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SEPARATION AND PURIFICATION TECHNOLOGY · 2022 · IF 9.136

Entropy enthalpy compensation in the SO2 absorption reaction and the optimal capture temperature range with amine alkyl siloxane as absorbent

Kai Wang,Guangzhen Li,Yanhong Li,Yuan Chen,Ling Zhang,Zhiying Zhu,Zhiyong Xu,Wenbo Zhao

In the present work, a kind of amine alkyl siloxane N -butyl-N-((1,1,3-trimethyl-3,3-diphenyldisiloxaneyl)methyl)butan-1-amine (BTDMBA) was synthesized and used to capture SO 2 . Its thermal decomposition temperature is 160℃, which is comparable with that of Ionic liquids (ILs), but its viscosity is only 125 mPa∙s at 25℃ after the absorption of SO 2 , which is much lower than that of ILs. The reaction mechanism is that BTDMBA reacted with SO 2 to form charge transfer complex BTDMBA∙SO 2 . The reaction enthalpy and entropy change are −83.95 kJ/mol and −240.48 J·mol −1 ·K −1 , respectively, which are more negative than that of ILs. By comparing the enthalpy and entropy change of amine alkyl siloxane and absorbents reported in literatures, an unexpected entropy enthalpy compensation phenomenon was discovered and the isokinetic temperature was found to be 371 K. Based on this phenomenon and the optimization objective function, it was also found that with the decrease of entropy change, the optimal absorption and desorption temperature difference increased initially and decreased afterwards. The maximum of entropy changes is −201 J·mol −1 ·K −1 for absorbent to achieve recycle absorption capacity 0.79 mol/mol under the condition of absorption pressure 0.002 bar and desorption pressure 1 bar.

研究领域: 物理化学 · 环境化学 · 分离科学 · 能源材料 · 工业气体净化 · 绿色化工
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2012 · IF 2.237

Efficient Conversion of Cellulose to Glucose, Levulinic Acid, and Other Products in Hot Water Using SO2 as a Recoverable Catalyst

Weina Liu,Yucui Hou,Weize Wu,Zhenyu Liu,Qingya Liu,Shidong Tian,Kenneth N. Marsh

Cellulose is the most widely distributed source of biomass, and its efficient conversion to a variety of chemicals is important for a sustainable future. In this work, sulfur dioxide (SO2) dissolved in hot water has been demonstrated to be an efficient catalyst for the selective conversion of cellulose to chemicals such as glucose and levulinic acid. The selectivity of products can be tuned by the SO2 concentration, temperature, and reaction time. SO2 acts both as a supply of H+ ions through ionization of H2SO3 when dissolved in water and as a Lewis acid catalyst that breaks the hydrogen bonds in cellulose. Importantly, SO2 in the reaction mixture can be recovered completely by stream stripping, thus avoiding the formation of acidic wastewater. This work provides a new, efficient, and environmentally benign way to convert cellulose to chemicals.

CAS / MDL: 98-01-1 67-47-0 123-76-2
研究领域: 化学工程 · 可持续化学 · 生物质转化
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2021 · IF 8.128

Confinement of MnOx@Fe2O3 core-shell catalyst with titania nanotubes: Enhanced N2 selectivity and SO2 tolerance in NH3- SCR process

Yifan Li,Yaqin Hou,Yongzhao Zhang,Yatao Yang,Zhanggen Huang

Surface interface regulation is an important research content in the field of heterogeneous catalysis. To improve the interface interaction between the active component and matrix, tremendous efforts have been dedicated to tailoring the morphology, size, and structure of composite catalysts. In this work, we report a confinement strategy to synthesize a series of core-shell catalysts loaded with metal oxides on titania nanotubes (TNTs), which were applied to the selective catalytic reduction of NO x with ammonia. Interestingly, the core-shell catalyst with confinement of TNTs exhibited the remarkable activity at low temperature region, N 2 selectivity and sulfur tolerance. Benefiting from the superior interfacial confinement characteristic of TNTs and Fe 2 O 3 , strong component interactions, the surface acid sites and strong oxidizability of MnO x were properly regulated, thus obtained the outstanding activity, N 2 selectivity and provide chemical protection to effectively prevent SO 2 poisoning. As far as the reaction mechanism, we found that the adsorption and reactivity of Lewis acid sites were the dominant factors affecting the activity in the NH 3 -SCR process by in situ DRIFT spectra. In general, our work provides an innovative strategy for constructing an TNTs-enwrapped nanocomposite with nano-confinement and core-shell structure to improve the low temperature SCR process.

