CHINESE JOURNAL OF CHEMISTRY
·
2022
·Vol. 41
·期 3
·307-313
·
IF 5.56
Run-Ze Yuan,Peng-Fei Cui,Yue-Jian Lin,Guo-Xin Jin
Comprehensive Summary Herein, we describe the synthesis of a carborane-supported octanuclear palladacycle complex, Pd 8 ( o -C 2 B 10 H 10 CS 2 CH 3 ) 4 Cl 4 (CH 3 CN) 4 (complex 1 ), with B(3)–H activations on o -carborane ligand. The substitution reaction of 1 has been explored, and three of its substituted complexes Pd 8 ( o -C 2 B 10 H 10 CS 2 CH 3 ) 4 Cl 4 (L) 4 (L = t BuNC, 2 ; L = C 5 H 5 N, 3 ; L = C 4 H 8 S, 4 ) have been synthesized. The m - and p -carborane disubstituted ligands m - and p -C 2 B 10 H 10 (CS 2 CH 3 ) 2 (ligands 5 and 6 ) as well as their B—H activated carborane complexes [ m -C 2 B 10 H 9 (CS 2 CH 3 ) 2 PdCl] ( 7 ) and [ p -C 2 B 10 H 8 (CS 2 CH 3 ) 2 ][PdCl( t BuNC)] 2 ( 8 ) have also been synthesized by the similar method. All of these complexes have been characterized, including X-ray single crystal diffraction, NMR spectroscopy, IR spectroscopy and elemental analysis methods.
研究领域:
无机化学
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材料科学
✓ 已验证
DOI
高影响因子
ChemistrySelect
·
2024
·Vol. 9
·期 28
·e202402061
·
IF 1.9
Jiankang Ou,Haoyu Liu,Zeguo Fang,Qian Zhang,Dong Li
Graphical Construction of C−C bonds of alkyl-substituted naphthoquinones through C−H/C−H cross dehydrogenation coupling of naphthoquinones with acetone and 1,3-dicarbonyl compounds was developed. A direct C−H alkylation of naphthoquinones with acetone and 1,3-dicarbonyl compounds was developed to construct C−C bonds of alkyl-substituted naphthoquinone derivatives. It proceeded through an oxidative radical cross dehydrogenation coupling process under simple and mild conditions. This method provides a facile and efficient route for synthesis of functionalized naphthoquinones from readily available feedstocks.
研究领域:
有机化学
·
合成化学
✓ 已验证
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2020
·Vol. 55
·期 35
·16455-16469
·
IF 3.553
Zhang Zengqi,Wang Qiang,Zhang Mingzhong,Huang Zongxian,Zhuang Shiyu
The filler effect is the most important physical mechanism of mineral admixtures in the early hydration of cement whose chemical properties greatly affect the precipitation of C–S–H. In this study, calcite, strontianite, magnesite, dolomite, quartz, whewellite and whitlockite were selected as the fillers. The morphology and reaction kinetics of synthetic C–S–H precipitated on the surfaces of different fillers were studied via electron microscopy observations and electrical conductivity and ion concentration measurements. The precipitation rate of C–S–H has a positive correlation with the affinity of Ca 2+ for adsorption on the fillers, which can be explained by the nucleation barrier of C–S–H. Extremely ordered honeycomb-like morphology of the C–S–H is found on calcite and strontianite surfaces, while less regular leaf-like or honeycomb-like C–S–H is found on whewellite and whitlockite. The ordered C–S–H pattern is related to the lattice cleavage of the ionic compound filler. In the case of quartz, C–S–H prefers growth along the tangential direction, which is quite different from the normal-direction growth on ionic compounds. The in-plane growth of C–S–H on quartz is believed to be induced by a layer of loosely physically adsorbed Ca 2+ .
研究领域:
材料科学
·
水泥化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2025
·
IF 13.1
Yu-Yang Liu,Shan Xu,Xiao-Xin Li,Run-Han Li,Xin-Ting Cai,Hui-Zhen Zhong,Jiang Liu,Qing Huang,Lei Zhang,Shun-Li Li,Ya-Qian Lan
Developing strategies and photocatalysts for C(sp3)-H bond functionalization under simple and mild conditions is important but challenging. Here, we report two redox heterocluster-based frameworks, named Ni5-PW12 and Ni5-V16, in which the terminal oxygen atoms of polyoxometalates are directly coordinated to metal atoms in metal–organic clusters. Due to the coexisting strong oxidation and reduction capacities, both of these photocatalysts achieve photocatalytic C(sp3)-H bond oxidative imination through combining oxidation of methyl aromatics and reduction of nitro aromatics reactions. The experimental and theoretical results reveal that benefiting from the short distance between the clusters, the rapid charge transfer and mass transfer processes would enhance the photocatalytic reactivity and inhibit side reactions. More importantly, all of the photocatalytic reactions are carried out in mild conditions at room temperature without any additional solvents, photosensitizers, oxidizing or reducing agents, or cocatalysts.
