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Catalysis Science & Technology · 2023 ·Vol. 13 ·期 10 ·3147-3157 · IF 5

Mn mixed oxide catalysts supported on Sn-doped CoAl-LDO for low-temperature NH3-SCR

Hange Wang,Wen Chen,Wei Jin,Yueli Liu

SCR technology is considered to be the most effective method for denitrification. However, the low NOx conversion rate of the current catalysts at low temperatures limits their further application. Herein, Sn-doped modified CoAl-LDH carriers are synthesized by a hydrothermal method, and the typical hexagonal sheet structure of the MnOx(0.25)/CoSn3Al-LDO catalyst achieves 100% NO conversion at a wide range of 120–330 °C with a GHSV of 30 000 h−1, and the 100% NO conversion may be maintained at 200 °C for 30 h. After the introduction of 150 ppm SO2 at 200 °C, the NO conversion of the MnOx(0.25)/CoSn3Al-LDO catalyst is maintained at 73.4%, which is greatly improved compared with those of CoAl-LDO and MnOx(0.25)/CoAL-LDO catalysts (64.8% and 38.6%, respectively). The active components such as MnOx and Co3O4 are highly dispersed in the MnOx(0.25)/CoSn3Al-LDO catalyst. Sn doping increases the ratios of Mn4+/Mn3+ and Co3+/Co2+ as well as the adsorbed oxygen amount on the catalyst surface, and improves the redox capacity of the catalyst and increases the number of acid sites, resulting in the excellent low-temperature NH3-SCR performance of MnOx(0.25)/CoSn3Al-LDO.

研究领域: 环境科学 · 催化化学
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Journal of Environmental Sciences · 2024 · IF 5.9

Significantly surfactant-enhanced photochemical conversion of SO2 to sulfates on photosensitive substances

Hongxing Yang,Wangjin Yang,Xiangli Nan,Ning Tang,Chong Han

The photochemical conversion of SO 2 to sulfates on 4–(benzoyl) benzoic acid (4–BBA) was investigated deeply in the presence of anionic and cationic surfactants. The types of surfactants determined their effect behaviors, and cationic surfactants can significantly enhance the SO 2 oxidation on 4–BBA under irradiation, as shown by larger SO 2 uptake coefficients and sulfate production. Hydrophilic moieties in cationic surfactants have a greater enhancement effect on the photochemical conversion of SO 2 to sulfates than the corresponding hydrophobic moieties. Cationic surfactants obviously increased the accumulation of H 2 O on the surface, which was proved to be the main factor influencing the SO 2 uptake and the sulfate formation on 4–BBA. SO 2 lifetime and sulfate formation rate in the mixture system of photosensitive substances with surfactants were evaluated to be 2.25 days and 0.09 μg/(m 3 ·h), respectively.

研究领域: 环境科学 · 大气化学
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MACROMOLECULES · 2016 · IF 5.554

SO2-Induced Solution Phase Transition of Water-Soluble and α-Helical Polypeptides

Mengxiang Zhu,Yan Wu,Chenglong Ge,Ying Ling,Haoyu Tang

Water-soluble random copolypeptides bearing pyridinium tetrafluoroborate (PyBF4) and oligo-ethylene glycol (OEG) pendants (PPLG-PyBF4-r-OEG) showed SO2-induced solution phase transition. They were prepared by sequential postpolymerizations including nucleophilic substitution of poly(γ-3-chloropropyl-l-glutamate) with sodium azide to partially convert chloro groups into azido groups, copper-mediated [2 + 3] alkyne–azide 1,3-dipolar cycloaddition to conjugate OEG pendants, another nucleophilic substitution to conjugate pyridinium chloride, and ion-exchange reaction. FTIR and CD analysis revealed that PPLG-PyBF4-r-OEG samples with suitable molar content of PyBF4 (x ≤ 0.4) were water-soluble and adopted α-helical conformation in both the solid-state and aqueous solution. UV–vis spectroscopy and dynamic light scattering (DLS) results revealed that PPLG-PyBF4-r-OEG aqueous solution underwent a reversible solution phase transition by sequentially bubbling SO2 and N2. 1H NMR analysis suggested that SO2 interacted with triazole groups and induced the solution phase transition.

