Materials Today Chemistry
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2022
·
IF 7.613
W. Sun,B. Shi,Z. Xia,C. Lü
Organic room-temperature phosphorescence (RTP) materials are very attractive, but there is still a challenge to achieve RTP for their practical applications under visible light excitation (λ > 400 nm) because of the implement for the most organic RTP is under ultraviolet light. Herein, a simple tactics for inhibiting the vibrational dissipation of three amorphous phenanthroline derivatives by doping them into polyvinyl alcohol (PVA) matrix was utilized to afford visible-light excitation RTP. By using this method, on account of the mutual H-bonding and confinement effect with PVA matrix, a series of organic RTP materials with blue-green phosphorescence emission were obtained under visible-light excitation. The afterglow colors of RTP materials can be adjusted by co-doping the available fluorescence dyes (RhB or Rh6G) into the PVA films through a triplet-to-singlet Förster resonance energy transfer. However, the H-bonding is easily broken by water molecules resulting in the RTP phenomenon disappears. Hence, Aphen-epoxy resin composite system was constructed to overcome this drawback. It is shown that the composite still has good phosphorescence properties after soaking in water for 7 days. The superior RTP of the amorphous phenanthroline derivatives in processable polymer matrices endows these materials with a highly potential for the night warning clothing coating and information encryption.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Kunyu Chen,Zhanguo Cui,Zhiqiang Zhang,Heliang Pang,Jing Yang,Xiaojiang Huang,Jinsuo Lu
The present study developed a prolonged oxidizable sulfur(IV)/ferrate(VI) system for the generation of hydroxyl radical ( OH) and sulfate radical (SO 4 − ) within 120 min, and proposed a reaction mechanism. In the presence of H + in solution, the S(IV)/Fe(IV) system provided excellent oxidation performance of refractory organics O,O-dimethyl-S-methylcarbamoyl methyl phosphorothioate (dimethoate, a widely used organophosphorus pesticide) within 120 min. The degradation efficiency of dimethoate in the bisulfite/Fe(VI) system (e.g., 90.06% dimethoate) was higher than that in the sulfite/Fe(VI) system (e.g., 51.03% dimethoate), while Fe(VI) alone degraded 27.81% of dimethoate. In the S(IV)/Fe(VI) system, the active species consisted of Fe(VI) (including the highly-reactive iron-based intermediate species, i.e. Fe(V) and Fe(IV)), OH and SO 4 − , with OH being identified as the main active species, contributing more than half of the total. The degradation mechanism of dimethoate in the S(IV)/Fe(VI) system mainly included the cleavage of the S-P bond, C-S bond and the oxidation of the P = S bond. Two plausible degradation pathways were proposed based on the detected transformation products. Dimethoate could be efficiently degraded when the [bisulfite]/[Fe(VI)] molar ratio was 4:1 with a low Fe(VI) dosage (218 µM), the changes in HA and HCO 3 − concentrations affected the transformation of dimethoate, the presence of Cl − , SO 4 2− and NO 3 − had a negligible effect, and the S(IV)/Fe(VI) system performed well in real waters. The S(IV)/Fe(VI) system has excellent oxidation performance for the removal of organic pollutants in water, with a final pH (pH = 6.6) close to neutral and ultimate products of SO 4 2− and Fe(OH) 3 , which has great potential for engineering applications.
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Reaction Chemistry & Engineering
·
2021
·Vol. 6
·期 10
·1900-1910
·
IF 4.239
Udayakumar Veerabagu,Gowsika Jaikumar,Fushen Lu,Franck Quero
Copper iodide (CuI) nanoparticles/boron nitride nanosheets (BNNSs) were prepared via an ultrasonication method and subsequently characterized. For the first time, these newly synthesized CuI/BNNS supports were used as heterogeneous catalysts for C–H difluoromethylation reactions, including the synthesis of heteroarenes and terminal alkynes. The versatility of the catalyst was demonstrated for the synthesis of diverse substituted difluoromethylated heteroarenes and terminal alkynes from electron-deficient and electron-rich groups, resulting in moderate to high yields (up to 91%). The reaction was carried out in a greener medium (cyrene instead of dimethylformamide and N-methyl-2-pyrrolidone) at room temperature using (difluoromethyl)trimethylsilane and 9,10-phenanthraquinone in the presence of the CuI/BNNS catalyst containing ∼3 wt% Cu and I. Notably, its activity was found to provide higher yield, shorter reaction time, and fewer usage of the catalyst, compared with commercial CuI catalysts. In addition, the CuI/BNNS catalyst could be easily recovered and recycled up to five times, with only a slight decrease (3%) in its catalytic activity, providing attractive features for chemical engineers to use this catalyst for the large-industrial scale synthesis of organic bioactive compounds involving C–H difluoromethylation reactions.
