SYNTHESIS-STUTTGART
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2019
·Vol. 51
·期 17
·3221-3230
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IF 2.867
Wei Sun,Mingjuan Zhang,Peilang Li,Yiqun Li
A novel and highly efficient one-pot synthesis of polysubstituted imidazoles from α-hydroxyphenylacetic acids, diphenylacetylene, and amines has been achieved by Pd(OAc)2/Ce(SO4)2/Bi(NO3)3 trimetallic catalytic system. A series of control experiments showed that this overall reaction occurs through a one-pot cascade process combining the steps of decarboxylation of α-hydroxyphenylacetic acids, Wacker-type oxidation of diphenylacetylene, and Debus–Radziszewski annulation of aryl aldehydes and benzil generated in situ, as well as amines. This reaction represents a novel multicomponent reaction using α-hydroxyphenylacetic acids and diphenylacetylene as sources of aryl aldehydes and a β-diketone. This process exhibits a broad substrate scope and a good functional group tolerance to assemble the corresponding polysubstituted imidazoles in excellent yields (72–88%) under mild conditions.
研究领域:
有机化学
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催化化学
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药物化学
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合成方法学
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杂环化学
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Jie Wu,Yuanyuan Zhang,Bin Zhang,Siwei Li,Ping Xu
Development of low-cost, efficient, and durable electrocatalysts for the oxygen evolution reaction (OER) is crucial for multiple energy conversions and storage devices. Herein, Zn-doped CoS2 nanoarrays supported on carbon cloth, Co(Zn)S2/CC, are fabricated through a facile sulfidization of CoZn metal–organic frameworks. This precatalyst, Co(Zn)S2/CC, with a well-defined nanoarray structure affords excellent OER catalytic activity (η = 248 mV at 10 mA/cm2) and long-term durability in 1 M KOH. X-ray photoelectron and in situ Raman spectroscopic studies indicate that Co(Zn)S2 undergoes surface reconstruction with the generation of Co(Zn)OOH adsorbed with SO42– at the surface during the OER process. The Zn dopant is calculated to impact on the electronic structure of Co species and further the adsorption of intermediates. This work not only provides a novel method for the synthesis of bimetallic sulfides but also gives insights into the doping effect on the OER performance of transition metal sulfides.
研究领域:
电化学
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材料科学
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能量转换与存储
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产品关联
DOI
PubMed
高影响因子
CRYSTAL GROWTH & DESIGN
·
2018
·
IF 3.972
Fangfang He,Qian Wang,Cuifang Hu,Wen He,Xueying Luo,Ling Huang,Daojiang Gao,Jian Bi,Xin Wang,Guohong Zou
Two new antimony sulfate chlorides named (NH4)2SbCl(SO4)2 and (NH4)SbCl2(SO4) were successfully synthesized through solvent-free synthesis method. (NH4)2SbCl(SO4)2 exhibits a three-dimensional framework constructed of [SbCl(SO4)2]2– chains and NH4+ ions. And the NH4+ cations play the role of charge balance and provide the hydrogen bond constructed with oxygen atoms. (NH4)SbCl2(SO4) shows a two-dimensional layer structure that is composed of the regularly stacked [SbCl2(SO4)]− chains via hydrogen-bonding interactions. Both of the titled compounds possess the same chemical composition and the similar Sb–Cl–SO4 chains, while hydrogen-bonding interactions and lone-pair cations play the synergistic effect on the framework structures and macroscopic centricities resulting in that the (NH4)2SbCl(SO4)2 is centrosymmetric and the (NH4)SbCl2(SO4) is non-centrosymmetric (NCS). Powder second harmonic generation (SHG) measurements indicated that the NCS compound (NH4)SbCl2(SO4) is type I phase-matchable and exhibits SHG responses of ∼1.7 times that of KH2PO4.
研究领域:
材料科学
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晶体学
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产品关联
DOI
高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2023
·
IF 5.9
Renjie Ji,Mingya Liu,Jingyun Zhang,Zewei Hu,Hanli Zheng,Yunxi Hou,Jianfeng Liu,Shitao Yu,Shiwei Liu,Lu Li,Yue Liu
A core-shell carbon-based catalyst mZSM-5@SO 4 2- /mC-1.5N with mZSM-5 as core and SO 4 2- /mC-1.5 N as shell was prepared using phenolic resin as carbon source. The conversion of xylose was 97.4% and the furfural yield was 75.4% at 140 ℃ for 1 h when the catalyst was used to the reaction of xylose to furfural. The high activity of mZSM-5@SO 4 2- /mC-1.5 N was attributed to the core-shell structure could construct a high activity Brønsted acid-Lewis acid (BA-LA) interface, which promoted the synergistic effect of LA and BA and was conducive to the xylose-furfural cascade reaction. In additon, the combination of HNO 3 activation and H 2 SO 4 grafting method adjusted the density of -OH, -COOH and -SO 3 H on the mC surface, improved the Brønsted/Lewis (B/L) and hydrophilicity of the catalyst, and promoted the adsorption, fixation and transformation of xylose. Then, the effect -OH, -COOH and -SO 3 H in the reaction of xylose-furfural was studied by characterization analysis. Finally, the experimental results showed that mZSM-5@SO 4 2- /mC-1.5 N could reduce the activation energy of the xylose-furfural reaction, and the catalyst could maintain good stability after recycling and regeneration.