研究领域: 生物化学 · 高分子化学
✓ 已验证 DOI 高影响因子
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ENVIRONMENTAL POLLUTION · 2025 · IF 7.3

NO2-promoted heterogeneous photochemical oxidation of SO2 to sulfates on brown carbon

Hongxing Yang,Wangjin Yang,Shiwei Lai,Fu Li,Shaojie Yang,Chong Han

The role of NO 2 in the heterogeneous photochemical formation of sulfates by SO 2 uptake on typical brown carbon (BrC) species (Fluoranthene, FL; 4-(benzoyl) benzoic acid , 4–BBA; 3,7-dihydroxy-2-naphthoic acid, 3,7–DHNA) was systemically explored in a flow tube reactor with the infrared spectroscopy , ion chromatography as well as theoretical calculation. NO 2 enhanced SO 2 uptake and sulfate generation on BrC under irradiation, as shown by larger steady-state uptake coefficients of SO 2 and sulfate formation rates. NO 2 − can be produced through the reduction of NO 2 by the photogenerated electrons on BrC, and it was proven to be the trigger that promoted the oxidation of SO 2 to sulfates. NO 2 − was more easily formed on FL, followed by 4−BBA and 3,7−DHNA, which can be evidenced by the energy barrier for NO 2 − production: FL (0.01 kJ mol −1 ) < 4−BBA (0.12 kJ mol −1 ) < 3,7−DHNA (1.33 kJ mol −1 ). SO 2 lifetimes and sulfate formation rates during the reaction of SO 2 /NO 2 with BrC were estimated to be 10.60–31.75 days and 0.02–0.04 μg m −3 h −1 , respectively.

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ACS Sensors · 2025 · IF 9.1

Detection of ppb-Level SO2 at Room Temperature Based on Bi2O2Se Nanosheets

Xinxin He,Xuanyu Ren,Xuyang An,Ping Guo,Yinhua Hu,Tiezhu Liu,Jia Zhang

Monitoring sulfur dioxide (SO2) is crucial for protecting human health as exposure to this pollutant can cause respiratory and cardiovascular illnesses, particularly in vulnerable populations. The primary materials currently used for detecting SO2 are metal oxides. However, it is still a challenge to detect SO2 at the parts per billion (ppb) level via these materials even when operated at high temperatures. Herein, we propose a highly sensitive SO2 sensor that operates at room temperature (RT). The sensing material employed is the hydrothermally synthesized bismuth oxyselenide (Bi2O2Se) nanosheets. The Bi2O2Se sensor exhibits a response value of 34% to 1 ppm SO2 and a detection limit of 20 ppb, which surpasses most SO2 sensors reported to date. The superior sensitivity and selectivity of Bi2O2Se nanoppbsheets toward SO2 are attributed to their strong adsorption energy (−0.76 eV) and significant electron transfer (2.205 e) between Bi2O2Se and SO2 molecules, as confirmed by density functional theory (DFT) calculations. Finally, a wireless SO2 sensing system is designed and implemented based on the SO2 sensor, enabling the detection of trace-level SO2 in indoor environments such as factories and laboratories, thereby protecting the well-being of personal further.

研究领域: 材料科学 · 环境监测
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JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES · 2024 ·Vol. 129 ·期 3 ·e2023JD040017 · IF 3.8

Unveiling the Role of Carbonate Radical Anions in Dust-Driven SO2 Oxidation

Yangyang Liu,Tao Wang,Qiuyue Ge,Wenbo You,Kejian Li,Wei Wang,Lifang Xie,Longqian Wang,Xiaozhong Fang,Xuejun Ruan,Le Yang,Runbo Wang,Liwu Zhang

