ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Fusheng Liu,Ran Ping,Yongqiang Gu,Penghui Zhao,Bin Liu,Jun Gao,Mengshuai Liu
CO2 capture and utilization (CCU) have aroused much attention. In this paper, several novel triazolium-based ionic liquids (ILs) were developed for highly efficient transformation of CO2 into quinazoline-2,4(1H,3H)-diones. The catalytic behaviors such as the effects of IL structures and reaction parameters, catalyst recyclability, and scope of substrates were studied in detail. As compared to the reported homogeneous and heterogeneous catalysts, the [HTMG][Triz] with a tetramethylguanidine cation and a triazole anion exhibited an exceptional activity at 50 °C and 1 atm CO2 without any organic solvents. On the basis of the CCU strategy, we first studied the equimolar CO2 capture by the [HTMG][Triz] and one pot conversion of activated CO2 into various quinazoline-2,4(1H,3H)-diones, and good to excellent product yields were obtained. In addition, the catalytic performance for synthesis of quinazoline-2,4(1H,3H)-dione under low concentration of CO2 using a simulated flue gas was studied. The developed triazolium-based ILs could realize simultaneous activation of CO2 and the substrates under ambient conditions, which also have been demonstrated to support the reaction mechanism well. The integrative protocol here shows great significance in the practical synthesis of quinazoline-2,4(1H,3H)-dione and their derivatives from captured CO2 waste under mild conditions.
研究领域:
化学工程
·
环境科学
·
有机合成
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Ran Ping,Penghui Zhao,Qianqian Zhang,Guangyu Zhang,Fusheng Liu,Mengshuai Liu
Novel aminophenol-based protic ionic liquids (APILs) were designed and synthesized via one-step neutralization, and they were used as catalysts for conversion of 2-aminobenzonitriles and CO2 from simulated flue gases to produce quinazoline-2,4(1H,3H)-diones under mild conditions. The effects of anion–cation structures of APILs, various solvents, reaction parameters, and water contents on the product yields were investigated in detail. The catalyst recyclability and general applicability to different substrates were examined. It showed that both the basicity of the reaction media and the synergistic activation of zwitterions to reactants played important roles during the catalysis. The optimum [HTMG][m-AP] catalyst cooperating with the dimethylformamide (DMF) solvent could selectively convert CO2 into various quinazoline-2,4(1H,3H)-diones with good to excellent product yields at 60 °C and in a 0.1 MPa simulated flue gas atmosphere. In addition, [HTMG][m-AP]/DMF was easily recycled and could be reused in up to five consecutive cycles without an obvious loss of activity. By comparison with the reported catalysts, [HTMG][m-AP]/DMF here showed a superior catalytic performance and a great potential for development. Finally, the activation behaviors of [HTMG][m-AP]/DMF to reactants were studied, and a synergistic catalytic mechanism was proposed.
研究领域:
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
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.
研究领域:
化学工程
·
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
ZEITSCHRIFT FUR NATURFORSCHUNG SECTION B-A JOURNAL OF CHEMICAL SCIENCES
·
2016
·Vol. 71
·期 8
·869-874
·
IF 0.686
Gao-Feng Wang,Xiao Zhang,Shu-Wen Sun,Hong Sun,Xia Yang,Hui Li,Chen-Zhong Yao,Shu-Gang Sun,Yu-Peng Tang,Li-Xin Meng
Two Mn(II) complexes, {[Mn(BIPMO) 2 Cl 2 ] · 2(H 2 O)} n ( 1 ) and {[Mn(BIPMO) 2 (SCN) 2 ] · 2(CH 3 OH)} n ( 2 ) (BIPMO = bis(4-(1 H -imidazol-1-yl)phenyl)methanone) with V-shaped BIPMO ligands, were synthesized and characterized by IR spectroscopy and elemental analyses along with their single-crystal X-ray diffraction analyses. The Mn(II) ions in 1 and 2 are both six-coordinated to four nitrogen atoms of four BIPMO ligands and two anions (Cl − for 1 , and SCN − for 2 ) to form a distorted octahedral geometry.
研究领域:
配位化学
·
晶体学
✓ 已验证
产品关联
DOI
高影响因子
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.