研究领域:
催化
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化学工程
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材料科学
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生物化学
✓ 已验证
产品关联
DOI
高影响因子
ChemSusChem
·
2020
·Vol. 13
·期 9
·2239-2244
·
IF 7.962
Yuwen Luo,Feipeng Zheng,Luojia Liu,Kaixiang Lei,Xuesen Hou,Gang Xu,Hui Meng,Jifu Shi,Fujun Li
Graphical Tunable operating voltage : The anion effect induces a varied redox ability of p-type organic radicals, leading to tunable operating voltage of Zn–organic radical batteries. DFT calculations reveal that the stronger interaction of the anion with the organic radical host, the higher the operating voltage of the Zn–organic radical battery. In contrast to traditional rechargeable rock-chair metal-ion batteries, dual-ion batteries (DIBs) involve redox reactions with anions rather than cations in p-type cathodes. In principle, regulating the electrochemical performance of the DIB by different anion species is highly feasible. Herein, the anion effect on the electrochemical performance of a DIB, the aqueous Zn– organic radical battery (Zn-ORB), consisting of a poly(2,2,6,6tetramethylpiperidinyloxy-4-yl vinyl ether) cathode and a Zn anode, was investigated by DFT calculations. SO 4 2− , CF 3 SO 3 − , and ClO 4 − with different molecular electrostatic potential values were selected as anion models. DFT calculations revealed that a stronger electrostatic interaction of the anion with the organic radical resulted in a higher operating voltage of the Zn-ORB, which was consistent with experimental results. These results bring new insight into the redox chemistry of p-type organic radicals with anions and will promote the development of high-power aqueous Zn-ORBs as well as inspire more investigations into the anion effect towards novel battery designs.
研究领域:
电化学
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电池技术
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材料科学
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计算化学
✓ 已验证
DOI
高影响因子
HYDROMETALLURGY
·
2025
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IF 5.3
Yanfei Fan,Dandan Gao,Dongdong Li,Dewen Zeng
Alum is an important intermediate for the extraction and purification of Cs or Rb chemicals, due to its excellent separation ability for Cs, Rb and K. Although the solubility sequence K-alum > Rb-alum > Cs-alum has been well known, the separation factors among Cs, Rb and K during the formation of alum have not been determined. The formation of solid solution of alum controls the Cs or Rb content and Cs/Rb/K ratio in the sequentially precipitated Cs, Rb and K alums. In this study, the thermodynamic equilibrium separation factors were determined from the solid solution-aqueous solution equilibrium data of the two mixed alum systems: (i) RbAl(SO 4 ) 2 , CsAl(SO 4 ) 2 , and H 2 O, and (ii) KAl(SO 4 ) 2 , RbAl(SO 4 ) 2 and H 2 O. The separation factor β Cs/Rb varied from 48 to 2 with the increase of the Rb/Cs ratio in system (i), and β Rb/K varied from 22 to 0.2 with the increase of the K/Rb ratio in system (ii). This suggests that the purification of Cs or Rb using alums is more efficient from raw materials containing high Cs/Rb or Rb/K ratio than that from low Cs/Rb or Rb/K ratio. In kinetic studies, the apparent separation factors β Cs/Rb and β Rb/K were highly affected by the recrystallization process of cooling or non-cooling and the initial composition of raw alum, showing asymmetric kinetic intensification. The separation factors β Cs/Rb or β Rb/K obtained in the “dissolution by heating and crystallization by cooling (DHCC)” process for the raw alum with high initial Cs/Rb or Rb/K molar ratio is several times larger than the equilibrium value expected from thermodynamics. Finally, CsAl(SO 4 ) 2 and RbAl(SO 4 ) 2 with a metal-based purity of 99.97 % and 99.94 %, respectively, were obtained by using the DHCC process 3–4 times.
研究领域:
化学工程
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材料科学
✓ 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）