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FUEL · 2019 · IF 5.128

Influenced factors study and evaluation for SO2/SO3 conversion rate in SCR process

Jianyi Lu,Zhiyong Zhou,Hanzhi Zhang,Zhe Yang

SO 3 generated in coal-fired boiler and selective catalytic reduction (SCR) process has become a significant problem due to its adverse effects on boiler facilities and air environment. The factors influenced conversion rate of SO 2 to SO 3 (SO 2 /SO 3 ) during SCR process were studied and evaluated, which included the effects of flue gas composition and SCR catalyst components on the conversion of SO 2 /SO 3 . SO 3 was trapped by the condensation and isopropanol absorption method, and SO 4 2− concentration was detected by spectrophotometer. The results showed that a certain concentration of NH 3 in the flue gas significantly promoted the conversion rate, but when NH 3 and NO coexisted, NO inhibited the catalytic action of NH 3 , while NO itself and O 2 had small effect on the conversion rate. Besides, the conversion rate of SO 2 increased with the increase of Ti and V content in the catalyst, and SiO 2 and BaO abated the catalytic oxidation of SO 2 , while WO 3 promoted the formation of SO 3 .

研究领域: 环境工程 · 化学工程 · 能源技术 · 空气污染控制
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SEPARATION AND PURIFICATION TECHNOLOGY · 2020 · IF 5.774

Aliphatic amine decorating metal–organic framework for durable SO2 capture from flue gas

Zhonghui Zhang,Bolun Yang,Heping Ma

The efficient capture of SO 2 using porous adsorbents is of great significance in flue gas desulfurization (FGD) process as the reversible physical adsorption can avoid solvents/water consumption and minimize waste generation. Metal organic frameworks (MOFs) are interesting and promising candidates to sequestrate SO 2 in flue gas as their high porosities, regular pore sizes and easy functionalization. However, the coordination bond nature of MOFs makes stably and persistently capture acidic SO 2 gas remains a challenge in MOF. Herein, an aliphatic amine decorating strategy was introduced in a MOF (MIL-101(Cr)) with open metal sites for reversible and durable SO 2 capture. The successful synthesis of N,N'-dimethylethylenediamine (mmen) decorated MIL-101(Cr) named mmen-MIL-101(Cr), was confirmed by powder X-ray diffraction (PXRD), Fourier transform-infrared spectroscopy (FTIR), scanning electron microscopy (SEM), energy-dispersive spectra (EDS) and nitrogen adsorption–desorption isotherm. Compared with chemisorption of SO 2 on open Cr sites in MIL-101(Cr), the SO 2 adsorption sites are transferred from Cr to N atom in mmen-MIL-101(Cr), leading to reversible SO 2 adsorption and desorption. The dipole–dipole interaction between N atom and S(SO 2 ) atom, combining with hydrogen bonding interaction between O(SO 2 ) and H in mmen can increase the SO 2 absorption capacity of mmen-MIL-101(Cr) under low SO 2 partial pressure. The SO 2 adsorption capacity and cycle stability properties were studied in detail by adsorption isotherm and dynamic breakthrough measurement. An unprecedented high SO 2 adsorb capacity (upto 4.27 mmol·g −1 ) at SO 2 partial pressure (0.5 mbar) is achieved in mmen-MIL-101(Cr), which is a great improvement compared to 2.92 mmol·g −1 SO 2 adsorption capacity for primordial MIL-101(Cr) under the same condition. Moreover, mmen-MIL-101(Cr) manifests reversible SO 2 adsorption–desorption performance while MIL-101(Cr) gradually loses its adsorption capacity during dynamic breakthrough cycles. The high SO 2 sorption capacity in low partial pressure and impressive cycle stability of mmen-MIL-101(Cr) demonstrate aliphatic amine decorating strategy is an efficient way to improve MOF’s SO 2 capture capability, which also can extend to other porous adsorbents for low concentration FGD process.

