ChemistrySelect
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2024
·Vol. 9
·期 41
·e202402919
·
IF 1.9
Wenyu Wang,Shouhong Wang,Juan Xu,Huigui Yang,Yi Liu,Mengrui Li,Yunfei Zhi
Graphical This study successfully prepared three environmentally friendly Schiff base network (SNW) polymers, SNW-1, SNW-2, and SNW-3, using melamine and aldehyde compounds as raw materials through a microwave-assisted synthesis method. The SNW materials were applied to catalyze the copolymerization reaction of SO 2 and epoxides. Through detailed analysis of the chemical structure and properties of SNW-1, SNW-2, and SNW-3, their catalytic efficiency was thoroughly investigated. Three thermal degradation kinetic models, FWO, Kissinger, and Coats–Redfern, were employed to calculate the kinetic parameters of the thermal degradation of PCS. Potential thermal degradation mechanisms were speculated. This study successfully prepared three environmentally friendly Schiff base network (SNW) polymers, SNW-1, SNW-2, and SNW-3, using melamine and aldehyde compounds as raw materials through a microwave-assisted synthesis method. The SNW materials were applied to catalyze the copolymerization reaction of SO 2 and epoxides. Through detailed analysis of the chemical structure and properties of SNW-1, SNW-2, and SNW-3, their catalytic efficiency was thoroughly investigated. Three thermal degradation kinetic models, Flynn–Wall–Ozawa (FWO), Kissinger, and Coats–Redfern, were employed to calculate the kinetic parameters of the thermal degradation of poly(cyclohexene sulfite) (PCS). Potential thermal degradation mechanisms were speculated. Additionally, the Kissinger model accurately described the thermal degradation kinetics features of PCS. Based on experimental results and kinetic analysis, this paper elucidates the potential mechanism of the copolymerization reaction of SO 2 and epoxides. The study indicates that microwave-assisted synthesis exhibits convenience and high efficiency in preparing efficient catalysts, demonstrating significant potential across various application domains.
研究领域:
材料科学
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化学工程
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环境科学
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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2019
·
IF 3.375
Yan Zhang,Zhonghang Chen,Xing Liu,Ze Dong,Peixin Zhang,Jun Wang,Qiang Deng,Zheling Zeng,Shuhua Zhang,Shuguang Deng
Removal of trace SO2 contaminants from gas mixtures by the molecular sieving effect is highly desired. Herein, a microporous metal–organic framework Cu2(pzdc)2(pyz) [CPL-1, pzdc = 2,3-pyrazinedicarboxylate; pyz = pyrazine] with a dumbbell-shaped 1D channel and specific binding sites is explored for deep desulfurization. The proper size of 4.1 × 6.2 Å and strong SO2 trapping sites on CPL-1 render a high adsorption uptake of SO2 (44.8 cm3 g–1) with a record-high selectivity for SO2/N2 (368) and SO2/CH4 (74.3) separation under ambient conditions. Moreover, the dispersion-corrected density functional theory calculations have identified the dual specific adsorption sites of SO2, such as Sδ+···Oδ− electrostatic interactions and Oδ−···Hδ+ hydrogen bonds. The feasibility of CPL-1 for SO2/N2, SO2/CH4, CO2/CH4, CO2/N2, and mimicked flue gas mixture separations was validated by dynamic breakthrough experiments. Water vapor and CO2 impurity were introduced to the gas feed streams to confirm the excellent separation performance of CPL-1. Moreover, a scale-up production of CPL-1 via a facile and green method was conducted, and a reproducible CPL-1 adsorbent with undamaged adsorption and separation performances was successfully manufactured in kilogram quantity. These unique features render CPL-1 a very promising adsorbent for practical desulfurization processes.
研究领域:
化学
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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
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Liam John France,Wan Li,Yanke Zhang,Wentao Mu,Zhihang Chen,Junjun Shi,Qiang Zeng,Xuehui Li
A series of Fe-Zr mixed-metal oxides were prepared and examined for the simultaneous reduction of NO and SO 2 with CO. The catalyst containing 40 mol% exhibited near-complete conversion of both pollutants at a minimum temperature of 350 °C and a GHSV of 90,000 h −1 . The addition of Fe 3+ to ZrO 2 decreased the crystallinity of the latter phase and significantly enhanced surface area. Concentrations of 30 mol% or greater produced segregated FeO x phases, which affected catalytic performance in distinctly different ways: supported Fe 3+ (30 mol%) possessed similar activity to doped Fe 3+ ; α-Fe 2 O 3 (50 mol%) inhibited activity due to its’ lower reducibility; an amorphous phase (40 mol%) promoted iron-weighted areal activity. A complete identification of the ambiguous component was not successfully established, but the obtained properties revealed that it exhibited weaker interaction with the support and had a size greater than that of oligomeric-Fe 2 O 3 yet smaller than 3 nm.
