CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yuling Ma,Airong Li,Cheng Wang
Metal-organic frameworks (MOFs) with a high specific surface area, an adjustable pore structure, and functionalized pore environment have a broad application prospect in gas adsorption and separation. In this work, a series of defective UiO-66 (UiO-66-monocarboxylic acid) samples were prepared by adding different monocarboxylic acids during the synthesis of UiO-66. UiO-66-monocarboxylic acid samples (UiO-66-formic acid, UiO-66-acetic acid, UiO-66-benzoic acid, UiO-66-acrylic acid, and UiO-66-cyanoacetic acid) had a high specific surface area (1200–1400 m 2 /g) and a good thermal stability (560 °C). In the desulfurization experiment of simulated flue gas (SO 2 /CO 2 /O 2 /N 2 , 0.3/10.0/5.5/84.2 vol%), the breakthrough time of UiO-66-cyanoacetic acid for SO 2 was higher (194 min/g), and the selectivity of SO 2 /CO 2 reached 33.8. Through optimizing the moles of cyanoacetic acid added, the breakthrough time of SO 2 on 18-UiO-66-cyanoacetic acid increased to 251 min/g. At a pressure of 1.0 bar and a temperature of 298 K, the adsorption capacity of SO 2 by 18-UiO-66-cyanoacetic acid reached 762.1 mg/g. In addition, the adsorption behavior of 18-UiO-66-cyanoacetic acid for SO 2 was considered as a combination of chemical and physical adsorption, and fractional chemisorption sites was provided by cyanoacetic acid.
研究领域:
材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Chengzhi Wang,Fengyu Gao,Songjin Ko,Hengheng Liu,Honghong Yi,Xiaolong Tang
The presence of SO 2 in industrial flue gases will cause permanent deactivation of the catalyst active centre. Therefore, an effective method to improve the SO 2 resistance of manganese-based catalysts at low temperatures is urgently needed. In this work, a hierarchical porous nanowire structure catalyst was designed by the in situ self-assembly method to inhibit SO 2 adsorption. This hierarchical porous nanowire aerogel catalyst with great BET surface area and surface acidity exhibited NOx conversion above 90% at 100–400 °C. Notably, the NOx conversion of the MnCe-N catalyst was almost not inhibited by SO 2 (250 ppm) compared to the 33% decrease of the MnCe-P catalyst. On the MnCe-P catalyst, SO 2 has strong competitive adsorption with NH 3 and NO, and the stronger adsorption capacity of SO 2 inhibits the adsorption activation of the reaction gas and hinders the reaction proceeding through the L-H mechanism. Meanwhile, a large quantity of sulfate is formed on the catalyst surface, which prevents the active centre to participate in the redox reaction. The structure of nanowires enhances the number of acid sites, facilitates the adsorption and activation of NH 3 , and effectively inhibits the adsorption of SO 2 on the MnCe-N catalyst. Fewer sulfate species are generated and difficult to deposit and aggregate on the catalyst surface, as a result, the active centre is less affected by sulfate species. The stable adsorption of NH 3 -related species ensures reliable reaction on MnCe-N through the E-R mechanism. This work emphasizes the importance of hierarchically porous structures in improving the NH 3 -SCR performance and SO 2 resistance of monolithic catalysts, and provides new insights into the design of highly efficient and stable catalytic materials.
研究领域:
催化
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环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2024
·
IF 5.9
Hongliang Sheng,Xiaoben Zhao,Shuainan Wang,Tao He,Jinfeng Zhang,Song He,Yajun Huang
In this paper, we investigated the properties of nitrogen-doped activated carbon produced via the co-activation of KSCN and KOH, using hydrothermal lignin as a precursor. The resulting activated carbon exhibited a high specific surface area of 3504 m 2 /g and contained 3.37 % nitrogen from KSCN, which enhanced its adsorption efficiency. The adsorption capacities for SO 2 and benzene at 273 K were measured at 2260.68 mg/g and 1668.90 mg/g, respectively. Competitive adsorption experiments at 298 K showed that in the presence of SO 2 , the activated carbon maintained a high adsorption capacity for benzene at 1008.81 mg/g, while the adsorption capacity for SO 2 decreased to only 12.31 mg/g, indicating a higher affinity for benzene. The selectivity coefficient, calculated using the Ideal Adsorbed Solution Theory (IAST), reached 44.76 at a benzene-to-SO 2 ratio of 2:1. To gain deeper insights into the selective adsorption mechanism, Density Functional Theory (DFT) simulations were conducted. These simulations confirmed the experimental findings, indicating that benzene can be selectively adsorbed and effectively separated from SO 2 flue gas.