CAS / MDL: 110-70-3 100-21-0
研究领域: 材料科学 · 环境科学
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Journal of the Taiwan Institute of Chemical Engineers · 2015 · IF 3

Reversible absorption of SO2 from simulated flue gas by aqueous calcium lactate solution

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

The capture of SO 2 by recyclable absorbents has drawn much attention all over the world. In this work, it was found that aqueous calcium lactate (CaL 2 ) solution can be used as a recyclable absorbent for the capture of SO 2 . The solution shows high SO 2 absorption capacities up to 24.8 g SO 2 /kg absorbent at 40 °C. The effects of temperature, excessive lactic acid and CaL 2 concentration on the absorption of SO 2 , the desorption of SO 2 , and the reuse of aqueous CaL 2 solution were systemically studied. Furthermore, the difference between CaL 2 method and traditional calcium method was discussed. Compared with traditional calcium method, there are some advantages, such as regeneration of absorbent, recovery of SO 2 and reduction of CaSO 4 . This work suggests that aqueous CaL 2 solution, which can be obtained at quite low cost, is a promising recyclable absorbent in the process of desulfurization of flue gas.

CAS / MDL: 50-21-5
研究领域: 环境科学 · 化学工程
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SEPARATION AND PURIFICATION TECHNOLOGY · 2020 · IF 5.774

Chemically tunable DILs: Physical properties and highly efficient capture of low-concentration SO2

Dan Li,Yong Kang,Jie Li,Zongchi Wang,Zhinan Yan,Kai Sheng

As a successive work towards exploring suitable IL-based absorbents for SO 2 absorption from flue gas, we developed a species of new dicationic ionic liquids (DILs) with the combination of ether-functionalized dication and N-heterocyclic anions. These dual-functionalized DILs possessed high thermal stability, low vapour pressure, and high SO 2 capacity. The solubilities of SO 2 in the DILs increased with declining of the temperature and elevating of the SO 2 concentration. Notably, the available loading capacity of SO 2 in DIL 4 was up to 0.267 g SO 2 ·(g DIL) -1 at 313.2 K when the concentration of SO 2 in the feed gas was 2000 ppm, which was exceedingly significant for trapping SO 2 from the flue gas with low content of SO 2 . The regeneration experiments demonstrated that the absorption capacities of SO 2 in DIL 4 kept unchanged after six successive cycles of absorption/desorption. The absorption mechanisms based on the results of 1 H NMR, FTIR analysis and quantum chemical calculations indicated that both physical and chemical interactions between the SO 2 molecules and DIL 4 could be found in spite of different concentrations of SO 2 .

研究领域: 化学工程 · 环境科学
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Atmospheric Pollution Research · 2018 · IF 2.152

Investigation of low concentration SO2 adsorption performance on different amine-modified Merrifield resins

Xiao Yu,Jinliang Hao,Zhicheng Xi,Taiyang Liu,Ying Lin,Bin Xu

Three amine-modified Merrifield resins (AMMRs) were synthesized with ethane diamine, methylamine and dimethylamine to assess the impact of amine group on SO 2 adsorption under low SO 2 concentration. The dimethylamine-modified Merrifield resin (DMAMR) grafting with tertiary amine groups showed the greatest SO 2 adsorption compared with ethane diamine-modified Merrifield resin (EDAMR) and methylamine-modified Merrifield resin (MAMR). Different amine groups had different reaction mechanisms with SO 2 . It was much easier for SO 2 to form noncovalent charge transfer complex with tertiary amine group than the zwitterion and ion/counterion products with primary and secondary amine groups under dry condition. The noncovalent charge transfer complex had a relatively weaker thermostability than the zwitterion and ion/counterion products. As the temperature increased from 25 °C to 75 °C, the SO 2 adsorption capacity on DMAMR decreased by 78.92%, which was much higher than that of EDAMR and MAMR (63.77% and 63.41% respectively). As SO 2 concentration increased from 40 ppm to 100 ppm, significant increase (∼100%) in SO 2 adsorption capacity was observed. Lower SO 2 flow rate led to a more sufficient reaction between SO 2 and amine groups, resulting the increase in SO 2 adsorption capacities. Water vapor enhanced the SO 2 adsorption performance of AMMRs significantly due to the formation of salt. However, it was more difficult for tertiary amine group to react with SO 2 in the presence of water due to its relatively weaker basicity . DMAMR showed a greater regeneration performance than EDAMR and MAMR under dry and humid condition.

