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CHEMICAL ENGINEERING JOURNAL · 2019 · IF 8.355

Simultaneous removal of NO and SO2 through heterogeneous catalytic oxidation-absorption process using magnetic Fe2.5M0.5O4 (M = Fe, Mn, Ti and Cu) catalysts with vaporized H2O2

Zijian Song,Ben Wang,Wu Yang,Tao Chen,Chuan Ma,Lushi Sun

Fe 2.5 M 0.5 O 4 (M = Mn, Ti and Cu) were investigated for the first time as the catalyst for simultaneous removal of NO and SO 2 through catalytic oxidation-absorption with vaporized H 2 O 2 . The physicochemical properties of as-prepared catalysts were comprehensively characterized by XRD, SEM, TEM, BET, XPS, TPR, VSM, TG and PL analyses. Activity test results showed that SO 2 can be completely removed under most conditions. However, NO removal was affected by catalyst, H 2 O 2 consumption, reaction temperature, GHSV and coexistence gases (i.e., H 2 O, O 2 , NO and SO 2 ). Mn, Ti and Cu doping in the magnetite can remarkably enhance NO removal. Redox pairs and oxygen vacancy of catalysts were considered as vital factors affecting OH generation. Base on the catalyst characterization and DFT calculation results, the main mechanism of Mn, Ti and Cu doping on the catalytic activity improvement was explained as follows: (a) Mn, Ti and Cu doping can increase the catalyst surface area; (b) Ti on the surface can directly promote the catalytic decomposition of H 2 O 2 ; and (c) Mn and Cu doping can promote the generation of oxygen vacancy and indirectly increase the activity. Moreover, two arrangement forms of an industrial simultaneous removal system for NO, SO 2 and Hg 0 were proposed.

CAS / MDL: 3317-61-1
研究领域: 环境科学 · 催化化学
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CHEMICAL ENGINEERING JOURNAL · 2018 · IF 6.735

Insights into the Sm/Zr co-doping effects on N2 selectivity and SO2 resistance of a MnOx-TiO2 catalyst for the NH3-SCR reaction

Chuanzhi Sun,Hao Liu,Wei Chen,Dezhan Chen,Shuohan Yu,Annai Liu,Lin Dong,Shuai Feng

A series of Sm- and/or Zr-doped MnO x -TiO 2 catalysts were prepared, and the catalysts exhibited better N 2 selectivity and SO 2 resistance than the undoped MnO x -TiO 2 catalyst for the selective catalytic reduction of NO by NH 3 (NH 3 -SCR). The reasons for the good N 2 selectivity and SO 2 resistance of the catalysts were proposed. X-ray photoelectron spectroscopy (XPS) combined with density functional theory (DFT) calculations suggested that electron transfer between the manganese and samarium species by Mn 4+  + Sm 2+  ↔ Mn 3+  + Sm 3+ redox cycles occurred in the Sm-containing catalysts. Furthermore, electron transfer from Sm 2+ to Mn 4+ suppressed electron transfer from NH 3 to Mn 4+ , inhibiting the formation of NH 2 or NH. Thus, the pathway for NH generation was removed, and the reaction of 2NH + 4NO → 3N 2 O + H 2 O was prevented. Consequently, the N 2 selectivity of the NH 3 -SCR reaction was enhanced. In situ diffused reflectance infrared Fourier transform spectroscopy ( in situ DRIFTS) combined with thermogravimetry, differential scanning calorimetry and mass spectrometry (TG-DSC-MS) results revealed that the deposition rate of sulfate species decreases after Sm doping, which was also attributed to the suppressed electron transfer from SO 2 to Mn 4+ , i.e., the oxidation of SO 2 to SO 3 . Thus, the catalysts exhibited better SO 2 resistance.

CAS / MDL: 13759-83-6
研究领域: 催化化学 · 环境科学
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Rationally engineered ReOx-CuSO4/TiO2 catalyst with superior NH3-SCO efficiency and remarkably boosted SO2 tolerance: Synergy of acid sites and surface adsorbed oxygen

