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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Experimental study on adsorption removal of SO2 in flue gas by defective UiO-66

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 · 环境科学
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Materials · 2023 ·Vol. 16 ·期 6 ·2343 · IF 3.4

Enhanced Desulfurization by Tannin Extract Absorption Assisted by Binuclear Sulfonated Phthalocyanine Cobalt Polymer: Performance and Mechanism

Bing Wang,Huanyu Chen,Xingguang Hao,Kai Li,Xin Sun,Yuan Li,Ping Ning

Removal of hydrogen sulfide (H2S) from coke oven gas has attracted increasing attention due to economic and environmental concerns. In this study, tannin extract (TE) absorption combined with binuclear sulfonated phthalocyanine cobalt organic polymer (OTS) and binuclear sulfonated phthalocyanine cobalt (PDS) with a fixed bed reactor is used for removal of H2S. The effect of gas flow rate, concentration of H2S, co-existence of organic sulfide compounds and O2were investigated. Then, the effect of total alkalinity content of TE, NaVO3, OTS and PDS was studied in detail. The experimental results demonstrated that 100% H2S conversion could maintain for 13 h at a total alkalinity of 5.0 g/L, TE concentration of 4.0 g/L, NaVO3concentration of 5 g/L, and OTS and PDS concentration of 0.2 g/L and 0.2 g/L, respectively. The OTS and PDS showed synergistic effect on boosting TE desulfurization efficiency. The results provide a new route for the investigation of liquid catalyzed oxidation desulfurization in an efficient and low-cost way.Keywords:coke oven flue gas;flue gas desulfurization;tannin extract desulfurization;polymer

研究领域: 环境科学 · 化学工程
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CHINESE JOURNAL OF CHEMICAL ENGINEERING · 2019 · IF 1.911

Manganese leaching in high concentration flue gas desulfurization process with semi-oxidized manganese ore

Dong Sun,Guangzhi Xin,Lu Yao,Lin Yang,Xia Jiang,Wenju Jiang

Manganese leaching during high concentration flue gas desulfurization process with semi-oxidized manganese ore was studied in this paper. It was found that there were different reaction pathways among which MnO 2, Mn 2 O 3 and MnCO 3 in semi-oxidized manganese ore during flue gas desulphurization and manganese leaching. High SO 2 concentration facilitated redox reaction between MnO 2 and SO 2 , and high concentration of H 2 SO 4 accelerated MnCO 3 /Mn 2 O 3 leaching from semi-oxidized ore. Kinetics study showed that manganese leaching in flue gas desulfurization process with semi-oxidized ore was controlled by a mixed-control model, that is the surface chemical reaction and mass diffusion dominated both the oxidation of SO 2 and manganese leaching process. The apparent activation energy was 13.05 kJ·mol −1 and the reaction orders with respect to SO 2 and H 2 SO 4 concentration were 1.38 and 0.10, respectively. Finally, a semi-empirical rate equation based on shrinking core model was derived to describe the process.

CAS / MDL: 598-62-9
研究领域: 化学工程 · 环境科学
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POWDER TECHNOLOGY · 2022 · IF 5.64

Effect of CO2 on the heterogeneous condensation of water vapor on insoluble fine particles

Jie Yin,Jun Zhang,Li Lv,Hui Zhong

Heterogeneous condensation preconditioning technology has generated broad interest in removing fine particles from coal-fired flue gas due to its economic and environmental advantages. Here, a flow cloud chamber was used to study the effect of 0%–90% CO 2 concentrations on the growth performance of insoluble fine particles with different operational conditions. The results suggest that a higher CO 2 concentration in the particle growth environment is detrimental to the fine particles growth. The higher the CO 2 concentration, the worse the growth performance. The adverse effect of CO 2 on the growth performance decreases with the increase of growth time and the increase of supersaturation caused by temperature, and does not change significantly with the increasing particle concentration.

研究领域: 环境科学 · 大气科学
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FUEL · 2014 · IF 3.406

The relationship between speciation and release ability of mercury in flue gas desulfurization (FGD) gypsum

Mingyang Sun,Jiaai Hou,Guanghuan Cheng,Shams Ali Baig,Lisha Tan,Xinhua Xu

Multipurpose utilization of flue gas desulfurization (FGD) gypsums releases mercury into environment and poses threats to public health. Determining Hg speciation is essential not only for predicting its toxicity and mobility but also for designing effective remediation strategies. Sequential chemical extraction (SCE) method was used to analyze Hg speciation in this study. The total Hg concentration in four samples ranged from 0.61 to 1.63   μg/g. XRD and EDX analysis revealed that the main chemical composition of FGD gypsum was calcium sulfate (CaSO 4 ). SCE result indicated that Hg was mainly distributed in the strong complex phase, ranging from 60% to 80%. Water soluble mercury in Sample SX accounted for 30% of the total extract, which might be attributed to the relatively high chlorine content in coal. Moreover, the mobility of Hg from FGD gypsum was also investigated in this study, which exhibited biphasic kinetics. The rapid release of Hg was related to the ratio of water soluble Hg at some extent ( R 2   =   0.818), which signified of more attentions for its stabilization. This study also suggested theoretical framework for the environmental risk associated with FGD gypsum during its usage and disposal.

