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 Chemistry
·
2023
·
IF 13.1
Yuzhu Qian,Hongrui Wang,Xinni Li,Ting Song,Yong Pei,Li Liu,Bei Long,Xiongwei Wu,Xianyou Wang
The development of insertion-type anodes is the key to designing “rocking chair” zinc-ion batteries. However, there is rare report on high mass loading anode with high performances. Here, {001}-oriented BiOCl nanosheets with Sn doping are proposed as a promising insertion-type anode. The designs of cross-linked CNTs conductive network, {001}-oriented nanosheet , and Sn doping significantly enhance ion/electron transport, proved via experimental tests and theoretical calculations (density of states and diffusion barrier). The H + /Zn 2+ synergistic co-insertion mechanism is proved via ex situ XRD, Raman, XPS, and SEM tests. Accordingly, this optimized electrode delivers a high reversible capacity of 194 mA h g −1 at 0.1 A g −1 with a voltage of ≈0.37 V and an impressive cyclability with 128 mA h g −1 over 2500 cycles at 1 A g −1 . It also shows satisfactory performances at an ultrahigh mass loading of 10 mg cm −2 . Moreover, the Sn-BiOCl//MnO 2 full cell displays a reversible capacity of 85 mA h g −1 at 0.2 A g −1 during cyclic test.
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
COLLOIDS AND SURFACES B-BIOINTERFACES
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2017
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IF 3.887
Zhili Deng,Menghuan Tang,Li Zhao,Yijuan Long,Zuhuang Wen,Yuan Cheng,Huzhi Zheng
A novel targeting drug delivery system for cancer therapy based on H + -triggered bubble-generating nanosystems (BGNSs) was engineered. First, hollow mesoporous silica nanoparticles (HMSNs) were used to load doxorubicin (DOX). Then, the obtained drug-loaded HMSNs were treated with NaHCO 3 to prepare the BGNSs. The BGNSs were coated with polydopamine (pDA), and finally, folic acids (FA) were anchored on the nanosystems to obtain the desired nanoscale drug delivery system ( [email protected] ). [email protected] was effectively internalized by cancer cells through folate receptor-mediated endocytosis and generated CO 2 bubbles under the acidic environment of the lysosomes, thus enhancing lysosomal membrane permeability (LMP) to release caspase-3 into the cytoplasm, resulting in cancer cell death via an apoptosis-like pathway. Notably, we demonstrated that the [email protected] exhibited a significant simultaneous synergetic cytotoxicity against MCF-7 cells and remarkably overcame the multidrug resistance (MDR) of MCF-7/ADR cells. Moreover, compared to free DOX and a nanosystem without FA modification (BGNSs), the [email protected] induced relatively minor side effects in the MCF-10A cells. Therefore, the results showed that [email protected] , as a targeted drug delivery system, have a good probability of overcoming the MDR of tumor cells with minor side effects on normal cells.
研究领域:
纳米技术
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药物科学
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癌症研究
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药物递送系统
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS A-GENERAL
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2021
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IF 5.706
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
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催化
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化学工程
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有机化学
✓ 已验证
DOI
高影响因子
ChemSusChem
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2019
·Vol. 12
·期 16
·3871-3877
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IF 7.804
Dan Wu,Xing Yu,Xinqing Chen,Gan Yu,Kun Zhang,Minghuang Qiu,Wenjie Xue,Chengguang Yang,Ziyu Liu,Yuhan Sun
Graphical Stacks on ! H-type MFI zeolite catalysts with a unique stacked structure are synthesized in a one-pot procedure in the presence of NH 4 F with the help of zeolite confinement through a solvent-free route without further ion-exchange procedures. The catalysts display excellent catalytic performance in methanol-to-gasoline reactions. H-type aluminosilicate zeolites are extensively used as solid-acid catalysts and support materials in industrial catalysis. However, the conventional synthesis methods involving hydrothermal syntheses and ion-exchange processes suffer from severe water pollution and toxic gas emissions. Herein, H-type MFI zeolite catalysts with a unique stacked structure were directly synthesized in the presence of NH 4 F and with the help of zeolite confinement through a solvent-free route without further ion-exchange procedures. A range of ex situ and in situ characterization procedures were used to provide evidence of the simultaneous use of pre-made ZSM-5 and NH 4 F as a confined Al source and mineralizer, respectively. The confined zeolite framework of ZSM-5 prevented the formation of AlF x species between NH 4 F and Al atoms, ensuring that the prepared samples had desirable acidic properties. Moreover, the resulting morphology could be controlled by using different silica substrates. The obtained H-type MFI zeolites showed excellent catalytic performance in methanol-to-gasoline reactions owing to their unique structure and directly exposed acidic sites. The developed one-pot strategy provides an alternative method for the facile synthesis of H-type zeolites with defined morphology.
