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ACS Omega · 2020 · IF 2.87

Electrosynthesis of Quinazolines and Quinazolinones via an Anodic Direct Oxidation C(sp3)-H Amination/C-N Cleavage of Tertiary Amine in Aqueous Medium

Zhenghong Zhou,Kangfei Hu,Jiawei Wang,Zhibin Li,Yan Zhang,Zhenggen Zha,Zhiyong Wang

An electrochemical synthesis for quinazolines and quinazolinones was developed via a C(sp3)-H amination/C-N cleavage by virtue of the anodic oxidation. The reaction can be carried out in aqueous media under mild conditions to afford the desired products with high yields. The reaction mechanism was proposed after detailed investigation.

研究领域: 有机化学 · 电化学
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ADVANCED FUNCTIONAL MATERIALS · 2022 ·Vol. 32 ·期 51 ·2208676 · IF 19.924

Ultraductile Cementitious Structural Health Monitoring Coating: Waterborne Polymer Biomimetic Muscle and Polyhedral Oligomeric Silsesquioxane-Assisted C-S-H Dispersion

Bo Pang,Zuquan Jin,Yunsheng Zhang,Zhiyong Liu,Wei She,Penggang Wang,Yong Yu,Xiaoying Zhang,Chuansheng Xiong,Ning Li,Guowen Sun,Peng Zhao,Guojian Liu,Xiaoyun Song,Song Gao

Cement-based sensors (CBSs) have demonstrated potential in structural health monitoring (SHM) despite rare applications due to their poor flexibility and sensing accuracy/protection with robustness. Herein, a promising strategy is reported to design a waterborne epoxy resin (WEP)-modified cement-based composite coating sensorcapable of simultaneous stable SHM and durable protection. The interpenetrating network (IPN) formed by WEP within cement paste is bionic to the toughness and crack resistance of biological muscle tissue and balances the ion permeation performance and polarization of hydration products. The polymerization-redispersion progress and mechanism of calcium silicate hydrate (C-S-H) gel modified with [3-(2-aminoethylamino)-propyl]trimethoxysilane silsesquioxane (C-POSS) are characterized and revealed. The results show that the muscle-like IPN increases the cement-based coatings’ maximum deflection angle to 30° and improves the monitoring accuracy of compressive, tensile, and fatigue microchanges of concrete structures to more than 95%. The POSS···Ca 2+ ···C-S-H interaction in C-POSS partially transferred the intra-adhesive hydrogen bonds surrounding the nanoconducer into electrostatic bridging ones to maintain an excellent electromechanical conductive dispersion.

研究领域: 土木工程 · 材料科学 · 传感器技术
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Near-infrared laser induced direct ignition of 4,4′,5,5′-tetranitro-1H,1′H-[2,2′-biimidazole]-1,1′-diamine by constructing diverse crystal structures

Ping Ye,Weimiao Wang,Xiaodong Li,Zhiqiang Qiao,Yirui Lu,Bing Huang,Liangfei Bai,Liang Chen,Xiaoqing Tu,Rui Li,Guangcheng Yang,Guoqing Lv

Although laser ignition is considered to be one of the most promising ways to detonate energetic materials due to its high safety and reliability, it is still a challenge to achieve direct ignition of energetic materials by a laser with low-power and near-infrared (NIR) band. In this paper, a molecular self-assembly strategy based on recrystallization was utilized to prepare 4,4′,5,5′-tetranitro-1H,1′H-[2,2′-biimidazole]-1,1′-diamine (DATNBI) crystals with various micro-nano structures. The characterization results suggest that DATNBI crystals with different degrees of roughness and defects by the induction of solvents and surfactants. The crystal defects can not only bring about the enhancement of light absorption of DATNBI in NIR band, but also advance its thermal decomposition, providing reliable support for direct laser ignition of DATNBI profit from the hot spot ignition theory. Combined with density functional theory, it is speculated that electrons of defect states achieve electron-hole recombination by laser radiation, thereby enhancing photothermal conversion. Compared with raw DATNBI, DATNBI crystals with rough surface and abundant defects can be directly ignited by a NIR laser and exhibits self-sustainable combustion. In summary, a direct NIR laser-ignitable energetic material has been prepared via appropriate crystal structure design.

