Molecular Catalysis
·
2023
·
IF 4.6
Ziliang Yuan,Xun Li,Guanghui Wang,Zhihua Zhu,Yuhe Liao,Zehui Zhang,Bing Liu
The selective hydrogenation of N -heteroarenes into N -heterocycles is a highly important organic transformation in fine chemical industry, as N -heterocycles are moieties in a variety of pharmaceutical and bioactive compounds. Here, we report highly efficient mesoporous CeO 2 supported Ni catalysts prepared by the incipient wet impregnation and following high-temperature reduction for the selective hydrogenation of N -heteroarenes. The experiments indicated that the synergistic effect between CeO 2 and Ni nanoparticles was responsible to the superior catalytic performance. Various kinds of N -heterocycles were obtained at 120 °C with yields of 86 ∼ >99%, demonstrating the versatility of the developed method. This work is valuable for guiding the design and manipulation of low metal loading, cost-effective and robust hydrogenation catalysts.
研究领域:
化学工程
·
材料科学
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产品关联
DOI
高影响因子
ACS ES&T Engineering
·
2025
·
IF 6.7
Baoqiang Hao,Renyuan Zhang,Genye He,Zishi An,Xiaoqing Li,Jing Li
The combined application of UV254 irradiation and chlorination (UV/chlorine) is considered to be a promising method for the disinfection and removal of organic pollutants. However, it is not clear how this process affects the formation of disinfection by-products (DBPs). In this study, the formation of DBPs from 11 of the most commonly used azoles in the UV/chlorine process has been investigated. The study demonstrated that dichloroacetylene, a previously unreported DBP, was identified as a coproduct of azoles. In addition to dichloroacetylene, another toxic DBP, cyanogen chloride (CNCl), was also detected in the process. However, neither dichloroacetylene nor CNCl was detected in the presence of azoles during chlorination alone. The results indicated that •OH and •Cl radicals resulting from UV/chlorine were the key factors in the production of dichloroacetylene and CNCl. Further studies have shown that dichloroacetylene was relatively stable in water with a hydrolysis half-life of 77 h and can be degraded in the presence of UV irradiation or high doses of chlorine. Additionally, bromochloroacetylene was observed in the UV/chlorine system in the presence of bromide. Furthermore, the presence of dichloroacetylene was detected in real UV/chlorine-treated water samples at concentrations ranging from 0.06 to 0.18 μM. This was found to be significantly increased by the addition of pyrazole, as was the case with CNCl. Dichloroacetylene and CNCl were detected in wastewater treatment plants at concentrations ranging from 0.15 to 0.31 μM. This finding suggested that the active species of the UV/chlorine process may alter the DBP formation pathway and lead to the emergence of novel toxic DBPs that have not yet been identified.
研究领域:
环境科学
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公共卫生
·
化学工程
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产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2021
·
IF 8.271
Fangjun Shao,Zihao Yao,Yijing Gao,Qiang Zhou,Zhikang Bao,Guilin Zhuang,Xing Zhong,Chuan Wu,Zhongzhe Wei,Jianguo Wang
The development of bifunctional catalysts for the efficient hydrogenation and acceptorless dehydrogenation of N -heterocycles is a challenge. In this study, Ru 2 P/AC effectively promoted reversible transformations between unsaturated and saturated N -heterocycles affording yields of 98% and 99%, respectively. Moreover, a remarkable enhancement in the reusability of Ru 2 P/AC was observed compared with other Ru-based catalysts. According to density functional theory calculations, the superior performance of Ru 2 P/AC was ascribed to specific synergistic factors, namely geometric and electronic effects induced by P. P greatly reduced the large Ru-Ru ensembles and finely modified the electronic structures, leading to a low reaction barrier and high desorption ability of the catalyst, further boosting the hydrogenation and acceptorless dehydrogenation processes.
研究领域:
催化化学
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材料科学
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理论化学
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DOI
高影响因子
Current Analytical Chemistry
·
2021
·Vol. 17
·期 7
·1027-1036
·
IF 1.892
Qiao Dan,Deng Qiliang,Wang Shuo
Background: The approach for the determination of aminoimidazo-azaarenes (AIAs) is urgently required due to their mutagenic activity and potential carcinogenicity. For this purpose, a CdSe/ZnS quantum dots (CdSe/ZnS QDs)-embedded molecularly imprinted silica gel with high selectivity
and sensitivity was successfully prepared and applied to analyze such target. Methods: Herein, CdSe/ZnS QDs acted as the fluorescent probe, and molecularly imprinted silica gel as a recognition probe was synthesized on the surface of QDs via sol-gel method. 2- Aminobenzimidazole, which
has a similar structure with AIAs, as well as low cost and low toxicity, was selected as the dummy template. Results: The material has a high imprinting factor (IF=6.15); the linear range of CdSe/ZnS@MIP as a fluorescent sensing material for AIAs is 0.5-20.0 μg L-1
with the limit of detection (LOD) of 0.25 μg L-1 (3σ/s). Moreover, the fluorescent materials have been further applied to determine AIAs in beef floss and grilled fish fillet with satisfactory recoveries (82.8-110.8 %), and the relative standard deviation (RSD)
is < 5.5%. Conclusion: The proposed CdSe/ZnS QDs-embedded molecularly imprinted silica gel can be used to easily and selectively detect AIAs.