研究领域: 环境科学 · 化学工程
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ANALYTICA CHIMICA ACTA · 2023 · IF 6.2

A multifunctionally reversible detector: Photoacoustic and dual-channel fluorescence sensing for SO2/H2O2

Yicai Zhu,Junjun Wang,Yingyong Ni,Qingpeng Rao,Xiaojiao Zhu,Jianhua Yu,Sen Wang,Hongping Zhou

In this work, the phenothiazine fragment with powerful electron-donating ability was specifically selected to construct a multifunctional detector (noted as T1 ) in double-organelle with near-infrared region I (NIR-I) absorption. The changes of SO 2 /H 2 O 2 content in mitochondria and lipid droplets were observed through red/green channels respectively, which was due to the reaction between benzopyrylium fragment of T1 and SO 2 /H 2 O 2 to achieve red/green fluorescence conversion. Additionally, T1 was endowed with photoacoustic properties deriving from NIR-I absorption to reversibly monitor SO 2 /H 2 O 2 in vivo . This work was significant for more accurately deciphering the physiological and pathological processes in living organisms.

研究领域: 分析化学 · 生物化学 · 生物医学工程 · 分子生物学
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JOURNAL OF HAZARDOUS MATERIALS · 2023 · IF 13.6

Deep eutectic solvent-based blended membranes for ultra-super selective separation of SO2

Ping Zhang,Zhuoheng Tu,Zhihao Yan,Xiaomin Zhang,Xingbang Hu,Youting Wu

SO 2 is a major atmospheric pollutant leading to acid rain and smog. As a new generation of green solvents, deep eutectic solvents (DESs) have been widely investigated for gas capture. Nevertheless, studies on DES-based membranes for SO 2 separation are yet minimal. Herein, we devised polymer/DES blended membranes comprising 1-butyl-3-methyl-imidazolium bromide ([Bmim]Br)/diethylene glycol (DEG) DES and poly (vinylidene fluoride) (PVDF), and these membranes were firstly used for selective separation of SO 2 from N 2 and CO 2 . The permeability of SO 2 reaches up to 17480 Barrer (0.20 bar, 40 ºC) in PVDF/DES blended membrane containing 50 wt% of [Bmim]Br/DEG (2:1), with ultrahigh SO 2 /N 2 and SO 2 /CO 2 selectivity of 3690 and 211 obtained, respectively, far exceeding those in the state-of-the-art membranes reported in literature. The highly-reversible multi-site interaction between SO 2 and [Bmim]Br/DEG DES was revealed by spectroscopic analysis . Furthermore, the PVDF/DES blended membrane was also able to efficiently and stably separate SO 2 /CO 2 /N 2 (2.5/15/82.5%) mixed gas for at least 100 h. This work demonstrates for the first time that [Bmim]Br-based DESs are very efficient media for membrane separation of SO 2 . The easy preparation, low cost and high performance enable polymer/DES blended membranes to be promising candidates for flue gas desulfurization .

CAS / MDL: 111-46-6
研究领域: 环境科学 · 材料科学
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ENVIRONMENTAL TECHNOLOGY · 2014 · IF 1.197

Low-temperature selective catalytic reduction of NO on CeO2–CuO/Al2O3 catalysts prepared by different methods

Rui-tang Guo,Wen-long Zhen,Wei-guo Pan,Jie-nan Hong,Qiang Jin,Cheng-gang Ding,Shi-yi Guo

