APPLIED CATALYSIS B-ENVIRONMENTAL
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2026
·
IF 19.7
Xiao-Hui Wang,Yue-Han Qin,Xue Xiao,Yu Chen,Shu-Ni Li
Histidine-functionalized Cu 2 O effectively stabilizes Cu + species under cathodic conditions. • The histidine functionalization enhances the co-adsorption of *CO and *NO x intermediates. • The formation of an interfacial hydrogen-bond network on the catalyst surface accelerates proton transfer kinetics. • The histidine-functionalized Cu 2 O catalyst achieves a high urea Faradaic efficiency alongside a notably high yield rate. Electrocatalytic C-N coupling for urea synthesis from CO 2 and nitrate (NO 3 - ) offers a sustainable alternative to the energy-intensive industrial process. Copper (Cu)-based catalysts are uniquely capable of activating both CO 2 and NO 3 - ; however, the catalytically active Cu + species is prone to over-reduction to Cu 0 under cathodic conditions, leading to poor selectivity and instability. Herein, we report a histidine-functionalized Cu 2 O nanospheres (His-Cu 2 O NSs) that stabilize Cu + under operating conditions. The preserved Cu + electronic structure promotes synchronized adsorption of *CO and *NO x intermediates, while protonated amino groups construct a hydrogen-bonded interfacial water network that accelerates proton transfer. As a result, the optimized catalyst achieves a urea Faradaic efficiency of 42.3% and a yield rate of 41.9 mmol h −1 g −1 at −1.1 V potential, with exceptional stability over 100 h in both H-type and flow cells. In situ spectroscopy and density functional theory calculations reveal that histidine coordination not only enhances *CO adsorption but also lowers the energy barrier for C-N coupling, thereby accelerating C-N bond formation. Meanwhile, the in-situ EXAFS results indicate that Cu + species can effectively be retained after histidine modification. This work establishes a molecular-level design principle for regulating complex multi-reactant electrocatalysis and provides a versatile strategy for promoting efficient C-N coupling reactions. Download: Download high-res image (156KB) Download: Download full-size image Functionalizing Cu 2 O nanospheres establishes a generalizable stabilization-via-delocalization principle providing a blueprint for designing durable organic-inorganic interfaces for electrocatalytic urea synthesis.
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Atmospheric Pollution Research
·
2022
·
IF 4.831
Mincong Zhu,Mingqiang Huang,Tingting Lu,Shunyou Cai,Xiaobin Shan,Liusi Sheng,Weixiong Zhao,Xuejun Gu,Weijun Zhang
Imidazole and its derivatives are the main heterocyclic nitrogen-containing brown carbon constituents in aerosol particles. Imidazoles of aqueous secondary organic aerosol (aqSOA) particles formed from the reaction of methylglyoxal and ammonium sulphate ((NH 4 ) 2 SO 4 ) are detected by vacuum ultraviolet photoionization aerosol mass spectrometer (VUV-PIMS) in real-time and verified off-line with optical spectrometry in current study. The experimental results showed that the single photon ionization mass spectrum of aqSOA particles measured by VUV-PIMS emerged the molecular ion peaks at m/z = 68, 82 and 110. While, the extraction solution of aqSOA particles detected by off-line techniques demonstrated that the characteristic peaks at 217 and 282 nm appeared in the UV–Vis spectrum; the strong emission in 405–480 nm with maximum emission wavelength at 435 nm contained in the 3D fluorescence spectra; and the chemical shift peaks of hydrogen atoms on N–H, C C and C N bond on imidazole ring and methyl group arised in the 1 H-NMR spectrum. In view of these spectral information, 4-methyl-imidazole and 4-methyl-imidazole-2-carbaldehyde are determined as the principal products of the aqueous reaction between methylglyoxal and (NH 4 ) 2 SO 4 . The possible reaction mechanism leading to the generation of imidazole compounds are also discussed. These will help to understand the formation process of imidazole compounds in atmospheric aerosol particles , and provide experimental basis for the model mechanism study of aqSOA particles.
