Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Zeyu Geng,Qin Xie,Zhongjiao Fan,Weining Sun,Wei Zhao,Junhao Zhang,Jianqiu Chen,Yun Xu
Four tertiary amine-based protic ionic liquids (PILs) have been carefully designed to investigate the performance of SO 2 uptake. Their physical properties of densities and viscosities were determined. In the four PILs, the highest capacity for SO 2 of the four PILs reached up to 5.64 mol/kg ILs (P = 1.0 bar, T = 313.2 K). The ideal selectivity of SO 2 /CO 2 was up to 250 in the separation application of SO 2 from CO 2 . The kinetic study demonstrated that the PILs could efficiently capture SO 2 quickly under the ambient pressure. Based on the SO 2 absorption capacity and selectivity, excellent recyclability , and fast absorption process, the PILs in this work are considered as a potential alternative to traditional absorbents in the flue gas desulfurization (FGD).
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
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2018
·
IF 3.141
Muyuan Chai,Wenbo Zhao,Genming Li,Shengchao Xu,Qingming Jia,Yuan Chen
In order to avoid the high energy consumption in SO2 capture with aqueous amine absorbents, a liquid–liquid SO2 phase-change absorbent (SPCA) was developed in the present work using N,N-dimethylaniline (DMA) as absorbent, and high-boiling liquid paraffin was used as solvent to adjust the boiling point of the solution. The homogeneous solution would form two immiscible liquid phases after SO2 bubbling, only the SO2-rich phase needed to be desorbed, which could effectively reduce the energy consumption. Different from the liquid–solid phase-change absorbents developed in our previous work, the liquid–liquid phase-change absorbent avoid their shortcomings such as difficulties in separation of absorption products. The absorption product of SPCA was proved to be a charge-transfer complex DMA·SO2 by NMR and FTIR characterization, and the phase-change mechanism was attributed to the polarity variation between DMA and DMA·SO2. The viscosities of SPCAs was lower than 11.65 mPa·s, and the viscosity of SO2-rich phase was 3.9 mPa·s at 30 °C. The mass absorption capacity was found to be 0.89 g SO2/g DMA at 1 atm and 20 °C by ignoring liquid paraffin. The SPCA exhibited extremely high mass selectivity of SO2/CO2 with the value of 351. In addition, it was found that water had no effect on the structure of the absorption product and the SO2 capacity of SPCA. SPCA could be completely regenerated in 50 min at 80 °C. All the results showed that the SPCAs composed of DMA/liquid paraffin have a good application prospect.
研究领域:
化学工程
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环境科学
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DOI
高影响因子
Catalysts
·
2022
·Vol. 12
·期 5
·534
·
IF 4.501
Zhaohui Teng,Shan Huang,Na Li,Qulan Zhou
Rice husk ash (RHA) has potential as a supporter of catalysts. In this research, we studied the activity and SO2tolerance of RHA-based Fe-Cu oxide in the reduction of NO by CO. Characterization methods were employed to study the properties of the catalysts and their SO2tolerance. Activity and SO2resistance were also tested at different temperatures. We recommend two catalysts with SO2resistance ability: Fe0.67Cu0.33/RHA (the highest catalytic activity) and Fe0.8Cu0.2/RHA. The NO removal rate hardly changed with the addition of SO2and was kept at about 100%. However, the CO conversion rate decreased with increasing SO2at the lower reaction temperatures, which may be due to the formation of sulfites. Fortunately, the deactivation was reversible and can be reduced with an increase in the reaction temperature. The results of our research may help promote the application of CO-SCR.Keywords:rice husk ash;Fe-Cu catalysts;NO reduction;SO2resistance;CO-SCR
研究领域:
环境科学
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催化化学
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DOI
高影响因子
Catalysts
·
2020
·Vol. 10
·期 1
·72
·
IF 3.52