研究领域: 催化化学 · 环境科学
✓ 已验证 DOI PubMed 高影响因子
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MACROMOLECULES · 2020 · IF 5.918

Sustainable and Biodegradable Copolymers from SO2 and Renewable Eugenol: A Novel Urea Fertilizer Coating Material with Superio Slow Release Performance

Limin Liu,Yonghao Ni,Yunfei Zhi,Wenbo Zhao,Manoj Pudukudy,Qingming Jia,Shaoyun Shan,Kaifu Zhang,Xuefen Li

To enhance SO2 utilization, improve fertilizer use efficiency, and minimize the negative environmental impact, the novel slow release sulfur-containing urea fertilizers with good biodegradation performance were developed by coating with the sustainable poly(eugenol sulfone) derived from renewable eugenol and SO2. The poly(eugenol sulfone) was synthesized by a simple free radical polymerization under mild conditions, and structural features of the synthesized copolymers were studied by various characterization techniques. Characterization results revealed that the copolymers exhibited the strict alternating copolymerization structures containing O═S═O. A set of systematically designed experiments were carried out to determine the influences of the amount of initiator, reaction time, and reaction temperature on the molecular structure, release, and biodegradation behavior of the coated fertilizers. The obtained results proved that the coated fertilizers showed excellent release and biodegradation features. Moreover, the release and biodegradation rate of the coated fertilizers can be adjusted by changing the molecular weight of poly(eugenol sulfone). In addition, the kinetic study on the slow release characteristics of poly(eugenol sulfone)-coated fertilizers showed that the best fitting effect was obtained by the Ritger–Peppas equation. This work offers a simple and useful strategy for designing sulfur-containing urea fertilizers with excellent slow release and biodegradation performance and provides a new route for sulfur recycling. In the future, the fertilizer will be deeply tested to evaluate their impact on plant growth, chemical, and biological soil properties.

研究领域: 材料科学 · 环境科学 · 农业科学
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY · 2023 · IF 6.1

Development of a Ratiometric Fluorescent Probe with Zero Cross-Talk for the Detection of SO2 Derivatives in Foods and Live Cells

Huan Peng,Suna Kong,Xia Deng,Qirong Deng,Fengpei Qi,Changhui Liu,Ruiren Tang

Sulfur dioxide (SO2) derivatives are extensively utilized as both a preservative for foods and an active gaseous signal molecule in various physiological and pathological processes, but their excessive intake would bring harmful effects on human health; so, the determination of SO2 derivatives is of great importance. Herein, we developed a ratiometric fluorescent probe named 2-(2′-hydroxyphenyl)benzothiazole-3-ethyl-1,1,2-trimethyl-1H-benzo[e]indolium (HBT-EMBI) by introducing a hemicyanine unit of EMBI to an HBT group for the detection of SO2 derivatives via an excited-state intramolecular proton transfer (ESIPT) and intramolecular charge transfer (ICT) effects. The probe displays some advantages, such as a colorimetric change from purple to colorless, a ratiometric fluorescence with zero cross-talk, and a remarkably large emission shift (Δλ = 164 nm) under a single-wavelength excitation. Accordingly, the probe HBT-EMBI has been successfully employed for the colorimetric and ratiometric determination of SO2 derivatives in real food samples and the quantitative visualization of SO2 derivative variations in HepG2 cells.