研究领域:
催化
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环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2024
·
IF 10.8
Yuwen Wang,Lingdong Kong,Jie Tan,Beibei Liu,Yixuan An,Lianghai Xia,Yu Lu,Qing Li,Lin Wang
Hydrogen peroxide (H2O2) plays a crucial role as an oxidizing agent within the tropospheric environment, making a substantial contribution to sulfate formation in hydrated aerosols and cloud and fog droplets. Field observations show that high levels of H2O2 are often observed in heavy haze events and polluted air. However, the source of H2O2 remains unclear. Here, using the droplets formed in situ by the deliquescence of hygroscopic compounds under a high relative humidity (RH), the formation of H2O2 by the photochemistry of imidazole-2-carbaldehyde (2-IC) under ultraviolet irradiation was explored. The results indicate that 2-IC produces IM–C•–OH and IM–C•═O radicals via H transfer itself to its excited triplet state and generates H2O2 and organic peroxides in the presence of O2, which has an evident oxidizing effect on SO2, suggesting the potential involvement of this pathway in the formation of atmospheric sulfate. H2O2 formation is limited in acidic droplets or droplets containing ammonium ions, and no H2O2 is detected in droplets containing nitrate, whereas droplets containing citric acid have an obvious promotion effect on H2O2 formation. These findings provide valuable insights into the behaviors of atmospheric photosensitizers, the source of H2O2, and the formation of sulfate in atmospheric droplets.
研究领域:
大气化学
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环境科学
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物理化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2017
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IF 4.9
Yuefei Ji,Yuanyuan Shi,Lu Wang,Junhe Lu,Corinne Ferronato,Jean-Marc Chovelon
The widespread occurrence of sulfonamide antibiotics in the environment has raised great concerns about their potential to proliferate antibacterial resistance. Sulfate radical (SO 4 •- ) based advanced oxidation processes (SR-AOPs) are promising in-situ chemical oxidation (ISCO) technologies for remediation of soil and groundwater contaminated by antibiotics. The present study reported that thermally activated persulfate oxidation of sulfonamides (SAs) bearing six-membered heterocyclic rings, e.g., sulfamethazine (SMZ), sulfapyridine (SPD), sulfadiazine (SDZ), sulfadimethoxine (SDM), and sulfachloropyridazine (SCP), all produced SO 2 extrusion products (SEPs), a phenomenon that is of potential importance, but not systematically studied. As an electrophilic oxidant, SO 4 •- tends to attack the aniline moiety, the reactive site of SAs, via electro-transfer mechanism. The resulting anilinyl radical cations are subjected to further intermolecular Smiles-type rearrangement to produce SEPs. Formation of SEPs is expected to occur in other SR-AOPs as well. The temperature-dependent evolution pattern of SEP of SMZ, 4-(2-imino-4,6-dimethylpyrimidin-1(2 H )-yl)aniline, can be well fitted by kinetic modeling concerning sequential formation and transformation of intermediate product. The presence of natural organic matter (NOM) influenced the evolution patterns of 4-(2-imino-4,6-dimethylpyrimidin-1(2 H )-yl)aniline significantly. Toxicological effects of SEPs on ecosystem and human health remain largely unknown, thus, further monitoring studies are highly desirable.
研究领域:
环境科学
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化学工程
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毒理学
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DOI
PubMed
高影响因子
Pharmaceutics
·
2024
·Vol. 16
·期 6
·833
·
IF 4.9
Zhiran Chen,Xiaoxiang Zhou,Bo Wu,Han Tang,Wei Wei,Daoming Zhu,Yi Ding,Longyun Chen
The inhibition of the immune response in the tumor microenvironment by therapy regimens can impede the eradication of tumors, potentially resulting in tumor metastasis. As a non-invasive therapeutic method, radiotherapy is utilized for tumor ablation. In this study, we aimed to improve the therapeutic impact of radiotherapy and trigger an immune response by formulating a benzothiazole sulfinate (BTS)-loaded fusion liposome (BFL) nanoplatform, which was then combined with radiotherapy for anti-cancer treatment. The platelet cell membrane, equipped with distinctive surface receptors, enables BFL to effectively target tumors while evading the immune system and adhering to tumor cells. This facilitates BFL’s engulfment by cancer cells, subsequently releasing BTS within them. Following the release, the BTS produces sulfur dioxide (SO2) for gas therapy, initiating the oxidation of intracellular glutathione (GSH). This process demonstrates efficacy in repairing damage post-radiotherapy, thereby achieving effective radiosensitization. It was revealed that an immune response was triggered following the enhanced radiosensitization facilitated by BFL. This approach facilitated the maturation of dendritic cell (DC) within lymph nodes, leading to an increase in the proportion of T cells in distant tumors. This resulted in significant eradication of primary tumors and inhibition of growth in distant tumors. In summary, the integration of personalized BFL with radiotherapy shows potential in enhancing both tumor immune response and the elimination of tumors, including metastasis.