研究领域: 材料科学 · 光学工程 · 化学工程
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Energy Storage Materials · 2018 · IF 0

Highly synergetic catalytic mechanism of Ni@g-C3N4 on the superior hydrogen storage performance of Li-Mg-B-H system

Xu Huang,Xuezhang Xiao,Xuancheng Wang,Zhendong Yao,Chuntao Wang,Xiulin Fan,Lixin Chen

Li-Mg-B-H system with the composition of 2LiBH 4 -MgH 2 is one of the most promising reversible hydrogen storage materials because of the extremely high hydrogen storage capacity (11.5 wt%). Yet, sluggish kinetics with high desorption temperature (~ 400 °C) hindered its practical applications. Herein, a highly efficient catalyst of nanoNi@g-C 3 N 4 , comprised of transition metal nanocatalyst and carbon-based nonmetal material, was designed and fabricated to dramatically reduce its initial hydrogen desorption temperature to as low as ~105 °C, and eliminate induction period between the two dehydrogenation steps of 2LiBH 4 -MgH 2 by reducing the activation energy for the dehydrogenation of LiBH 4 from 200±6 to 126±7 kJ/mol. Multiple postmortem analyses revealed that the in situ formed MgNi 3 B 2 NPs and the H + defects on g-C 3 N 4 play the key role in synergically enhancing the hydrogen reversible desorption/absorption kinetics at low temperature: 1) in situ formed MgNi 3 B 2 acts as nucleation center of MgB 2 and leads to an excellent catalytic effect to accelerate the dehydrogenation kinetics of 2LiBH 4 -MgH 2 ; 2) the H + defects on g-C 3 N 4 , will interact with the H – in LiBH 4 to trigger the release of H 2 at low temperature and destabilize LiBH 4 and MgH 2 to form Li 3 N and Mg 3 N 2 respectively for the high electronegativity of N: 3) these in situ formed intermediates of Li 3 N and Mg 3 N 2 will be readily rehydrogenated as highly reversible Mg(NH 2 ) 2 and LiH. This novel transition metal and g-C 3 N 4 catalytic composites could provide alternative insights into designing nanosized catalytic hydrogen storage system with low desorption temperature and high capacity for hydrogen-fueled applications.

研究领域: 材料科学 · 能源化学
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JOURNAL OF MOLECULAR LIQUIDS · 2024 · IF 5.3

Research on the effect of DES properties on the preparation of h-BN nanosheets by electrochemical-liquid phase exfoliation method

Qihui Ding,Qian Shan,Qi Zhang,Mengda Chen,Ding Cai,Wei Wu

Hexagonal boron nitride (h-BN) with a large specific surface area and unique optoelectronic properties has good application prospects in many fields. The liquid phase exfoliation method is considered the most promising method for achieving controllable preparation of boron nitride nanosheets (BNNSs), but the low-cost, relatively environmentally friendly and efficient liquid phase exfoliation is still difficult to achieve. Choosing a suitable solvent system is the key to achieving efficient exfoliation. Deep eutectic solvents (DESs) have the advantages of simple synthesis, low cost, high thermal and chemical stability and strong biocompatibility and are expected to be green solvents for preparation of BNNSs . In this paper, it was found that the properties of DESs and its interaction with h-BN had a significant impact on the electrochemical exfoliation of h-BN. The intercalation effect of DES and the compatibility between DES and h-BN were the main factors affecting the yield, while the quality of BNNSs mainly depended on the decomposition and expansion effect of DES. This rule also can be applied to prepare highly conductive and hydrophilic two-dimensional material Ti-MXene. This research explores the structure–activity relationship between two-dimensional materials and DESs, and provides a theoretical basis for the environmentally friendly and efficient preparation of two-dimensional materials using DESs as exfoliation solvents.

