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APPLIED CATALYSIS A-GENERAL · 2021 · IF 5.706

Microporous cobaltporphyrin covalent polymer mediated Co3O4@PNC nanocomposites for efficient catalytic C-H bond activation

Mingyang Tan,Liang Zhu,Hao Liu,Yajun Fu,Shuang-Feng Yin,Weijun Yang

A Cobalt porphyrin conjugated porous polymer (Co/PCP) was obtained by hybrid polymerization of a mixture of Co(II)(5,10,15,20-tetrakis(4-bromophenyl)-21H,23H-porphyrin) (CoTBPP) and 5,10,15,20-tetrakis(4-bromophenyl)-21H,23H-porphyrin (TBPP) (3:7 M ratio) with the coupling reagent of p-phenyldiboric acid. This Co/PCP was carbonized at 400 °C and the obtained catalyst (denoted as Co 3 O 4 @PNC-400) was composed of Co 3 O 4 nanoclusters wrapped in the nitrogen-carbon materials. This catalyst has an extremely high catalytic activity for the aerobic oxidation of C–H bonds. It can efficiently catalyze the oxidation of the C–H bonds in toluene and cyclohexane with high conversion and high selectivity of (alcohol + aldehyde), (alcohol + ketone) compounds, respectively. When heat-treated at 400 °C, the porous framework structure of the porphyrin polymer was partially retained, and the highly active Co 3 O 4 nanoclusters were generated in situ. The reaction of C N to C N and connection with the Co 3 O 4 nanoclusters also occurred. Co 3 O 4 @PNC-400 has obvious synergistic catalytic effect between Co 3 O 4 and nitrogen-carbon framework during the catalytic reaction. The defective structure caused by the migration of cobalt also greatly improved the catalytic activity. Co/PCPs with different cobalt contents were also synthesized and heat treated at different temperature. These catalysts were a new type of efficient C–H oxidation catalysts with excellent potential application value.

研究领域: 材料科学 · 催化 · 化学工程 · 有机化学
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Journal of Energy Storage · 2024 · IF 8.9

In-situ synthesis and application of hollow H-SnS/MXene@C nanobox for advanced LIBs and NIBs anodes

Wei-Xiang Cheng,Ting-Ting Mao,Yi-Zhao Chen,Shuai-Fu Cui,Jing Chen,Dao-Ren Deng,Ru-Ming Feng,Song-Yi Liao,Yong-Gang Min

In this paper, cubic ZnSn(OH) 6 with MXene were firstly in-situ synthesized, and subsequently vulcanized and etched to obtain hollow SnS nanoboxes with MXene coating by carbon layer (referred to as H-SnS/MXene@C). The composition and surface chemical state of H-SnS/MXene@C were characterized by XRD and XPS , respectively. The microscopic morphology of H-SnS/MXene@C was analyzed and characterized in detail by SEM and TEM, and the results show that the hollow SnS nano-boxes formed an effective connection with the MXene nanosheets . When used as LIBs anode, the H-SnS/MXene@C maintained ∼707 mAh/g after 200 cycles at 0.5 A/g current density. As a NIBs anode material, the H-SnS/MXene@C delivered ∼402 mAh/g after 150 cycles at 0.5 A/g current density. In addition, a detail simulation/calculation revealed that H-SnS/MXene@C demonstrated a higher pseudocapacitance (83.2 % for LIBs and 74.4 % for NIBs at a scan rate of 2 mV/s, respectively). The synergistic effect of the highly conductive MXene and the three-dimensional hollow cubic structure could effectively provide an efficient channel for charge transfer and ionic diffusion in H-SnS/MXene@C anode.

研究领域: 材料科学 · 电化学 · 能源存储
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JOURNAL OF ORGANIC CHEMISTRY · 2025 · IF 3.6

I2-Induced Metal-Free C(sp2)–H Functionalization of Indoles via One-Pot and Two-Step Reaction with 1-(2-Hydroxyphenyl)-propargyl Alcohols: Access to 3-(Benzofuran-3-yl)-1H-indoles

Yang Zhu,Guisheng Deng

The I2-catalyzed reaction of 1-(2-hydroxyphenyl)-propargyl alcohols with indoles and subsequent treatment with K2CO3 provided (benzofuran-3-yl)-1H-indoles in good to excellent yields with high regioselectivity. This one-pot and two-step strategy proved to be suitable for a wide range of substrates except for aliphatic alkynyl alcohols as well as the indoles bearing N-protected groups such as the Ts group possessing strong electron-withdrawing feature. The reaction procedure involved a cross-coupling and the construction of a benzofuran framework via 5-exo-dig cyclization.

