RSC Advances
·
2017
·Vol. 7
·期 82
·51831-51837
·
IF 3.108
Yunrui Zhang,Haihong Niu,Xiangjie Zhang,Junxiu Pan,Yang Dong,Haijun Wang,Yongjun Gao
A kind of magnetic N-containing carbon material was synthesized by a simple method using sustainable N-acetyl-D-glucosamine (NAG) and iron nitrate as the raw materials. In C–H oxidation reactions such as the epoxidation of stilbene and styrene, and the oxidation of ethylbenzene, the carbon catalyst exhibited excellent catalytic activity and selectivity for the target products. The superparamagnetic properties at room temperature facilitated catalyst recycling and reusability when it was used as a catalyst. The relationship between the catalytic results and the N 1s XPS analysis indicated that the graphitic N species located in the carbon skeleton was the key accelerating factor which promoted the catalytic C–H oxidation. Density functional theory (DFT) calculations further indicated that the iron species were not an essential factor but they acted as promoters for the catalytic performance of the catalyst. This study will expand the application of biomass-based heteroatom-containing compounds.
研究领域:
材料科学
·
催化
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可持续化学
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无机化学
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理论化学
✓ 已验证
产品关联
DOI
高影响因子
Molecular Catalysis
·
2019
·
IF 2.938
Qiaoyun Liu,Fei Liu,Yaru Zhang,Yang Su,Aiqin Wang,Tao Zhang
A highly active and robust catalyst composed of Ru nanoparticles highly dispersed on zeolite H-beta was developed for transforming furfural into 3-acetyl-1-propanol (3-AP) in good yield (81%)under mild conditions (80 °C, 1 MPa H 2 ). Both the support nature and the preparation methods had significant impacts on the dispersion of Ru, eventually on the yield of 3-AP. Ion-exchange method proved best for obtaining the highly active and selective catalyst for this reaction. Moreover, the catalyst can be regenerated easily by calcination and reduction. This catalyst was further explored for the one-pot conversion of xylose and xylan to 3-AP with a yield of 46% and 31%, respectively, thus opening a new feasible pathway from biomass to valuable fine chemicals.
研究领域:
催化化学
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生物质转化
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绿色化学
✓ 已验证
DOI
高影响因子
BMC Chemistry
·
2019
·Vol. 13
·期 1
·1-15
·
IF 0
Guo J.,Ma Yu L.,Yu Jia Y.,Gao Yu J.,Ma Ning X.,Wu Xiao Y.
Herein, 2-(2-methoxyphenoxy)-1-phenylethanol (β- O -4), 2-methoxyphenyl anisole (α- O -4) and 4-phenoxyphenol (4- O -5) were selected as typical lignin model compounds. Given the effectiveness of traditional acid–base catalysts for lignin depolymerisation, a novel Ni/CaO–H-ZSM-5(60) catalyst was prepared to investigate the difficulty level of C–O bond of three model compounds cleavage in ethanol. It was observed that Ni/CaO–H-ZSM-5(60) had prominent performance on the C–O bond cleavage at very mild conditions (140 °C, 1 MPa H 2 ). Among them, the C–O bond of α- O -4 and β- O -4 could be completely cleaved within 60 min. Although the C–O bond of 4- O -5 had high bond energy, 41.2% of conversion was occurred in 60 min. The introduction of CaO could regulate the acidity of H-ZSM-5 to enhance the ability to break C–O bonds. Moreover, the possible pathways of C–O ether bonds in three lignin model compounds cleavage were proposed in order to selectively obtain target products from the raw lignin degradation.
