ATMOSPHERIC ENVIRONMENT
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2024
·
IF 4.2
Hongxing Yang,Wangjin Yang,Jiawei Ma,Chong Han
The heterogeneous reactions of SO 2 on organic aerosols (OA) have been proposed as a significant source of sulfates. The photochemical conversion of SO 2 to sulfates on the surface of light-absorbing OA, i.e., brown carbon (BrC), remained slight understanding. Herein, the photochemical uptake of SO 2 on typical BrC species, including aromatic carbonyl compounds (ACs), polycyclic aromatic hydrocarbons (PAHs) and phenols (PHs), was systematically investigated by a flow tube reactor. Light can significantly promote the uptake of SO 2 on all BrC species used here, especially for ACs. The initial and steady-state uptake coefficients (γ i and γ ss ) of SO 2 exhibited positive relationships with the light intensity, whereas they negatively correlated with the initial SO 2 concentration. Significant sulfate formation was clearly observed with in situ attenuated total internal reflection infrared (ATR-IR) spectrometer, and H 2 O and O 2 had obvious enhancement effects on the sulfate production. Photoinduced •OH, which primarily originated from •O 2 − that was generated through an electron transfer process on BrC under irradiation, was determined to be a key driver for the oxidation of SO 2 to sulfates. Finally, SO 2 lifetime and sulfate formation rate were evaluated on the basis of experimental results, highlighting potential contributions of BrC photochemistry to atmospheric SO 2 loss and sulfate sources.
研究领域:
大气科学
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环境化学
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
·
IF 9.7
Zhujiang Wang,Jun Wu,Jieyu Li,Yingxue Fu,Jiaqi Long,Lin Wu,Fenghua Shen,Hao Chen,Kaisong Xiang,Hui Liu,Liyuan Chai
The electrocatalytic reduction of sulfur dioxide (SO 2 ) to hydrogen sulfide (H 2 S) is a promising strategy for efficient sulfur resource utilization. Copper (Cu) catalysts show high selectivity for SO 2 reduction, but their limited hydrogenation capacity restricts H 2 S production. Palladium (Pd), known for its hydrogenation efficiency, was incorporated to overcome this limitation. We synthesized CuPd bimetallic catalysts to enhance hydrogenation efficiency in SO 2 electroreduction. Among these, Cu 67 Pd 33 exhibited superior catalytic performance, achieving a H 2 S partial current density of 201.56 mA·cm −2 (1.08 mmol·cm −2 ·h −1 ), a 120 % increase over Cu and 154 % over Pd. In-situ Fourier-transform infrared spectroscopy (FTIR) and density functional theory (DFT) calculations revealed that Cu primarily catalyzes the reduction of *SOH to *S, while Pd facilitates the activation and dissociation of interfacial water to provide hydrogen and reduces the energy barrier for the conversion of *S to *H 2 S. The synergistic catalysis between Cu and Pd ensures efficient transformation of intermediates and facilitates the conversion of SO 2 to H 2 S. This study highlights a novel strategy for enhancing hydrogenation in SO 2 electroreduction and provides insights into the synergistic mechanisms of CuPd bimetallic catalysts, emphasizing the critical role of interfacial interactions in catalytic performance.
研究领域:
电化学
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催化材料
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环境科学
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DOI
PubMed
高影响因子
AICHE JOURNAL
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2025
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IF 4
Bo Wang,Shuangjiang Li,Xiandong Hao,Wenbo Zhao,Zhiyong Xu,Yongming Luo
Traditional amine scrubbing for SO 2 capture typically dilutes alcohol amines with water to improve mass transfer, resulting in high volatility and desorption energy consumption. Inspired by the exceptional properties of ionic liquid (IL) 1-ethyl-3-methylimidazolium thiocyanate ([EMIM][SCN]), we herein propose substituting water with [EMIM][SCN] in a novel SO 2 absorbent system based on N -methyl ethanolamine (MDEA). MDEA acts as the primary SO 2 absorbent, while [EMIM][SCN] serves as an auxiliary absorption component and physical properties regulator. Performance evaluations reveal that MDEA-[EMIM][SCN] achieves high thermal stability (~483.15 K), low viscosity (~26 mPa s), excellent absorption capacity (~1.64 mol/kg at 298.15 K and 2000 ppm SO 2 ), high SO 2 /CO 2 selectivity (~101), and low desorption energy (approximately −95.6 kJ/mol). Thermodynamic modeling illustrates MDEA and [EMIM][SCN] contribute independently to absorption. Optimal energy consumption was determined by the proposed objective function. This work exemplifies the non-aqueous alkanolamine/IL system for SO 2 capture, offering a promising approach for developing efficient, low-energy SO 2 absorbents.