研究领域:
材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
MICROCHEMICAL JOURNAL
·
2025
·
IF 5.1
Yueru Chen,Zongning Guo,Xuelin Huang,Jiangying Qu,Feng Gao,Kai Wan,You Zhang,Xiaofang Zhao,Zhe Jiao
In this study, we designed a fluorescent Por-COF-MF, for selective detection SO 2 in wine. The fluorescence was quenched due to the intramolecular charge transfer (ICT) process blocked by SO 2 . A good linear relationship of fluorescent intensity with SO 2 in the concentration range of 0.01–1 ppm was found. To achieve facile solid-state detection, Por-COF-MF was loaded on polyvinyl alcohol (PVA) to fabricate a uniform fluorescent film Por-COF-MF@PVA. Then a portable device was designed by 3D printing technology. The device exhibited good linearity in the SO 2 concentration range of 0.5–3 ppm, with a detection limit of 0.06 ppm. The relative standard deviation (RSD) was less than 8 % when measuring SO 2 in three different types of wine. Compared to other portable technologies, our 3D-printed fluorescent device allowed for direct detection of SO 2 content in wine, which provided a more effective and economical method for food safety monitoring.
研究领域:
食品安全
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化学传感器
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL PROCESSING TECHNOLOGY
·
2019
·
IF 4.507
Haotian Li,Feng Liu,Shuhui Wang,Fengjia Wang,Xin Qian,Caiduan Zhang,Yongliang Ma,Lidong Wang
Based on advanced oxidation technology, a new method for the simultaneous removal of SO 2 and NO x from industrial flue gas using Na 2 S 2 O 8 /MgO was proposed. The method does not require the body structure of the wet desulfurization device is changed but adds Na 2 S 2 O 8 to the original equipment to realize simultaneous desulfurization and denitrification. After determining Cl − was additive, the effects of various reaction factors on the simultaneous removal of SO 2 and NO x were investigated, including the Cl − concentration, the initial concentration of the oxidant, the initial pH value of the solution, and the reaction temperature. According to the characterization of removal products and the types of free radicals involved in the reaction by XRD , XPS , and EPR , the reaction mechanism was elucidated. The experimental results indicated that the removal products were mainly sulfates and nitrates. The free radicals involved in the reaction were SO 4 ·− , ·OH, and Cl·, and the key free radical was Cl·.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
ANALYTICAL CHEMISTRY
·
2025
·
IF 6.7
Yingcui Bu,Yingyu Zhu,Yuxin Yang,Ting Wang,Xiaojiao Zhu,Xingxing Chen,Qiong Zhang,Mingdi Yang,Hongping Zhou
At present, some progress has been made in developing NIR light-responsive free radical generators. However, the efficacy of theranostics continues to be hindered by tumor-associated inflammatory reactions. Hence, fulfilling the in situ release of free radicals upon NIR light excitation specifically activated by the inflammation microenvironment would be an ideal strategy for efficient inflammation eradication and tumor suppression but remains a challenge. Herein, a SO2 (overexpressed reactive sulfur species in inflamed site)-stimulated phototheranostic agent (CVS) is successfully developed. Through a specific response to both endogenous and exogenous SO2 with a low LOD (31.7 nM), CVS demonstrates the “switch on” two-photon activity as well as efficient OH· generation. Remarkably, in CVS-treated H22-tumor-bearing mice, the NIR light-activated accurate inflammation eradication and tumor suppression are accomplished. This reactive phototheranostic platform not only facilitates the quantification of SO2 during inflammation but also renders it a potent NIR antihypoxic tumor agent.
