ADVANCED SYNTHESIS & CATALYSIS
·
2017
·Vol. 359
·期 3
·454-466
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IF 5.646
Xu Cheng,Weijian Li,Ruifang Nie,Xiaojun Ma,Rui Sang,Li Guo,Yong Wu
A micron-scale palladium(II) material has been successfully prepared using Schiff base-modified hexagonal boron nitride as a support and used for the first time as an efficient and recyclable catalyst in organic synthesis. The morphology, composition, metal loading and thermal stability of the catalyst were studied using scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), infrared spectroscopy (FT-IR), inductively coupled plasma (ICP) and thermogravimetric (TG) analyses. Then, the micron material was tested in various C–C cross-coupling reactions and exhibited excellent catalytic activities in the Suzuki and Heck reactions. Moreover, the catalyst could be easily recovered by simple filtration and reused at least ten times without significant loss of its catalytic activity. In general, this work demonstrates the possibility of using Schiff-base@hexagonal boron nitride as an efficient support for heterogeneous catalysts.
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ANALYTICA CHIMICA ACTA
·
2019
·
IF 5.256
Chao Song,Dan Gao,Shangfu Li,Liping Liu,Xiaowu Chen,Yuyang Jiang
The location of double bond in unsaturated fatty acids (FAs) plays a critical role in their physiological properties. However, structural identification and quantification of unsaturated FAs by mass spectrometry are still challenging. In this work, we reported the coupling of epoxidation reaction of the C=C in unsaturated FAs and liquid chromatography-mass spectrometry (LC-MS) with multiple reaction monitoring (MRM) mode for accurate identification and quantification of C=C isomers of FAs. Epoxidation of the C=C in unsaturated FAs was induced by a dioxide of ketone , tetrahydrothiopyran-4-one 1,1-dioxide, as a catalyst and Oxone as an oxidant in less than 5 min with nearly 100% yield. All the C=C bonds were epoxidized to obtain a single product, simplifying the chromatographic separation of epoxidation products to enable more accurate quantification analysis. The epoxidation products were stable at room temperature and can produce highly abundant diagnostic ions indicative of C=C locations by tandem mass spectrometry using collision-induced association (CID). The application of this approach for the analysis of FAs isomers in human plasma demonstrated the potential of our method for the qualitative and quantitative analysis of unsaturated FAs in complex biological samples, which is valuable in biological and medical analysis.
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ACS Catalysis
·
2017
·
IF 10.614
Tingting Hou,Nengchao Luo,Hongji Li,Marc Heggen,Jianmin Lu,Yehong Wang,Feng Wang
Selective cleavage of C–C bonds is pursued as a useful chemical transformation method in biomass utilization. Herein, we report a hybrid CuOx/ceria/anatase nanotube catalyst in the selective oxidation of C–C bonds under visible light irradiation. Using the lignin β-1 model as a substrate offers 96% yields of benzaldehydes. Characterization results by high angle annular dark field scanning transmission electron microscopy (HAADF-STEM) and energy-dispersive X-ray spectroscopy element (EDX) mapping reveal that CuOx clusters are highly dispersed on the exposed anatase surface as well as on the nanosized ceria domains. In-depth investigations by Raman and ultraviolet visible diffuse reflectance spectra (UV−vis DRS), together with density functional theory (DFT) calculations, further verify that the CuOx clusters present on the ceria domains increase the concentration of surface defects (Ce3+ ions and oxygen vacancies) and accordingly improve the photocatalytic activity (Yang character); the CuOx clusters decorating on anatase suppress the side reaction (oxy-dehydrogenation without C–C bond cleavage) because of an upward shift in the valence band (VB) edge of anatase (Yin character). Mechanism investigation indicates hydrogen abstraction from β-carbon by photogenerated holes is a vital step in the conversion.
