CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Guokai Cui,Yisha Xu,Daqing Hu,Ying Zhou,Chunliang Ge,Huayan Liu,Wenyang Fan,Zekai Zhang,Biao Chen,Quanli Ke,Yaoji Chen,Bing Zhou,Wei Zhang,Ruina Zhang,Hanfeng Lu
A series of functional ionic deep eutectic solvents (iDESs) containing pyridinolate anions were reported as green sorbents , solvents, and catalysts for highly efficient capture and transformation of CO 2 to quinazoline-2,4(1 H ,3 H )-dione and its derivatives at mild conditions via tuning the structures of iDESs. Physical properties, such as density and viscosity, as well as flow activation energy and thermal expansion coefficient, were systematically investigated. Effects of the partial pressure of CO 2 and the absorption temperature on the CO 2 absorption capacity using these functional iDESs as sorbents were studied, and the different absorption mechanisms, including carbamate and carbonate pathways, were analyzed by FT-IR and 13 C NMR spectroscopy. Additionally, thermodynamics analysis of CO 2 absorption was performed according to the chemical reaction mechanism, and K θ ,Δ r G θ m), Δ r H θ m, and Δ r S θ m were calculated. Furthermore, the effects of cations, anions, HBDs, reaction temperature, and the molar ratio of catalyst to substrate ( n Cat. / n Sub . ) on CO 2 conversion were systematically studied, and excellent isolated yield of up to 97.1% at mild conditions could be obtained with only 0.25 equiv. DES as the solvent as well as the sorbent and the catalyst. Plausible “simultaneous CO 2 activation and substrate activation” reaction mechanism of capture and transformation of CO 2 to quinazoline-2,4(1 H ,3 H )-diones by [N 2222 ][4-PyO]/DMSO (1:4) was verified by the spectra of FT-IR and based on previous reports. To the best of our knowledge, these are the first examples of tuning functional iDESs for the capture and transformation of CO 2 to quinazoline-2,4-(1 H ,3 H )-dione and its derivatives with only 0.25 equiv. DES. The method may also open a door to obtain the high efficiency of capture and transformation of such gases as NO x , SO 2 , CO, H 2 S, and CO 2 by functional DESs.
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ACS Sustainable Chemistry & Engineering
·
2022
·
IF 9.224
Tingting Chen,Yunfei Zhang,Yingjie Xu
A novel basic anion-functionalized ionic liquid with a 1-methylhydantoin anion ([1-MHy]−) and [P4442]+ cation was synthesized for efficient CO2 capture and catalytic conversion of CO2 to quinazoline-2,4(1H,3H)-dione, and CO2 absorption and conversion mechanisms were investigated by NMR, FT-IR, and DFT calculations. CO2 absorption results show that the capture capacity of [P4442][1-MHy] at 303.15 K and 0.1 MPa is up to 1.58 molCO2/molIL, which is attributed to the multiple-site cooperative interactions between CO2 with N– and C═O of [1-MHy]− originated from the electron conjugation effect, resulting in a decrease in the CO2 absorption enthalpy (−51.4 kJ/mol) and an increase in the activation of CO2. Moreover, the high yield of quinazoline-2,4(1H,3H)-dione obtained by using [P4442][1-MHy] to catalyze 2-aminobenzonitrile with atmospheric-pressure CO2 was 97% and is solvent- and metal-free. The reaction mechanism indicates that [1-MHy]− with the multiple-site cooperative interactions can not only activate CO2 but also can activate 2-aminobenzonitrile by forming two types of hydrogen bonds with −NH2 (N–H···N– and N–H···O═C), thus ensuring the excellent catalytic performance of [P4442][1-MHy]. Furthermore, due to the similar basicity of [1-MHy]− to the quinazolide anion ([Quinazolide]−), it can effectively prevent the deprotonation of the acidic quinazoline-2,4-dione into [Quinazolide]−, thereby improving its yield. In addition, [P4442][1-MHy] has good recycling performance during CO2 capture and conversion. The physicochemical properties of [P4442][1-MHy] are also reported. The obtained results may provide a new strategy for converting CO2 into value-added chemicals under green conditions.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2024
·
IF 2.7
Zhen Liu,Heng Xu,Zhijie Fan,Xiandie Zhang,Xuxu Cui,Jie Ji,Haozhe Li,Xiaode Guo