Yanke Yu,Desheng Wei,Zhaojian Tong,Jinxiu Wang,Jinsheng Chen,Chi He

Ammonia (NH 3 ) is a critical component causing environmental problems like haze and water pollution. Selective catalytic oxidation of ammonia (NH 3 -SCO) to N 2 and H 2 O is a promising method to abate NH 3 emission. However, inferior SO 2 tolerance is still a tremendous challenge to be conquered for present NH 3 -SCO catalysts regarding practical applications. Application of materials which was difficult to be sulfated by SO 2 should be an effective way to solve this problem. Here, a ReO x -CuSO 4 /TiO 2 catalyst which coupled the advantages of ReO x (Rhenium oxides, supplying highly active adsorbed surface oxygen enhancing NH 3 -SCO reaction) and CuSO 4 (providing Brønsted acid sites inhibiting the formation of N 2 O) was rationally fabricated. Results indicated that ReO x -CuSO 4 /TiO 2 catalyst exhibited excellent catalytic performance in NH 3 -SCO with almost 100% of NH 3 oxidized at 300 °C (N 2 selectivity as high as 96%). Crucially, the composite catalyst exhibited incredible activity and stability under harsh reaction conditions toward SO 2 (600 ppm) and H 2 O (4.0 vol%) owing to the superior inhibition capability for SO 2 adsorption. In situ DRIFTS, in situ Raman and in situ XPS demonstrated that the NH 3 -SCO reaction over ReO x -CuSO 4 /TiO 2 catalyst mainly obeyed a N 2 H 4 reaction mechanism and oxidation–reduction circle between Re 7+ and Re 6+ played a vital role. Moreover, SO 2 would not affect this reaction mechanism on ReO x -CuSO 4 /TiO 2 catalyst. The knowledge and understanding reported could provide critical insights for the design and optimization of efficient materials for industrial NH 3 oxidative elimination.

CAS / MDL: 13463-67-7 7758-99-8
研究领域: 催化化学 · 环境科学 · 材料科学
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JOURNAL OF NANOPARTICLE RESEARCH · 2019 ·Vol. 21 ·期 4 ·1-7 · IF 2.009

The influence of the pore structure on the SO2 tolerance for selective catalytic reduction of NOx with NH3 over MnOx-TiO2/MWCNTs catalysts

Xie Chong,Shi Jian-Wen,Yang Shenghui,Li Xifei

The MnO x -TiO 2 /MWCNTs nanocomposites were used as De-NO x catalysts to study the deep-rooted reason for the deactivation. Based on a series of characterization on as-prepared catalyst and poisoned catalyst, the results showed that the chief culprit for the deactivation is the micropores in the De-NO x catalyst. The formed ammonium (bi)sulfate in the micropores during the SCR reaction process could not be took away by the gas flow soon and then deposited on the catalyst surface gradually, and further covered the active sites. And the poisoned catalysts could be recovered partly rather than fully by heat treatment at 500 °C because of the decomposition of the ammonium (bi)sulfate and the phase transition of the TiO 2 .

研究领域: 环境催化 · 纳米材料科学 · 大气污染控制
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY · 2022 · IF 4.831

A dual-site multifunctional fluorescent probe for selective detection of endogenous H2O2 and SO2 derivatives based on ICT process and its bioimaging application

Xue-Liang Liu,Mengdi Yan,Zhi-guo Chen,Bingxin Zhang,Ningcong Yao,Shan Zhao,Xiaoxia Zhao,Tao Zhang,Guangfan Hai

In this paper, we reported a coumarin-based fluorescent probe for selective detection of H 2 O 2 /SO 2 derivatives via ICT process. To the best of our knowledge, it was few reported with the same probe to enable visual detection of H 2 O 2 /SO 2 derivatives in vivo and in vitro. H 2 O 2 and SO 3 2− were selectively sensed over other analytes, and the probe displayed 20-fold and 220-fold relative fluorescence intensity respectively, as well as the good linear relationship and the excellent detection limits of 2.7 * 10 3 nM and 19.3 nM. Furthermore, the probe was successfully used for fluorescence imaging of the HeLa cells and the mice to monitor exogenous and endogenous H 2 O 2 and SO 3 2− , suggesting its potential biomedical application for investigation and detection the intermediate indicator of oxidative stress in vitro and in vivo.

研究领域: 分析化学 · 生物医学工程 · 细胞生物学
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APPLIED CATALYSIS A-GENERAL · 2021 · IF 5.706

Excellent low-temperature NH3-SCR of NO activity and resistance to H2O and SO2 over WaCeOx (a = 0.06, 0.12, 0.18, 0.24) catalysts: Key role of acidity derived from tungsten addition

Huansheng Tan,Shibo Ma,Xiaoyu Zhao,Yushi Li,Chen Zhao,Yujun Zhu

Bimetallic W a CeO x (a = 0.06, 0.12, 0.18, 0.24) catalysts were synthesized for selective catalytic reduction of NO x with NH 3 (NH 3 -SCR). The influences of W on structure, activity and surface properties were investigated by XRF, XRD, Raman, TEM, N 2 adsorption-desorption, H 2 -TPR, O 2 /NH 3 /SO 2 -TPD, XPS, and in-situ DRIFTS. The characterization results show that the W/Ce ratio has a great effect on the NH 3 -SCR activity. The different catalytic activities of W a CeO x are mainly attributed to the acidity change, especially the increase of B-acid content plays a major role in enhancing low temperature activity. W 0.18 CeO x exhibits excellent low-temperature NH 3 -SCR activity, SO 2 /H 2 O resistance and N 2 selectivity with a broad activity window (190–490 °C) with 5%H 2 O. Moreover, good activity window (235–460 °C) can be maintained even the catalyst treated with 5% H 2 O at 800 °C for 12 h, showing especial hydrothermal stability. Thus, it can be summarized that W 0.18 CeO x is regarded as outstanding catalyst for low-temperature NH 3 -SCR of NO.