CAS / MDL: 120-72-9
研究领域: 有机化学 · 合成化学
✓ 已验证 产品关联 DOI PubMed 高影响因子
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CELL BIOLOGY INTERNATIONAL · 2024 · IF 3.3

DEAD/H-box helicase 11 is transcriptionally activated by Yin Yang-1 and accelerates oral squamous cell carcinoma progression

Guang Yang,Xin Shi,Meixia Zhang,Kaiwen Wang,Xin Tian,Xiaofeng Wang

Oral squamous cell carcinoma (OSCC) is the most common oral malignancy. DEAD/H-box helicase 11 (DDX11), a DNA helicase, has been implicated in the progression of several cancers. Yet, the precise function of DDX11 in OSCC is poorly understood. The DDX11 expression in OSCC cells and normal oral keratinocytes was evaluated in the Gene Expression Omnibus database (GSE146483 and GSE31853). SCC-4 and CAL-27 cells expressing doxycycline-inducible DDX11 or DDX11 shRNA were generated by lentiviral infection. The role of DDX11 in OSCC cells was determined by 3-(4, 5-Dimethylthiazol-2-yl)-2, 5-diphenyltetrazolium bromide assay, colony formation assay, flow cytometry assay, TUNEL staining, and western blot. The effects of DDX11 on tumor growth were explored in a xenograft nude mouse model. The relationship between DDX11 and transcription factor Yin Yang-1 (YY1) was researched using the dual luciferase report assay and chromatin immunoprecipitation assay. DDX11 expression was significantly upregulated in OSCC cells. Knockdown of DDX11 inhibited cell proliferation, induced cell cycle arrest, and suppressed PI3K-AKT pathway, while DDX11 overexpression showed opposite effects. The number of apoptotic cells was increased in DDX11 silenced cells. DDX11 upregulation or knockdown accelerated or suppressed tumor growth in vivo, respectively. Moreover, the YY1 bound and activated the DDX11 promoter, resulting in increasing DDX11 expression. Forced expression DDX11 reversed the anticancer effects of YY1 silencing on OSCC cells. DDX11 has tumor-promoting function in OSCC and is transcriptionally regulated by YY1, indicating that DDX11 may serve as a potential target for the OSCC treatment.

研究领域: 肿瘤学 · 分子生物学 · 细胞生物学 · 转化医学
✓ 已验证 DOI PubMed 高影响因子
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JOURNAL OF ORGANIC CHEMISTRY · 2023 · IF 3.6

Organocalcium Hydride-Catalyzed Intramolecular C(sp3)–H Annulation of Functionalized 2,6-Lutidines

Shuo Li,Xian Xu,Qianlin Sun,Xin Xu

This work reports an intramolecular C(sp3)–H annulation of functionalized 2,6-lutidines catalyzed by an organocalcium hydride [{(DIPPnacnac)CaH(thf)}2] (DIPPnacnac = CH{(CMe)(2,6-iPr2–C6H3N)}2). This reaction constitutes a streamlined approach for producing a new family of tetrahydro-1,5-naphthyridines and hexahydropyrido[3,2-b]azocines derivatives in good to excellent yields with high atom efficiency and broad substrates scope. A calcium alkyl complex was isolated from the stoichiometric reaction between calcium hydride and the substrate through deprotonation, which was structurally characterized and confirmed as the catalytic intermediate.

研究领域: 有机化学 · 催化 · 合成化学
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Science China-Chemistry · 2022 ·Vol. 66 ·期 2 ·548-561 · IF 10.138

The marriage of dual-acceptor strategy and C-H activation polymerization: naphthalene diimide-based n-type polymers with adjustable molar mass and decent performance