Self-healing materials have not been able to solve the problem of the coexistence of mechanical strength and self-healing function. Despite years of research, high-strength self-healing materials still require external factors to accelerate their self-healing process. For this reason, in this study, two kinds of chain extenders were inserted into the hard segment to design the molecular structure of polyurethane. The introduction of two chain extenders not only provided multiple binding modes for hydrogen bond recombination, but also formed more types of hydrogen bonds. Based on the design, a polyurethane elastomer PUGI-D 3 B 2 with high strength and excellent self-healing properties was synthesized. Data such as FTIR and 1 H NMR spectra clearly demonstrate the successful synthesis of PUGI-D 3 B 2 . The mechanical strength of PUGI-D 3 B 2 is 15.34 MPa, and its surface scratches can completely disappear after self-healing at 60°C for 10 h，and 98.02% of the mechanical strength is restored after 12 h of heal. Therefore, combining the excellent self-healing properties of PUGI-D 3 B 2 , we prepared a multifunctional superhydrophobic material (SHN-SiO 2 /PUGI-D 3 B 2 ). It can be used in a wide range of applications such as waterproof coatings, biomedicine and flexible electronics, which provides a new idea for the future direction of multifunctional materials.
研究领域:
材料科学
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高分子化学
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表面科学
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高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2015
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IF 4.097
Kangming Xiong,Fangjun Huo,Caixia Yin,Yueying Chu,Yutao Yang,Jianbin Chao,Anmin Zheng
We have developed two new colorimetric and fluorescent probes for hypochlorite based on a novel recognition mechanism: amido oxidized nitroso-group by hypochlorites, which realized the preparation of nitroso compounds. Furthermore, 1 H NMR, ESI-MS and theoretical calculation proved the recognition mechanism. In addition, the probe 2 was applied in practical applications such as detecting the hypochlorite concentration of sodium hypochlorite disinfectant and bioimagings.
研究领域:
分析化学
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生物化学
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材料科学
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高影响因子
INORGANIC CHEMISTRY
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2015
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IF 4.762
Fugang Li,Yangang Bi,Wenyuan Zhao,Tonglai Zhang,Zunning Zhou,Li Yang
Nitrogen-rich energetic salts involving various cations (lithium, 1; ammonium, 2; hydrazinium, 3; hydroxylammonium, 4; guanidinium, 5; aminoguanidinium, 6; diaminoguanidinium, 7; and triaminoguanidinium, 8) based on nitrogen-rich anion [Zn(BTA)2(H2O)]2– (N% = 65.37, BTA = N,N-bis[1H-tetrazol-5-yl]amine anion) were synthesized with a simple method. The crystal structures of all compounds except 1, 2, and 6 were determined by single-crystal X-ray diffraction and fully characterized by elemental analysis and FT-IR spectroscopy. The thermal stabilities were investigated by differential scanning calorimetry (DSC). The DSC results show that all compounds exhibit high thermal stabilities (decomposition temperature >200 °C). Additionally, the heats of formation were calculated on the basis of the experimental constant-volume energies of combustion measured by using bomb calorimetry. Lastly, the sensitivities toward impact and friction were assessed according to Bundesamt für Materialforschung (BAM) standard methods.
研究领域:
含能材料
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无机化学
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材料科学
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热分析
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晶体学
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高影响因子
JOURNAL OF CHEMICAL AND ENGINEERING DATA
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2014
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IF 2.045
Jia-rong Guo,Ling-Hua Zhuang,Guo-Wei Wang,Yan Wang,Jie Sun
The chemical structure of a new gemini dicationic imidazolium ionic liquid, 1,1′-[1,2-ethanediylbis(oxy-1,2-ethanediyl)]bis-[3-methyl-1H-imidazolium-1-yl] dihexafluorophosphate ([C6O2(mim)2][PF6]2), was established by 1HNMR. The thermal stability of [C6O2(mim)2][PF6]2 was studied with differential scanning calorimetry and thermogravimetric analyses. With the use of the analytical stirred-flask method at atmospheric pressure, the solubilities of [C6O2(mim)2][PF6]2 in water, methanol, ethanol, dimethylformamide, dimethyl sulfoxide, and (acetone + water) binary solvent mixtures were measured from (283.00 to 323.00) K. The experimental data was correlated with the modified Apelblat equation.