研究领域:
化学工程
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环境科学
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热力学
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绿色化学
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DOI
高影响因子
MOLECULES
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2018
·Vol. 23
·期 4
·871
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IF 3.098
Ming-Yu Wu,Jing Wu,Yue Wang,Yan-Hong Liu,Xiao-Qi Yu
A novel chromenylium-based fluorescent probe was exploited for sulphur dioxide (SO2) detecting. The probe displayed a remarkable fluorescence turn-on response towards SO2based on the nucleophilic addition reaction to the carbon-carbon double bond with 105 nm Stock shift. The probe was successfully applied for the quantification of SO2.The linear detection range was from 0–160 μM with the detection limit as low as 99.27 nM. It also exhibited high selectivity for SO2than other reactive species and amino acids. Furthermore, cell staining experiments indicated that the probe was cell membrane permeable and could be used for high-performance imaging of SO2in living cells. The superior properties of the probe made it highly promising for use in chemical and biological applications.
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DOI
高影响因子
International Journal of Electrochemical Science
·
2023
·Vol. 13
·期 4
·3613-3624
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IF 1.5
Yong Xiang,Chen Li,Zhengwei Long,Canwen Zhang,Zhongli Ji
Although steel corrosion in a SO 2 -containing atmospheric environment has been extensively investigated, its electrochemical behavior still needs to be addressed, especially when it coexists with CO 2 in a carbon capture, utilization and storage system. In this work, electrochemical experiments with 316L stainless steel corrosion in a CO 2 -saturated solution were conducted by adding different amounts of SO 2 to a solution at 25 °C under different pH conditions. The effect of SO 2 on the cathodic reactions of 316L stainless steel corrosion in a CO 2 -saturated solution was investigated by electrochemical methods, including potentiodynamic sweep, linear polarization resistance and electrochemical impedance spectroscopy. The results showed that the presence of SO 2 increased the cathodic limiting current and corrosion rates of 316L stainless steel at the same pH. There was a “second-wave” phenomenon that appeared before the second limiting current and this new “wave” was demonstrated to be related to the direct reduction of both hydrate of SO 2 and bisulfite on the steel surface.
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DOI
高影响因子
Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Zai-Dong Shao,Peng Wu,Fang Liu,Qi-Jun Zhang,Chao-Yang Guo,Rui-Sang Liu,Jiang Lu,Xiao-Meng Ren,Yu-Ming Zheng
Sulfur dioxide (SO 2 ) emissions present significant environmental and health risks, yet efficiently capturing SO 2 remains challenging due to its corrosive nature and the limited performance of conventional adsorbents. In this study, we developed multivariate metal-organic frameworks (MTV-MOFs) based on UiO-66(Zr) for effective SO 2 capture. Through systematic ligand functionalization with -OH, -NH 2 , -SO 3 H, and -(NH 2 ) 2 groups on terephthalic acid linker, we developed a series of MTV-UiO-66 materials with tailored pore environments and adsorption characteristics. UiO-66-NH 2 exhibited superior performance with an SO 2 uptake of 252.9 mL g −1 at 298 K and 1 bar. Ideal adsorbed solution theory (IAST) calculations demonstrated improved selectivity for SO 2 over N 2 (847) and CO 2 (31), surpassing that of the parent UiO-66. Dynamic breakthrough experiments further confirmed the practical viability of MTV-UiO-66 materials for SO 2 capture under both dry and humid (50 % RH) conditions, with UiO-66-NH 2 retaining a capacity of 30.73 mL g −1 in dry settings and exhibiting robust performance in moisture-rich environments. Grand Canonical Monte Carlo (GCMC) simulations and density functional theory (DFT) calculations provided molecular-level insights into the adsorption mechanisms, revealing that functional groups play a crucial role in modulating binding interactions through hydrogen bonding, dipole-dipole interactions, and spatial confinement effects. The computational binding energies corroborated the experimental isosteric heats of adsorption, validating the integrated experimental-computational approach.