研究领域:
分析化学
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环境科学
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食品安全
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产品关联
DOI
高影响因子
Journal of Energy Chemistry
·
2025
·
IF 14.9
Dengqi Zhou,Ke Zeng,Liqiang Wang,Feiying Tang
The development of highly efficient non-noble metal catalysts for the hydrogenation of N-heteroarenes under mild condition is of great importance for both theoretical and industrial applications, which can efficiently reduce energy consumption and environmental pollution. In this work, we found that the prepared CoCu nano-alloy catalyst after exposed in the air over 24 h (named Co 1 Cu 1 /C) exhibited a dramatically improved catalytic performance (yield from trace to >99%) for quinoline hydrogenation under mild reaction conditions (60 °C, 3 MPa H 2 ). According to the characterization, the catalyst Co 1 Cu 1 /C exhibited the strong interaction between Co and Cu. Meanwhile, it was endowed with a stable partial oxidation surface. The unsaturated oxygen coordinated surface of Co 1 Cu 1 /C presented a moderate binding for quinoline and 1, 2, 3, 4-tetrahydroquinoline, which could efficiently avoid the deactivation of catalyst and favor the hydrogenation kinetics. The density functional theory (DFT) calculations coupled with X ray-based structural analyses suggested that the unsaturated oxygen coordinated surface could lower the diffusion energy of the active hydrogen species and the reaction barrier for quinoline hydrogenation which resulted from the d - p orbital electron coupling. This work revealed that the catalytic performance of nano-alloy catalysts might not only be ascribed to the interaction between metals, while the unsaturated oxygen coordination of metallic surfaces played an important role.
研究领域:
催化化学
·
材料科学
·
理论化学
✓ 已验证
DOI
高影响因子
FOOD CHEMISTRY
·
2022
·
IF 9.231
Xiang-Rong Cheng,Jia-Hui Ma,Issoufou Amadou,Wei Zhao,Yu-Yao Chen,Chen-Xi Zhang,Bin Guan
Xiaoheiyao is the rhizome of Inula nervosa Wall., a traditional spice and medicinal herb in China. In this study, the creatinine inhibitor from Xiaoheiyao extract and also the effects and mechanism on the production of heterocyclic aromatic amines (HAAs) were investigated. Xiaoheiyao extract inhibited the total contents of seven detected HAAs in grilled beef patties, particularly aminoimidazole-azaarenes (AIAs) in a dose-dependent manner, reaching a maximum inhibition rate of 62% for total HAAs and 73% for AIAs. The most effective subfraction of Xiaoheiyao extract (IER80) contained abundant potential creatinine inhibitors, as revealed by immobilized creatinine probe, HPLC and UPLC-MS/MS analyses. Moreover, electrophilic p -coumaric acid derivatives were discovered from IER80 by feature based molecular networking. p -Coumaric acid was demonstrated to inhibit the contents of total HAAs and AIAs in grilled beef patties and model system. Quantitative analyses of the precursor and intermediates of AIAs in model system revealed that p -coumaric acid mainly affected the generation of AIAs by inhibiting creatinine.
研究领域:
食品科学
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药理学
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化学
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产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2017
·Vol. 8
·期 1
·1-7
·
IF 12.124
Lin Jin,Li Zhi,Kan Jian,Huang Shijun,Su Weiping,Li Yadong
Catalytic oxidative C–H bond functionalization reactions that proceed without requiring stoichiometric amounts of external oxidants or pre-functionalized oxidizing reagents could maximize the atom- and step-economy in chemical syntheses. However, such a transformation remains elusive. Here, we report that a photo-driven catalytic process enables decarboxylative C–H trifluoromethylation of (hetero)arenes with trifluoroacetic acid as a trifluoromethyl source in good yields in the presence of an external oxidant in far lower than stoichiometric amounts (for example, 0.2 equivalents of Na 2 S 2 O 8 ) using Rh-modified TiO 2 nanoparticles as a photocatalyst, in which H 2 release is an important driving force for the reaction. Our findings not only provide an approach to accessing valuable decarboxylative C–H trifluoromethylations via activation of abundant but inert trifluoroacetic acid towards oxidative decarboxylation and trifluoromethyl radical formation, but also demonstrate that a photo-driven catalytic process is a promising way to achieve external oxidant-free C–H functionalization reactions.
研究领域:
有机化学
·
催化
·
光化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）