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Molecular Catalysis
·
2022
·
IF 5.089
Shengnan Zhao,Song Song,Yong You,Yingtian Zhang,Wei Luo,Kaijie Han,Tong Ding,Ye Tian,Xingang Li
Heterogeneous photocatalytic C-C coupling is a green and efficient approach to producing valuable chemicals. The strategies for guiding effective photocatalyst design are desired but still limited. Here, we report visible-light-driven highly selective photocatalytic C-C coupling of benzyl alcohol over surfactant-modified Zn 3 In 2 S 6 semiconductors. A complete switch of product selectivity from benzyl aldehyde (91.5 %) to C-C coupling products (96.5 %) is obtained by the modification of Zn 3 In 2 S 6 with stearyl trimethyl ammonium bromide (STAB). This modification assists the formation of sulfur vacancies on Zn 3 In 2 S 6 to enhance charge carrier separation, thereby increasing the photocatalytic activity. The selectivity switch is mainly attributed to increasing conduction band position of Zn 3 In 2 S 6 by surfactant modification which strengthens the reduction ability of photogenerated electrons to induce the reversible reduction of benzyl aldehyde to ketyl radicals, and partially to the poor oxidation ability of the material that inhibits the oxidation of ketyl radicals to benzyl aldehyde. Encouragingly, this universal protocol has been successfully applied to a series of aromatic alcohols and biomass-derived furanic alcohols to selectively produce C-C coupling products.
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JOURNAL OF MOLECULAR STRUCTURE
·
2023
·
IF 3.8
Peng Xiong,Tong-Wei Zhang,Shi-Ming Li,Mei-Yu Xu,Guang-Ming -Liang,Liu-Cheng Gui,Xiu-Jian Wang
Two tetranuclear copper cages with tubular type, [Cu 4 (BMBA) 4 ((CH 3 ) 2 N) 2 (H 2 O) 2 ] ( 1 ) and [Cu 4 (BMBA) 4 (Bipy)(H 2 O) 2 ] ( 2 ), were successfully constructed by the reaction of Cu(NO 3 ) 2 with dicarboxylic acid 4,4′-[( ethylazanediyl ) bis ( methylene )]-bis[(1,1′-biphenyl)-2-carboxylic acid] (H 2 BMBA) under solvothermal conditions. The complexes 1 and 2 exhibit a similar cage structure, formed by four ligands connecting two binuclear copper paddle-wheel secondary building units (SBUs). Interestingly, the complex 2 was obtained by appropriately binding of 4, 4′-bipyridine (Bipy) molecule on the axial positions of two Cu paddle-wheels inside the cage. For this reason, the complex 2 exhibits excellent stability in some common organic solvents at room temperature and aqueous solutions with a pH of 2 to 12. Upon thermal activation of complex 2 , the coordinated water molecules can be removed, and its exposed metal active-sites show Lewis acid character, which can be used an efficient heterogeneous catalysis of Knoevenagel condensation (C C) and Clauson-Kaas (C N) reactions.
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JOURNAL OF POLYMER SCIENCE PART A-POLYMER CHEMISTRY
·
2018
·Vol. 56
·期 20
·2344-2353
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IF 2.588
Jiajun Bi,Jian Chen,Yahao Dong,Wen Guo,Dajian Zhu,Tao Li
A new polymer was prepared from 1,3,5-triformylphloroglucinol (noted as TDTB) and o -phenylenediamine through Schiff base condensation reaction, and palladium (II) was immobilized on the polymer (noted as TbPo-Pd(II)). This process was easy to work-up and cost-effective. The structure and composition of TbPo-Pd(II) were fully characterized by FTIR, TGA, XPS, AAS, SEM, and TEM analyses. Meanwhile, this catalyst showed desired thermal stability and excellent performance in water/methanol system for Suzuki and Sonogashira coupling reactions. In addition, this heterogeneous catalyst can be readily recovered by simple filtration with no appreciable Pd leaching in the reaction. This work provides a powerful protocol for rapid access to asymmetrical biphenyls and aryl alkynes. © 2018 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2018 , 56 , 2344–2353
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2022
·
IF 10.319
B. Li,H.J. Li,X.Y. Yao,X.F. Tian,Y.J. Jia,G.H. Feng
A (ZrC/SiC) 3 alternate coating was deposited on sharp leading edge (SLE) C/C composites by chemical vapor deposition (CVD). The ablation behavior was examined via oxyacetylene torch with heat flux of 2.38 MW/m 2 . The results indicated that the alternate coating exhibited great ablation resistance, providing an effective protection for C/C composites. In initial rapid heating stage, the (ZrC/SiC) 3 alternate coating can relieve thermal stress, avoiding the peeling of coating and keeping an intact coating structure. In subsequent ablation, the SiC layers in central region were consumed rapidly, leaving layered interspaces. Three stacked ZrO 2 layers were reserved with the assistance of the release of thermal stress by interspaces, offering a great anti-scouring effect. In transition and border regions, the alternate SiC layers can delay oxygen erosion of inner coating and C/C substrate by the formation of SiO 2 . It is believed that the results would be helpful for the design and application of anti-ablation coatings on SLE C/C composites.