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Frontiers in Neurology
·
2019
·
IF 2.635
Zhang Jie,Jiang Yunyao,Liu Nan,Shen Ting,Jung Hyo Won,Liu Jianxun,Yan Bing Chun
Senkyunolide-H (SEH), a major bioactive compound extracted from Ligusticum chuanxiong, has been reported to be effective in preventing cerebral ischemic stroke (CIS). In this study, we employed network pharmacology to reveal potential mechanism of SEH against CIS on a system level and confirmed the therapeutic effects of SEH on CIS by models of cerebral ischemia-reperfusion in vivo and in vitro. Through protein-protein interaction networks construction of SEH- and CIS-related targets, a total of 62 key targets were obtained by screening topological indices and analyzed for Gene Ontology and Kyoto Encyclopedia of Genes and Genomes pathway enrichment. Gene Ontology analysis indicated that SEH might have a role in treating CIS via regulating some biological processes including regulation of transcription from RNA polymerase II promoter, epidermal growth factor receptor signaling pathway, phosphatidylinositol-mediated signaling, and some molecular function, such as transcription factor and protein phosphatase binding and nitric oxide synthase regulator activity. Meanwhile, the Kyoto Encyclopedia of Genes and Genomes analysis showed that phosphoinositide 3-kinase (PI3K)/protein kinase B (Akt) signaling pathway was significantly enriched. In addition, our result showed that SEH posttreatment significantly decreased the neurological scores, infarct volume, and neuronal death in the middle cerebral artery occlusion mice. Moreover, the PI3K/Akt/nuclear factor kappa B signaling pathway was activated by intragastric administration of 40 mg/kg SEH, as verified by Western blot. In vitro, treatment of PC12 cells with 100 μM SEH markedly reduced cell death induced by oxygen-glucose deprivation through the activation of PI3K/Akt/nuclear factor kappa B pathway, and the therapeutic effect of SEH was obviously inhibited by 10 μM LY294002. In summary, these results suggested that SEH carries a therapeutic potential in CIS involving multiple targets and pathways, and the most crucial mechanism might be through the activation of PI3K/Akt/nuclear factor kappa B (NF-κB) signaling pathway to inhibit inflammatory factor releases and increase the antiapoptosis capacity. Our study furnishes the future traditional Chinese medicine research with a network pharmacology framework.
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Surfaces and Interfaces
·
2023
·
IF 6.2
Xiangyue Wei,Yixin Pan,Jisheng Kou,Rui Huang
The removal of selenium (IV) from aqueous solutions was the focus of research that led to the discovery of a novel type of composite adsorbent called FeS@h-BN nanocomposite . This adsorbent was studied, characterized, and put to use in a fixed bed column. SEM, FTIR, XRD, and XPS analyses were conducted to learn more about the coated layer's surface properties. The effect of several adsorbent materials on the remediation of Se(IV) in dynamic water was examined. The Adams-Bohart model, the Thomas model, and the Yoon-Nelson model were all utilized to get optimal fits to the kinetic data obtained from the adsorption process. Moreover, the Adams-Bohart model was only applicable to the beginning portion of the dynamic behavior of the FeS and FeS@h-BN columns. The Thomas and Yoon-Nelson models were sufficient for describing the breakthrough curve under all experimental conditions. For this dynamic process, the theoretical breakthrough curve profile was compared to an experimentally derived profile. It was discovered that FeS@h-BN nanocomposites are the most effective at removing Se(IV), and the adsorption of Se(IV) by a variety of adsorbent materials is enough for all three dynamic models.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2023
·
IF 5.2
Xinyu Li,Shunyu Han,Jingzhe Xu,Nanzhe Jiang
The synthesis of zeolites from natural aluminosilicate minerals is environmentally sustainable. However, the preparation of nano-ZSM-5 zeolite single crystals via the facile “silica–alumina homologation” of natural clay remains challenging. This paper highlights a novel strategy for the synthesis of defect-free, highly crystalline nano-H-ZSM-5 with a uniform morphology through the kinetically controlled in situ reconstruction of the topology of natural clay within a solid-state-like system. Crystal nucleation and growth were decoupled by aging to control the crystal size. The “homogeneous silica–alumina” property of natural clay was found to be directly inherited by nano-H-ZSM-5 to provide uniformly distributed acidic sites for catalysis. This was demonstrated by methanol-to-propylene conversion, wherein the performance of the obtained crystals was superior to that of commercial ZSM-5. This strategy promotes the development of natural silica–aluminate clay resources and allows the scalable production of high-quality nano-H-ZSM-5 single crystals for heterogeneous catalysis .