研究领域:
材料科学
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环境化学
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吸附技术
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金属有机框架材料（MOFs）
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计算化学
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DOI
高影响因子
ANALYST
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2020
·Vol. 145
·期 24
·7985-7992
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IF 3.978
Mengya Lv,Yanhao Zhang,Jiayi Fan,Yanyun Yang,Sheng Chen,Gaolin Liang,Shusheng Zhang
Developing suitable molecular tools for monitoring SO2 and its derivatives in living organisms is attractive due to their importance for human health. Herein, the first near-infrared fluorescent probe Mito-HN with aggregation-induced emission enhancement (AIEE) characteristics for ratiometric sensing of SO2 derivatives in vitro, in cells, and in zebrafish was designed and synthesized. By connecting the electron-donating naphthopyran and electron-withdrawing hemicyanine via the alkenyl group, this probe displays a near-infrared fluorescence emission and notable solid-state luminescence with AIEE features. Based on the specific 1,4-addition reaction of HSO3−/SO32− with the CC double bond of Mito-HN, this probe can specifically sense HSO3− in real time with an excellent near-infrared ratiometric fluorescence effect, a low detection limit of 0.17 μM, and a fast response time of less than 30 s. Cell imaging and zebrafish imaging results demonstrate that Mito-HN can ratiometrically not only sense endogenous SO2 derivatives in mitochondria but also monitor SO2 in living organisms. We anticipate that Mito-HN could be applied for the diagnosis of SO2-related diseases in the future.
研究领域:
分析化学
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生物化学
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分子生物学
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医学诊断
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产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2019
·
IF 5.107
Wenbo Zhao,Ling Chen,Qian Zhao,Yuan Chen,Zhiyong Zeng
Phase-change absorption was considered to be a new promising strategy for capture of acid gas since only the rich-phase needed to be disposed and the lean-phase could be reused directly. In the present work, liquid-solid phase-change absorption of SO 2 with a series of tertiary diamines as absorbent was investigated. Long-chain alkane was found to be the best one among the tested solvents. Among the investigated diamines, tetramethylhexanediamine has the highest SO 2 molar absorption capacity of ~2.6 mol/mol. The SO 2 absorption products of diamines were demonstrated to be pyrosulfites based on the FTIR and elemental analysis . Among them, the single crystal of dimethylpiperazine pyrosulfite was obtained through recrystallization. These results indicated that the absorption mechanism of tertiary diamines is different from that of primary and secondary diamines. The effect of absorption conditions such as concentration of absorbent, temperature and partial pressure on the capacity was also investigated. The variation tendency of diamines in liquid along with SO 2 loading indicated that the absorbed SO 2 would force diamines to be separated from liquid phase completely. TG analysis indicated that the initial decomposition temperature sequence of absorption products is C 10 H 26 N 2 S 2 O 5 > C 7 H 20 N 2 S 2 O 5 > C 6 H 16 N 2 S 2 O 5 ·H 2 O > C 6 H 18 N 2 S 2 O 5 .
研究领域:
化学工程
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环境科学
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产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2021
·
IF 5.455
Rong Pan,Yining Tang,Yanni Guo,Jun Shang,Lei Zhou,Wei Dong,Deliang He
To develop effective SO 2 adsorbents, HKUST-1 and HKUST-1 @ GO were synthesized by hydrothermal and room-temperature methods, and characterized by SEM, BET, XRD , TG and FTIR. The preparation method of the adsorbent, amount of adsorbent, initial concentration of SO 2 , and the influence of time and temperature on the adsorption of SO 2 by HKUST-1 and HKUST-1@GO were studied. The results showed that the hydrothermally synthesized HKUST-1@1.2%GO was the best adsorbent for SO 2 , the SO 2 concentration did not affect the final adsorption efficiency, the best adsorption time was 20 min, and the best adsorbent dose was 200 mg. The kinetics and isotherms of HKUST-1@1.2%GO were studied, and the thermodynamic parameters were calculated. The static SO 2 adsorption of HKUST-1@1.2%GO conformed to the pseudo-first-order model and Freundlich model, and was a spontaneous exothermic process. Lowering the temperature is beneficial to the adsorption. At 288 K, the maximum theoretical SO 2 adsorption capacity of HKUST-1 @1.2% GO was 72.49 mmol g −1 . After five adsorption cycles, the adsorption efficiency only decreased by 0.8%, indicating that the adsorbent has excellent repeatability and cyclic stability.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2014