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Reaction Kinetics Mechanisms and Catalysis
·
2022
·Vol. 135
·期 6
·3243-3256
·
IF 1.843
Zhou Lin,Wang Ruo-Bing
Nitrogen doped mesoporous carbon (N-MPC)-supported monometallic and bimetallic catalysts were synthesized by using hydrothermal and impregnation method, and the catalytic activity of the catalyst to carbon–carbon bond-forming reactions (Suzuki, Heck and Sonogashira reactions) was studied. The bimetallic catalyst Pd-Ni@N-MPC with high Ni to Pd atomic ratios showed highly activity in the C–C coupling reactions of aryl halide under optimized condition. In contrast to their monometallic counterparts, such Pd-Ni@N-MPC catalyst not only show higher catalytic activity but also show more economic and stable. The catalysts were characterized by powder X-ray diffraction, X-ray photoelectron spectroscopy, scanning electron microscope and transmission electron microscopy, which demonstrated that the Pd–Ni NPs highly dispersed and possessed uniform size.
Graphical abstract
研究领域:
催化化学
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材料科学
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有机化学
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纳米技术
·
物理化学
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LANGMUIR
·
2026
·
IF 4.4
Zhouxuan Zang,Feifan Zheng,Yi Yu,Li Xu,Guoji Liu
The direct synthesis of bioaviation fuel precursors from furfural (FF) aqueous solutions represents a promising and more sustainable approach. Herein, we report MgAlSnO mixed oxides derived from MgAlSn-LDH intercalated with various interlayer anions, exhibiting favorable activity for the aqueous C–C coupling of FF and methyl isobutyl ketone (MIBK). MgAlSnO-CA demonstrates optimal resistance to water poisoning, achieving 96% conversion of FF in high-water-content systems (MH2O/FF = 7). Furthermore, the excellent catalytic activity of MgAlSnO-CA in various aqueous-phase C–C couplings of biomass-derived molecules confirms broad applicability. In situ DRIFTS studies and contact angle measurements reveal that water dissociation enables the catalyst to exhibit superior resistance to water poisoning. Poisoning experiments confirmed that the acidic sites on the catalyst served as the active sites for water dissociation. DFT calculations reveal that the charge density of Sn influences the strength of the p-p orbital, which plays a decisive role in determining the water dissociation rate and water-poisoning resistance. This study provides guidance for the direct resource utilization of FF aqueous solutions and suggests a novel strategy to mitigate the water poisoning of metal oxides.