CAS / MDL: 13762-51-1
研究领域: 环境科学 · 化学
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ADSORPTION-JOURNAL OF THE INTERNATIONAL ADSORPTION SOCIETY · 2024 ·Vol. 30 ·期 3 ·377-387 · IF 3

Preparation of UiO-66-type adsorbents for the separation of SO2 from flue gas

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 · 材料科学 · 化学工程
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CONSTRUCTION AND BUILDING MATERIALS · 2025 · IF 8

Environmentally friendly thermal insulation composite material derived from flue gas desulfurization gypsum and fly ash

Zhiming Zhang,Lianzheng Gui,Zhuo Chen,Xingwu Li,Junda Quan,Sha Liang,Yibing Zuo,Jiakuan Yang,Yin Yang

Fly ash (FA) and flue gas desulfurization gypsum (FGD) are major solid wastes from coal-fired power plants, with high production and low utilization, leading to environmental pollution when stockpiled. Meanwhile, with the increase in energy consumption and the growing demand for building energy efficiency, there is an urgent need to develop safe and stable thermal insulation materials. In this study, an insulation composite material was developed using FGD building gypsum (FGDBG), combined with fly ash-based aerogel (FAA) with a low thermal conductivity of 0.0179 W/(m·K). At a FAA content of 25 wt%, the thermal conductivity of the FGDBG@FAA composite insulation material was as low as 0.080 W/(m·K), which is 83.71 % reduction compared to FGDBG without FAA, while the compressive strength and flexural strength reached 2.11 and 0.83 MPa, respectively. The heat transfer behavior of the FGDBG@FAA composites was further investigated by COMSOL software, and the results show that the FAA changed the heat transfer path and enhanced the overall thermal resistance of the FGDBG@FAA composites. By hydrophobically modifying the surface of the FGDBG@FAA composites, the softening coefficient increased from 0.34 to 0.85, which is sufficient to resist humid environments, while the thermal insulation and mechanical properties of the FGDBG@FAA composites kept stable. The evaluation of heavy metal leaching toxicity and radioactive nuclides indicates that the FGDBG@FAA composites are environmentally friendly. The composites developed in this study can be used for interior thermal insulation in buildings, enabling the co-disposal of FA and FGD gypsum while reducing environmental risks.

CAS / MDL: 112-04-9 84992-49-4
研究领域: 建筑材料 · 环境科学 · 能源工程
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SCIENCE OF THE TOTAL ENVIRONMENT · 2019 · IF 5.589

Simultaneous desulfurization and denitrification from flue gas by catalytic ozonation combined with NH3/(NH4)2S2O8 absorption: Mechanisms and recovery of compound fertilizer

Bing Liu,Xiaochen Xu,Yuan Xue,Lifen Liu,Fenglin Yang

An integrated method of simultaneous desulfurization and denitrification from flue gas by catalytic ozonation combined with NH 3 /(NH 4 ) 2 S 2 O 8 absorption was developed for the first time. It consisted of two parts: (1) the catalytic ozonation of NO over FeO x /SAPO-34 to study the effects of the various influencing factors, and (2) the absorption–oxidation of NO x and SO 2 induced by ozone combined with a NH 3 /(NH 4 ) 2 S 2 O 8 solution in a bubble column reactor. In Part 1, results showed that under the optimal condition of a molar ratio of 0.5 for O 3 /NO, a residence time of 3 s, a water vapor volume fraction of 4%, a NO initial concentration of 536 mg/m 3 , and a SO 2 initial concentration of 343 mg/m 3 , the oxidation rate of NO was 55%. The characterizations of poisoned catalyst are briefly discussed. In Part 2, as the gas passed sequentially through the ozonizing reactor and the absorber (NH 3 /(NH 4 ) 2 S 2 O 8 solution of 0.8% ammonia and 0.2 mol/L (NH 4 ) 2 S 2 O 8 ), a NO conversion rate of approximately 92.6% and SO 2 conversion rate of 100% were obtained. The pH of the NH 3 /(NH 4 ) 2 S 2 O 8 solution had a significant impact on the NO conversion. According to the analysis of the composition of products under different pHs, a mechanism of desulfurization and denitrification based on NH 3 /(NH 4 ) 2 S 2 O 8 solutions was proposed. The reaction product as a compound fertilizer contained up to 24.5% nitrogen.