研究领域:
光催化
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有机合成
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材料化学
·
簇化学
✓ 已验证
产品关联
DOI
高影响因子
Catalysts
·
2024
·Vol. 14
·期 4
·248
·
IF 3.8
Xinyi Xing,Wanni Liu,Siquan Xu,Jianxiu Hao
H-Beta zeolite is a solid acid catalyst commonly utilized in the catalytic conversion of biomass resources. In this study, H-Beta zeolite was calcined at different temperatures (350, 550, 750, and 1000 °C) to explore the effects of high temperature-induced dealumination on its physicochemical properties and its catalytic ability to convert glucose into 5-hydroxymethylfurfural (HMF). It was shown that as the calcination temperature increased, the Si-O-Al bond of H-Beta zeolite was broken and its dealumination effect was enhanced. Dealumination led to the collapse of the framework of H-Beta zeolite and a reduction in the number of acid sites, which in turn reduced its catalytic performance and the efficiency of HMF formation from glucose. Furthermore, H-Beta zeolite exhibited an extraordinary catalytic ability for the production of HMF from carbohydrates. Using glucose and cellulose as substrates, superior HMF yields of 91% and 46%, respectively, were achieved under optimal reaction conditions. Further, calcination removes carbon deposits in the recovered H-Beta zeolite, but it affects the cycling stability of the catalyst. Meanwhile, the by-products formed during the synthesis of HMF from glucose catalyzed by H-Beta zeolite catalyst were also clearly detected.
研究领域:
催化化学
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生物质转化
✓ 已验证
产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2022
·Vol. 12
·期 20
·6268-6284
·
IF 6.177
Tingyu Liang,Jialing Chen,Sen Wang,Pengfei Wang,Zhangfeng Qin,Fang Jin,Mei Dong,Jianguo Wang,Weibin Fan
A series of H-MCM-22 zeolites with different Si/Al ratios (H-M22-x, x = 15–90) were hydrothermally synthesized by boron incorporation to investigate the influences of acid density on the methanol-to-hydrocarbon (MTH) performances and deactivation behaviors. The acid density of H-M22-x zeolites is nearly proportional to their aluminum contents; the residual boron barely affects the overall acidity of H-M22-x zeolites. 27Al and 29Si MAS NMR experiments support the existence of competitive occupancy of various framework T sites among boron, aluminum and silicon during zeolite synthesis, which leads to different distribution of Brønsted acid sites/framework aluminum among three types of pores in H-MCM-22 zeolites. Increasing the Si/Al ratio of H-M22-x zeolites leads to a gradual increase in the proportion of Brønsted acid sites in supercages while those in sinusoidal channels decrease. However, the acid density has a significantly larger impact than acid distribution on the MTH performances of H-M22-x zeolites. Increasing the acid density can accelerate the hydrogen transfer reactions in the MTH conversion and promote the formation of aromatics, ethene, and alkanes. The deactivation of H-M22-x zeolites with low acid density (x = 50–90) is mainly ascribed to coke covering the acid sites inside the micropores and partly blocking the pore mouths. Nevertheless, the deactivation of H-M22-x zeolites with high acid density (x = 15–30) is mainly caused by massive coke deposition on the external surface which blocks the pore mouths of inner micropores. The coke on the external surface exhibits a lower decomposition temperature than that inside the micropores. The deactivation behaviors of H-M22-x zeolites for the MTH reaction can be divided into three stages. Firstly, rapid deactivation of supercages occurred for all the H-M22-x zeolites in spite of their different acid densities, suggesting a much stronger influence of pore structure than acidity on the initial deactivation behaviors of H-M22-x zeolites. Secondly, the acid sites in sinusoidal channels of H-M22-x zeolites are highly resistant to coke formation, which dominates the MTH reaction in the second stage. Finally, with the continuous formation of coke in the surface pockets, which gradually covers the acid sites and pore mouths of sinusoidal channels, complete deactivation of H-M22-x zeolites can be observed. GC-MS and UV-vis analysis of partly or completely deactivated H-M22-x zeolites reveals that the retained species in H-M22-x zeolites gradually condense into bulky hydrocarbon species through successive hydrogen transfer reactions and form methylbenzenes, naphthalene, polymethylnaphthalenes, phenalenone, pyrenes and eventually graphite-like carbonaceous species.