研究领域:
化学工程
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催化科学
✓ 已验证
DOI
Journal of the American Chemical Society
·
2015
·
IF 12.113
Xiao-Li Pei,Yang Yang,Zhen Lei,Shan-Shan Chang,Zong-Jie Guan,Xian-Kai Wan,Ting-Bin Wen,Quan-Ming Wang
The activation of C(sp3)–H bonds is challenging, due to their high bond dissociation energy, low proton acidity, and highly nonpolar character. Herein we report a unique gold(I)–silver(I) oxo cluster protected by hemilabile phosphine ligands [OAu3Ag3(PPhpy2)3](BF4)4 (1), which can activate C(sp3)–H bonds under mild conditions for a broad scope of methyl ketones (RCOCH3, R = methyl, phenyl, 2-methylphenyl, 2-aminophenyl, 2-hydroxylphenyl, 2-pyridyl, 2-thiazolyl, tert-butyl, ethyl, isopropyl). Activation happens via triple deprotonation of the methyl group, leading to formation of heterometallic Au(I)–Ag(I) clusters with formula RCOCAu4Ag4(PPhpy2)4(BF4)5 (PPhpy2 = bis(2-pyridyl)phenylphosphine). Cluster 1 can be generated in situ via the reaction of [OAu3Ag(PPhpy2)3](BF4)2 with 2 equiv of AgBF4. The oxo ion and the metal centers are found to be essential in the cleavage of sp3 C–H bonds of methyl ketones. Interestingly, cluster 1 selectively activates the C–H bonds in −CH3 rather than the N–H bonds in −NH2 or the O–H bond in −OH which is traditionally thought to be more reactive than C–H bonds. Control experiments with butanone, 3-methylbutanone, and cyclopentanone as substrates show that the auration of the C–H bond of the terminal methyl group is preferred over secondary or tertiary sp3 C–H bonds; in other words, the C–H bond activation is influenced by steric effect. This work highlights the powerful reactivity of metal clusters toward C–H activation and sheds new light on gold(I)-mediated catalysis.
研究领域:
无机化学
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有机金属化学
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催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Energy Storage
·
2024
·
IF 8.9
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
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电化学
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能源存储
✓ 已验证
DOI
高影响因子
JOURNAL OF ORGANIC CHEMISTRY
·
2025
·
IF 3.6
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.
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
JOURNAL OF HAZARDOUS MATERIALS
·
2025
·
IF 11.3
Guoqiang Zhao,Wenjing Chen,Rongrong Zhang,Rui Zhang,Bo Jiang,Ruyan Hou,Xing Huang
Cypermethrin, a common pyrethroid insecticide, raises significant ecological concerns due to its widespread use. In this study, a highly efficient cypermethrin-degrading strain, Rhodococcus sp. H-3, was isolated. The strain was capable of degrading 30 mg/L cypermethrin at the rate of 83.48 % within 7 days and it could hydrolyze cypermethrin into 3-phenoxybenzoic acid (3-PBA) and permethric acid (DCVA). A novel cypermethrin degradation gene, cymE1 , was identified in strain H-3 through genome analysis, and its highest level of amino acid sequence similarity observed was 33.50 % in the Swiss-Prot database. The functional strain, SCK6-E, which could secrete CymE1, was successfully constructed by using double-exchange strategies. Strain SCK6-E could be applied for the removal of cypermethrin residues from tea plant leaves with a removal rate of 57.83 % within 2 h. Furthermore, strain H-3 demonstrated the capability to remediate cypermethrin-contaminated soil, exhibiting a degradation rate of 65.80 % over 10 days. The results of the 16S rRNA high-throughput sequencing indicated that strain H-3 was conducive to the restoration of the diversity and richness of the bacterial community in the soil. This study provides novel strain and gene resources for researching the degradation mechanism of pyrethroids, and offers valuable insights for developing effective pesticide residue remediation strategies.