CAS / MDL: 57-13-6
研究领域: 材料科学 · 化学工程 · 纳米技术
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RSC Advances · 2019 ·Vol. 9 ·期 25 ·14286-14295 · IF 3.049

Enhanced charge separation and increased oxygen vacancies of h-BN/OV-BiOCl for improved visible-light photocatalytic performance

Wenhui He,Yawen Wang,Caimei Fan,Yunfang Wang,Xiaochao Zhang,Jianxin Liu,Rui Li

The introduction of oxygen vacancies (OVs) on the surface of photocatalysts has already been proven to be an effective way to extend the light response to visible light and trap charge carriers, thereby promoting the photocatalytic performance. In this study, h-BN/OV-BiOCl composites were prepared using hexagonal boron nitride (h-BN) to further improve the visible-light photocatalytic activity of oxygen-vacancy-enriched bismuth oxychloride (OV-BiOCl). The composition and morphology of these materials were investigated, and the photocatalytic performance experiments showed that the introduction of h-BN could significantly improve the visible-light photocatalytic activity of OV-BiOCl, which was 1.7 and 1.4 times that of pure OV-BiOCl for the degradation of rhodamine B (RhB) and bisphenol A (BPA) when the h-BN content was 5 wt%, respectively. The role of h-BN was comprehensively investigated, and the results revealed that the presence of negatively charged h-BN could improve the separation efficiency of photoinduced electrons (e−) and holes (h+) by promoting the migration of positively charged h+ to the surface of the photocatalyst, as expected. Moreover, the oxygen vacancies in OV-BiOCl were increased in the presence of h-BN; this favored the activation of more adsorbed O2 for the oxidation of pollutants. Finally, a probable mechanism was proposed for the improved photocatalytic activity of the h-BN/OV-BiOCl composites. This study provides an insight into the roles of h-BN in oxygen-vacancy-enriched photocatalysts.

研究领域: 材料科学 · 环境科学
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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
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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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JOURNAL OF CATALYSIS · 2019 · IF 7.723

Visible-light-driven selective oxidation of glucose in water with H-ZSM-5 zeolite supported biomimetic photocatalyst

Rui Chen,Changjun Yang,Quanquan Zhang,Bingguang Zhang,Kejian Deng

A new iron tetra(2,3-bis(butylthio)maleonitrile)porphyrazine (FePz(SBu) 8 ) has been synthesized, then it was loaded on H-ZSM-5 zeolite to obtain a supported biomimetic photocatalyst H-ZSM-5/FePz(SBu) 8 . Using H 2 O 2 as oxidant, the photocatalytic selective oxidation of glucose in water under visible light (λ ≥ 420 nm) irradiation was carried out in presence of H-ZSM-5/FePz(SBu) 8 . Under such conditions, the glucose can be efficiently converted into value-added chemicals such as glucaric acid, gluconic acid, arabinose, glycerol and formic acid . More importantly, in comparison with pure FePz(SBu) 8 and pure H-ZSM-5 zeolite, the H-ZSM-5/FePz(SBu) 8 exhibited a higher photocatalytic activity for glucose oxidation and the formation of glucaric acid was observed only when H-ZSM-5/FePz(SBu) 8 was used, deriving from the synergistic effect between FePz(SBu) 8 and H-ZSM-5 zeolite. Some reaction parameters of glucose oxidation catalyzed by the H-ZSM-5/FePz(SBu) 8 were discussed, such as loading amount of FePz(SBu) 8 , H 2 O 2 :glucose ratio, glucose concentration, and so on. It was demonstrated that the Soret-band of FePz(SBu) 8 contributed more to the visible light photocatalytic activity than the Q-band during the photocatalytic process. The stability of H-ZSM-5/FePz(SBu) 8 during the photocatalytic process was further evaluated by the reusability test. In addition, the generation of reactive oxygen species was determined by electron spin resonance (ESR) technology and scavenger experiments. A possible reaction pathway of glucose oxidation was also discussed.

研究领域: 化学工程 · 环境科学
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JOURNAL OF ENZYME INHIBITION AND MEDICINAL CHEMISTRY · 2025 · IF 5.4

Discovery of conformation constrained tetracyclic compounds as potent chitinase OfChi-h inhibitors with a novel binding mode

Pengtao Yuan,Xi Jiang,Xintong Ni,Xusheng Shao,Xuhong Qian,Qing Yang

Chitinase h (Chi-h) has been identified as a promising pesticide target due to its exclusive distribution in lepidopteran insects and its essential role in the moulting processes. In this study, we leverage OfChi-h from destructive agricultural pest Ostrinia furnacalis (Asian corn borer) as a model target to identify novel chitinase inhibitors. A conformational restriction approach was employed to design a series of novel OfChi-h inhibitors. Among these, compound 6a showed the highest inhibitory activity against OfChi-h, with a Ki value of 58 nM. Molecular docking analysis suggested that 6a tightly bound to three subsites (-3 to −1) of OfChi-h. The binding mode is further confirmed by the co-crystallization data of 6a with the SmChiA, a bacterial homologue of OfChi-h, at a resolution of 1.8 Å. This research presents a novel approach for the development of highly potent insect chitinase inhibitors, offering potential tools for effective pest control.