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JOURNAL OF MOLECULAR LIQUIDS
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2021
·
IF 6.165
Ke Li,Hao Fang,Xiuzhi Duan,Dongshun Deng
Development of high-efficient solvents for NH 3 capture to improve the quality of atmosphere and ecological environment is a hot research topic. Deep eutectic solvents (DESs) as NH 3 absorbents can overcome some problems troubling the traditional NH 3 capture process. In this work, NH 4 SCN was paired with imidazole (Im) DESs to form low viscous DESs with dual active sites for highly efficient NH 3 absorption. The effects of absorption temperature, gas flow rate, water content, molar ratio on NH 3 absorption performance as well as physical properties of NH 4 SCN/Im DESs were systematically investigated. The results show that NH 4 SCN/Im DESs can rapidly capture NH 3 with good recycling performance, while the gas flow rate only shortens the absorption time. The NH 3 absorption capacity of NH 4 SCN/Im DESs decreased with increasing temperature and NH 4 SCN/Im molar ratio. The absorption capacity of NH 4 SCN/Im (1:2) DES reaches 9.65 mol NH 3 /kg DESs for atmospheric NH 3 . Based on 1 H NMR and IR spectroscopy analysis, the strong hydrogen bond between protic ammonium cation and NH 3 plays the major essence of efficient NH 3 capture for NH 4 SCN/Im DESs.
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ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Jiajia Liu,Xiaochen Tang,Huiling Lu,Yingjie Xu
To reveal the interactions between azole-anion-based ionic liquids (AILs) and propargyl alcohol (PA) and their effect on the carboxylative cyclization reaction of PA with CO2, three AILs, namely, [P66614][Im], [P66614][4-MeIm], and [P66614][4-BrIm], were synthesized and characterized. The interactions between the AILs with 2-methyl-3-butyn-2-ol (MBY) were investigated through IR and 1H NMR spectra and DFT calculations. The results indicate that azole-based anions can form H-bonds with the hydroxyl (O–H) and the alkynyl hydrogen atoms (C≡C–H) of MBY simultaneously, with the former much stronger than the latter, which is supported by the interaction energy and the distance of the H-bond from DFT calculations. Interestingly, the strength of the former always increases with the mole fraction of AIL (xAIL), while that of the latter first decreases and then increases, reaching a minimum at xAIL ≈ 0.4. Furthermore, the order of the strength of the two H-bonds is as follows: [P66614][Im] > [P66614][4-MeIm] > [P66614][4-BrIm], which is in good agreement with their basicity. According to the interactions between the AILs with MBY and combined with the reaction mechanism of MBY with CO2 promoted by AILs, it is evident that the increase in the basicity of the AILs enhances the H-bond between the AILs with O–H, thereby enhancing the activation of MBY and the subsequent CO2 conversion. However, this will also increase the interaction between AILs and C≡C–H, resulting in the deprotonation of C≡C–H and hindering the activation of MBY. Therefore, choosing a suitable basic AIL and controlling its ratio are the keys to the reaction of PA and CO2.
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Nanoscale
·
2021
·Vol. 13
·期 7
·4140-4150
·
IF 7.79
Yongjie Zhang,Ning Feng,Shujin Zhou,Xia Xin
Gold nanoclusters (AuNCs) are among the most promising organic–inorganic hybrid luminescent materials for various applications. The current development of AuNCs majorly focuses on controlling their luminescence properties. Herein, we report a new strategy to facilely construct two different nanocomposites featuring enhanced photoluminescence based on mercaptopropionic acid-protected AuNCs (MPA-AuNCs). Through co-assembly with Zn2+ and 2-methylimidazole (2M-IM), the weak luminescence of MPA-AuNCs evolved into either intense blue-green or orange emission at different concentration ratios of additives. HR-TEM and spectroscopic characterization studies revealed that the intense blue-green emission was ascribed to the formation of ZnS quantum dots (QDs) on the outer surface of AuNCs (AuNCs@ZnS), while the strong orange emission originated from the primitive MPA-AuNC core encapsulated by a cubic ZIF-8 shell (AuNCs@ZIF-8). The AuNCs@ZnS nanocomposite was further applied as an exceptional chemical sensor for selective detection of Pb2+ and Fe3+via different quenching mechanisms, and the AuNCs@ZIF-8 composite was applied for fabricating light-converting devices. The co-assembly of AuNCs with Zn2+ and imidazole derivatives provides a facile strategy for acquiring differentiated nanomaterials that have versatile potential applications in chemical detection and light-converting devices.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2020
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IF 5.774
Dan Li,Yong Kang,Jie Li,Zongchi Wang,Zhinan Yan,Kai Sheng
As a successive work towards exploring suitable IL-based absorbents for SO 2 absorption from flue gas, we developed a species of new dicationic ionic liquids (DILs) with the combination of ether-functionalized dication and N-heterocyclic anions. These dual-functionalized DILs possessed high thermal stability, low vapour pressure, and high SO 2 capacity. The solubilities of SO 2 in the DILs increased with declining of the temperature and elevating of the SO 2 concentration. Notably, the available loading capacity of SO 2 in DIL 4 was up to 0.267 g SO 2 ·(g DIL) -1 at 313.2 K when the concentration of SO 2 in the feed gas was 2000 ppm, which was exceedingly significant for trapping SO 2 from the flue gas with low content of SO 2 . The regeneration experiments demonstrated that the absorption capacities of SO 2 in DIL 4 kept unchanged after six successive cycles of absorption/desorption. The absorption mechanisms based on the results of 1 H NMR, FTIR analysis and quantum chemical calculations indicated that both physical and chemical interactions between the SO 2 molecules and DIL 4 could be found in spite of different concentrations of SO 2 .
