ into the RbNa3(Li3SiO4)4:Eu2+ phosphor to partially or completely replace Rb+ allows the emission spectrum to be modulated from blue (λ = 473 nm, FWHM = 22.5 nm) to a narrow cyan band (λ = 485 nm, FWHM = 21.1 nm). As the K+ ion content increases, the space group of the phosphor evolves from I4/M to I41/A. The complete replacement of Rb+ by K+ results in the KNa3(Li3SiO4)4:Eu2+ cyan phosphor, which shows excellent thermal stability (the comprehensive emission loss is only 8% at 150 °C) and can be used to fill the cyan light gap in white LED devices. By adding the KNa3(Li3SiO4)4:Eu2+ cyan phosphor in packaging with yellow and red phosphors, the color rendering index is increased from 90.2 to 97.1 and the correlated color temperature improved to 3658 K. These results indicate that the cyan phosphor has important application value in full-spectrum white LEDs.
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