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ACS Omega
·
2018
·
IF 0
Tingting Cheng,Jian Chen,Aofei Cai,Jian Wang,Haiyan Liu,Yuandong Hu,Xiaojun Bao,Pei Yuan
A series of silica supported Pd (Pd/SiO2) catalysts were prepared in various HCl concentrations (CHCl) of the impregnation solution with different electrostatic interactions between Pd precursor and support, and their catalytic properties were evaluated by the selective hydrogenation of nitrile butadiene rubber (NBR). The results show that with the CHCl increasing from 0.1 to 5 M, the particle size of Pd nanoparticles dramatically decreases from 24.2 to 5.1 nm and stabilizes at ∼5 nm when CHCl is higher than 2 M. Using the catalysts prepared with a high CHCl (>2 M), an excellent hydrogenation degree (HD) of ∼94% with 100% selectivity to C═C can be acquired under mild conditions. Interestingly, the HD could be remarkably increased from 65 to 92% by increasing only CCl– from 0.1 to 2 M with the addition of NaCl while keeping CH+ at 0.1 M. This is because PdCl42– is the predominant existing form of precursor at high CCl–, which has a strong electrostatic attraction with the positively charged support favorable for the formation of small-sized Pd nanoparticles over silica. Notably, Pd leaching behavior during the hydrogenation reaction is closely related to CH+, and the higher the CH+, the less Pd residues are detected in the hydrogenated NBR. Our contribution is to provide a facile strategy to synthesize effective and stable Pd/SiO2 catalysts via adjusting the electrostatic interaction, which exhibits a high activity and selectivity for NBR hydrogenation.
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PubMed
Chemical Science
·
2019
·Vol. 10
·期 35
·8179-8186
·
IF 9.556
Xiaohong Pan,Yuehui Zhao,Tingting Cheng,Aishan Zheng,Anbin Ge,Lixin Zang,Kehua Xu,Bo Tang
Reductive stress, the opposite of oxidative stress, represents a disorder in the redox balance state which is harmful to biological systems. For decades, the role of oxidative stress in tumor therapy has been the focus of attention, while the effects of reductive stress have been rarely studied. Here, we report the anti-cancer effects of reductive stress induced by three natural antioxidants (resveratrol, curcumin and celastrol). Considering the fact that the solid tumor microenvironment suffers from hypoxia, we performed cell experiments under hypoxic conditions. In order to observe the reductive stress, we first developed an ultrasensitive fluorescent probe (TCF-MQ) for specifically imaging NAD(P)H which is a marker of reductive stress. TCF-MQ responded to NAD(P)H rapidly and exhibited high sensitivity with a detection limit of 6 nM. With the help of TCF-MQ, we found that upon the treatment of HepG2 cells with pharmacological doses of three natural antioxidants under hypoxic conditions, high levels of NAD(P)H were produced before cell death. The excess NAD(P)H resulted in reductive stress instead of oxidative stress. In contrast, under normoxic conditions, there was no reductive stress involved in the process of cell death induced by three natural antioxidants. Therefore, we hypothesize that the mechanism of cancer cell death induced by natural antioxidants under hypoxia should be attributed to the reductive stress.
