FUEL
·
2024
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IF 6.7
Yurou Shao,Yangyang Jiang,Dong Wang,Benshuai Guo,Jingyan Zhao,Zhibin Zhou,Jianqiu Chen,Ruixin Guo,Yuntao Lei,Lili Jin
Capturing and recovering carbon dioxide (CO 2 ) from the combustion of fossil fuels is an effective way to reduce carbon emissions, as CO 2 is not only a threat to the environment but also an important C1 feedstock. In the current work, a series of trioctylphosphine oxide (TOPO)-based azole deep eutectic solvents (DESs) have been synthesized for the efficient absorption of CO 2 . The solid–liquid phase diagrams of the DESs were projected using the prediction data from COSMO-RS, and the experimental melting temperature was found to be lower than that of the prediction. These DESs exhibit satisfactory physical properties, including low viscosities (20–60 mPa·s) and high thermal decomposition temperatures (up to 192.5 °C). Furthermore, the CO 2 uptake process was carried out at 35 °C and 0.1 MPa, and the results demonstrated that the CO 2 uptake capacity was positively influenced by hydrogen bond donors (HBDs), mole fraction of HBDs, temperatures, and humidity. Among the DESs, TOPO-imidazole (1:1) was notable for its high absorption capacity of 0.062 mol CO 2 /mol DES, as well as its excellent recyclability. There was no discernible decline in the CO 2 uptake capacity after four absorption–desorption cycles. In this work, NMR and FT-IR investigations indicated the physical absorption mechanism of this system. The designed DESs have the potential to be effective absorbents for efficient reversible CO 2 capture.
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JOURNAL OF FLUORESCENCE
·
2017
·Vol. 27
·期 5
·1721-1727
·
IF 1.461
Wang Fanwei,Duan Hongdong,Xing Dianxiang,Yang Geng
One novel turn-on fluorescence probe founded on conjugated pyrazole Schiff base for detecting Al 3+ was invented. The UV–vis and fluorescence spectrometer were employed to explore optical properties of this probe. The results got from those experiments indicated that this fluorescence probe manifested excellent sensitivity and selectivity for Al 3+ compared with other cations examined(Ag + , Co 2+ , Mg 2+ , Cu 2+ , Ni 2+ , Pb 2+ ,and Zn 2+ ). In addition, this probe displayed a more rapid response and remained stable between pH 6 and 9 by investigating the fluorescence intensity under different response time and various pH values. Remarkably, the detection limit for Al 3+ could lower to 1.0×10 −9 M. Therefore, the probe could be potentially applied to the environment for the detection of Al 3+ , and the availability in biological range of pH that could be further studied to make this probe apply to biological systems in the future.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Xiaojiang Li,Xingqiao Zhang,Chengwei Zuo,Han Zhang,Zhenfu Jia
Cleaner recovery of petroleum hydrocarbons is a key process for waste oil and gas resources, especially oily waste solid. However, the direct recovery of petroleum hydrocarbons is difficult with deep eutectic solvents (DES) without other additives (such as water). In this work, ionic liquid-based DESs (ILs-DESs) with a controllable polarity were prepared for the sustainable recovery of petroleum hydrocarbons. Here, CO2-responsive ionic liquids were prepared by the neutralization reaction of 1,8-diazabicyclo[5.4.0]undec-7-ene and iminazole (Im), pyrazol (Py), or triazole (Tri). Then, the ILs-DESs were separately prepared by using ionic liquids as proton acceptors and straight-chain alcohols (carbon number = 4, 6, 8, 10, and 12) as proton donors. The polarity transformation of the ILs-DESs was regulated only by the introduction and removal of CO2, which was caused by the reversible transformation from ILs-DESs with a lower polarity to alkyl carbonate and carbamate with higher polarity upon CO2. Because of the polarity changes, the simulated oil (such as n-dodecane or diesel oil) was mixed with ILs-DESs, and the samples were directly separated by introducing CO2. Finally, a sustainable process for treating oil sands and oily sludge by using ILs-DESs was developed, where the ILs-DESs were also reused more than twice. This implies that a sustainable approach for petroleum hydrocarbon recovery was realized by using DESs.
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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.
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INORGANIC CHEMISTRY
·
2025
·
IF 4.7
Yu-Lei Gao,Li-Xing Zhao,Qing-Yu Du,Lei-Lei Guo,Han-Xue Sun,Si-Zhe Li,Hao-Wen Cui,Xue-Yun Geng,Xiao-Yu Li,Guo-Ming Wang
In this paper, a polynuclear heterometallic compound (H3O)[Al3Ni4(OH)6(MBA-NO2)6(H2O)6] (Al3Ni4, H2MBA-NO2 = 2-hydroxy-3-methoxy-5-nitrobenzoic acid) with a seven-star disk metal core has been synthesized by the solvothermal method. Al3Ni4 has good stability in water and several organic solvents, and its solid powder shows a good photothermal effect under 980 nm laser irradiation, and the temperature can reach 138.8 °C within 100 s under 1.0 W cm–2 power irradiation. Considering its good photothermal effect, water evaporation of Al3Ni4 was measured. It can be further used as a photothermal material in seawater evaporation.