研究领域:
化学工程
·
催化化学
·
绿色化学
✓ 已验证
产品关联
DOI
高影响因子
ZEITSCHRIFT FUR NATURFORSCHUNG SECTION B-A JOURNAL OF CHEMICAL SCIENCES
·
2020
·
IF 0.839
Gao-Feng Wang,Shu-Wen Sun,Hong Sun,Bing-Wei Chang,Jing Song,Xia Yang
Two coordination polymers (CPs), [Mn(bipmo)(pbtda)(H 2 O)] n ( 1 ), {[Cd(bipmo)(btda)]·2(H 2 O)]} n ( 2 ), (bipmo = bis(4-(1 H -imidazol-1-yl)phenyl)methanone, H 2 pbtda = 2-phenylbutanedioic acid, H 2 btda = butanedioic acid), were synthesized by solvothermal methods. The products have been characterized by elemental analyses, IR spectroscopy, and single-crystal X-ray diffraction. The topological structure of 1 is based on 2-nodal nets with the Schläfli symbol {6 3 }{6 9 ·8}, while that of 2 features a system with a sixfold penetration with the Schläfli symbol {6 6 }.
研究领域:
化学
·
材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF HETEROCYCLIC CHEMISTRY
·
2023
·
IF 2.4
Ping Zhao,Qingle Zeng
We have developed a diversity-oriented, substrate-controlled, chemoselective synthetic method for a variety of structurally diverse 1-sulfonylquinazoline-2,4(1H,3H)-diones and 2-sulfonamidobenzonitriles. This substrate-controlled synthesis is accomplished through the condensation reaction of 2-(sulfonamido)benzamides with or without an N-methyl group on the amides. The reactions are fulfilled within half an hour at room temperature with solid triphosgene as a convenient condensing agent and pyridine as an acid acceptor. This protocol features easily available starting materials, mild reaction conditions, easy experimental operation, and moderate to excellent yields of products.
研究领域:
有机化学
·
药物化学
✓ 已验证
DOI
高影响因子
ZEITSCHRIFT FUR NATURFORSCHUNG SECTION B-A JOURNAL OF CHEMICAL SCIENCES
·
2019
·Vol. 74
·期 3
·261-265
·
IF 0.961
Gao-Feng Wang,Shu-Wen Sun,Wei-Bing Wang,Hong Sun,Shao-Fei Song
Two coordination polymers, {[Co(bipmo)(tbip)]·3H 2 O} n ( 1 ) and {[Cd(bipmo)(tbip)]·3H 2 O} n ( 2 ) (bipmo=bis(4-(1 H -imidazol-1-yl)phenyl)methanone, H 2 tbip=5- tert -butylisophthalic acid), were synthesized by solvothermal methods and structurally characterized by elemental analyses, infrared spectroscopy, and single-crystal X-ray diffraction. The results from single-crystal X-ray diffraction data indicate that the solid state structures of 1 and 2 consist of metal-aromatic carboxylate layers, which are pillared by weak interactions to generate a three-dimensional network. The topological structures of 1 and 2 are uninodal nets based on 3-connected nodes with the Schläfli symbol of {6 3 }.
研究领域:
无机化学
·
材料科学
✓ 已验证
DOI
高影响因子
EUROPEAN JOURNAL OF MEDICINAL CHEMISTRY
·
2021
·
IF 6.514
Xing-Rong Wang,Shuai Wang,Wen-Bo Li,Kai-Yan Xu,Xue-Peng Qiao,Xue-Li Jing,Zi-Xiao Wang,Chang-jiang Yang,Shi-Wu Chen
Vascular endothelial growth factor-2 (VEGFR-2) plays a pivotal role in tumor angiogenesis . Herein, a library of novel 2-(4-(1 H -indazol-6-yl)-1 H -pyrazol -1-yl)acetamide derivatives were designed and synthesized as VEGFR-2 inhibitors based on scaffold hopping strategy. These compounds exhibited the excellent inhibitory in both VEGFR-2 and tumor cells proliferation . Especially, compound W13 possessed potent VEGFR-2 inhibition with IC 50 = 1.6 nM and anti-proliferation against HGC-27 tumor cells with IC 50 = 0.36 ± 0.11 μM, as well as less toxicity against normal GES-1 cells with IC 50 = 187.46 ± 10.13 μM. Moreover, W13 obviously inhibited colony formation, migration and invasion of HGC-27 cells by adjusting the expression of MMP-9 and E-cadherin, and induced HGC-27 cells apoptosis by increasing ROS production and regulating the expression of apoptotic proteins. Furthermore, W13 blocked the PI3K-Akt-mTOR signaling pathway in HGC-27 cells. In addition, anti-angiogenesis of W13 was proved by inhibiting tube formation and the expression of p-VEGFR-2 in HUVEC cells. All the results demonstrated that W13 could be developing as a promising anticancer agent for gastric cancer therapy.