研究领域: 分析化学 · 生物医学 · 食品安全
✓ 已验证 DOI PubMed 高影响因子
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CERAMICS INTERNATIONAL · 2026 · IF 6

The effect of Nb deficiency and YSZ composite on the response characteristics of MnNb2O6 sensing electrodes in mixed potential SO2 sensors

Jiaxin Li,Qunwei Guo,Jiangtao Feng,Yinwen Gu,Bo Chi,Jian Pu

Accurate and real-time detection of SO 2 at industrial emission sources is important for emission control, yet reliable sensing under high-temperature and relatively high-concentration conditions remains challenging. In this study, a YSZ-based mixed-potential SO 2 sensor was developed by regulating Nb nonstoichiometry in MnNb 2-x O 6 sensing electrodes and YSZ compositing. Nb deficiency altered particle coarsening, the apparent pore architecture of the electrode layer, and the defect chemistry. Among the single-phase sensing electrodes, MnNb 1.9 O 6 exhibited larger pore sizes and the highest oxygen-vacancy concentration, achieving a sensitivity of −14.76 mV/decade over 50-500 ppm SO 2 at 400 °C. Further compositing with YSZ produced more uniformed pore structure and increased the electrochemically active triple-phase-boundary (TPB) region, with MnNb 1.8 O 6 /20 wt% YSZ achieved the highest sensitivity of −18.74 mV/decade. A comparison of the composition series and YSZ-composite electrodes indicates that electrode microstructure and accessible TPB sites are the primary determinants of the electrochemical response, which enhance SO 2 diffusion and increase the number of active sites. Additionally, the increased oxygen vacancies also provide a synergistic contribution by promoting oxygen ion transport, further enhancing the overall reaction rate. The optimized sensor also showed good repeatability and 15-day stability, highlighting its potential for high-concentration SO 2 monitoring under industrially relevant dynamic-flow conditions.

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Journal of Physical Chemistry C · 2024 · IF 3.3

Insights into Migration and Transformation of Cu Species during SO2 Poisoning and Hydrothermal Aging of Cu/SAPO-34 NH3–SCR Catalysts

Fumei Wang,Qi Cai,Xinhua He,Boxiong Shen,Leila Negahdar,Shuo Feng,Andrew M. Beale

Cu/SAPO-34 catalysts have been widely used for the reduction of NOx from diesel exhaust by ammonia-selective catalytic reduction (SCR). Sulfur poisoning remains a challenge for Cu/SAPO-34 catalysts in NH3–SCR, restricting its application. In this study, Cu/SAPO-34 samples containing a mixture of Cu species comprising isolated Cu2+ located in the 6MR, Cu(OH)+ in 8MR, CuO clusters/nanoparticles, and Cu+ species were prepared. The Cu speciation during SO2 and hydrothermal aging of Cu/SAPO-34 SCR catalysts was subsequently studied. While hydrothermal aging had little effect on catalytic activity, the sulfur-aged sample exhibited deterioration in NH3–SCR activity over the temperature range of 100–575 °C. The breakage and collapse of the zeotype framework and chemical deactivation of the Cu/SAPO-34 catalyst after exposure to SO2 and H2O took place. A combination of X-ray photoelectron spectroscopy (XPS) and TGA-DT-DSC revealed the presence of ammonium bisulfate, copper bisulfate/sulfate, aluminum sulfate, and sulfuric acid after SO2 and H2O copoisoning under SCR conditions. Furthermore, Cu(OH)+ tended to migrate to form isolated Cu2+ and Cu+, as well as agglomerate to form CuO particles. Density functional theory (DFT) calculations revealed that SO2 and O2 could readily be absorbed by CuO particles to form stable copper bisulfate/sulfate species with the following order of preference: CuO > Cu+ > Cu2+ > Cu(OH)+. In contrast, Cu(OH)+ was less prone to be poisoned by easily releasing SO3 than other Cu species sites.

研究领域: 环境科学 · 催化化学
✓ 已验证 DOI 高影响因子
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MICROCHEMICAL JOURNAL · 2026 · IF 5.2

LDs-targeting multifunctional fluorescent probe toward polarity, viscosity, and SO2 and bioimaging in cancer, inflammation, ferroptosis, and acute alcoholic liver injury