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2020
·Vol. 22
·期 5
·2849-2857
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IF 3.43
Chaoyue Zhao,Xianliang Qiao,Zenghuimin Yi,Qingxin Guan,Wei Li
A green catalyst for acetylene hydrochlorination yielding a VCM is presented using imidazole as a single component metal-free catalyst. The mechanisms and reactivities of imidazole-catalyzed acetylene hydrochlorination have been investigated by combined computational and experimental studies. The electronic effects of ortho-substituents on the reactivities have also been investigated. Through theoretical calculations and experimental studies, the nitrogen-atom including a lone pair active site of single component imidazole for metal-free acetylene hydrochlorination is proposed. It is suggested that the nitrogen-atom including a lone pair of imidazole adsorbs an HCl molecule to form an imidazole-HCl complex, which serves as the active catalyst to participate in the reaction process of acetylene hydrochlorination. Besides, the results show that C2H2 assists in the electrophilic addition of HCl, undergoing an almost planar six-membered ring transition state. Computational studies on the ortho-substitution of the active sites will have an important impact on the catalytic efficiency.
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Communications Biology
·
2019
·Vol. 2
·期 1
·1-11
·
IF 0
Lin Yanke,Wang Shuai,Zhou Ziyue,Guo Lianxia,Yu Fangjun,Wu Baojian
Metabolism is a major defense mechanism of the body against xenobiotic threats. Here we unravel a critical role of Bmal1 for circadian clock-controlled Cyp3a11 expression and xenobiotic metabolism. Bmal1 deficiency decreases the mRNA, protein and microsomal activity of Cyp3a11, and blunts their circadian rhythms in mice. A screen for Cyp3a11 regulators identifies two circadian genes Dbp and Hnf4α as potential regulatory mediators. Cell-based experiments confirm that Dbp and Hnf4α activate Cyp3a11 transcription by their binding to a D-box and a DR1 element in the Cyp3a11 promoter, respectively. Bmal1 binds to the P1 distal promoter to regulate Hnf4α transcriptionally. Cellular regulation of Cyp3a11 by Bmal1 is Dbp- and Hnf4α-dependent. Bmal1 deficiency sensitizes mice to toxicities of drugs such as aconitine and triptolide (and blunts circadian toxicity rhythmicities) due to elevated drug exposure. In summary, Bmal1 connects circadian clock and Cyp3a11 metabolism, thereby impacting drug detoxification as a function of daily time.
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JOURNAL OF CHROMATOGRAPHY A
·
2023
·
IF 4.1
Rihui Su,Xiaohua Xiao,Gongke Li
Poly(N-isopropylacrylamide) thermosensitive hydrogel tube tip solid-phase extraction/ultra-high liquid chromatography-mass spectrometry (UPLC-MS/MS) method was developed for analysis of methylimidazoles in beverages. Thermosensitive poly(N-isopropylacrylamide) (PNIPA) hydrogel solid-phase extraction (SPE) medium was prepared on the surface of highly internal phase emulsion (HIPE) porous polymer by thermally initiated polymerization in a tube tip. The temperature sensitive SPE medium has the characteristics of high porosity and high specific surface area. When the temperature is higher than 30.0℃, it can well adsorb polar molecular, and could quickly desorb polar molecular when the temperature was less than 20.0℃. The tube tip SPE coupled with UPLC-MS/MS method was established for the determination of three polar molecules including 1-methylimidazole, 4-methylimidazole and 2-methylimidazole, with linear ranges of 2.50 – 240 μg/L, and detection limits of 1.20, 1.20 and 0.65 μg/L, respectively. The method was applied to the determination of three methylimidazoles in beverages with the spiked recoveries of 81.5%-115.5% and the RSD of 0.6%-5.0%, and the relative errors of the results with the national standard UPLC-MS/MS method were in the range of -8.5%-8.9%.