研究领域:
癌症治疗
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纳米技术
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免疫疗法
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放射治疗
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药学
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2020
·
IF 9.038
Can Cheng,Jianjun Li,Jinyan Cao,Jiaxiu Guo,Wanglai Cen
The absorption properties of N-(2-hydroxyethyl) morpholine (HEM), morpholine (MP) and N-(2-aminoethyl) morpholine (AEM) for SO 2 were studied using sulfolane (SUL) as solvent in this work. Among these solvent combinations, HEM/SUL shows the best cyclic absorption performance, and the capacity of HEM-SUL-40 (40 wt% of HEM and 60 wt% of SUL) to absorb 8580 mg/m 3 SO 2 (the remainder is N 2 ) is 192.18 mg/g at 293.15 K. The absorption capacity of the second cycle is 97.5% of the first absorption cycle, which is higher than 70% of the Cansolv amine solution in a commercial application with similar experimental conditions. However, MP/SUL is difficult to desorb at high temperature, and the absorption capacity of AEM/SUL is much lower than HEM/SUL and MP/SUL. According to the FTIR , 1 H NMR and 13 C NMR, all three cyclic amines have charge transfer effects with SO 2 . The structure of HEM/SUL can be recovered after heating, but MP cannot be recovered. Δ r G m ° in the reaction against HEM with SO 2 increases significantly with increasing temperature. The Δ r G m ° of HEM-SO 2 and MP-SO 2 at 353.15 K is −12.56 kJ/mol and −16.29 kJ/mol, respectively, which further explains the easy desorption of HEM-SO 2 and the difficult desorption of MP-SO 2 at high temperature.
研究领域:
化学工程
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环境科学
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物理化学
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产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2018
·
IF 4.439
Weiyuan Yao,Yue Liu,Zhongbiao Wu
A series of CeO 2 @Ce-O-P “multi-core@shell” catalysts were synthesized in this paper for selective catalytic reduction (SCR) of NO with NH 3 . The experimental results had showed that CeO 2 @Ce-O-P-30:3 yielded best SO 2 tolerance of an over 70% deNO x efficiency at 250 °C in the presence of 100 ppm SO 2 for 20 h, which was much higher compared to pure Ce-O-P and CeO 2 samples. Further characterization results indicated that Ce-O-P coating layer could somewhat inhibit sulfur depositing on the catalysts during SCR reaction in the presence of SO 2 , thereby protecting the active sites from SO 2 poisoning. Especially, O 2 -TPD results illustrated that a great amount of active oxygen species were retained on used CeO 2 @Ce-O-P catalyst after a long term reaction. The synergetic effect of “multi-core@shell” structure could be attributed to such enhanced performances. The “core” CeO 2 devoted abundant active oxygen sites to fulfill the SCR reaction. And the “shell” Ce-O-P could not only provide acid sites, but also protect the active oxygen species by avoiding the over-adsorption of SO 2 on the catalyst. This work could provide a new way to increase the sulfur resistance for low temperature SCR catalysts.
研究领域:
催化化学
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环境科学
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产品关联
DOI
高影响因子
ANALYTICAL CHEMISTRY
·
2025
·
IF 6.7
Hong Wang,Tong Zhu,Wanying Li,Zhangjun Hu,Xin Yang,Qiong Zhang,Peng Huang,Jiwen Hu,Zhihui Feng
As a key signaling molecule, sulfur dioxide (SO2) plays a crucial role in maintaining physiological homeostasis. In this work, we designed a mitochondria-targeted fluorescent probe (MIC) for independently detect SO2 (short-wavelength) and DNA (long-wavelength) in real time. It is worth noting that our research reveals a dual role of that SO2 in regulating oxidative stress. At appropriate levels, it acts as a modulator, whereas excessive amounts induce apoptosis by reducing mitochondrial membrane potential, upregulating p53/Bax, downregulating Bcl-2, and activating the caspase-3 cascade. The apoptotic process induces mitochondrial membrane permeability changes, triggering the release and nuclear translocation of the probe MIC, which subsequently emits red fluorescence. Using time-resolved fluorescence imaging technology, we further observed a significant increase in the average fluorescence lifetime of the DNA channel. This finding demonstrates that the MIC probe not only enables dual-channel monitoring of mitochondrial SO2 and nuclear DNA but also precisely evaluates the apoptotic process through changes in fluorescence lifetime. This innovative tool provides an important means for in-depth study of the SO2-mediated apoptotic mechanism and opens up new strategies for the diagnosis of mitochondrial-related diseases.