CAS / MDL: 4637-24-5
研究领域: 农药研究 · 酶抑制 · 结构生物学 · 农业化学 · 昆虫生物化学
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ACS Sustainable Chemistry & Engineering · 2022 · IF 9.224

Nano-H-ZSM-5 with Short b-Axis Channels as a Highly Efficient Catalyst for the Synthesis of Ethyl Levulinate from Furfuryl Alcohol

Yafei Li,Shiqing Wang,Shunxin Fan,Babar Ali,Xiaocheng Lan,Tiefeng Wang

For the ethanolysis of biomass-derived furfuryl alcohol (FA) to value-added ethyl levulinate (EL), the development of an efficient solid acid catalyst is very important for industrial application with high FA concentration. Herein, a H-ZSM-5 catalyst with nano b-axis channels (NB-H-ZSM-5) was synthesized and used for the conversion of FA. Detailed catalyst characterization proved that the NB-H-ZSM-5 catalysts (Si/Al = 25∼125) with ∼70 nm b-axis channels were successfully prepared. The NB-H-ZSM-5 catalyst with Si/Al = 75 showed the highest activity. Its structural characteristics allowed for fast diffusion of reactants and products and full utilization of active sites, which endowed it with higher activity compared to commercial H-ZSM-5 (C-H-ZSM-5). Its moderate acidity effectively inhibited the polymerization of FA even at a high FA concentration of 20 wt %. The spent catalyst was easily regenerated by coke burn-off to give a good recyclability. Furthermore, based on the proposed reaction network, a method of physically mixing the NB-H-ZSM-5 (75) catalyst with a small amount of Amberlyst-15 was proposed to further increase the EL yield from 64.7 to 82.1% at an FA concentration of 6 wt %.

研究领域: 催化化学 · 可再生资源化学 · 材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Mixed matrix composite membranes comprising nanocage-like hollow ZIF-71(h) polyhedral nanocrystals in poly(ether-block-amide) membranes for phenol/water separation

Zhongming Zhang,Enfang Gou,Zhiying Zhao,Rui Wu,Rui Fang,Weipeng Guo,Jie Yao

Organophilic pervaporation (PV) mixed matrix membranes (MMMs) have enormous potential for organic wastewater treatment due to their environmental friendliness and high efficiency. However, developing a high-flux PV membrane remains challenging. In this work, the nanocage-like hollow ZIF-71(h) (HZIF-71(h)) polyhedral nanocrystals were synthesized by heteroepitaxial growth of a ZIF-71(h) shell and successive excavation of a ZIF-67 core. The resultant HZIF-71(h) nanocrystals were blended with poly (ether block amide) (PEBA) matrix to fabricate MMMs for phenol/water separation. Results from several characterization techniques confirmed the successful preparation and formation mechanism of HZIF-71(h). Further, a series of experiments were conducted using the composite membranes to explore the impact of filler type, filler loading, operating temperature, and feed concentration on the separation performance. The incorporation of ZIFs facilitated phenol permeation while limited water transport, thereby resulting in increased separation factor. Notably, the HZIF-71(h)/PEBA-21 MMM exhibits a higher phenol flux in comparison to ZIF-71/PEBA-21 and ZIF-67/PEBA-21 MMMs, indicating the importance of the low-resistance hollow structure. The HZIF-71(h)/PEBA-21 MMM exhibits outstanding pervaporation performance with a separation factor of 15.86 and a phenol flux of 17.32 g·m −2 ·h −1 , respectively, displaying an improvement of 41.2 % and 6.4 % compared to the PEBA/PVDF membrane. Furthermore, this composite membrane demonstrated outstanding durability during continuous testing for 84 h, implying a promising potential for phenol separation.

研究领域: 材料科学 · 环境工程
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