研究领域:
生物医学工程
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药理学
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肿瘤学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 29
·期 19
·29117-29129
·
IF 5.19
Huang Xinlei,Li Hongxian,Wang Ling,Tang Minghui,Lu Shengyong
The coal combustion produces a large amount of pollutants such as organic compounds pollutants (such as VOCs, SVOCs) and conventional pollutants (such as SO 2 , NOx) which need to be controlled in coal-fired plants. Currently, there have been mature emission control technologies for conventional pollutants in coal-combustion flue gas. The complicated conditions of flue gas will have great effects on the property of VOCs adsorbents. Thus, high-quality adsorbents with great adsorption properties and selectivity of VOCs are urgently needed. In this work, a biomass-derived hierarchical porous carbon (HPC-A) with high adsorption capacity (585 mg/g) and great selectivity of toluene was proposed. Analyses through the competitive adsorption tests between toluene and SO 2 indicated that the pore size distributions of adsorbents dominate the adsorption capacity and selectivity. The ultramicropores (< 0.7 nm) determine the SO 2 adsorption capacity and promote the SO 2 adsorption selectivity, while the micropores of 0.7 ~ 2 nm and mesopores are beneficial for toluene adsorption. Intriguingly, the SO 2 molecules can promote the toluene adsorption kinetics on hierarchical porous carbons through occupying ultramicropores when competitive adsorption. Besides, we indicated the mechanism of adsorption capacity, selectivity, and kinetics of toluene and SO 2 , and great reusability of HPC-A was found through toluene cyclic adsorption tests. The HPC-A could be a potential adsorbent for VOCs removal from coal-combustion flue gas.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2020
·
IF 9.038
Xuan Liu,Chang’an Wang,Tao Zhu,Qiang Lv,Defu Che
In this paper, the simultaneous removal of SO 2 and NO x catalyzed by Fe-Mo mixed oxides at varying Mo/Fe atomic ratios was reported for the first time with the aim of reducing H 2 O 2 consumption and elucidating the roles of Fe and Mo species in the catalytic process. Fe-Mo mixed oxides with varying Mo/Fe atomic ratios were synthesized and the catalytic performances were systematically studied. The catalyst with Mo/Fe atomic ratio of 2.0 exhibited the highest activity, with which removal efficiencies of 89.4 % for NO x and 100 % for SO 2 can be attained at extremely low H 2 O 2 dosage. Products analysis revealed that SO 2 was mainly removed via wet scrubber, while the adequate oxidation resulting from OH radicals was the prerequisite for NO x removal. The redox pair of Fe 2+ /Fe 3+ played a significant role in decomposing H 2 O 2 , while Mo species had double effect on catalytic activity. Higher Mo content resulted in abundant oxygen vacancies and stronger surface acidity, which favored OH formation. However, the excessive Mo content involved severe surface Mo enrichment and remarkably reduced the active sites of Fe species. The H 2 O 2 /Fe-Mo catalyst system showed excellent stability and had a promising prospect for simultaneously removing SO 2 and NO x in coal-fired flue gas.
研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
FUEL
·
2022
·
IF 8.035
Shengji Wu,Yalun Ma,Wangsheng Yu,Hui Wang,Wei Yang,Lei Che,Zhongxi Han
How to enhance the SO 2 tolerance of transition metal oxide-supported activated carbon is one of the hottest issues in the field of mercury capture from flue gas. Addition of a foreign metal ion to prepare bimetallic adsorbent is a common method of improving the SO 2 tolerance of adsorbent. However, this approach suffers from high cost and a complex preparation process. In this study, CeO 2 - and Co 3 O 4 -supported activated carbon ( m %CeO 2 /AC and m %Co 3 O 4 /AC), with various loading values of active center, were prepared by an incipient wetness impregnation method, and their SO 2 tolerances were compared. The mercury removal performance and SO 2 tolerance of both CeO 2 /AC and Co 3 O 4 /AC could be remarkably improved through increasing the loading amount of the active center. Co 3 O 4 /AC exhibited high affinity with SO 2 , and the chemisorbed oxygen in Co 3 O 4 would be largely consumed, when SO 2 was present in the flue gas, resulting in a significant decrease of mercury removal efficiency. The mercury removal efficiencies of 20%CeO 2 /AC, 40%CeO 2 /AC and 60%CeO 2 /AC were 86.1%, 93.7% and 93.7%, respectively, during removal of mercury from flue gas at 150 °C in the presence of SO 2 . 20%CeO 2 /AC was the optimal adsorbent for mercury capture from flue gas, owing to its excellent mercury removal efficiency, strong SO 2 tolerance and relatively lower cost. The mercury species formed over spent 20%CeO 2 /AC were HgO and HgSO 4 . The HgO was generated through the reaction of mercury and chemisorbed oxygen, while the formation of HgSO 4 was due to the reaction between mercury, SO 2 and chemisorbed oxygen. The regeneration investigation indicated that the activity of spent 20%CeO 2 /AC could be almost fully recovered through a temperature-programmed decomposition and desorption process. The present study showed that the SO 2 tolerance of CeO 2 /AC could be easily improved through regulation of the loading amount of the active center.