✓ 已验证
DOI
PubMed
高影响因子
EUROPEAN JOURNAL OF MEDICINAL CHEMISTRY
·
2024
·
IF 6
Yong-Jun Huang,Yi-Peng Zang,Li-Jun Peng,Ming-Han Yang,Jing Lin,Wei-Min Chen
The low permeability of the outer membrane of Gram-negative bacteria is a serious obstacle to the development of new antibiotics against them. Conjugation of antibiotic with siderophore based on the “Trojan horse strategy” is a promising strategy to overcome the outer membrane obstacle. In this study, series of antibacterial agents were designed and synthesized by conjugating the 3-hydroxypyridin-4(1 H )-one based siderophores with cajaninstilbene acid ( CSA ) derivative 4 which shows good activity against Gram-positive bacteria by targeting their cell membranes but is ineffective against Gram-negative bacteria. Compared to the inactive parent compound 4 , the conjugates 45c or 45d exhibits significant improvement in activity against Gram-negative bacteria, including Escherichia coli , Klebsiella pneumoniae and especially P. aeruginosa (minimum inhibitory concentrations, MICs = 7.8–31.25 μM). The antibacterial activity of the conjugates is attributed to the CSA derivative moiety, and the action mechanism is by disruption of bacterial cell membranes. Further studies on the uptake mechanisms showed that the bacterial siderophore-dependent iron transport system was involved in the uptake of the conjugates. In addition, the conjugates 45c and 45d showed a lower cytotoxic effects in vivo and in vitro and a positive therapeutic effect in the treatment of C. elegans infected by P. aeruginosa . Overall, our work describes a new class and a promising 3-hydroxypyridin-4(1 H )-one- CSA derivative conjugates for further development as antibacterial agents against Gram-negative bacteria.
研究领域:
微生物学
·
药理学
·
传染病学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ZEITSCHRIFT FUR NATURFORSCHUNG SECTION B-A JOURNAL OF CHEMICAL SCIENCES
·
2020
·Vol. 75
·期 8
·733-737
·
IF 0.839
Gao-Feng Wang,Shu-Wen Sun,Hong Sun,Bo-Hui Wei,Yan-Fei Zhao,Li-Xin Meng
A three-dimensional (3D) two-fold interpenetrated coordination polymer, {[Cd(bipmo)(bpda)]·1.25(H 2 O)} n ( 1 ), (bipmo = bis(4-(1H-imidazol-1-yl)phenyl)methanone, H 2 bpda = 1,1ʹ-biphenyl-2,2ʹ-dicarboxylic acid), was synthesized by a solvothermal method. It has been characterized by elemental analyses, infrared (IR) spectroscopy, and single-crystal X-ray diffraction. The topological structure of 1 consists of uninodal dia nets with two-fold penetration. The thermal stability and the luminescence properties of complex 1 were investigated.
研究领域:
化学
·
材料科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Zongxu Liu,Wenyan Wang,Jin Liu,Baolei Zhu,Guoxian Zhang,Jinxin Wang,Hepeng Zhang,Qiuyu Zhang
Nacre-mimetic strategy provides an enlightening approach to design high-performance bioinspired nanocomposites. Yet, it is still a big challenge to integrate excellent mechanical properties and tunable multifunctionality into artificial nacre materials. Herein, we develop a pioneering strategy to simultaneously modulate the electrical conductivity and mechanical properties of nacre-mimetic nanocomposite films by controlling interlay supramolecular interactions. A series of novel waterborne polyurethanes with 2-ureido-4[1H]-pyrimidinone (UPy) quadruple hydrogen bonding motifs in the side-chains were elaborately designed and synthesized, and further assembled with Ti 3 C 2 T x MXene nanosheets to construct lamellar nacre-mimetic nanocomposite films with highly ordered nanostructure. This research revealed for the first time that merely varying the content of UPy groups on polyurethane realize significant modulation of mechanical properties, electrical conductivity, and even the electromagnetic shielding effectiveness of nacre-mimetic nanocomposites. Strikingly, the tensile strength of the nanocomposites can be improved from 87.91 to 136.96 MPa and the electrical conductivity from 3214.0 to 4136.1 S cm −1 when the UPy content is increased from 0 to 15%. Additionally, the nacre-mimetic nanocomposite film is capable of fast responsive Joule heating performance at low trigger voltage. This work would open up a new avenue for fabricating multifunctional and mechanically robust biomimetic nanocomposites.
研究领域:
材料科学
·
纳米技术
·
复合材料
·
仿生学
✓ 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）