CAS / MDL: 7727-54-0 3317-61-1
研究领域: 环境科学 · 化学工程
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Journal of Environmental Chemical Engineering · 2021 · IF 5.909

Investigation of tertiary amine-based PILs for ideal efficient SO2 capture from CO2

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 · 环境科学
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FUEL · 2014 · IF 3.406

Study of mercury re-emission in a simulated WFGD solution containing thiocyanate and sulfide ions

Qingfeng Wang,Yue Liu,Zhenmei Yang,Haiqiang Wang,Xiaole Weng,Yuejun Wang,Zhongbiao Wu

In this paper, elemental mercury (Hg 0 ) re-emissions from simulated wet flue gas desulfurization (WFGD) solutions were evaluated in the presence of thiocyanate ions (SCN − ) or sulfide ions (S 2− and HS − ). Experimental results revealed that both thiocyanate ions and sulfide ions could inhibit the reduction of oxidized mercury to Hg 0 . The inhibition effect of SCN − was mainly attributed to the formation of HgSO 3 SCN − and HgSCN X −( X – 2) ( X   =   2–4). It was found that the mercury reduction process in the presence of sulfide ions followed different mechanism under acidic or alkaline condition, though the formation of stable HgS could be ascribed to the main inhibition reason. Under acidic condition, the bivalent mercury ions may not directly combine with sulfide ions to form HgS. This had led to a weaker inhibition effect under the acidic condition compared to that under alkaline condition.

CAS / MDL: 10257-55-3 540-72-7
研究领域: 环境科学 · 化学工程
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HYDROMETALLURGY · 2020 · IF 3.338

Promotion of manganese extraction and flue gas desulfurization with manganese ore by iron in the anodic solution of electrolytic manganese

Lu Yao,Guangzhi Xin,Pengyan Pu,Lin Yang,Xia Jiang,Zhicheng Jiang,Wenju Jiang

In this work, Mn ore was mixed with the wastewater anode solution of electrolytic Mn (ASEM, instead of water) and utilized as the desulfurizer for simultaneous SO 2 removal from flue gas and Mn extraction. The effects of Fe 2+ and Fe 3+ on Mn leaching and flue gas desulfurization were investigated. For MnO 2 and Mn 2 O 3 (mixed with ASEM), the introduction of Fe 2+ could simultaneously increase Mn extraction efficiency and flue gas desulfurization efficiency when MnO 2 and Mn 2 O 3 mixed with ASEM was used. Fe 3+ addition could improve desulfurization efficiency obviously for MnCO 3 . Fe 2+ could react with MnO 2 and H + to form Mn 2+ and Fe 3+ . This reaction further improved Mn extraction and simultaneously decreased the acidity of ASEM, thus promoting SO 2 removal. The introduced Fe 3+ could react with SO 2 , when MnO 2 was absent from the desulfurizer slurry. The resulting Fe 2+ was then oxidized by O 2 to form Fe 3+ , which underwent a Fe 3+ ↔ Fe 2+ cycle to promote flue gas desulfurization. Thus, the introduction of Fe ions, especially Fe 2+ , could promote simultaneous Mn leaching and flue gas desulfurization with Mn ore. This work provided not only a new way for effective SO 2 removal from flue gas and Mn extraction but also for recycling ASEM.

研究领域: 环境科学 · 冶金工程
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

NH2-MIL-125 filled mixed matrix membrane contactor with SO2 enrichment for flue gas desulphurization

Xu Li,Yanli Zhang,Qingping Xin,Xiaoli Ding,Lizhi Zhao,Hui Ye,Ligang Lin,Hong Li,Yuzhong Zhang

Membrane absorption is a convenient and efficient flue SO 2 capture technology . In this study, NH 2 -MIL-125 filled mixed matrix membrane contactor (MMMC) is constructed by Non-solvent Induced Phase Separation (NIPS) method. The functional groups and metal active sites on the surface of NH 2 -MIL-125(Ti) exhibit high affinity for SO 2 . The microporous structure of NH 2 -MIL-125(Ti) provides storage for adsorbed SO 2 , which is conducive to the formation of SO 2 enrichment zone in the membrane. The membrane morphology, wetting resistance, and light responsiveness et al of MMMC have been tested. The combination of NH 2 -MIL-125(Ti) adsorption and membrane absorption process effectively promotes the transfer of gas molecules in the membrane pores. The SO 2 absorption flux of MMMC filled by NH 2 -MIL-125(Ti) has a significant increment, reaching 8.81 × 10 −4 mol·m −2 ·s −1 and 9.77 × 10 −4 mol·m −2 ·s −1 under non-light and visible light conditions respectively, which is comparability with results in literature. The membrane phase mass transfer coefficient calculated by Wilson model is 149.6 s·m −1 , which shows the low resistance in membrane. The SO 2 absorption flux keep stable after 4 cycles of tests. The membrane contactor coupled with function fillers enhances the SO 2 capture ability and further promotes the enrichment of SO 2 , which has favorable development foreground.

研究领域: 环境科学 · 材料科学
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