Zhao Ying-Han,Li Wenhao,Shen Tao,Zhao Yan,Liu Yunqi,Wang Yang

The development of readily accessible high-mobility n-type semiconducting polymers is in great demand for realizing high-performance p-n junction-based organic electronics. In this study, we demonstrate that with the combination of dual-acceptor strategy and C-H direct arylation polymerization (DArP), unipolar n-type semiconducting polymers can be conveniently synthesized. By tuning the monomer concentration, three dual-acceptor polymers, namely, poly(naphthalene diimide- alt -dithiophenyl pyrrolopyrrole-dione) (PNDI-DPP), poly(naphthalene diimide- alt -dithiophenyl isoindigo) (PNDI-IID), and poly (naphthalene diimide- alt -dithiophenyl bezothiadiazole) (PNDI-BT) can be obtained via C-H activation with decent number average molecular weight of ∼10 to 30 kg mol −1 and relatively narrow polydispersity index of ∼2. In addition, these polymers are defect-free in nature as evidenced by the nuclear magnetic resonance. Moreover, we attribute the different molar masses of the three copolymers under the same DArP condition to the different α-C-H acidity, which may stem from different electron-withdrawing capability of the hydrogenated acceptor units. Furthermore, the influence of the hydrogenated acceptor monomers on the optical, electrochemical and charge transporting properties is comprehensively studied. Among the three dual-acceptor polymers, PNDI-BT demonstrates the highest electron mobilities of up to 0.6 cm 2 V −1 s −1 in unipolar n-type organic transistors because of its relatively planar backbone, larger overlaps of the lowest unoccupied molecular orbital and strong H-aggregation. Note that the transistor performance of PNDI-BT synthesized via C-H activation in this study is at least comparable to the one made by conventional C(sp 2 )-C(sp 2 ) Stille or Suzuki cross-coupling polymerization. This study demonstrates the presented protocol can be a useful platform for sustainable and convenient synthesis of high-performance n-type semiconducting polymers.

研究领域: 材料科学 · 有机电子学
✓ 已验证 DOI 高影响因子
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GREEN CHEMISTRY · 2021 ·Vol. 24 ·期 1 ·384-393 · IF 10.182

Cu@CuCl-visible light co-catalysed chlorination of C(sp3)–H bonds with MCln solution and photocatalytic serial reactor-based synthesis of benzyl chloride

Qi Zhang,Shouxin Liu,Xia Tian,Yidong Liu,Shiming Fan,Baibiao Huang,Andrew Whiting

A highly selective, green and sustainable chlorination of aliphatic C–H bonds is reported using MCln under the co-catalysis of visible light and nano-Cu@CuCl, which was synthesised via a one-step, hydrothermal strategy using copper(II) sulfate and D-glucose as the reducing agent in a KCl solution. A novel cascade method of producing Cl2 occurs in situ chlorinating C(sp3)–Hs, achieved through nano-Cu@CuCl catalysis using inorganic chloride MCln as a chlorine source under visible light and without the need for a strong oxidant. The reaction was applied to the chlorination of different alkylarene α-Hs and cyclic hydrocarbons C–HS and was developed for use in a photocatalytic serial reactor system which accomplished the chlorination of toluene α-Hs to give 92% conversion, 90% yield and 98% selectivity. Electron spin resonance (ESR) studies of DMPO-Cl. revealed that the reaction mechanism belonged to a free radical process.

研究领域: 有机化学 · 绿色化学 · 材料科学
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MATERIALS LETTERS · 2022 · IF 3.574

Synthesis of C-S-H seeds using the waste solution of acid treatment of recycled concrete aggregates and black liquor

Feifei Zhou,Ganghua Pan,Haining Meng,Hailong Sun

For preparing finer and well-dispersed calcium-silicate-hydrate (C-S-H) seeds at a lower cost, the waste solution of acid treatment of recycled concrete aggregates (RCAs) and black liquor from pulping were used for the synthesis of C-S-H seeds. The results show that C-S-H seeds can be successfully fabricated by chemical co-precipitation reaction using the two waste solutions. Interestingly, it was globular rather than traditional foil-like. Furthermore, C-S-H seeds synthesized using the two waste solutions had smaller particle size and better dispersibility. More importantly, it had a more prominent accelerating effect to the strength development of mortar, significantly enhancing the early and long-term compressive strength of mortar.

研究领域: 材料科学 · 土木工程 · 环境科学
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ORGANOMETALLICS · 2020 · IF 3.804

Palladium-Catalyzed Cyclobutanation of Aryl Sulfonates through both C–O and C–H Cleavage

Liangwei Zhang,Long Liu,Tianzeng Huang,Qizhi Dong,Tieqiao Chen

A palladium-catalyzed cyclobutanation of aryl sulfonates with strained alkenes has been developed. The methodology is featured to achieve the cleavage of both C–O and C–H bonds of phenol derivatives in one pot. Under the reaction conditions, in addition to reactive triflates, the relatively inactive tosylates and mesylates can also be transformed into the corresponding benzocyclobutanes in high yields. This reaction can be carried out in gram-scale experiments with a low loading of the palladium catalyst and is applicable to the cyclobutanative modification of bioactive molecules, highlighting its synthetic value in organic synthesis.