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INORGANIC CHEMISTRY
·
2025
·
IF 4.7
Qiang-Qiang Ma,Peng Zhou,Yizhen Liu,Zuowei Xie
Transition metal catalyzed selective cage B–H functionalization of carboranes has made significant progress in recent years, giving rise to the efficient synthesis of a large variety of cage B-functionalized carboranes including alkenylation, arylation, alkynylation, borylation, hydroxylation, acyloxylation, amination, and halogenation. However, the mechanisms of these catalytic B–X coupling reactions are not well understood. Herein, we describe the isolation and characterization of the catalytically relevant o-carborane based palladium(II) metallacycle, disclosing the details of Pd-catalyzed B–H functionalization of o-carboranes. As a result, highly selective catalytic B(3,6)-dihalogenation, -dimethylation, and -diarylation of o-carboranes have been achieved.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Tao Shan,Sunzai Ke,Xin Yang,Xuhui Yang,Bo Weng,Lijuan Shen,Min-Quan Yang
Photocatalytic selective oxidation of aromatic hydrocarbons plays an important role in the production of value-added chemicals. A key step in this process is the activation of C(sp 3 )-H bond by photogenerated holes. However, the inadequate hole generation and lack of surface adsorption-activation sites severely hinders the improvement in photocatalytic C-H bond oxidation. In particular, the random charge migration to the surface impedes the effective capture of holes by surface active sites to dissociate the C(sp 3 )-H bond. Here, we design and fabricate a Co 3 O 4 /Cs 3 Sb 2 Br 9 p-n heterojunction that effectively addresses these challenges. The p-n heterojunction forms strong built-in electric fields (BEF) facilitating spatial charge separation. Holes are accumulated on Co 3 O 4 , while electrons are accumulated on Cs 3 Sb 2 Br 9 , thereby offering abundant active holes and electrons. Moreover, Co 3 O 4 shows stronger adsorption and activation capacity for the C(sp³)-H bond, enabling the C(sp 3 )-H bond dissociation with low reaction energy barrier. Consequently, the holes are directionally extracted from photoactive Cs 3 Sb 2 Br 9 to catalytically active Co 3 O 4 under visible light irradiation, thereby accelerating the toluene oxidation. The optimized 5 % Co 3 O 4 /Cs 3 Sb 2 Br 9 exhibits a benzyl aldehyde (BAD) evolution rate of 5044 μmol g −1 h −1 and a benzyl alcohol (BA) production rate of 1820 μmol g −1 h −1 , which are 12 and 17 times higher than that of blank Cs 3 Sb 2 Br 9 , respectively.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Xinqi Luan,Xuehui Jia,Syed Jalil Shah,Jingyu Bao,Shunxiang Qin,Ruimeng Wang,Jiguang Deng,Zhongxing Zhao,Zhenxia Zhao
Low adsorption efficiency and secondary pollution release pose a bottleneck for the efficient capture of radioactive iodine vapor during nuclear utilization via adsorption. In addition, the simultaneous adsorption of iodine vapor alongside other harmful vapors in complex systems has been rarely reported. In this work, an electron/H-donating defective pore construction strategy involving MIL-101 modification via amino acids (AAs) was proposed to enhance its simultaneous adsorption efficiency for iodine and formaldehyde vapors. These defective microenvironments possessed microporous property with 11.3 Å, which not only formed strong affinity for I 2 molecules itself but also enhanced its adsorption interaction towards polyiodide anion (I 3 - and I 5 - ) through electron donation of AAs. Moreover, these adsorbed polyiodide anions and AAs-SL within the MOFs, resulting in multisite capture of FA via NH…O-H…I hydrogen bonding. The results revealed that AAs coordinated MIL-101 exhibited superior removal rate ( k 80% = 0.61–1.15 g g −1 h −1 ) for iodine vapor than that of the original MIL-101, which was 3.6–30.8 times higher that of state-of-the-art adsorbents under similar conditions. Notably, a high-capacity superior retention rate of 94.8 % was achieved for its I 2 adsorption after exposure to air for 7 days. After adsorption of iodine, AAs coordinated MIL-101 retained high FA adsorption capacity up to 9.7–12.9 mg/g, representing 75.1 %–87.7 % of the original AAs@MIL adsorption capacity for FA. This defective engineering strategy in MOFs supplied an efficient method for removing multiple harmful gases from the surrounding nuclear waste atmosphere.
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ENVIRONMENTAL POLLUTION
·
2024
·
IF 7.6
Kuang Wang,Zhanqiang Fang
In the homologous series of polybrominated diphenyl ethers (PBDEs), the debromination of low-brominated diphenyl ethers with higher toxicity remains a challenge. Nano zero-valent iron (nZVI) has been extensively studied for the debromination of PBDEs, but its inherent direct electron transfer mechanism is less efficient for low-brominated diphenyl ethers, and there are issues with high preparation costs. In this work, we synthesize Ni-doped oxalated submicron ZVI (Fe OX bm /Ni) using a low-cost ball-milling method. Fe OX bm /Ni exhibits a debromination rate constant of 0.48 day −1 for 2,2′,4,4′-tetrabromodiphenyl ether (BDE-47) in tetrahydrofuran (THF)/water. The debromination rate of Fe OX bm /Ni for BDE-47 in water is even faster (0.98 day −1 ), with the yield of the complete debromination product, diphenyl ether, reaching 76.71%. In real groundwater, Fe OX bm /Ni also shows high reactivity toward BDE-47, with a rate constant of 0.33 day −1 . Kinetic experiments, quenching experiments, and degradation pathway indicate that the attack of atomic hydrogen on C-Br bonds is the primary degradation mechanism. Electrochemical analysis further show that Ni 0 sites could cleave hydrogen into absorbed atomic hydrogen (H∗ ABS ) and adsorbed atomic hydrogen (H∗ ADS ), with H∗ ADS playing the main role. These findings contribute valuable insights into advancing the large-scale application of ZVI and offer promising strategies for thorough remediation of PBDEs pollution.
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