Shizeng Pei,Huiling Wang,Jing Liu,Gang Nie,W.M.W.W. Kandegama,Chunrong Liu

Sulfur dioxide (SO₂), as well as microenvironmental viscosity and polarity are indispensable for redox equilibrium, biomolecular trafficking, and metabolic signaling, yet holistic analysis tools are lacking. Herein, we developed a multifunctional fluorescent probe TPA-TOB for simultaneous detection of polarity, viscosity, and SO₂. In the D-π-A structured TPA-TOB , triphenylamine (TPA) functioned as the donor, with 2-thiobarbituric acid serving as the acceptor, linked by a thiophene vinyl π-bridge. This architecture targeted lipid droplets (LDs), while the C C bond served as the site of the Michael addition reaction for the recognition of SO 2 . The D-π-A structure of TPA-TOB with twisted intramolecular charge transfer (TICT) characteristics enabled it to respond to polarity and viscosity (≥620 nm fluorescence enhancement with higher viscosity/lower polarity). For SO₂, TPA-TOB exhibited 47-fold fluorescence enhancement at 420 nm (response time ~ 10 min, LOD 0.87 μM), with 95.78%–100.58% recovery for SO₂ detection in rock sugar. Furthermore, TPA-TOB facilitated dynamic monitoring of intracellular SO 2 redox dynamics and fluctuation of LDs microenvironment (polarity and viscosity) spanning cell, tissue, and organism levels. Significantly, we realized the dual-channel mapping of acute alcoholic liver injury (AALI) with this probe, as well as identification of pathological signatures in cancer, inflammation, and ferroptosis. Therefore, we have established an integrative analytical platform to elucidate the interplay between SO 2 signaling and LDs microenvironment, thereby deepening the understanding of their roles in the pathogenesis of multiple diseases, and providing novel avenues for mechanistic investigation and therapeutic discovery.

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SEPARATION AND PURIFICATION TECHNOLOGY · 2022 · IF 9.136

Unexpectedly efficient absorption of low-concentration SO2 with phase-transition mechanism using deep eutectic solvent consisting of tetraethylammonium chloride and imidazole

Ping Zhang,Guangzhi Xu,Mingzhen Shi,Zongheng Wang,Zhuoheng Tu,Xingbang Hu,Xiaomin Zhang,Youting Wu

Deep eutectic solvents (DESs) are environmentally friendly solvents with excellent affinity to acidic gases and have broad application prospect in the field of SO 2 capture. In this work, four inexpensive DESs comprising of tetraethylammonium chloride (TEACl) and azoles (imidazole, pyrazole and tetrazole) were designed and prepared for highly efficient and reversible absorption of SO 2 . Physical properties and chemical structures of the prepared DESs were characterized. High SO 2 capacity ranging from 0.756 to 1.251 g/g (3.610–7.231 mol/mol) were obtained at 20 °C and 1.0 bar. Surprisingly, owing to the accompanying phase transition, available SO 2 capacity of TEACl-Im (1:3) reaches 0.438 g/g (2.532 mol/mol) at 2000 ppm and 20 °C, which is the highest value reported so far. The absorption mechanism and phase transition were further investigated using FTIR, NMR and XRD, revealing the generation and precipitation of SO 2 -imdazole adduct. In addition, no significant drop in SO 2 absorption capacity was observed after five successive absorption–desorption cycles. Overall, TEACl-Im (1:3) exhibits good absorption performance especially for low-concentration SO 2 , providing potential alternatives for flue gas desulfurization.

研究领域: 环境化学 · 气体分离 · 可持续溶剂 · 碳捕集与封存 · 化学工程
✓ 已验证 DOI 高影响因子
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CHEMICAL ENGINEERING JOURNAL · 2016 · IF 5.31

Efficacious means for inhibiting the deactivation of K2CO3/AC for low-concentration CO2 removal in the presence of SO2 and NO2