研究领域:
化学
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材料科学
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ANALYST
·
2019
·Vol. 145
·期 3
·1025-1032
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IF 4.019
Hui Xu,Zijie Feng,Yingxiang Du
Recently, ionic liquids have been widely used for chiral separation. However, several papers have reported the use of ionic liquids as the sole chiral selector. In this work, a novel capillary electrophoresis method using the ionic liquid 3-methyl-1-(3-sulfopropyl)-1H-imidazol-3-ium lactobionate (MSI-LA) as a chiral selector was developed for the enantioseparation of propranolol, metoprolol, bisoprolol, esmolol, atenolol, sotalol, terbutaline and clenbuterol. Method optimization was conducted and the optimized method (40 mM borax buffer, v/v 30% methanol, pH 8.5, 160 mM MSI-LA; +10 kV voltage; capillary temperature, 15 °C; 50 mbar/5 s injection; detection wavelength, 230 nm) was successful for the baseline separation of the eight basic drugs. The LA (lactobionic acid) system was compared. The possible mechanisms of enantioseparation were investigated using molecular modeling. Both the cation and anion of MSI-LA provided interactions between the chiral selector and analytes, and finally enhanced chiral recognition capability compared with LA.
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PubMed
高影响因子
Research
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2022
·
IF 11.036
Jin-Meng Heng,Hao-Lin Zhu,Zhen-Hua Zhao,Da-Shuai Huang,Jun-Yi Li,Pei-Qin Liao,Xiao-Ming Chen
Inorganic solids are a kind of important catalysts, and their activities usually come from sparse active sites, which are structurally different from inactive bulk. Therefore, the rational optimization of activity depends on studying these active sites. Copper is a widely used catalyst and is expected to be a promising catalyst for the electroreduction of CO2 to C2H4. Here, we report a conductive dinuclear cuprous complex with a short Cu···Cu contact for the electroreduction of CO2 to C2H4. By using 1H-[1,10]phenanthrolin-2-one and Cu(I) ions, a dinuclear cuprous complex [Cu2(ophen)2] (Cuophen) with a remarkable conductivity (3.9 × 10−4 S m−1) and a short intramolecular Cu···Cu contact (2.62 Å) was obtained. Such a short Cu···Cu contact is close to the distance of 2.54 Å between 2 adjacent Cu atoms in the edge of the copper(100)/(111) plane. Detailed examination of Cuophen revealed a high activity for the electroreduction of CO2 to C2H4 with a Faradaic efficiency of 55(1)% and a current density of 580 mA cm−2, and no obvious degradation was observed over 50 h of continuous operation. Comparing the properties and mechanisms of Cuophen and 2 other copper complexes with different Cu···Cu distances, we found that the shorter Cu···Cu distance is conducive not only for a *CO species to bridge 2 copper ions into a more stable intermediate transition state but also for C–C coupling.
研究领域:
无机化学
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电催化
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材料科学
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能源转换
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高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-12
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IF 15.7
Hu Yaqi,Liu Runze,Lu Kaiyun,Wu Daoning,Gao Pan,Hou Guangjin,Zhang Hongbo,Dai Weili
Hydrated hydronium ions formed in the pores/cages of zeolite catalysts are suggested as the active species that could impact the adsorption of reactant, the stability of intermediates or transition states, and the reaction mechanism in the aqueous phase alcohol dehydration. Nevertheless, under a typical vapor phase reaction condition, the relevant situation is still debatable. Herein, the promotion of water on cyclohexanol (CyOH) adsorption and dehydration under a vapor phase condition was clarified by in situ 1 H MAS NMR, 2D 1 H DQ MAS NMR and 2D 1 H- 27 Al HMQC NMR spectroscopy, systematic kinetic studies, isotope tracing and thermodynamic measurements. The water promoting effects were ascribed to water facilitating the formation of H 3 O + cluster (H 3 O + (H 2 O) n-1 ), and per Brønsted acid site (BAS) could be saturated by about 5 water at ambient temperature. The CyOH dehydration pathway was found to be highly dependent on the water concentrations, and a dimer reaction route with the C-H bond rupture as the kinetically relevant step (KRS) was verified as the main reaction pathway at high water concentrations. All these findings provide the deep insights into how water regulating the zeolite catalyzed dehydration reaction at a molecular level.
