Nature Communications
·
2026
·
IF 18.1
He Yingchun,Li Qing,Zhang Shao,Zhang Bo,Ma Dong-Dong,Wu Xin-Tao,Zhu Qi-Long
Electrosynthesis of N , N -dimethylformamide (DMF) combines sustainability with economic viability. However, its implementation is hindered by challenges in electrode engineering and reaction control. Herein, a redox-mediated domino electrosynthesis strategy is explored for efficient C–N coupling production of DMF over a binder-free single-molecule-integrated electrode engineered with designed cobalt phthalocyanines. This integrated electrode, featuring enhanced site accessibility and charge transfer capacity, exhibits high and selective methanol oxidation activity, initiating the domino process synergistically facilitated by in situ electrogenerated iodine as a redox mediator. The system operates stably at 50 mA cm –2 for over 150 h, achieving >90% Faradaic efficiency and a consistent DMF productivity of 839 μmol h –1 cm –2 . In a flow cell, pairing anodic DMF production with cathodic CO 2 -to-amide conversion yields industrial-scale DMF productivity up to 2.75 mmol h –1 cm –2 and gram-level amide-containing generic drug production at –200 mA cm –2 . Furthermore, comprehensive spectroscopic analysis and theoretical calculations elucidate a domino reaction sequence involving several key intermediates, namely *CH 2 O, iododiamine and iminium cation for DMF generation.
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高影响因子
POLYMER
·
2013
·Vol. 54
·期 18
·4902-4908
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IF 3.379
Peng Liu,Wang Tang,Hailiang Zhang
A series of water-soluble thermoresponsive copolymers , i.e., poly[( N -isopropylacrylamide- co -bis( N -hydroxyisopropyl pyrrolidone) 2-vinylterephthalate] [P(NIPAm- co -HIPPVTA)], with well-defined comonomer content have been synthesized via conventional free-radical copolymerization at low conversion. The liquid crystalline behavior of the copolymers was investigated using polarized light microscope and differential scanning calorimetry . The results revealed that the P(NIPAm- co -HIPPVTA) exhibit liquid crystallinity when the NIPAm content is lower than 52.2 mol%, which was obviously different from that of previous papers. In addition, thermo-responsive behaviors of copolymer also demonstrated by dynamic light scattering . The cloud points of these copolymers can be tuned over a broad range (i.e., 9.9–81.2 °C) by simply altering the molar content of the HIPPVTA. It is noted that the cloud point of the copolymers showed unexpected trend (i.e., parabolicaly other than linearly or exponentially) with the increasing of HIPPVTA content. That is, with an increase of HIPPVTA molar content, the cloud point of copolymer decreases at first and then increases.
研究领域:
高分子化学
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材料科学
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温敏高分子
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软物质物理
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KEY ENGINEERING MATERIALS
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2012
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IF 0
Xuan Min Zhu,Xiu Jian Zhao,Zhi Yong Ning,Xiao Tao Sui
Nanosized silver (Ag) was synthesized by reducing high concentration AgNO3 in N, N-dimethylformamide (DMF), in the presence of stabilizer polyvinyl pyrrolidone (PVP). PVP of two different molecular weights (MW=40000, 1300000) at the reaction temperature of 80°C and 100°C were tested for the effect on the formation of diverse silver nanoparticles. Our results indicated that the PVP with different molecular weights plays different role in the controlling of the Ag nanostructure owing to the PVP molecular selective adsorption on different crystal facets, thus affecting the growth rate of different facets of Ag nanoparticles. When all the other conditions kept the same and the temperature of 100°C, if PVP (Mw=40,000) was used, only a small amount of Ag decahedra were found. However, when the PVP with larger molecular weight such as PVP K88 (Mw=1300, 000), a large quantity of the triangular nanoprisms existed in the final solution in spite of the minority of quasi-sphere. The growth process and causation of different silver morphology with two distinct PVP have been briefly discussed.