研究领域:
催化化学
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材料科学
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能源化学
✓ 已验证
产品关联
DOI
高影响因子
PLoS One
·
2024
·Vol. 19
·期 8
·e0306043
·
IF 2.9
Yuping Liao,Feng Zhang,Fang Yang,Shijin Huang,Sha Su,Xuemei Tan,Linlin Zhong,Lingjie Deng,Lihong Pang
Background
Haemoglobin H (HbH) disease is caused by a disorder of α-globin synthesis, and it results in a wide range of clinical symptoms. M 6 A methylation modification may be one of the mechanisms of heterogeneity. Therefore, this article explored the role of methyltransferase like 16 (METTL16) in HbH disease.
Method
The results of epigenetic transcriptome microarray were analysed and verified through bioinformatic methods and qRT-PCR, respectively. The overexpression or knock down of METTL16 in K562 cells was examined to determine its role in reactive oxygen species (ROS), cell cycle processes or iron overload. YTH domain family protein 3 (YTHDF3) was knocked down in K562 cells and K562 cells overexpressing METTL16 via siRNA to investigate its function. In addition, haemoglobin expression was detected through benzidine staining. qRT-PCR, WB, methylated RNA Immunoprecipitation (MeRIP) and (RNA Immunoprecipitation) RIP experiments were conducted to explore the mechanism of intermolecular interaction.
Results
METTL16, YTHDF3 and solute carrier family 5 member 3 (SLC5A3) mRNA and the methylation level of SLC5A3 mRNA were downregulated in HbH patients. Insulin-like growth factor 2 mRNA-binding protein 3 (IGF2BP3) mRNA expression was negatively correlated with HGB content among patients with HbH-CS disease. Overexpression of METTL16 increased ROS and intracellular iron contents in K562 cells, changed the K562 cell cycle, reduced hemin-induced haemoglobin synthesis, increased the expressions of SLC5A3 and HBG and increased SLC5A3 mRNA methylation levels. Knockdown of METTL16 reduced ROS and intracellular iron contents in K562 cells. Hemin treatment of K562 cells for more than 14 days reduced the protein expressions of METTL16 and SLC5A3 and SLC5A3 mRNA methylation levels. Knockdown of YTHDF3 rescued the intracellular iron content changes induced by the overexpression of METTL16. The RIP experiment revealed that SLC5A3 mRNA can be enriched by METTL16 antibody.
Conclusion
METTL16 may affect the expression of SLC5A3 by changing its m 6 A modification level and regulating ROS synthesis, intracellular iron and cycle of red blood cells. Moreover, METTL16 possibly affects the expression of haemoglobin through IGF2BP3, which regulates the clinical phenotype of HbH disease.
研究领域:
分子生物学
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血液学
·
表观遗传学
·
细胞生物学
✓ 已验证
DOI
PubMed
高影响因子
Materials
·
2021
·Vol. 14
·期 11
·2741
·
IF 3.623
Pengcheng Lv,Ruihong Meng,Zhongyang Mao,Min Deng
In this study, the hydrated sodium aluminosilicate material was synthesized by one-step hydrothermal alkaline desilication using fly ash (FA) as raw material. The synthesized materials were characterized by XRD, XRF, FT-IR and SEM. The characterization results showed that the alkali-soluble desilication successfully had synthesized the sodium aluminosilicate crystalline (N-A-S-H) phase of sodalite-type (SOD), and the modified material had good ionic affinity and adsorption capacity. In order to figure out the suitability of SOD as an adsorbent for the removal of ammonium and phosphorus from wastewater, the effects of material dosing, contact time, ambient pH and initial solute concentration on the simultaneous removal of ammonium and phosphorus are investigated by intermittent adsorption tests. Under the optimal adsorption conditions, the removal rate of ammonium was 73.3%, the removal rate of phosphate was 85.8% and the unit adsorption capacity reached 9.15 mg/L and 2.14 mg/L, respectively. Adsorption kinetic studies showed that the adsorption of ammonium and phosphorus by SOD was consistent with a quasi-secondary kinetic model. The adsorption isotherm analysis showed that the equilibrium data were in good agreement with the Langmuir and Freundlich model. According to thermodynamic calculations, the adsorption of ammonium and phosphorus was found to be a heat-absorbing and spontaneous process. Therefore, the preparation of SOD by modified FA has good adsorption properties as adsorbent and has excellent potential for application in the removal of contaminants from wastewater.Keywords:N-A-S-H;sodalite;simultaneous removal;ammonium;phosphorus
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CEMENT & CONCRETE COMPOSITES
·
2023
·
IF 10.5
Zhongtao Luo,Tianyi Zhi,Xiaohai Liu,Kunpeng Yin,Han Pan,Hu Feng,Yatao Song,Yanfeng Su
The early hydration of UHPC can be retarded by the low water/binder ratio, the high polycarboxylate superplasticizers dosage, and the large supplementary cementitious materials (SCM) content. In this study, the effects of the prepared nanoscale C–S–H seeds and nano-silica (NS) on the early performance of UHPC were compared. The mechanism of nanomaterials influencing the early hydration of UHPC was further characterized by calorimetry , thermal analysis, nuclear magnetic resonance (NMR), and mercury intrusion porosimetry . The results showed that the 1-day compressive strength of UHPC samples with 0.3 wt% C–S–H seeds and NS increased by 457% and 25% respectively compared to the control sample. Compared to NS, C–S–H seeds were more effective in accelerating the early (before 3 d) hydration to produce hydrates and refine the pore structure of UHPC. The NMR results further implied that compared with the NS, the C–S–H seeds was 12% and 343% more efficient in accelerating the early hydration of cement and SCMs, respectively. However, the performance enhancement of nanomaterials was effective at 1 d and had little effect thereafter.