研究领域:
生物化学
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细胞生物学
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分子生物学
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生物物理学
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医学诊断
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENERGY & FUELS
·
2017
·
IF 3.091
Yongli Sun,Yanling Zhang,Luhong Zhang,Bin Jiang,Wenhao Gu,Huawei Yang
In this work, a kind of aqueous solution of novel protic triamine-based ionic liquid was proposed for efficient SO2 capture. The mixed absorbents were prepared by blending 1,1,4,7,7-pentaethyldiethylene (PEDETA) with sulfuric acid and water, and their physicochemical properties were studied by various methods. Remarkably, the viscosities of the mixed absorbents are in the range of 1.44–1.85 mPa s at 293.2 K, which is as low as water. Detailed SO2 absorption experiments were carried out to investigate the influence of some important factors, including temperature (298.2, 313.2, and 328.2 K), SO2 partial pressure (0–1 bar), and sulfuric acid proportion. It is worth noting that the mixed absorbents showed excellent absorption capacity, especially at a low partial pressure. All absorbed SO2 could be released easily and completely by the method of heating reflux. More importantly, the absorbent could be reused for at least 5 cycles without noticeable changes in both absorption performance and chemical structure. A thermogravimetric analysis further confirmed its good thermal stability. The detailed absorption mechanism was proposed and demonstrated by an infrared spectrum. In the end, the pKa values and reaction enthalpy of the protonation reaction of PEDETA were determined by acid titration and parameter analysis based on the reaction equilibrium model. In summary, the mixed absorbents, which possess low viscosities, good resistance to sulfuric acid, excellent capacity, and reusability, may have a good perspective in industrial SO2 capture.
研究领域:
环境科学
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化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2025
·
IF 11.3
Wenjie Liao,Ling Zhou,Xiaoqiang Wang,Yue Liu,Zhongbiao Wu
Both improving the activity and reducing SO3 emissions during selective catalytic reduction of NOx by the NH3 (NH3–SCR) process over commercial V–Ti-based catalysts remain a challenge. Herein, Ce and P cooperatively modified the VMo/Ti catalyst to address this challenge. Within the temperature range of 250–350 °C, the optimal VMoCeP/Ti catalyst achieved a NO conversion of more than 95% and maintained a SO2 oxidation ratio below 1.0%. The enhanced SCR activity of the modified catalyst could be attributed to the improvement in surface acidity and redox capacity by the addition of Ce and P, which would promote NH3 adsorption and activation. Meanwhile, Ce and P coaddition could regulate the surface structure of vanadyl species from predominantly polymeric to a more dimeric form, which could also promote the SCR reaction. More importantly, except for the suppressed sulfation of vanadium species, both a lower proportion of polymeric vanadyl species and the strong interactions among V–Ce–P species could raise the energy barrier of the decomposition of sulfated vanadium species into SO3, thereby inhibiting SO2 oxidation. This work provided novel insights into developing efficient SCR catalysts with low SO2 oxidation ratios for both the academic and industrial fields.
研究领域:
催化化学
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环境化学
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Physical Chemistry C
·
2023
·
IF 3.7
Xinbo Jing,Zhe Chen,Xue Cao,Qishen Huang,Pai Liu,Yun-hong Zhang
Sulfate formation is arguably the most important chemical process during urban haze events in China; however, the complex mechanism of sulfate formation from SO2 remains unresolved. Recent studies showed regionally transported sea spray aerosols (SSAs) and transition-metal ions (TMI)-catalyzed SO2 oxidation are major contributors to sulfate in haze events near coastal regions. To better understand the role of SSA and TMI catalysis, we investigated the reaction kinetics of Mn2+-catalyzed SO2 oxidation in NaCl microdroplets using confocal Raman spectroscopy coupled with a relative humidity (RH) and trace gas control system. We demonstrated that the reaction occurred on the droplet surface according to the linear correlation between the reaction rate and the droplet radius. The saturation concentration for both Mn2+ (0.001 mol/L at 1 ppm SO2) and SO2 (2 ppm at 10–5 mol/L Mn2+) implies the existence of an upper limit of the SO2 uptake coefficient, which is intercorrelated with Mn2+ and SO2 concentrations. The uptake coefficient increased with high ionic strength, while it remained constant when the pH ranged from 5 to 8. The uptake coefficient was on the order of 10–5 to 10–4, which is 10 to 100 times larger than that of the uncatalyzed autoxidation of SO2 and is overall higher than other mineral dust oxidation pathways.
研究领域:
大气化学
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环境科学
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气溶胶科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）