Carbonate radical anion ( C O 3 . − ${\mathrm{C}{\mathrm{O}}_{3}}^{.-}$ ) is generally overlooked in atmospheric chemistry. Our recent work emphasizes the important role of carbonate radicals produced on mineral dust surfaces in fast sulfate production under solar irradiation in the presence of CO 2 at specifically low RH and light intensity. Yet so far how C O 3 . − ${\mathrm{C}{\mathrm{O}}_{3}}^{.-}$ involves and affects secondary sulfate production under diverse RH, light intensity, and complex constituent matrix remains unknown, which essentially limits our comprehensive knowledge of C O 3 . − ${\mathrm{C}{\mathrm{O}}_{3}}^{.-}$ initiated SO 2 oxidation scheme in the atmosphere. Herein, we explored the heterogeneous SO 2 oxidation over both model and authentic dust and clays in the presence of CO 2 at atmospheric relevant RHs and light intensities. Interestingly, we observe that CO 2 promotes sulfate yield over authentic dust and clays at atmospheric-relevant RH and light intensity. This observation relates to the favorable kinetic between SO 2 oxidation and C O 3 . − ${\mathrm{C}{\mathrm{O}}_{3}}^{.-}$ while auto-quenching of these radical ions is largely minimized due to the sufficient sites of crustal constituents. Furthermore, employing a suite of authentic dust and machine learning strategies, we evaluated the relative importance of each constituent within airborne minerals or clays as well as environmental conditions including relative humidity, light intensity, and CO 2 concentration in affecting SO 2 uptake capability. On this basis, sulfate formation mediated by dust-driven pathway, accounting for nearly ∼20.9% of overall contribution by the end of this century during some pollution episodes, even higher than gas-phase · OH $\cdot \text{OH}$ (∼16.9%), will be increased by 163% if CO 2 -initiated SO 2 oxidation scheme is incorporated. Key Points Carbonate radical-initiated SO 2 heterogeneous oxidation is sensitive to RH, CO 2 concentration, light intensity, and dust constituents Carbonate radicals promote atmospheric sulfate production on authentic dust and clay particles at haze-relevant conditions This previously unrecognized scheme will account for ∼20.9% of overall atmospheric sulfate formation by the end of this century Plain Language Summary How carbonate radical ions involve and affect sulfate formation under different RHs, light intensities, and complex component matrices remains an open question. Secondary sulfate production is facilitated by C O 3 . − ${\mathrm{C}{\mathrm{O}}_{3}}^{.-}$ over authentic dust particles in atmospheric relevant RH and light intensity. More importantly, this research emphasizes that CO 2 is not an inert greenhouse gas that rarely participates in atmospheric chemistry but a strong oxidant precursor that will produce C O 3 . − ${\mathrm{C}{\mathrm{O}}_{3}}^{.-}$ and subsequently trigger quick SO 2 oxidation via chain reactions. This dust-driven reaction channel mediated by C O 3 . − ${\mathrm{C}{\mathrm{O}}_{3}}^{.-}$ potentially contributes to nearly ∼1/5 of secondary sulfate production during some pollution hours if the growing intensive anthropogenic activities continue.

研究领域: 大气化学 · 环境科学
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Plants-Basel · 2024 ·Vol. 13 ·期 21 ·3061 · IF 4

Effects of Postharvest SO2 Treatment on Longan Aril Flavor and Glucosinolate Metabolites

Rob Md Mahfuzur,Dongmei Han,Jianhang Xu,Yuqiong Lin,Xiaomeng Guo,Tao Luo,Zhenxian Wu,Shilian Huang,Xinmin Lv,Junbin Wei

SO 2 fumigation treatment (commonly known as sulfur treatment, ST) is a key method in the postharvest preservation of imported and exported fresh longan fruits, effectively reducing pericarp browning and enhancing color. Nonetheless, distinctive aromas, often referred to as “sulfur flavor”, may develop in the aril during the extended preservation period. This study employed “Caopu” longan as the test material and patented SO 2 -releasing paper (ZL201610227848.7) as a treatment to perform a 35-day low-temperature (5 °C) storage of the fruit. The changes in glucosinolates (GSLs) and associated metabolites in the aril of treated fruit (ST) were examined utilizing ultra-high-performance liquid chromatography-tandem mass spectrometry (UPLC-MS/MS) detection and widely targeted metabolomics technology. The findings indicated that following 35 days of storage, nearly all control (CK) fruit pericarp turned to brown, resulting in an edible fruit rate of 75.41% and a commercial fruit rate of 0%. In contrast, the treated (ST) fruit demonstrated an edible fruit rate and a commercial rate of 99.44%, while the pericarp color changed from dark yellow-brown to light earthy yellow. The sulfur-containing metabolites identified in longan fruit aril predominantly consist of amino acids and their derivatives (60.44%), followed by alkaloids (15.38%), nucleotides and their derivatives (1.10%), and other types (23.08%), which include GSLs. SO 2 treatment significantly reduced the content of oxidized glutathione in fruit aril but increased the content of GSLs and related amino acids and their derivatives. Via screening, 19 differential sulfur-containing metabolites were obtained between ST and CK, including 11 GSLs. The identified differential metabolites of GSLs were all increased, primarily comprising aliphatic GSLs, such as 1-hydroxymethyl glucosinolate, 2-Propenyl glucosinolate (Sinigrin), and 4-Methylsulfinylbutyl glucosinolate (Glucoraphanin). Pathway analysis showed that these differential metabolites were mainly involved in coenzyme factor synthesis, cysteine and methionine metabolism, and amino acid synthesis, among other pathways. To the best of our knowledge, this is the first study to reveal the causes of the special flavor of longan aril after SO 2 treatment, which is a great concern for longan consumers. Moreover, this study provides a scientific basis for exploring the reasons and mechanisms for the development of the sulfur flavor in the SO 2 -treated fruits during postharvest storage.