CeO2–CuO/Al2O3 catalysts were prepared by three different methods and their activities for selective catalytic reduction (SCR) of NO with NH3 were investigated. As can be seen from the experimental results, the catalyst prepared by the single-step sol–gel (SG) method showed the best SCR activity and resistance to SO2 and H2O. In order to investigate the relationship between the preparation method and the performance of SCR catalysts, the catalysts were characterized by using Brunauer–Emmett–Teller, X-ray diffraction, temperature programmed reduction with hydrogen, temperature programmed desorption with ammonia, X-ray photoelectron spectroscopy, Fourier transform infrared and thermo-gravimetric analysis techniques. It was found that the excellent performance of CeO2–CuO/Al2O3 catalyst prepared by the single-step SG method should be resulted from its large surface area, low crystallinity, high oxygen storage capacity, high NH3 adsorption capacity, high concentration of surface chemisorbed oxygen, weak sulphation process and weak water absorption.

研究领域: 环境科学 · 催化材料科学
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Journal of Environmental Sciences · 2020 · IF 4.302

Effects of calcination temperature on physicochemical property and activity of CuSO4/TiO2 ammonia-selective catalytic reduction catalysts

Yanke Yu,Jiali Zhang,Changwei Chen,Chi He,Jifa Miao,Huirong Li,Jinsheng Chen

CuSO 4 /TiO 2 catalysts with high catalytic activity and excellent resistant to SO 2 and H 2 O, were thought to be promising catalysts used in Selective catalytic reduction of nitrogen oxides by NH 3 . The performance of catalysts is largely affected by calcination temperature. Here, effects of calcination temperature on physicochemical property and catalytic activity of CuSO 4 /TiO 2 catalysts were investigated in depth. Catalyst samples calcined at different temperatures were prepared first and then physicochemical properties of the catalyst were characterized by N 2 adsorption-desorption, X-ray diffraction, thermogravimetric analysis , Raman spectra , Fourier-transform infrared spectroscopy, X-ray photoelectron spectroscopy, temperature-programmed desorption of NH 3 , temperature-programmed reduction of H 2 and in situ diffuse reflectance infrared Fourier transform spectroscopy . Results revealed that high calcination temperature had three main effects on the catalyst. First, sintering and anatase transform into rutile with increase of calcination temperature, causing a decrement of specific surface area. Second, decomposition of CuSO 4 under higher calcination temperature, resulting in disappears of Brønsted acid sites (S–OH), which had an adverse effect on surface acidity. Third, CuO from the decomposition of CuSO 4 changed surface reducibility of the catalyst and favored the process of NH 3 oxidation to nitrogen oxides (NO x ). Thus, catalytic activity of the catalyst calcined under high temperatures (≥600°C) decreased largely.

CAS / MDL: 13463-67-7
研究领域: 催化 · 环境化学 · 材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Fabrication of SiC catalytic filter with low vanadium loading and highly uniform structure for efficient NO reduction and dust removal

Xiangsen Xu,Jiangxiao Qiao,Shibo Yu,Jiahao Chen,Yiqing Zeng,Feng Zhang,Zhaoxiang Zhong,Weihong Xing

The rational design of catalysts and the establishment of uniform filter structure are key points in the development of high-performance catalytic filters. To resolve the issue of increased N 2 O concentration in catalysts with high vanadium content at high temperatures, a range of catalytic filters with low vanadium loading were fabricated by partially substituting vanadium in 6VWTi catalysts with transition metals (Mn, Cu, Co and Ce). The experimental results show that the introduction of Ce, which leads to rich surface-adsorbed reactive oxygen species, good redox properties and appropriate surface acidity, thus the 1V5CeWTi/SiC catalytic filter exhibits the highest denitration efficiency (NO conversion >90 % at the temperature of 300–500 °C without N 2 O production), presenting significant advantages in contrast to 1VWTi/SiC and 6VWTi/SiC. Furthermore, the preparation technology was optimized to obtain a more uniform structure, which enhanced NH 3 -SCR performance and reduced filter pressure drop. The optimized 1V5CeWTi/SiC also exhibited exceptional resistance to SO 2  + H 2 O and long-term stability for a duration of 200 h at 300 °C, as well as displays a noteworthy efficiency in filtering particulate matter (10 μm SiO 2 ). Therefore, the optimized 1V5CeWTi/SiC catalytic filter holds great potential in the realm of gas purification.