研究领域: 有机化学 · 催化化学 · 合成化学
✓ 已验证 DOI 高影响因子
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Advanced Science · 2024 · IF 14.3

H. Pylori-Facilitated TERT/Wnt/β-Catenin Triggers Spasmolytic Polypeptide-Expressing Metaplasia and Oxyntic Atrophy

Lijiao He,Xiao Zhang,Shengwei Zhang,Yi Wang,Weichao Hu,Jie Li,Yunyi Liu,Yu Liao,Xue Peng,Jianjun Li,Haiyan Zhao,Liting Wang,Yang-Fan Lv,Chang-Jiang Hu,Shi-Ming Yang

Persistent H. pylori infection triggers the repair program of the mucosa, such as spasmolytic polypeptide-expressing metaplasia (SPEM). However, the mechanism underlying the initiation of SPEM in gastric tissues by H. pylori remains unclear. Here, an increase in telomerase reverse transcriptase (TERT) protein expression is observed in chief cells upon infection with cagA -positive H. pylori . Tert knockout significantly ameliorated H. pylori -induced SPEM and single-cell RNA sequencing demonstrated that the Wnt/β-Catenin pathway is suppressed in gastric cells with Tert knockout. Mechanism study revealed that CagA elevated TERT abundance by disrupting the interaction between TERT and its novel E3 ligase, SYVN1. Interestingly, Nitazoxanide effectively relieved SPEM via inhibition of the Wnt/β-Catenin signaling in vivo. This results clarified the mechanism underlying which CagA activated the TERT/Wnt/β-Catenin pathway, thus promoting the dedifferentiation of chief cells and the occurrence of SPEM in gastric mucosa. This highlights a molecular basis for targeting CagA-activated Wnt signaling in chief cells for the treatment of gastric precancerous lesions.

研究领域: 胃肠病学 · 分子生物学 · 肿瘤学 · 病理学
✓ 已验证 DOI PubMed 高影响因子
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MedChemComm · 2013 ·Vol. 5 ·期 2 ·147-152 · IF 2.722

Self-assembled, redox-sensitive, H-shaped pegylated methotrexate conjugates with high drug-carrying capability for intracellular drug delivery

Haiqing Dong,Chunyan Dong,Wenjuan Xia,Yongyong Li,Tianbin Ren

A novel prodrug of pegylated methotrexate conjugates (PMCs) with a high drug-carrying capability and a redox sensitive drug release mechanism was reported for intracellular drug delivery. The PMC was structured in a H-shape with four molecules of anticancer drug methotrexate (MTX) linked to both ends of the PEG main chain via disulfide linkers, resulting in the conjugates with a high and constant drug loading efficiency of up to 26 wt%. The amphiphilic property of PMCs enables them to self-assemble into nanoparticles in aqueous solution, while the cleavable disulfide linkers allow the conjugated MTX to exert its therapeutic activity due to the fast cleavage of disulfide linkers when exposed to the intracellular concentration of glutathione (GSH). Cell proliferation assays performed with HepG2 cancer cells confirmed the pharmacological efficacy.

研究领域: 药理学 · 癌症研究 · 纳米医学 · 药物递送系统
✓ 已验证 DOI 高影响因子
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2023 · IF 9.9

Ni-doped Bi2O2CO3 nanosheet with H+/Zn2+ co-insertion for “rocking chair” zinc-ion battery

Mengwei Han,Yuzhu Qian,Xinni Li,Nailiang Wang,Ting Song,Li Liu,Xianyou Wang,Xiongwei Wu,Man-Kay Law,Bei Long

Developing insertion-type anode is key to advancing “rocking chair” zinc-ion batteries, though there are few reported insertion-type anodes. Herein, the Bi 2 O 2 CO 3 is a high-potential anode, with a special layered structure. A one-step hydrothermal method was used to prepare Ni-doped Bi 2 O 2 CO 3 nanosheet , and also a free-standing electrode consisting of Ni-Bi 2 O 2 CO 3 and CNTs was designed. Both cross-linked CNTs conductive networks and Ni doping improve charge transfer. Ex situ tests (XRD, XPS, TEM, etc.) reveal the H + /Zn 2+ co-insertion mechanism of Bi 2 O 2 CO 3 and that Ni doping improves its electrochemical reversibility and structural stability. Therefore, this optimized electrode offers a high specific capacity of 159 mAh g −1 at 100 mA g −1 , a suitable average discharge voltage of ≈0.400 V, and a long-term cycling stability of 2200 cycles at 700 mA g −1 . Besides, the Ni-Bi 2 O 2 CO 3 //MnO 2 “rocking chair” zinc-ion battery (based on the total mass of cathode and anode) delivers a high capacity of ≈100 mAh g −1 at 50.0 mA g −1 . This work provides a reference for designing high-performance anode in zinc-ion batteries.

研究领域: 材料科学 · 电化学 · 能源存储
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