研究领域:
纳米材料
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纳米粒子合成
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胶体化学
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材料科学
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CATALYSIS TODAY
·
2012
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IF 3.407
Anlian Zhu,Ruixia Liu,Lingjun Li,Liangyun Li,Lan Wang,Jianji Wang
In this work, the hydrogen bond formation ability of cation and anion of the ILs was determined by using the solvatochromic method and was found to be responsible for their catalytic activity in the Knoevenagel reactions. The enhancement in the hydrogen bond donor ability of the cations and the hydrogen bond acceptor ability of the anions can both lead to the increase in the catalytic activity of the ILs. From the proposed reaction mechanism, it was deduced that the cations of the ILs can form hydrogen bond with aldehyde to activate the C O bond as electrophile, and the anions of the ILs can promote active methylene compound to produce carboanion as nucleophile, showing dual function activation effect in the catalytic processes. In addition, the optimized N,N-dimethylethanolamnium acetate as dual function activator for the Koevenagel reactions benefits from wide substrates tolerance, ambient reaction temperature, easy work-up procedure, and easy reuse of the IL.
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JOURNAL OF CHEMICAL THERMODYNAMICS
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2022
·
IF 3.269
Jian Wang,Shuan Wu,Wenlin Xu,Hongkun Zhao
Switchable-hydrophilicity solvents (SHSs) are an emerging class of solvents with switchable phase behavior. They can be used as a substitute for volatile solvents and can be removed from organic products without distillation. However, the detailed physical properties data of SHSs are still very scarce in the literature. In this work, the experimental values densities, dynamic viscosities, refractive indices as well as conductivities of switchable hydrophilicity solvent (SHS) systems ( N , N -Dimethylbutylamine (DMBA), water, and carbon dioxide) are investigated at temperatures (283.15, 288.15, 293.15, 298.15, 303.15 and 308.15) K and at atmospheric pressure. VLE of the CO 2 loaded DMBA solutions are measured at 298.15 K over the partial pressure range of carbon dioxide from 17.0 to 98.0 kPa. Density data have been used to calculate the apparent molar volumes ( V ϕ ), limiting apparent molar volumes ( V ϕ 0 ) and limiting partial molar expansivity of solute ( E ϕ 0 ). The Jones-Dole coefficients B, the Gibbs free energies of activation of viscous flow per mole of solvent ( Δ μ 1 0 ≠ ) and per mole of solute ( Δ μ 2 0 ≠ ), entropies ( Δ S 2 0 ≠ ) and enthalpies ( Δ H 2 0 ≠ ) of activation of viscous flow were calculated from experimental viscosity data and discussed in terms of transition state theory. The Walden's product was calculated from the conductance and dynamic viscosity data. The results are valuable sources of information on the design and development of SHSs for novel industrial applications.
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RESEARCH ON CHEMICAL INTERMEDIATES
·
2022
·Vol. 48
·期 7
·2987-3006
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IF 3.134
Zhao Yifan,Li Wensi,Rehman Mooeez Ur,Wang Shengping,Li Guobing,Xu Yan
A series of N-modified Ru/N x -AC catalysts were prepared by ammonia treatment method and applied in dioctyl phthalate hydrogenation, which is a cascade reaction system involving partial hydrogenation of aromatic ring and the further saturated hydrogenation of the formed intermediate bis(2-ethylhexyl) cyclohexene-1,2-dicar-boxylate (DH 4 ) to dioctyl di-2-ethylhexylcyclohexane-1,4-dicar-boxylate (DEHCH). N doping was found to be able to increase the nitrogen-containing pyridine groups on the activated carbon (AC) surface, resulting in the abundance of binding sites for anchoring Ru and exceptionally enhancing the dispersion of Ru nanoparticles. Furthermore, the N-modified Ru/N 12 -AC catalyst exhibited a significantly higher turnover frequency value (1260.06 h −1 ) than Ru/AC catalyst (913.64 h −1 ). It was deduced that the presence of the pyridine groups could improve the adsorption of intermediate DH 4 by promoting the coverage of DH 4 on the catalyst surface. The environment of surface-enriched DH 4 accelerated the reaction rate of DH 4 hydrogenation and increased the selectivity to DEHCH. Therefore, the cooperation between highly dispersed Ru nanoparticles and pyridine groups supports remarkably enhanced the activity and selectivity. In addition, the Ru/N 12 -AC catalyst presented excellent catalytic activity and versatility in the hydrogenation of other phthalates such as dimethyl phthalate, diethyl phthalate, and dibutyl phthalate, demonstrating its prospective application in phthalate esters hydrogenation. Graphical abstract
Description N-doping exceptionally improved Ru dispersion and the adsorption of the intermediate product in DOP hydrogenation, leading to a higher activity and selectivity to saturated product.