研究领域:
材料科学
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催化
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Energy Storage
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2024
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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
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Ji Shu,Yichong Zhang,Kanming Wang,Jianli Wang,Jiaxuan Ying,Hongyu Wang
Membrane filtration is regarded as one of the promising technologies for water treatment. However, insufficient micropollutants removal and membrane fouling still limited the further application. Herein, this study engineered a novel membrane hybrid system integrating typical pharmaceuticals removal and membrane self-cleaning by assembled layered MXene and hexagonal boron nitride (h-BN). By doping a small amount of MXene into h-BN (mass ratio of 1 to 10), the synergetic process of adsorption and photocatalytic degradation were achieved. Based on experimental and density functional theory (DFT) calculation results, the chemisorption-photodegradation performance of the membrane hybrid system assembled with 1/10 MXene@h-BN was significantly enhanced due to the termination group and conductive property of MXene. In addition, trimethoprim (TMP) degradation by the above membrane followed the Langmuir–Hinshelwood model, indicating pollutants removal initiated not only on the membrane surface but also in the bulk solution under simulated solar irradiation. This phenomenon was attributed to the generation of •OH and 1 O 2 by forming Ohmic contact with altered internal band structure. The durability and practical experiments with secondary effluent from local wastewater treatment were also tested. The exceptional self-cleaning performance of the membrane hybrid system assembled with 1/10 MXene@h-BN was demonstrated by lower membrane fouling and maintaining durability even after five cycles. Furthermore, the performance (both pollutants removal and flux) of the modified membrane for secondary effluent treatment was also considerable, validating its potential for practical application. Owing to the excellent features, the membrane assembled with MXene@h-BN is anticipated to be an ideal candidate for advanced wastewater treatment.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ORGANIC CHEMISTRY
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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
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合成化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CATALYSIS TODAY
·
2018
·
IF 4.667
Lingcong Li,Xiaojun Liu,Hong He,Ningqiang Zhang,Ziwen Liu,Guizhen Zhang
The MgO-doped hexagonal boron nitride (MgO-h-BN) nanomaterials were designed as a support for Palladium (Pd) catalysts for CO oxidation reaction. The catalytic properties of Pd/MgO(5)-h-BN catalyst was investigated and compared with Pd/h-BN catalyst. Transmission electron microscopy (TEM) results suggested that the PdO nanoparticles with small grain sizes (ca. 8 nm) were effectively dispersed on the surface of MgO, and the MgO were deposited on the h-BN nanosheets in the Pd/MgO(5)-h-BN catalyst. X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) analyses revealed that a small amount of Mg 2+ embedded into the B vacancies of h-BN nanosheets in the Pd/MgO(5)-h-BN catalyst. More significantly, a large amount of adsorbed oxygen appeared near the B vacancies of Pd/MgO(5)-h-BN catalyst. The experiments outcomes of diffuse reflectance fourier transform spectra analysis of CO (CO-DRIFT) indicated that the carbonate/formate species were easily decomposed to CO 2 on the Pd/MgO(5)-h-BN catalyst than Pd/h-BN catalyst, which might be a reason why the Pd/MgO(5)-h-BN catalyst had high CO oxidation activity. According to above analyses, we provide a new insight for the MgO-h-BN nanomaterials for Pd catalysts for application in CO oxidation reaction.
研究领域:
催化
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材料科学
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化学
·
纳米技术
✓ 已验证
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2025
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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
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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
危险品化学品经营许可证（带存储）