研究领域: 食品科学 · 采后技术 · 代谢组学 · 植物生理学
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JOURNAL OF CHEMICAL THERMODYNAMICS · 2017 · IF 2.726

Investigation of SO2 solubilities in some biobased solvents and their thermodynamic properties

Dongshun Deng,Xiaobang Liu,Yanhong Cui,Yaotai Jiang

Solubilities of SO 2 have been determined in four biobased solvents (BBSs) at temperatures between 293.15 K and 323.15 K with 10 K intervals and pressure scope of (0–120.0) kPa using isochoric saturation method. The BBSs were selected from butyl lactate (BL), glyceryl triacetate (GT), triethyl citrate (TEC), and acetyl triethyl citrate (ATEC). Henry’s constants and thermodynamic properties such as Gibbs free energy , enthalpy and entropy of dissolution were derived from the solubility data. The gravimetric solubilities of SO 2 in BBSs were in the range of (0.07–8.52) mol.kg −1 and changed with the sequence of GT > BL > TEC ≈ ATEC. All the dissolution enthalpies were negative at each condition. The performances of SO 2 absorption in these solvents were further compared with those in some ionic liquids as well as common absorbents. The results illustrated that present BBSs possessed the potentiality as SO 2 absorbents due to their relatively large absorption ability, small absorption enthalpy, low toxicity, and biodegradability.

研究领域: 化学工程 · 环境化学 · 热力学 · 绿色溶剂 · 气体吸收
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2014 · IF 2.235

Highly Efficient and Reversible Absorption of SO2 by Aqueous Triethylenetetramine Tetralactate Solutions

Jianguo Qian,Shuhang Ren,Shidong Tian,Yucui Hou,Chenxing Wang,Weize Wu

The capture of SO2 by ionic liquids (ILs) has drawn much attention. In this work, a series of triethylenetetramine (lactate)n ([TETA]Ln) was synthesized and triethylenetetramine tetralactate ([TETA]L4) was selected to prepare aqueous IL solutions to absorb SO2. It has been found that the aqueous IL solutions can absorb large amounts of SO2; the saturated mole ratio of SO2 to IL in the aqueous IL solution decreases with increasing temperature, and increases with increasing water content of the aqueous IL solution; the density and viscosity of the aqueous IL solution decreases with increasing temperature and water content, and the density and viscosity of aqueous IL solution after SO2 absorption is higher than that before SO2 absorption. The absorption of SO2 by the aqueous IL solution is reversible. Compared with other ILs, [TETA]L4 has many advantages in application, including inexpensive synthetic materials, uncomplicated synthetic procedures, high SO2 capacity, and excellent reversibility.

研究领域: 环境化学 · 绿色化学 · 气体分离 · 材料科学
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IEEE SENSORS JOURNAL · 2023 ·Vol. 23 ·期 24 ·30504-30515 · IF 4.3

Smart SO2 Sensor Based on Cs3Cu2I5@Fe2O3 Nanocrystals for Eliminating Humidity Interference

Yuyan Zhuang,Jintuo Zhu,Danhong Gao,Shasha Gao,Zijiang Yang,Sheng Huang,Xinjian He