Xiaopeng Zhang,Xiangkai Han,Chengfeng Li,Xinxin Song,Hongda Zhu,Junjiang Bao,Ning Zhang,Gaohong He
Sorbent of αMnO2nanorods coating TiO2shell (denoted as αMnO2-NR@TiO2) was prepared to investigate the elemental mercury (Hg0) removal performance in the presence of SO2. Due the core-shell structure, αMnO2-NR@TiO2has a better SO2resistance when compared to αMnO2nanorods (denoted as αMnO2-NR). Kinetic studies have shown that both the sorption rates of αMnO2-NR and αMnO2-NR@TiO2, which can be described by pseudo second-order models and SO2treatment, did not change the kinetic models for both the two catalysts. In contrast, X-ray photoelectron spectroscopy (XPS) results showed that, after reaction in the presence of SO2, S concentration on αMnO2-NR@TiO2surface is lower than on αMnO2-NR surface, which demonstrated that TiO2shell could effectively inhibit the SO2diffusion onto MnO2surface. Thermogravimetry-differential thermosgravimetry (TG-DTG) results further pointed that SO2mainly react with TiO2forming Ti(SO4)O in αMnO2-NR@TiO2, which will protect Mn from being deactivated by SO2. These results were the reason for the better SO2resistance of αMnO2-NR@TiO2.Keywords:core-shell structure;αMnO2nanorods;elemental mercury removal;SO2resistance
研究领域:
环境科学
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材料科学
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化学工程
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产品关联
DOI
高影响因子
FUEL PROCESSING TECHNOLOGY
·
2020
·
IF 4.982
Hongyuan Xi,Song Zhou,Zhao Zhang
A novel method based on a Na 2 S 2 O 8 /urea composite system was used to both synchronously absorb SO 2 and NO from marine diesel engine emissions and reduce the nitrate residues in cleaning wastewater. In the Na 2 S 2 O 8 /urea solution, a temperature of over 60 °C and a Na 2 S 2 O 8 concentration of >0.05 mol/L were found to fully absorb SO 2 by overcoming the SO 2 release and effectively absorb NO. Urea successfully reduced the residual nitrate concentration and improves NO absorption at a concentration below 2 mol/L. The NO and SO 2 removal efficiencies reached 97.8 ± 1.5% and 100%, respectively, at 70 °C in 0.1 mol/L Na 2 S 2 O 8 and 1.5 mol/L urea solutions. The residual nitrate concentration was 8.12 ± 0.25 mg/L, far below the regulatory limit of 60 mg/L. Acidic conditions (pH ≤ 5.5) could be conducive to absorbing NO and reducing the residual nitrate concentration. Based on the experimental results, this novel method is highly promising for reducing ship emissions.
研究领域:
环境科学
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化学工程
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Hui Liu,Zhujiang Wang,Hao Chen,Yushan Tu,Jun Wu,Fenghua Shen,Xudong Liu,Yingxue Fu,Lin Wu,Jiaqi Long,Kaisong Xiang
The electrocatalytic reduction of SO2 to produce H2S is a critical approach for achieving the efficient utilization of sulfur resources. At the core of this approach for commercial applications lies the imperative need to elevate current density. However, the challenges posed by high current density manifest in the rapid depletion of protons, leading to a decrease in SO2 partial pressure, consequently hampering the generation and separation of H2S. Here, we demonstrate an effective solution to alleviate the problem of insufficient supply of protons by employing Nafion polymer as the proton conductor to modified Cu catalysts surface, creating a proton-enriched layer to boost H2S generation. It was observed that Nafion shortens the hydrogen bonds with water molecules in the electrolyte via its sulfonic acid groups, benefiting the proton transfer and consequently increasing the proton density on the electrode surface by 5-fold. With the Nafion-modified catalyst, the H2S partial current density and separation efficiency reached 205.9 mA·cm–2 (1.01 mmol·cm–2·h–1) and 87.8%, which were 1.34 and 1.22 times that on unmodified Cu, respectively. This work highlights the practicality of fabricating a proton conductor via ionic polymer for the control over product selectivity in pH-sensitive reactions under high current density.