研究领域:
土木工程
·
材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF ORGANIC CHEMISTRY
·
2023
·
IF 3.6
Huanhuan Song,Jingwen Li,Yinbin Zhang,Ke Chen,Le Liu,Junjie Zhang,Xin-Hua Duan,Mingyou Hu
Difluoromethylated heterocyclic compounds have found broad applications in numerous bioactive molecules. Herein, we report photoredox catalysis-induced direct C–H difluoromethylation of heterocycles by using bis(difluoromethyl) pentacoordinate phosphorane (PPh3(CF2H)2, 1) as the reagent. A variety of heterocycles, such as quinoxalin-2(1H)-one, thiophene, indole, and coumarin, are readily tailored with a difluoromethyl group. The method is featured as transition-metal-free by using an organic compound Erythrosin B as the catalyst and O2 as the oxidant.
研究领域:
有机化学
·
药物化学
✓ 已验证
DOI
PubMed
高影响因子
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2020
·
IF 3.232
Chenxiao Yan,Qingqing Zhang,Heng Gao,Xiong Zheng,Tong Yang,Guoxiang Zheng,Xiaoshun Zhou,Yong Shao
DNA templated dye assemblies pave an easy way to regulate the optical properties of molecular aggregates. G-quadruplexes (G4s) provide versatile DNA platforms for the dye assemblies since their foldings can be easily tuned by cation ions and sequences. In this work, we found that the G4 handedness can be used to control the aggregate chirality of a dye of 3,3′-diethylthiacarbocyanine (DiSC 2 (3)). The left-handed and right-handed G4s can template the concurrent formation of the J- and H-aggregates of DiSC 2 (3) with emergence of the featured absorption spectra. However, the chiral J-aggregate of DiSC 2 (3) can be formed only on the left-handed G4s, while the chiral H-aggregate is otherwise grown only on the right-handed G4s, as confirmed by the induced circular dichroism (ICD) spectra with the characteristic splitting bands. Additionally, these G4s even at tens of nM level are efficient to produce these chiral aggregates, demonstrating the high sensitivity of G4s in creating these optically active dye assemblies. The possible growth sites of the aggregates are proposed by the sequence length-dependent assemblies. Our work will provide a new way to control the chiral assemblies of dye aggregates via the G4 handedness.
研究领域:
化学
·
材料科学
·
生物物理
·
纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ChemistrySelect
·
2025
·Vol. 10
·期 7
·e202405464
·
IF 2
Kun Jia,Peng Jia
Graphical The asymmetric activation of anhydrous methanol molecules is realized by exogenous protons, the position and protonation position of asymmetric activation are determined, and the C─H bonding energy and reaction activation energy of some methanol molecules are reduced, and the asymmetric regulation of the non-oxidation dehydrogenation reaction process of anhydrous methanol molecules was realized. The activation of C─H bonds under mild conditions is a crucial step in the conversion of organic molecules. However, the simultaneous activation of C─H bonds in methanol can result in excessive oxidation, thereby diminishing the selectivity for formaldehyde production. We achieved selective activation of the C─H bonds in methanol under mild conditions by adjusting the proton concentration in an anhydrous methanol solution, which significantly enhanced the dehydrogenation rate of methanol. Additionally, we constructed related molecular models to identify the sites of asymmetric oxidation, providing new insights for further studies on C─H bond activation.
研究领域:
化学
·
催化反应
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）