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IF 4.331
Shidong Tian,Yucui Hou,Weize Wu,Shuhang Ren,Jianguo Qian
The capture of SO 2 by ionic liquids (ILs) has drawn much attention all over the world. However, ILs can absorb not only SO 2 but also water from flue gas. The removal of water from ILs is necessary for reusing the absorbent. In order to reduce the energy costs of removing water, it would be helpful to weaken the interactions between ILs and water. In this work, two kinds of hydrophobic task-specific ILs, 1-(2-diethyl-aminoethyl)-3-methylimidazolium hexafluorophosphate ([Et 2 NEmim] [PF 6 ]) and 1-(2-diethyl-aminoethyl)-1-methylpyrrolidinium hexafluorophosphate ([Et 2 NEmpyr][PF 6 ]), were designed and synthesized. Thermal stability and physical properties of the ILs were studied. Furthermore, the application of the ILs for the capture of SO 2 and the absorption mechanism were systematically investigated. It has been found that both of the ILs are immiscible with water, and [Et 2 NEmim][PF 6 ] has much lower viscosity, much higher thermal stability and much higher SO 2 absorption rate than [Et 2 NEmpyr][PF 6 ]. [Et 2 NEmim][PF 6 ] shows high SO 2 absorption capacities up to 2.11 mol SO 2 per mole IL (pure SO 2 ) and 0.94 mol SO 2 per mole IL (3% SO 2 ) under hydrous conditions at 30 °C. The result suggests that [Et 2 NEmim][PF 6 ] is a promising recyclable absorbent for the capture of SO 2 .
研究领域:
化学工程
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环境科学
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产品关联
DOI
PubMed
高影响因子
Journal of the Taiwan Institute of Chemical Engineers
·
2018
·
IF 3.849
Bin Jiang,Yang Chen,Luhong Zhang,Xiaowei Tantai,Haozhen Dou,Yongli Sun
In this work, a novel strategy was reported for improving SO 2 capture through multiple-site interactions of N-imidazole derivative. The tris (2-(1-H-imidazole-1-y1)ethyl) amine (TIA) was designed, synthesised and mixed with water to form the mixed absorbents for SO 2 absorption. The physical properties were determined and the mixed absorbents exhibited low densities and viscosities, which are beneficial to the mass and heat transfer. The SO 2 absorption reached equilibrium rapidly within 60 s and as high as 2.09 mol SO 2 per mol TIA could be absorbed at low SO 2 concentration (<2 kPa). With increasing the mass ratio of TIA in the aqueous absorbents to 50%, more than 6.2 mol/kg absorbent absorption performance was obtained. The desorption was carried out at 80 °C and the recycling performance was excellent without any change during 5 cycles. High SO 2 /CO 2 selectivity was achieved due to the suitable basicity of the absorbents. In addition, the absorption mechanism was established and proved by FTIR and 1 H NMR. Thermodynamic analysis was determined using gPROMS, which suggested the pK a of the TIA varied in a proper range for SO 2 capture. Overall, the novel mixed absorbents with excellent physical properties and high SO 2 absorption capacity have much potential for flue gas desulfurization.
研究领域:
化学工程
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环境科学
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产品关联
DOI
高影响因子
ENERGY & FUELS
·
2018
·
IF 3.024
Jie Li,Yong Kang,Bohao Li,Xin Wang,Dan Li
In this work, four novel PEG-linked dicationic ionic liquids (DILs) with one kind of thiocyanate anion and chloride anion and a traditional DIL with thiocyanate anion were synthesized and used for SO2 absorption. The physicochemical properties of PEG-linked DILs with thiocyanate anion were measured. The performance of SO2 absorption by the five DILs at different pressures, temperatures, and water contents was also investigated. The results showed that the absorption process was fast and the absorption capacities of the DILs were much higher than those of monocationic ILs; especially, [E3Eim2][Cl]2 had the absorption capacity up to 6.779 mol SO2/mol IL at 20 °C and 1 bar. The mechanism of SO2 absorption by DILs was also studied with FT-IR and NMR, which revealed there just existed physical interaction between DILs and SO2. PEG-linked DILs have a high selectivity between SO2 and CO2. Meanwhile, the good absorption performance of PEG-linked DILs could be maintained after five successive absorption/desorption cycles, implying these ILs show great potential as candidate absorbents for SO2 absorption.
研究领域:
化学工程
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环境科学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）