研究领域:
催化化学
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物理化学
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材料科学
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核磁共振波谱学
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反应机理
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表面化学
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高影响因子
JOURNAL OF MOLECULAR LIQUIDS
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2024
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IF 5.3
Yanrong Cheng,Chunyang Liu,Xia Guo
An aqueous two-phase system (ATPS) has been considered a green separation system. How to improve the separation efficiency and selectivity of ATPS has always been a widely concerned issue. However, so far, the construction of selective ATPS still remains a challenging task. Calixarenes are the third generation of supramolecular compounds. They exhibit significant advantages in recognizing small molecules. In the present study, calixarene was used for the first time to prepare selective ATPSs, which are sulfonatocalix[4]arene (SC[4])/1-decyl (or hexyl)-3-methylimidazolium bromide ([C n mim]Br)/trisodium citrate (Na 3 C 6 H 5 O 7 ) ATPS and SC[4]/1-decyl-3-methylimidazolium bromide ([C 10 mim]Br) ATPS. Ten aromatic molecules, including theobromine, syringic acid, vanillin, vanillic acid, theophylline, cephalexin, L-tyrosine, L-phenylalanine, S-mandelic acid, and L-tryptophan, were selected as model extracts to evaluate the selectivity of these SC[4]-based ATPSs. The results showed that among these 10 extracts, the SC[4]/[C n mim]Br/Na 3 C 6 H 5 O 7 ATPS has high selectivity toward vanillin, and the SC[4]/[C 10 mim]Br ATPS has high selectivity toward L-phenylalanine. Specifically, in the SC[4]/[C n mim]Br/Na 3 C 6 H 5 O 7 ATPS, the partition coefficient of vanillin can reach 315.7, while the partition coefficients of the other 9 extracts are around 2.4–23.1 In the SC[4]/[C 10 mim]Br ATPS, the partition coefficient of L-phenylalanine is much higher than 1 (i.e., 4.38–5.55), while the partition coefficients of the other extracts are below or around 1. The 1 H NMR spectra and response surface plots based on the Box-Behnken design further demonstrate the role of [C n mim]Br-SC[4] complex in the selectivity of these ATPSs.
研究领域:
化学
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分离科学
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超分子化学
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分析化学
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高影响因子
EUROPEAN JOURNAL OF PHARMACOLOGY
·
2019
·
IF 3.17
Qi-meng Liu,Qing Xiao,Xiang Zhu,Kai-feng Chen,Xia-wen Liu,Ru-chao Jiang,Dan Wu,Jun-min Shi,Li-jun Dai,Jun-jun Huang
Benign prostatic hyperplasia (BPH) is a common disorder of the urinary system in aging men. 2-(1H-indol-3-yl)-N-[3-(4-(2-methoxyphenyl) piperazinyl) propyl] acetamide (HJZ-3), which is derived from naftopidil , exhibited 97.7- and 64.6-fold greater inhibitory effects for a 1D adrenoceptor than for a 1B - and a 1A -adrenoceptors in vitro, respectively. To investigate the therapeutic potential for treating BPH, we evaluated the pharmacological activity of HJZ-3. Specifically, we evaluated through estrogen/androgen-induced rat benign prostatic hyperplasia model in vivo. HJZ-3 effectively prevented the progression of rat prostatic hyperplasia by suppressing the increase in prostate index and reducing the quantitative analysis of the relative acinus volume, relative stroma, epithelial volume and epithelial thickness and expression of proliferating cell nuclear antigen and α -smooth muscle actin. HJZ-3 decreased α 1A - and α 1D -adrenoceptor protein expressions in prostate tissue. HJZ-3 is a good alternative for α 1A - and α 1D -adrenoceptor blocker. It may relax smooth muscle tone and relieve symptoms of BPH.
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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
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合成化学
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PubMed
高影响因子
危险品化学品经营许可证（带存储）