Sulfur dioxide is a colorless gas with strong pungent odor, and prolonged inhalation can damage the respiratory system and heart. Precise measurement of sulfur dioxide is very important for the human health. While the current sulfur dioxide sensor works at a high temperature and is easily interfered by humidity. Therefore, in this work, we used a solution method to coat perovskite nanocrystals Cs3Cu2I5 with metal oxides Fe2O3 and obtained the room-temperature sulfur dioxide gas-sensitive materials Cs3Cu2I5@Fe2O3 nanocrystals. Meanwhile, combined with machine learning, the sensor has the ability of self-calibrating under different humidity environment, realizing the high precision and anti-interference measurement of sulfur dioxide. In addition, in this structure, the coating Fe2O3 not only helps to improve water stability but also transfers the interaction of sulfur dioxide to the inner Cs3Cu2I5 and lowers the gas-sensitive temperature to room temperature. The response/recovery time of the sulfur dioxide sensor based on Cs3Cu2I5@Fe2O3 is 31/816 s, and the sensitivity is 0.19 at 10 ppm. Then, intelligent classification algorithm was used for recognition, and the accurate recognition rate was up to 95.0%. Furthermore, density functional theory (DFT) was implemented to reveal the gas-sensitive mechanism that sulfur dioxide was adsorbed by Cs3Cu2I5@Fe2O3 nanocrystals, the good response was attributed to the band structure changes significantly, and the hybridization of electron orbitals was appeared between gas and nanocrystals. We believe that the sensor will have potential in sulfur dioxide, and the idea of using machine learning to intelligent eliminate humidity interference can also be extended to other gas sensor.

研究领域: 材料科学 · 气体传感 · 纳米技术 · 环境健康 · 智能传感系统 · 计算材料学
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Fabrication of metal oxides-based adsorbents for SO2 capture with equimolar adsorption

Yuqi Yang,Xiandong Hao,Zhongxiao Sun,Yuan Chen,Zhiyong Xu,Wenbo Zhao

A series of novel porous metal oxides (MO, M = Mg, Ca, Ba, Mn and Zn) adsorbents were synthesized through simple thermal treatment of the corresponding metal sulfite for the remotion of sulfur dioxide (SO 2 ). The obtained MO adsorbents were characterized by various techniques including scanning electron microscopy (SEM), thermal gravimetric analyzer (TGA), X-ray diffraction (XRD) and nitrogen adsorption studies. The results show that the SO 2 adsorption capacity of manganese oxide (MnO) is much higher than that of other MO. And due to its highly dispersed and large specific surface area, especially its well-developed pore structure, equimolar adsorption of SO 2 can be achieved for the first time among similar SO 2 adsorbents. In addition, different sources of MnO were explored and it was found that the MnO obtained from the decomposition of MnSO 3 had the highest SO 2 adsorption capacity. Adsorption kinetic studies show that the reaction between MnO and SO 2 conforms to the pseudo-second-order kinetic equation. Furthermore, it was found through seven-cycle experiments that the adsorption amount tended to stabilize in each of the following cycles, except for the first high temperature, which led to changes in the adsorbent and a decrease in cycling performance. This strategy has three advantages: one-step preparation at low temperatures, equimolar adsorption of SO 2 as well as good reusability and selectivity.

研究领域: 环境科学 · 材料科学
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JOURNAL OF CHEMICAL AND ENGINEERING DATA · 2018 · IF 2.196

Absorption of SO2 in Furoate Ionic Liquids/PEG200 Mixtures and Thermodynamic Analysis

Yaotai Jiang,Xiaobang Liu,Dongshun Deng

Carboxylate ionic liquid (IL) and polyethylene glycol 200 (PEG200) mixtures are suitable for the absorption of acidic SO2 because of their unique properties. In the present work, tetraethylammonium furoate ([N2222][FA]) and choline furoate ([Ch][FA]) were blended with PEG200 to form 40 wt % ILs/PEG200 mixtures as SO2 absorbents. The solubilities of SO2 in these two ILs/PEG200 mixtures were measured at T = (303.15, 313.15, 323.15, and 333.15) K and pressure up to 1.2 bar. [N2222][FA]/PEG200 demonstrated the high SO2 absorption capacity of 7.224 mol per kg absorbent at 303.15 K and 1.0 bar. The chemisorption mechanism of SO2 by mixture was studied by Fourier transform infrared and nuclear magnetic resonance spectra, and the influence of cations on the SO2 absorption capacity was analyzed. Furthermore, the reaction equilibrium thermodynamic model was used to correlate the experimental data, and Henry’s law constant (H), reaction equilibrium constant (K0), and thermodynamic properties (ΔrGm0, ΔrHm0, and ΔrSm0) were derived. The absorption enthalpies of the two binary mixtures are −46.39 and −23.07 kJ·mol–1 for the two mixtures, respectively. Considering the low cost, biodegradability of the materials, high capacity, and low absorption enthalpy, the [N2222][FA]/PEG200 mixture was regarded to be an attractive and promising alternative to pure ILs and ordinary solvent as a desulfurizer.

研究领域: 环境科学 · 化学工程
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