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ACS Catalysis
·
2026
·
IF 13.6
Wentao Hao,Zhuqian Wang,Hui Cao,Jia Qiao,Qingde Zhang,Kun Xiong,Xingchen Liu,Yong Qin,Chaoqiu Chen
The selective oxidation of CH4 to C2 oxygenates under mild conditions is a significant pathway for CH4 valorization, yet it remains extremely challenging due to the inertness of methane, the competing overoxidation, and sluggish C–C coupling kinetics. Here, we show that the N,S co-doped carbon nanotube-supported Fe5 clusters catalyst (Fe5/NSC) with adjacent Fe sites drives sequential C–H activation and C–C coupling to ethanol with a C2H5OH productivity of 1939.6 μmol·gcat–1·h–1 and a selectivity of 83.9% at 25 °C and 0.5 MPa CH4 without the assistance of CO. Comprehensive experimental investigation and density functional theory calculations reveal the critical role of adjacent Fe sites in the selective formation of C2H5OH. The adjacent Fe sites featured in Fe5/NSC synergistically facilitate the dissociation and/or partial oxidation of CH4 to distinct C1 intermediates (*OCH2 and *CH3) and subsequent OCHx–CHx coupling between them to form the key CH3CH2O* intermediate for C2H5OH production, as opposed to the conventional CHx–CO coupling pathway that primarily yields acetic acid.
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产品关联
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高影响因子
ACS Applied Nano Materials
·
2026
·
IF 5.8
Shuibo Wang,Zixiang Tong,Yanle Li,Yichao Lin,Jingjing Wang,Ziqi Tian,Hongfeng Yin,Liang Chen
The glycerol electro-oxidation reaction (GEOR) to formate represents an attractive technology for the concurrent production of hydrogen and the valorization of biomass. However, the intricate pathway of GEOR and the high cost associated with noble metal electrocatalysts hinder its progress. Herein, ultrathin CuCoNiW medium-entropy oxide nanosheets (CuCoNiWOx UNS) serve as an effective noble-metal-free catalyst for this transformation. It delivers a high mass activity mass activity of 632.9 mA mgmetal–1, a low potential of 1.0 V vs RHE at 10 mA cm–2, and a formate selectivity of 83.1%, with remarkable stability over 40 h. The high performance is attributed to the distinct roles of each metal within the medium-entropy structure: subsurface W atoms ensure structural stability; Co and Ni sites optimize the adsorption of glycerol and intermediates; and Cu sites promote C–C bond cleavage. The reaction pathway involves the sequential conversion of glycerol to glyceraldehyde, glyceraldehyde to glycolaldehyde/formate, and glycolaldehyde to formate. These findings emphasize the efficacy of implementing medium-entropy structures as a viable strategy for biomass electrooxidation reactions.
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ACS Sustainable Chemistry & Engineering
·
2026
·
IF 7.6
Yiquan Zhou,Yongtao Wang,Youguang Feng,Quanjie Du,Huanliang Lu,Kaixin Li,Yong Yan,Tan Giin Yu Amy,Hong He
Abstract Catalytic oxidation of biomass waste is a key environmental engineering route for waste valorization. However, it is typically conducted in alkaline media and is often limited by insufficient catalytic activity. Here, we report an efficient strategy for converting shrimp shell (a chitin-rich waste, denoted SS) through selective C–C bond scission over a stable biochar-supported Ru catalyst featuring synergistic Ru-base catalysis. This system affords an acetic acid (AA) yield of 43.2% and 7.6% of 4-hydroxypyridine directly from demineralized SS without adding alkaline media in the oxidation process. The sustainability metrics of this process is evaluated and yield an Environmental Factor (E-factor) of 2.37, highlighting its green superiority over conventional routes. In situ DRIFTS, density functional theory (DFT) calculations, and ESR characterization further reveal that clustered basic sites facilitate H abstraction at the Cα/Cβ positions of sugar intermediates, while RuOx species promote subsequent oxidative C–C bond scission via a Mars−van Krevelen mechanism. A planar adsorption configuration between the reactant and RuOx is identified, which favors C–C bond rupture and enhances reaction efficiency. Kinetic analysis further supports the mechanistic results and reveals that oxidative Cα–Cβ bond cleavage is the rate-determining step. Overall, this work delivers a high-activity and green platform for the selective oxidation of chitinous waste and provides a clue for upgrading solid waste through cooperative catalysis.
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