研究领域:
电化学
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材料科学
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催化
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环境化学
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DOI
PubMed
高影响因子
Chemical Physics Impact
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2022
·
IF 0
Yanke Yu,Mengqiao Geng,Jiahang Li,Jingjing Wang,Desheng Wei,Chi He
Commercial V 2 O 5 -WO 3 /TiO 2 (VWTi) catalysts used in NH 3 -SCR reaction with varied Zn loading were prepared and then effect of SO 2 on Zn-poisoned VWTi catalysts was investigated. Zn could cause the deactivation of VWTi catalysts. Nevertheless, the effect of SO 2 on Zn-poisoned VWTi catalysts varied with Zn loading. For Zn-poisoned catalyst with low content of Zn (1.0 wt.%, ZnL), SO 2 would promote the activity recovery of the catalyst. However, SO 2 had no influence on the Zn-poisoned catalyst with high Zn content (4.0 wt.%, ZnH). The catalyst was characterized by N 2 adsorption-desorption, XRD, XPS, SO 2 -TPD, NH 3 -TPD, H 2 -TPR and in situ DRIFTS. Tri-coordinated sulfate species were formed on ZnL sample in the presence of SO 2 , and the sulfate species could form new Brønsted acid sites, causing the recovery of activity. But ZnSO 4 was appeared and no Brønsted acid sites formed on ZnH sample under SO 2 , thus the activity of ZnH sample changed little.
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
ADSORPTION-JOURNAL OF THE INTERNATIONAL ADSORPTION SOCIETY
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2024
·Vol. 30
·期 3
·377-387
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IF 3
Ma Yuling,Li Airong,Wang Zhihong,Wang Cheng
There is an urgent need to address sulfur dioxide (SO 2 ) from the burning of fossil fuels, which poses a serious hazard to the surrounding environment due to its emission. In this work, UiO-66-type metal–organic framework materials (MOFs) were prepared by hydrothermal method and applied to flue gas desulfurization. Through characterization analysis, it was found that UiO-66 sample had high crystallinity and good thermal stability. Besides, UiO-66 sample had a large specific surface area (1423 m 2 /g) and a large pore volume (0.69 cm 3 /g). In the desulfurization experiments of SO 2 /CO 2 /O 2 /N 2 gas mixture (0.3/10.0/5.5/84.2 vol.%), UiO-66 had a breakthrough time of 137.6 min/g for SO 2 , the high selectivity of SO 2 /CO 2 (36.0), and strong acid resistance. Besides, the adsorption thermodynamic analysis can confirm that the adsorption process of UiO-66 for SO 2 was a combination of physical adsorption and chemical adsorption. At 1.0 bar and 298 K, the adsorption capacity of SO 2 on UiO-66 reached 8.12 mmol/g.
研究领域:
环境科学
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材料科学
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化学工程
✓ 已验证
DOI
高影响因子
AICHE JOURNAL
·
2015
·Vol. 61
·期 6
·2028-2034
·
IF 2.748
Kaihong Chen,Wenjun Lin,Xini Yu,Xiaoyan Luo,Fang Ding,Xi He,Haoran Li,Congmin Wang
Five kinds of anion-functionalized ionic liquids (ILs) with different basicity and substituent were selected, prepared and applied in the capture of SO 2 from flue gas, where the concentration of SO 2 is only 2000 ppm. The effect of the anion on SO 2 absorption capacity, desorption residue, and available absorption capacity under 2000 ppm was investigated. The relationship between available absorption capacity and absorption enthalpy was also studied. Through a combination of thermodynamic analysis and quantum calculation, the results indicated that the effect of the cation in the IL on absorption enthalpy was significant. However, the effect of chain length in the cation was weak. Hence, a new IL with low molecular weight, [P 4442 ][Tetz], was further designed and applied for the capture of SO 2 , which shows the high absorption capacity of 0.18 g SO 2 per g IL and excellent reversibility for 2000 ppm SO 2 . © 2015 American Institute of Chemical Engineers AIChE J , 61: 2028–2034, 2015
研究领域:
环境科学
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化学工程
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产品关联
DOI
高影响因子
RSC Advances
·
2017
·Vol. 7
·期 30
·18500-18507
·
IF 3.108
Xuecheng Liu,Yugo Osaka,Hongyu Huang,Jun Li,Zhaohong He,Xixian Yang,Huhetaoli,Shijie Li,Noriyuki Kobayashi
Increasing concern about sulfur dioxide (SO2) from diesel vehicle exhausts causing detrimental effects on NOx removal catalysts has resulted in the development of dry desulfurization filters for complete removal of SO2. In this study, a compact MnO2 filter was developed for diesel emission control. The SO2-capture behavior of the compact MnO2 filter was investigated by using a volumetric device in a low temperature range (200–400 °C) and low SO2 pressure conditions. The maximal capacity of the MnO2 filter was 304.1 mgSO2 per gMnO2 at 400 °C. Based on the experimental results, the required volume of the MnO2 filter was estimated as only 0.6 L for a diesel car with 30 000 km distance traveled per year. The thickness of the MnO2 filter had significant influence on its SO2-capture performance. The sulfate reaction mechanism was also discussed by using a grain model under four reaction temperature conditions for improving the efficiency of the design of the desulfurization filter. The sulfate process can be divided into two control stages (the chemical reaction control stage and the solid diffusion control stage) and the prediction models fit the experimental data well for both control stages, indicating that the two-stage grain model is suitable for the sulfate reaction between the MnO2 filter and SO2. The calculated apparent activation energy of 18.8 kJ mol−1 indicates that the MnO2 filter exhibits high activity for SO2 adsorption in a pure SO2 atmosphere.