CAS / MDL: 12333-11-8 10294-41-4
研究领域: 催化化学 · 环境科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2020 · IF 5.774

Investigation on amino distribution in porous resins for low concentration SO2 purification

Bin Xu,Lu Chen,Xiao Yu,Tao Zhou,Youcai Zhao

Effective purification of low concentration SO 2 at cathode air stream side is essential for Proton exchange membrane fuel cells performance in the real-world application. Amino modification porous material is the effective purification media. The modifier distribution along the pore channels is one of the most influencing parameters that determine the purification performance. Amino-modified porous resins are synthesized to assess the mechanism of modifier distribution along the pore channel. Modifier concentration, modification time, modification temperature, and intersolubility between solvent and modifier are found to significantly affect the modifier distribution. Increased modifier concentration within a relatively low range (0–200 g/L) is favorable to grafting modifier in external pore channel. However, no more significant modifier grafting was found for higher modifier concentration due to the higher solvent viscosity and lower modifier diffusion. Increased modification time leads to more amino groups grafted in deep pore channel. However, after the modification time is longer than 6 h, the modifier no longer diffuses into deeper pore channel due to the diffusion limitation. Solvent property significantly affects the modifier solubility and the swelling degree of porous resin. Larger intersolubility between solvent and modifier enhances the modifier diffusion into pore channel.

研究领域: 环境科学 · 材料科学 · 化学工程 · 能源技术
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Chemical Engineering Journal Advances · 2020 · IF 0

In/H-Beta modified by Co3O4 and its superior performance in the presence of H2O and SO2 for selective catalytic reduction of NOx with CH4

Jiuhu Zhao,Zhengzhong Wen,Rongshu Zhu,Zhi Li,Ran Ding,Yongji Zhu,Tingkun Gu,Rong Yang,Zhenye Zhu

In this paper, In-metal oxide/H-Beta catalysts were synthesized by ion exchange method and In-Co 3 O 4 /H-Beta exhibited the highest catalytic activity for the selective catalytic reduction of NO x with CH 4 in presence of H 2 O and SO 2 . Thus, the synthesis conditions of In-Co 3 O 4 /H-Beta were optimized. The results showed that In-Co 3 O 4 /H-Beta exhibited excellent catalytic performance and high CH 4 selectively when the synthesis was carried out by ion exchange method, the ratio of Si and Al in H-Beta was 25, the ratio of Co 3 O 4 and H-Beta was 5:40, the concentration of ion exchange liquid was 0.033 M and calcination temperature was 500 °C. The NO x removal efficiency was about 87.6 % and N 2 selectivity could reach 96.3% in the presence of H 2 O and SO 2 . Through a series of characterizations, it was concluded that In-Co 3 O 4 /H-Beta owned stable catalyst structure, abundant Brønsted acid sites and the highest ratio of InO + /In 2 O 3 under the optimal synthesis conditions. In addition, the doped of Co 3 O 4 could inhibit the adsorption of sulfate species on the surface of In/H-Beta catalyst, leading to the excellent H 2 O and SO 2 resistance property.

研究领域: 环境科学 · 催化化学
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PHYSICS AND CHEMISTRY OF LIQUIDS · 2019 · IF 1.526

Absorption, desorption and interaction of SO2 with the binary system tetraethylene glycol + dimethyl sulfoxide

Huihu Shi,Yunyun Fan,Xianshu Qiao,Chang Liu,Shuai Zhang,Zhaojun Wu

The gas-liquid equilibrium (GLE) data were determined for the mixture SO2 + N2 in the binary system of tetraethylene glycol (TeEG) + dimethyl sulfoxide (DMSO) at T = 298.15–313.15 K and p = 123.15 kPa with the SO2 partial pressures of 0.4–150 Pa. From GLE data, Henry’s law constants (HLCs) were obtained. When the SO2 concentration in the gas phase was designed at ySO2 = 500 ppmv, the SO2 solubility in the binary system is located in a minimum of 9.36 mol m−3 in TeEG and a maximum of 80.34 mol m−3 in DMSO. The SO2 absorption process was reversible from the five absorption–desorption cycles, and the solvents could repeat utilisation without obvious loss of absorption capacity and the homologous SO2 desorption efficiency was nearby 98.7%. Furthermore, the spectral consequences illustrated that H-bonding was formed among TeEG, DMSO and SO2.