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SENSORS AND ACTUATORS B-CHEMICAL
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2022
·
IF 9.221
Shuang Li,Yuchi Zhang,Le Han,Xianliang Li,Yan Xu
Heterojunction formation has been considered as an effective way for exploring ultrahigh sensitive multi-metal oxide based gas sensors. Herein, unique hierarchical radial CeO 2 /ZnO heterostructures with excellent triethylamine (TEA) gas-sensing performance were successfully prepared via a feasible solvothermal method . The morphology, microstructure and gas-sensing performance of the composite were systematically characterized and investigated. The selective TEA gas response of the radial CeO 2 /ZnO heterostructure was increased by ten times as compared to that of pure ZnO phase, ascribing to the abundant reactive sites induced by the formation of n-n heterojunction . Furthermore, the radial CeO 2 /ZnO n-n heterojunction exhibited the best TEA gas sensitivity with R a /R g = 92.17 at an operating temperature of 200 °C, a fast response/recovery time of 29 s/23 s, and a long-term stable repeatability for at least 60 days. The excellent selectivity of CeO 2 /ZnO heterojunction for TEA sensing is also remained even when mixing with other interferent gases. The interface-dependent and enhanced TEA sensing property of CeO 2 /ZnO can be ascribed to its intriguing radial morphology, for which the CeO 2 nanoparticles located in the internal structure of the composite while the ZnO hexagonal prism grew radially outward. The well assembled hierarchical CeO 2 /ZnO n-n heterojunction with abundant accessible active sites significantly facilitate the surface reaction and diffusion of target gas molecules at the interface between CeO 2 and ZnO during gas sensing process.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
·
IF 19.503
Shanyong Chen,Shiyan Wang,Panpan Hao,Muhong Li,Yu Zhang,Jia Guo,Weiping Ding,Min Liu,Jinlan Wang,Xuefeng Guo
Development of high-performance and stable electrocatalysts for hydrogen evolution reaction (HER) is crucial for hydrogen economy. Inspired by hydrogen evolution behavior on hydrogenase enzyme, in which the azadithiolate bridging ligand of active center facilitates fast proton shuttling and catalytic turnover, here we present an efficient approach to enhance both HER kinetics and stability realizing on an IrNi@N,O-C catalyst with individual IrNi nanoparticle separately confined in N and O co-doped carbon (N,O-C) nanocage. Experimental and theoretical investigations indicate that the N,O-C nanocage provides proton-adsorbing functionality on raising H* coverage over IrNi active centers, resulting in much accelerated HER kinetics. The IrNi@N,O-C presents superior HER performances compared to all reported Ir-based catalysts, with overpotential of 22 mV at 100 mA cm −2 , ultrahigh mass activity of 9.82 A mg Ir −1 (−0.050 V vs. RHE) and outstanding durability of 200 h at large current density. This work affords fresh insights/strategies for design of high-performance electrocatalysts
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2021
·
IF 6.953
Shuai Wang,Hao Wang,Jiali Tang,Yingbi Chen,Shixing Wang,Libo Zhang
The recovery of gold from wastewater has always been a research hotspot. Here, a novel chitosan-based adsorbent (CS-DPDM) was successfully synthesized by functionalizing chitosan with (N, N-(2-aminoethyl))-2,6-pyridinedicarboxamide. The adsorbent was analyzed by fourier transform infrared spectroscopy (FT-IR), nuclear magnetic resonance spectroscopy ( 1 H NMR), scanning electron microscope (SEM), energy dispersive X-ray spectroscopy (EDS), X-ray diffraction (XRD) and zeta potential method (Zeta). To investigate the adsorption performance of CS-DPDM for Au(III), the effects of pH, temperature, adsorption time and initial concentration were discussed. The maximum adsorption capacity of CS-DPDM for Au(III) at pH 5.0 is 659.02 mg/g at 318 K. The adsorption is a spontaneous endothermic behavior, and the adsorption process follows the quasi-second-order kinetic and Langmuir isotherm models, indicating that a single layer of chemical adsorption may have occurred on the surface of the adsorbent. The competitive adsorption and repetitive experiments show that CS-DPDM has considerable selectivity and reusability for Au(III). X-ray photoelectron spectroscopy (XPS) results show that N and O functional groups adsorb Au(III) on the surface of CS-DPDM through electrostatic, chelation and reduction. These results indicate that CS-DPDM has broad application prospects in recovering gold ions from aqueous solutions.