研究领域:
环境科学
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化学工程
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产品关联
DOI
高影响因子
DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 18
·6129-6137
·
IF 4
Peipei Wang,Jin Tong,Cong Meng,Qing Yuan,Wei Deng,Shu-Yan Yu,Hong-Wei Ma
Owing to their structural designability and tuneable properties, supramolecular metal–organic complexes have recently emerged as promising candidates for the sensing and detection of molecules and anions. Herein, we synthesised three tripyrazolate-linked [M6L2] metallocages with the formulas [(bpyPd)6L2](NO3)6 (1), [(dmbpyPd)6L2](NO3)6 (2), and [(phenPd)6L2](NO3)6 (3) (H3L = tris(4-(5-(trifluoromethyl)-1H-pyrazol-3-yl)phenyl)amine, bpy = 2,2′-bipyridine, dmbpy = 4,4′-dimethylbipyridine, phen = 1,10-phenanthroline). Crystallography revealed that metal-directed coordination and the bidentate chelate behaviour of the ligand induced the self-assembly of supramolecular metal–organic cages. Notably, these cages were employed as turn-on fluorescence sensors for SO2 and its derivative (HSO3−) through a disassembly mechanism. Cages 1, 2, and 3 showed a highly selective and sensitive detection of HSO3− over other common anions in aqueous solutions and of SO2 gas over other common gasses, with an excellent anti-interference ability. These metallocages were subsequently applied as sensors in environmental and biological samples. This study not only enriches the ongoing research on metal–organic supramolecular materials but also facilitates the future preparation of stimuli-responsive supramolecular coordination complexes.
研究领域:
超分子化学
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分析化学
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DOI
PubMed
高影响因子
Journal of Environmental Sciences
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2022
·
IF 6.796
Peng Lu,Xianhui Yan,Lyumeng Ye,Dingsheng Chen,Dongyao Chen,Jianhang Huang,Chaoping Cen
The co-removal of CO 2 while removing SO 2 and NO x from industrial flue gas has great potential of carbon emission reduction but related research is lacking. In this study, a wet scrubbing process with various urea solutions for desulfurization and denitrification was explored for the possibility of CO 2 absorption. The results showed that the urea-additive solutions were efficient for NO x and SO 2 abatement, but delivered < 10% CO 2 absorption efficiency. The addition of Ca(OH) 2 dramatically enhanced the CO 2 absorption, remained the desulfurization efficiency, unfortunately restricted the denitrification efficiency. Among various operating parameters, pH of solution played a determining role during the absorption. The contradictory pH demands of CO 2 absorption and denitrification were observed and discussed in detail. A higher pH of solution than 10 was favorable for CO 2 absorption, while the oxidizing of NO to NO 2 , NO 2 − or NO 3 − by NaClO 2 was inhibited in this condition. When 7 < pH < 10, it was favorable for the conversion and absorption of NO and NO x . However, the conversion of HCO 3 − to CO 3 2− was significantly inhibited, hence preventing the absorption of CO 2 . Large part of Ca(OH) 2 became CaCO 3 with a finer particle size, which covered the unreacted Ca(OH) 2 surface after the reaction. Kinetic analysis showed that the CO 2 absorption in urea-NaClO 2 -Ca(OH) 2 absorbent was controlled by chemical reaction in early stage, then by ash layer diffusion in later stage.
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）