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JOURNAL OF MOLECULAR LIQUIDS
·
2024
·
IF 5.3
Bin Chen,Hegang Shu,Yujun Guo,Yingjie Xu
In this work, the effect of the structure and substitution of azole-based anion on the CO 2 capture and viscosity ( η ) of metal chelate-based dual functional ionic liquids (DFILs) with [K(DGA) 2 ] + cation was investigated. The CO 2 absorption capacity of DFILs at 0.1 MPa and 333.2 K shows that methyl and nitro groups on the azole-based anion, such as pyrazolide ([Pyr] − ) and imidazolide ([Im] − ), attenuate their reactivity with CO 2 through the steric hindrance and electron-withdrawing effects, respectively. Furthermore, the CO 2 absorption capacity of [K(DGA) 2 ][Pyr] is larger than that of [K(DGA) 2 ][Im], which is due to the interaction of the two adjacent N atoms in the [Pyr] − anion with CO 2 , as confirmed by DFT calculations. The CO 2 absorption mechanism shows that both [Pyr] − anion and [K(DGA) 2 ] + cation of [K(DGA) 2 ][Pyr] can chemically interact with CO 2 , making its saturated uptake at 333.2 K as high as 1.47 mol CO 2 per mole IL. Moreover, CO 2 interacts preferentially with [Pyr] − , and the [K(DGA) 2 ] + –CO 2 interaction is enhanced when the CO 2 uptake is greater than 0.5 mol CO 2 per mole IL. η of pure [K(DGA) 2 ][Pyr] is lower than that of pure [K(DGA) 2 ][Im]. η of [K(DGA) 2 ][Pyr] increases with the increase of CO 2 absorption, and the rapid increase in η after CO 2 uptake greater than 0.5 is attributed to the formation of [K(DGA) 2 ] + –CO 2 interactions.
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JOURNAL OF HAZARDOUS MATERIALS
·
2013
·
IF 3.925
Zhike Wang,Cunling Ye,Juan Li,Heping Wang,Han Zhang
The objective of this work was to improve the understanding the influence of the methyl group at different positions of imidazolium ring on the adsorption behaviors of imidazole-modified silica adsorbents. Five adsorbents named as SilprImCl, SilprM 1 ImCl, SilprM 2 ImCl, SilprM 4 ImCl and SilprM 1 M 2 ImCl were synthesized using imidazole , 1-methylimidazole, 2-methylimidazole, 4-methylimidazole and 1,2-dimethylimidazole, respectively. These adsorbents were characterized by scanning electron microscope, infrared spectra, thermogravimetric analysis, elemental analysis and BET analysis. Firstly, phenol, 2-nitrophenol (2-NP), 3-nitrophenol (3-NP), 4-nitrophenol (4-NP) and 2,4-dinitrophenol (2,4-DNP) were used as adsorbates to investigate the selectivity of SilprImCl and its adsorption capacities followed the order of 2,4-DNP ≫ 4-NP > 2-NP ≫ 3-NP > phenol. Therefore, 2,4-DNP was used to investigate the adsorption behaviors of the five adsorbents. It was inferred that the adsorbents are of primary anion-exchange and electrostatic nature. The electrostatic nature was affected significantly by the methyl group at different positions of imidazolium ring. The adsorbed amounts of 2,4-DNP decreased in the order of: SilprM 1 M 2 ImCl ≈ SilprM 1 ImCl > SilprM 4 ImCl > SilprM 2 ImCl > SilprImCl. The adsorption–elution experiments indicated that 2,4-DNP can be removed from aqueous solutions by a SilprM 4 ImCl packed column and the recovery of 91.6% was obtained. The adsorbent could be regenerated and reused ten times at least by simple washings with HCl and water in turn.
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TALANTA
·
2025
·
IF 6.1
Yifei Ma,Lijie Zhang,Hong Yang,Shanshan Zhu,Jinhua Liu
Highly selective and sensitive determination of dopamine (DA) from multiple sources remains a persistent and significant challenge. Here, we develop an imidazole-triggered in situ fluorescence reaction system for highly selective and sensitive determination of DA from various sources (human, horse, dog, rabbit, and mouse). The system operates by catalyzing the oxidation of DA with 1,5-Dihydroxynaphthalene (1,5-DHA) through a Lewis base formed by imidazole, leading to the rapid generation of yellow azamonardine fluorescent compounds (AFC). Notably, the system demonstrates minimal background noise and a high signal-to-noise ratio of up to 300-fold with a determination limit of 33.33 pM, making it 10-100 times more sensitive than conventional enzyme-linked immunosorbent assay (ELISA) methods. Moreover, selectivity tests reveal that our system can effectively distinguish between several common interfering substances, even at concentrations as low as 10 nM. The developed system shows promising results in detecting DA from diverse sources (humans, horses, dogs, rabbits, and mice), including urine samples from clinical patients, exhibiting good agreement with traditional ELISA kits. Therefore, the established in situ fluorescence reaction system holds great potential for the determination of DA-related disorders due to its impressive analytical capabilities.
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