Yafei Guo,Changhai Li,Shouxiang Lu,Chuanwen Zhao

K 2 CO 3 supported on activated carbon (K 2 CO 3 /AC) shows promise as a potential candidate for removing low-concentration CO 2 from environmental control and life support systems (ECLSS). However, K 2 CO 3 /AC would suffer a decreased CO 2 sorption capacity due to sorbent deactivation in acid impurities such as SO 2 and NO 2 . To solve this problem, water vapor pretreatment, KOH addition and polyethyleneimine (PEI) modification were proposed as efficacious means for improving its CO 2 sorption capacity and mitigating the sorbent deactivation in these acid impurities. CO 2 sorption performances of the pretreated and modified sorbents were evaluated in a fixed-bed reactor under simulated ECLSS conditions of 20   °C, 1.0% CO 2 , 2.0% H 2 O, 30   ppm SO 2 , 20   ppm NO 2 and balanced N 2 . The mechanisms for sorbent deactivation inhibition by water vapor pretreatment, KOH addition and PEI modification were revealed by N 2 adsorption-desorption, X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM) and Fourier transform infrared spectroscopy (FT-IR). Effects of water vapor pretreatment duration, KOH addition and PEI loading on sorbent deactivation inhibition performances were demonstrated. Furthermore, the long-term working stabilities of the pretreated and modified sorbents in impurities were evaluated. The results will provide fundamental support on practical application of K 2 CO 3 /AC for low-concentration CO 2 removal in ECLSS.

研究领域: 环境控制与生命支持系统 · 气体吸附 · 材料化学 · 空气净化技术 · 二氧化碳捕集
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ENERGY & FUELS · 2018 · IF 3.024

Phase-Change Absorption of SO2 by N,N,N′,N′-Tetramethyl-p-phenylenediamine in Organic Solvents and Utilization of Absorption Product

Qian Zhao,Wenbo Zhao,Muyuan Chai,Ling Chen,Yang Wang,Qingming Jia,Yuan Chen

As SO2 removal via traditional aqueous amine scrubbing requires large amounts of energy for absorbent regeneration, phase-change absorption was considered to be a promising alternative, as regeneration of only the SO2-rich phase is needed. The SO2-lean phase can be directly reused, thus greatly reducing energy requirements. We herein investigated the phase-change absorption behavior of N,N,N′,N′-tetramethyl-p-phenylenediamine (TPD) in organic solvents. In general, the TPD absorption rate in organic solvents followed the order: dimethylformamide > diethylene glycol dimethyl ether > propylene carbonate > butanol, which is related to their Henry’s constant. Our results indicated that TPD reacted with SO2 to form the charge-transfer complex TPD·SO2, which was further converted into TPD·2SO2 upon increasing the absorption time. Furthermore, the addition of H2O promoted the formation of TPD·2SO2, but it exhibited a negative effect on the absorption rate. Moreover, in the presence of O2 and H2O, TPD·SO2 in solution was converted slowly into [H2TPD][HSO4]2. TPD·SO2 decomposed into TPD and SO2 at ∼100 °C and exhibited a relatively stable recyclability for SO2 absorption. At last, TPD·SO2 was used as a surrogate of SO2 to synthesize sulfonamide; its activity was higher than that of a reported complex of triethylenediamine and SO2.

CAS / MDL: 111-96-6 35065-28-2
研究领域: 化学工程 · 环境科学
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FUEL PROCESSING TECHNOLOGY · 2019 · IF 4.507

Catalytic conversion of cellulose to C5/C6 alkanes over Ir-VOx/SO2 combined with HZSM-5 in n-dodecane/water system

Lele Jin,Wenzhi Li,Qiying Liu,Longlong Ma,Song Li,Yang Liu,Baikai Zhang,Qi Zhang

The liquid fuel (made of C 5 /C 6 alkanes) was obtained directly from the hydrogenolysis of microcrystalline cellulose (MCC) with Ir-VO x /SiO 2 combined with HZSM-5 as the composite catalyst in a biphasic system (n-dodecane + H 2 O). The performance of the catalyst was investigated by carrying out a series of experiments using various V/Ir molar ratios , catalyst dosages, reaction temperatures, reaction time, hydrogen pressure and substrates. At the optimized conditions, the cellulose was almost completely converted, and at the same time, a high C 5 /C 6 yield of 85.1% was obtained at 210 °C for 24 h and 6 MPa with the V/Ir molar ratio being 0.13. These results not only proved that Ir-VO x /SiO 2 (V/Ir = 0.13) has excellent performance for the hydrogenolysis of MCC to liquid alkanes, but also indicated that vanadium is a good metal promoter for iridium . In addition, it was proven the C5/C6 alkanes were obtained via sorbitol through the combined effect of Ir-VO x /SiO 2 and HZSM-5.

研究领域: 催化化学 · 可再生资源转化
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