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高影响因子
JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2019
·
IF 2.298
Daofan Ma,Chunying Zhu,Taotao Fu,Xigang Yuan,Youguang Ma
The experimental values of density and viscosity for binary solutions diethylenetriamine (DETA) + H2O, DETA + N,N-diethylethanolamine (DEEA), and ternary solution DETA + DEEA + H2O over the entire concentration range were reported at atmospheric pressure and T = (293.15, 303.15, 313.15, 323.15, 333.15) K. The measured densities and viscosities were used to calculate the thermal expansion coefficient, excess molar volume, partial molar volume, apparent molar volume, partial molar volume at infinite dilution, viscosity deviation, and excess Gibbs free energy of activation for viscous flow. The molecular interactions in mixtures were discussed based on the volumetric and viscometric properties.
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Soft Matter
·
2023
·
IF 3.4
Chuanjiang Zhou,Yijia Yu,Wenjuan Xia,Shengjie Liu,Xiao Song,Zhaoqiang Wu,Hong Chen
Strain/pressure sensors with high sensitivity and a wide operation range have broad application prospects in wearable medical equipment, human-computer interactions, electronic skin, and so on. In this work, based on the different solubilities of Zr4+ in the aqueous phase and the hydrophobic ionic liquid [BMIM][Tf2N], we used N,N-dimethylacrylamide (DMA) as a vinyl monomer to prepare a Janus-type ionic conductive gel with one-sided adhesion through “one-step” UV irradiation polymerization. The Janus-type gel has satisfactory mechanical properties (tensile strength: 217.06 kPa, elongation at break: 1121.01%), electrical conductivity (conductivity: 0.10 S m−1), one-sided adhesion (adhesion strength to glass: 72.35 kPa) and antibacterial properties. The sensor based on the Janus gel can be used not only for real-time monitoring of strain changes caused by various movements of the human body (such as finger bending, muscle contraction, smiling, and swallowing) but also for real-time monitoring of pressure changes (such as pressing, water droplets, and writing movements). Therefore, based on the simplicity of this method for constructing Janus-type ionic conductive gels and the excellent electromechanical properties of the prepared gel, we believe that the method provided in this study has broad application prospects in the field of multifunctional wearable sensors.
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高影响因子
JOURNAL OF MOLECULAR LIQUIDS
·
2023
·
IF 6
Hui Liu,Jing He,Kun Zhu,Dongao Zhu,Linhua Zhu,Wenshuai Zhu,Huaming Li,Wei Jiang
Elaborate design of high stability catalytic active site is of great concern for the development of advanced organic–inorganic composite catalysts. Herein, cobalt-doped mesoporous molecular sieve grafted with N,N-dihydroxypyromellitimide catalyst (Co-SBA-15-NDHPI) is developed for the catalytic oxidative desulfurization (ODS) in diesel fuels. The close integration of organic active components and porous supports strengthens the synergistic catalytic effect, resulting enhancement of selective oxidation of sulfides to sulfone derivatives. In detail, N,N-dihydroxypyromellitimide is bonded to a Co-based mesoporous molecular sieve by 3-glycidyloxypropyltrimethoxysilane as the coupling agent allowing exclusive retention of NHPI, which serve as the active sites that result in boosted catalytic ODS performance. Meanwhile, taking advantage of strong chemical anchoring strategies, the Co-SBA-15-NDHPI catalyst exhibits the highest stability compared to other NHPI-containing desulfurization catalysts. This work opens the way for the development of a more stable organic–inorganic hybrid desulfurization catalyst.
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