研究领域: 环境工程 · 催化 · 材料科学
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Integrations of desulfurization, carbon capture, and methanation at an isothermal intermediate temperature

Zihao Gao,Yongjun Jiang,Zheyi Sun,Bin Shao,Rongting Ma,Zhonghao Jia,Lihui Zhou,Sheng Dai,Jun Hu

Integrated CO 2 capture and conversion (iCCC) technology has been recognized as the most efficient technology for Carbon Capture, Utilization, and Storage (CCUS). However, its industrialization is hindered by some unsolved engineering problems. Typically, sulfur impurities in most industrial flue gas will have significant poisoning effects on the process. Herein, we report integrations of SO 2 removal, CO 2 capture and conversion (iSCCC) at an isothermal intermediate temperature in a two-fixed-bed column system. By rationally developing the SO 2 adsorbent pellets of ZnO-CaO, the CO 2 adsorbent pellets of AMS-MgO, and the methanation catalyst pellets of Ni-La/Al 2 O 3 , each individual unit is optimized. Specifically, the in-situ dynamic structure evolution observed by the atmospheric aberration-corrected scanning transmission electron microscopy as well as the theoretical dynamics calculation provide an in-depth understanding of the CO 2 desorption performance changing with the temperature on the AMS-MgO pellets, which builds a bridge for a successful 99.3 % CO 2 methanation efficiency. As a result, the matched iSCCC process demonstrates exceptional performance from simulated flue gas containing 1000 ppm SO 2 and 20 vol% CO 2 , with full desulfurization and decarbonation and a CO 2 conversion efficiency of 93.6 % after 20 cycles isothermally at 400 °C, superior to all the reported performance so far as we know, providing a promising route to practical large-scale iSCCC towards carbon neutrality.

研究领域: 化学工程 · 环境科学 · 材料科学
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Journal of Environmental Chemical Engineering · 2025 · IF 7.2

Tailored SO2 capture in multivariate UiO-66(Zr) MOFs: Experimental insights and theoretical mechanisms

Zai-Dong Shao,Peng Wu,Fang Liu,Qi-Jun Zhang,Chao-Yang Guo,Rui-Sang Liu,Jiang Lu,Xiao-Meng Ren,Yu-Ming Zheng

Sulfur dioxide (SO 2 ) emissions present significant environmental and health risks, yet efficiently capturing SO 2 remains challenging due to its corrosive nature and the limited performance of conventional adsorbents. In this study, we developed multivariate metal-organic frameworks (MTV-MOFs) based on UiO-66(Zr) for effective SO 2 capture. Through systematic ligand functionalization with -OH, -NH 2 , -SO 3 H, and -(NH 2 ) 2 groups on terephthalic acid linker, we developed a series of MTV-UiO-66 materials with tailored pore environments and adsorption characteristics. UiO-66-NH 2 exhibited superior performance with an SO 2 uptake of 252.9 mL g −1 at 298 K and 1 bar. Ideal adsorbed solution theory (IAST) calculations demonstrated improved selectivity for SO 2 over N 2 (847) and CO 2 (31), surpassing that of the parent UiO-66. Dynamic breakthrough experiments further confirmed the practical viability of MTV-UiO-66 materials for SO 2 capture under both dry and humid (50 % RH) conditions, with UiO-66-NH 2 retaining a capacity of 30.73 mL g −1 in dry settings and exhibiting robust performance in moisture-rich environments. Grand Canonical Monte Carlo (GCMC) simulations and density functional theory (DFT) calculations provided molecular-level insights into the adsorption mechanisms, revealing that functional groups play a crucial role in modulating binding interactions through hydrogen bonding, dipole-dipole interactions, and spatial confinement effects. The computational binding energies corroborated the experimental isosteric heats of adsorption, validating the integrated experimental-computational approach.

研究领域: 材料科学 · 环境化学 · 吸附技术 · 金属有机框架材料(MOFs) · 计算化学
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