CAS / MDL: 112-27-6
研究领域: 化学工程 · 环境科学 · 物理化学
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JOURNAL OF HAZARDOUS MATERIALS · 2024 · IF 12.2

Ratiometric SERS quantification of SO2 vapor based on Au@Ag-Au with Raman reporter as internal standard

Yu Lu,Xiufang Mo,Geng Zhu,Yan Huang,Yingchao Wang,Zhenzhong Yang,Liqiong Gao,Guofang Shen,Yi Wang,Xiangwei Zhao

Practical gas sensing application requires sensors to quantify target analytes with high sensitivity and reproducibility. However, conventional surface enhanced Raman scattering (SERS) sensor lacks reproducibility and quantification arising from variations of "hot spot" distribution and measurement conditions. Here, a ratio-dependent SERS sensor was developed for quantitative label-free gas sensing. Au@Ag-Au nanoparticles (NPs) were filtered onto anodic aluminum oxide (AAO) forming Au@Ag-Au@AAO SERS substrate. 4-MBA was encapsulated in the gap of Au@Ag-Au and served as the internal standard (IS) to calibrate SERS signal fluctuation for improved quantification ability. Combined with headspace sampling method, SO 2 residue in traditional Chinese medicine (TCM) can be extracted and captured on the immediate vicinity of Au@Ag-Au surface. The intensity ratio I 613 cm −1 /I 1078 cm −1 showed excellent linearity within the range of 0.5 mg/kg-500 mg/kg, demonstrating superior quantification performance for SO 2 detection. Signals for concentration as low as 0.05 mg/kg of SO 2 could be effectively collected, much lower than the strictest limit 10 mg/kg in Chinese Pharmacopoeia. Combined with a handheld Raman spectrometer, handy and quantitative TCM quality evaluation in aspect of SO 2 residue was realized. This ratiometric SERS sensor functioned well in rapid on-site SO 2 quantification, exhibiting excellent sensitivity and simple operability.

CAS / MDL: 50-81-7 1074-36-8
研究领域: 分析化学 · 材料科学 · 环境科学 · 药学
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FUEL · 2025 · IF 7.5

Highly efficient NOx reduction with superior H2O and SO2 resistance on Ce-Ti/γ-Fe2O3 dual single-atom Catalysts: Synergistic interactions and mechanistic insights

Jianping Ding,Xiaoyan Zhou,Zhengzheng Yang,Changgeng Liu,Mingchao Sun,Congling Yang,Lu Fan

In this study, a novel strategy was proposed for synthesizing dual single-atom Ce-Ti catalysts supported on γ-Fe 2 O 3 via ball milling and calcination. Compared to γ-Fe 2 O 3 and single-atom Ce/γ-Fe 2 O 3 and Ti/γ-Fe 2 O 3 catalysts, the Ce-Ti/γ-Fe 2 O 3 catalyst exhibits superior NO conversion rates and significantly enhanced tolerance to H 2 O and SO 2 at 200–240 °C. These advancements are attributed to the synergistic interactions between Ce and Ti, which enhance redox properties, increase Lewis acid site density, and facilitate the Langmuir-Hinshelwood reaction pathway. In-situ DRIFTS and density functional theory (DFT) analyses revealed the mechanistic role of surface-active oxygen species and intermediate formation in promoting the SCR reaction. The findings provide valuable mechanistic insights and establish a scalable approach for the development of high-performance, environmentally friendly catalysts for industrial NO x removal.

研究领域: 催化化学 · 环境科学 · 材料科学
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Green Energy & Environment · 2020 · IF 6.395

Design and prediction for highly efficient SO2 capture from flue gas by imidazolium ionic liquids

Lili Jiang,Ke Mei,Kaihong Chen,Rina Dao,Haoran Li,Congmin Wang

An efficient method for prediction in the capture of SO 2 from flue gas by imidazolium ionic liquids was reported, where the concentration of SO 2 is 2000 ppm. On the basis of quantitative calculations through a combination of Langmuir simulation, theoretical calculation and quantum chemical method, SO 2 absorption and desorption performance from flue gas by twelve kinds of imidazolium ionic liquids with different anions were designed and predicted. Then, among them, five kinds of imidazolium ionic liquids were chosen and prepared to investigate their behavior of SO 2 absorption capacity , desorption residue, and available absorption capacity. The results indicated that the experimental values were in good agreement with the predicted values. Thus, an ideal ionic liquid [Emim][Tetz] was obtained through the predictive method for the capture of SO 2 of 2000 ppm, which showed high available absorption capacity of 0.24 g SO 2 per g ionic liquid and excellent reversibility .

CAS / MDL: 74-96-4 288-88-0
研究领域: 环境科学 · 化学工程 · 材料科学
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