研究领域:
环境微生物学
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生物修复
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基因组学
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分子生物学
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农业科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Xiaoyu Wang,Mengchao Feng,Rui Cao,Yuchang Wang,Kai Ma,Jianbin Zhang
A new CeCO 3 OH@(hexagonal/cubic phases–CdS) (CeCO 3 OH@(H/C–CdS)) composite catalyst was facilely synthesized by a simple microinjection titration–stirring method, in which CdS nanoparticles were dispersed on the surface of CeCO 3 OH nanolines. The optimal conditions for the preparation of composite catalysts with high photocatalytic performance were determined by single-factor experiments and response surface experiments. Under these conditions, the degradation rate of 30 mL 2.000 g/L rhodamine B (Rh B) by CeCO 3 OH@(H/C-CdS) in a photocatalytic reaction for 1 h at 25 °C was up to 86.81 % and its degradation rate in a photocatalytic reaction for 150 min was up to 99.62 %. The degradation rate could be maintained above 80 % even after six times recycling. Especially, the photocatalytic degradation efficiency of 2.000 g/L Rh B on the composite catalyst under sunlight and at room temperature for 30 min reached 97.66 %. Meanwhile, the large size of CeCO 3 OH considerably alleviated the agglomeration of CdS, providing more adsorption and active sites for visible light-mediated degradation of Rh B. Importantly, the Z-scheme charge transfer realized by CdS and CeCO 3 OH enhanced the efficient separation of photogenerated electrons and holes, and successfully inhibited the recombination of photogenerated electrons with holes. At the same time, owing to the low energy band difference between the two phases of CdS, charge was transferred between the hexagonal and cubic phases, leaving more effective photogenerated charge to participate in the degradation of Rh B. The synergism of the heterophase junction and heterojunction and the presence of oxygen and sulfur vacancies considerably enhanced the degradation performance of the catalyst. Thus, this study provides a new strategy for the modification and enhanced visible-light catalysis performance of CdS-based catalysts.
研究领域:
材料科学
·
环境科学
·
化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHINESE JOURNAL OF POLYMER SCIENCE
·
2024
·
IF 4.1
Luo Fang-Hua,Dong Zhi-Tao,Chen Guo-Hua,Ma Chen,Wang Huai-Yuan
Janus films with asymmetric physical/chemical properties have attracted considerable attention due to their promising applications in personal thermal management, electronic skins, sensors, actuators, etc. However, traditional methods for fabricating Janus films conventionally need the assistance of an interface or auxiliary equipment, which are usually complex and time-consuming. Herein, flexible poly(vinyl alcohol) (PVA)/graphene oxide (GO)/h-BN (recorded as PVA/GO/h-BN) Janus films with thermally, optically, and electrically anisotropic properties are fabricated by a simple density deposition self-assembly method, which just utilizes the density difference between GO and h-BN during water evaporation. Experimental results show that the two sides of the acquired Janus films have obvious asymmetric characteristics. In the original state of the PVA/GO/h-BN Janus films, the thermal conductivity of the GO side (10.06 W·m −1 ·K −1 ) is generally lower than that of the h-BN side (10.48 W·m −1 ·K −1 ). But after GO is reduced, the thermal conductivity of the rGO side reaches 12.17 W·m −1 ·K −1 , surpassing that of the h-BN side. In addition, the relative reflectance of the h-BN side of Janus film is also significantly higher than that of the rGO side, and the surface resistance difference between the two sides is about 4 orders of magnitude. The prepared PVA/GO/h-BN Janus films show great application potential in human thermal management, light conversion switches, and electronic skins. This study provides a simple and versatile strategy for fabricating Janus films with multifunctional (such as thermal, optical, and electrical) anisotropies.
研究领域:
材料科学
·
纳米技术
·
热管理材料
✓ 已验证
产品关联
DOI
高影响因子
CELL BIOLOGY INTERNATIONAL
·
2024
·
IF 3.3
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
JOURNAL OF ORGANIC CHEMISTRY
·
2023
·
IF 3.6
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
✓ 已验证
DOI
高影响因子
Science China-Chemistry
·
2022
·Vol. 66
·期 2
·548-561
·
IF 10.138
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
危险品化学品经营许可证（带存储）