研究领域:
环境科学
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化学工程
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2016
·Vol. 24
·期 1
·676-684
·
IF 2.76
Tu Baosheng,Shi Nian,Sun Wei,Cao Limei,Yang Ji
In this paper, Pt supports on carbon black powder (Vulcan XC-72) were synthesized via a hydrothermal method for selective catalytic reduction (SCR) of NO with H 2 in the presence of 2 vol% O 2 over a wide temperature of 20–300 °C. The results showed that the 3 and 5 wt% Pt/C catalysts resulted in high NO conversion (>90 %) over a temperature range of 120 to 300 °C, and the maximum NO conversion of 98.6 % was achieved over 5 wt% Pt/C at 120 °C. Meanwhile, the influence of SO 2 and H 2 O on the catalyst performance of 3 wt% Pt/C was investigated. The catalysts exhibited good SO 2 poisoning resistance when the SO 2 concentration was lower than 260 ppm. Moreover, a positive effect on NO conversion was detected with the addition of 3 and 5 vol% H 2 O in the feed gas stream.
TEM image and good NO conversion performance of the Pt/C catalysts
研究领域:
催化化学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FUEL
·
2025
·
IF 7.5
Jie Gao,Zijun Ran,Jingyu Ran,Xin Huang,Chuan Ma,Yunlin Shao
The catalysts utilized for low-temperature catalytic oxidation of Hg 0 from flue gas typically suffer from issues related to H 2 O and SO 2 poisoning. This study focused on doping modification of La 0.875 Ce 0.125 CoO 3 perovskite with promoters and conducted a thorough investigation on the H 2 O and SO 2 resistance through characterization and DFT methods. Experimental results demonstrated that the LCeCO/30 wt% ZrO 2 possessed optimal H 2 O and SO 2 resistance. Under high sulfur (1500 ppm SO 2 ) and high humidity (10 % H 2 O(g)) conditions, it maintained approximately 91 % Hg 0 removal efficiency after thermal regeneration cycles. Characterization results indicated that ZrO 2 doping facilitated the formation of three-dimensional macroporous structure and protected active Co 3+ sites on the surface. Based on DFT calculations, the H 2 O poisoning is attributed to competitive adsorption between H 2 O(g) and Hg 0 on the active sites. Also, the SO 2 poisoning occurs due to competitive adsorption of SO 2 and the toxicity of sulfates to the surface active sites. Meanwhile, ZrO 2 doping can lower the adsorption energies of H 2 O(g) and SO 2 by modifying their adsorption configuration, thus weakening the competitive adsorption of H 2 O(g) and SO 2 with Hg 0 . Overall, LCeCO/ZrO 2 is a promising Hg 0 removal catalyst with superior H 2 O and SO 2 resistance.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ENERGY & FUELS
·
2021
·
IF 3.605
Hairong Tang,Yong He,Peixi Liu,Jiaming Shao,Fawei Lin,Zhihua Wang
Zeolitic-imidazolate framework precursors (ZIF-67) were synthesized in an inorganic solution with triethylamine as a deprotonating agent for N2O decomposition, and the catalytic activities of the pyrolysis products under different conditions were investigated. Among them, the Co/CoOx@carbon catalyst pyrolyzed at 650 °C in a N2 atmosphere (Co-650N) exhibited excellent low-temperature catalytic activity and stability, achieving 50% decomposition efficiency at 305 °C and ∼100% at 400 °C, which benefitted from its large specific surface area, great reduction performance, abundant cobalt active sites, and surface oxygen species. Further, utilizing temperature-programmed desorption (TPD) and in situ diffused reflectance infrared Fourier transform spectroscopy (DRIFTS) results, it was found that N2O molecules preferentially combined with oxygen species bound to cobalt sites. The absorbed N2O was decomposed into N2 and oxygen species, and the latter was subsequently transferred to carbon frameworks. Interestingly, the amorphous graphitic carbon frameworks played an important role in transferring/storing active oxygen and regenerating cobalt sites. Moreover, Co-650N exhibited better resistance to SO2, and the efficiency could be recovered via heating and finally stabilized at 100%. Finally, the mechanisms of N2O decomposition and sulfur poisoning-reactivation on Co/CoOx@carbon catalysts were proposed for the first time.
研究领域:
催化化学
·
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
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