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Green Energy & Environment
·
2025
·
IF 14.6
Xiang Hui,Jianhui Shi,Jiajun Zhang,Yan Cao,Huiquan Li,Peng He,Liguo Wang
The carbonylation of amines offers a promising route for synthesizing N-substituted carbamates with high atom economy. However, conventional catalysts exhibit limited catalytic efficiency, and the underlying proton transfer mechanism remains elusive. Herein, we reported a metal-free, room-temperature strategy utilizing 1,5,7-triazabicyclo[4.4.0]dec-5-ene (TBD) as a dual hydrogen bond catalyst to synergistically activate propylamine (PA) and dimethyl carbonate (DMC). This green catalytic system achieves a 10-fold acceleration in reaction rate compared to other hydrogen bonding catalysts under mild conditions. This is enabled by dual hydrogen bonding of TBD with PA and DMC, which facilitates rapid proton transfer and stabilizes tetrahedral intermediates. Theoretical calculations confirm that the dual hydrogen bond system significantly lowers activation energy compared to single hydrogen bond analogs. Furthermore, it was revealed that the hydrogen bonding network within the product is the primary factor responsible for the sluggish reaction rate. This study demonstrates the effectiveness of a dual hydrogen bond system in accelerating the carbonylation of amines and provides a green route to access carbamates.
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Advanced Science
·
2025
·
IF 14.1
Guo-Shan Zhu,Ren-Jie Hui,Jun Hu
The electrochemically generated carbocations are pivotal yet elusive intermediates in electrosynthesis. By coupling nanoelectrospray ionization with a tip-confined electrochemical microreactor, the ultrafast transfer of the electrogenerated species into the charged microdroplets is achieved. Interestingly, the highly reactive carbocations become abnormally inert in the electrosprayed microdroplets, and made a survival throughout the entire lifespans of the microdroplets. By taking full advantage of the newfangled stabilizing effect of the microdroplets, the direct mass spectrometric identification of the electrogenerated transient benzylic and phenylic carbocations, whose half-lives in bulk solutions are on the nanosecond level is achieved. The detailed paths of the carbocation-driven C(sp 3 )–H and C(sp 2 )–H aminations are also revealed by the stepwise evaluation of their initial electrochemical generation and their ultrafast succedent chemical transformations. With its high sensitivity, excellent specificity, and minimal time delay, the wide applications of the in situ electrochemical mass spectrometry is anticipated as a powerful tool for not only the identification of previously unseen intermediates but also the in-depth exploration of the intricate electrochemical transformations.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Wanting Zhang,Jiawei Ruan,Xinzi Wu,Qian Liu,Kunchi Xie,Lifang Chen,Zhiwen Qi
The transformation of captured CO 2 into highly-valued dimethyl carbonate (DMC) is a promising approach for CO 2 capture and utilization. However, the direct synthesis of DMC from CO 2 and methanol is limited by high activation barrier derived from inert CO 2 and thermodynamic equilibrium constraints. Herein, three 1-butyl-1-methylpyrrolidinium (BMP)-based ionic liquid (ILs) with polar pyrrole, pyrazole, and 1,2,4-triazole (Tz) azole anions were designed to integrate CO 2 absorption and transformation into DMC. [BMP][Tz] exhibits a relatively high CO 2 uptake capacity of 0.6 mol·mol IL −1 and DMC yield reaches 12.2 % under mild reaction conditions of atmospheric temperature and pressure in 12 h. The reaction equilibrium thermodynamic model reveals that the process involves a combination of 1:1 and 2:1 stoichiometric reaction between [BMP][Tz] and CO 2 . Density functional theory calculations verify that [BMP][Tz] with increased absorption efficiency of azole anions promotes critical bond activation (particular C − O and O − H bonds), thereby enhancing catalytic efficiency. Besides, the reaction mechanism is clarified by the calculation of intermediates and transition state, wherein [BMP][Tz] can efficiently decrease the energy barrier of the rate-controlled step, which involves the insertion of CH 3 O − into CH 3 OCOO − species. Furthermore, polarity-induced phase separation of DMC from the IL phase to solvent phase favors DMC generation by breaking through the reaction equilibrium. The integration of CO 2 absorption-reaction-extraction based on basic and polar ILs, provides a promising approach for CO 2 capture and utilization.
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INORGANIC CHEMISTRY
·
2025
·
IF 4.7
Bao-Yi Jian,Xin-Ye Ren,Chen-Yu Dong,Lian-Cai An,Song-De Han,Guo-Ming Wang
Molecular piezoelectrics have garnered significant attention in energy harvesting and sensing fields due to their high intrinsic piezoelectricity, low elastic properties, and excellent solution processability. Recent efforts have primarily focused on rationally tuning the piezoelectric performance of these materials through the molecular predesign of organic components. However, the regulation of piezoelectric properties via the central metal ion has remained relatively underexplored. Herein, we report the mechanical properties and the piezoelectric output performances of three isostructural molecular piezoelectrics, [PhB(pz)3]2TM (PhB = phenylboronic acid, pz = pyrazole, TM = Fe(II), 1-Fe; Co, 2-Co; Ni, 3-Ni), via first-principles calculations and piezoelectric experiments. Compared with 1-Fe and 3-Ni, 2-Co shows an enhanced structural distortions arising from Jahn–Teller effect, the unequal occupancy of degenerate orbitals of 3d7 and enhanced polarization degree. The composite films of 2-Co dispersed in poly(butyleneadipate-co-terephthalate) (PBAT) are fabricated as piezoelectric generators (PEGs) and display enhanced performances with open-circuit voltages (Voc) of 3.5 V, and short-circuit current (Isc) of 1.4 μA. Moreover, 2-Co PEG can successfully detect human motion sensing including fingertip taping, finger bending, and walking. This work emphasizes the importance of the Jahn–Teller effect in molecular piezoelectrics and provides a strong tool to design and engineer the piezoelectric performance.
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