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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH · 2019 ·Vol. 26 ·期 28 ·28808-28816 · IF 2.914

Simultaneous removal of SO2 and NO by FeII(EDTA) solution: promotion of Mn powder and mechanism of reduction

Duo Yankai,Wang Xiaoping,He Jinjia,Zhang Shihan,Pan Hua,Chen Jianmeng,Chen Jun

The effect of Mn powder addition on the simultaneous removal of SO 2 and NO coupled with Fe II (EDTA) absorption was investigated in this work. In the NO absorption system with Fe II (EDTA), SO 2 reduced Fe II (EDTA)-NO to Fe II (EDTA) with a reduction efficiency reaching 88.5% under the conditions of 4000 mg/m 3 SO 2 , pH 8.0, 44 °C, and the flow rate of 1.2 L/min within 60 min. Introducing 0.1 M Mn powder with SO 2 increased the Fe II (EDTA)-NO reduction efficiency to 96.8% within 5 min. SO 2 was also removed by reducing Fe II (EDTA)-NO and converted into SO 4 2- at a removal efficiency of 100%. After adding Mn powder, NO was removed through the following reaction: \( 5\mathrm{Mn}+2{\mathrm{Fe}}^{\mathrm{II}}\left(\mathrm{EDTA}\right)-\mathrm{NO}+12{\mathrm{H}}^{+}\longrightarrow 2{\mathrm{Fe}}^{\mathrm{II}}\left(\mathrm{EDTA}\right)+5{\mathrm{Mn}}^{2+}+2{\mathrm{NH}}_4^{+}+2{\mathrm{H}}_2\mathrm{O} \) . Mn powder functioned as a reductant to regenerate the absorption of solution, and the coordinated NO in Fe II (EDTA)-NO was reduced to NH 4 + . The resource utilization rate of N reached approximately 77.2%. The integrated technology is a potential solution for flue gas treatment in industrial sectors with coal-fired power plants and industrial boiler. Graphical abstract

研究领域: 环境工程 · 化学工程 · 污染控制技术
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Minerals · 2019 ·Vol. 9 ·期 2 ·119 · IF 2.25

Cleaner Extraction of Lead from Complex Lead-Containing Wastes by Reductive Sulfur-Fixing Smelting with Low SO2 Emission

Yun Li,Shenghai Yang,Wenrong Lin,Pekka Taskinen,Jing He,Yuejun Wang,Junjie Shi,Yongming Chen,Chaobo Tang,Ari Jokilaakso

A novel and cleaner process for lead and silver recycling from multiple lead-containing wastes, e.g., lead ash, lead sludge, lead slag, and ferric sludge, by reductive sulfur-fixing smelting was proposed. In this process, coke and iron-containing wastes were employed as reductive agent and sulfur-fixing agent, respectively. A Na2CO3-Na2SO4mixture was added as flux. The feasibility of this process was detected from thermodynamic and experimental perspectives. The influence of Fe/SiO2and CaO/SiO2, composition of the molten salt, coke addition, smelting temperature, and smelting time on direct Pb recovery and sulfur-fixation efficiency were investigated. The optimal process conditions were determined as follows:WCoke= 15%WPb wastes,WNa2CO3/WNa2SO4= 0.7/0.3, Fe/SiO2= 1.10, CaO/SiO2= 0.30, smelting temperature 1200 °C, and smelting time 2 h, whereWrepresents weight. Under these optimum conditions, 92.4% Pb and 98.8% Ag were directly recovered in crude lead bullion in one step treatment, and total 98.6% sulfur was fixed. The generation and emissions of SO2can be avoided. The main phases in ferrous matte obtained were FeS, NaFeS2, Fe2Zn3S5, and a little entrained Pb. The slag was a FeO-SiO2-CaO-Na2O quaternary melt.Keywords:SO2-free sulfur fixing smelting;lead recycling;wastes co-treatment and recycling;lead-iron-containing wastes;molten salt;PbO-FeO-SiO2-CaO-Na2O phase diagram

研究领域: 冶金学 · 环境科学
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2016 · IF 2.567

Cyano-Containing Protic Ionic Liquids for Highly Selective Absorption of SO2 from CO2: Experimental Study and Theoretical Analysis

Xiaomin Zhang,Xi Feng,He Li,Jing Peng,Youting Wu,Xingbang Hu

The solubility of SO2 and CO2 in four cyano-containing protic ionic liquids (PILs) was experimentally measured at temperatures from 303.2 to 333.2 K and pressures up to 3.0 bar. Their physical properties, such as density, viscosity, and decomposition temperature, were also determined. It is found that [DMPANH][MOAc] and [DMAPNH][EOAc] have the best selective absorption of SO2 from CO2 at 303.2 K and 1.0 bar among the investigated PILs, and the ideal selectivities (119 and 107, respectively) of SO2/CO2 are significantly higher than those reported in literature for other ILs. The temperature-dependent Krichevsky–Kasarnovsky (K–K equation) and PR-NRTL equations are used to calculate the solubility data of SO2 and CO2, and the interactions between PILs and acid gases are analyzed thermodynamically. Quantum chemical calculations are also done to obtain the interaction configurations and energies. It is shown from the themodynamic analysis and the quantum chemical calculations that the interaction between SO2 and PILs is more energy favorable than that between CO2 and PILs, primarily due to the existence of the cyano group on the cation of PILs. The protic ionic liquids were reused for five absorption–desorption cycles without obvious loss in the absorption capacity, showing their potential as selective absorbents of SO2.

研究领域: 化学工程 · 环境科学
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JOURNAL OF HAZARDOUS MATERIALS · 2018 · IF 6.434

Liquid–liquid phase-change absorption of SO2 using N, N-dimethylcyclohexylamine as absorbent and liquid paraffin as solvent

Genming Li,Wenbo Zhao,Muyuan Chai,Yanhong Li,Qingming Jia,Yuan Chen

In the present work, liquid-liquid phase-change absorption of SO 2 was investigated using N , N -dimethylcyclohexylamine (DMCHA) as an absorbent, and high boiling liquid paraffin (LP) as a solvent to reduce volatilization of the absorbent. The homogenous solution was split into two immiscible phases upon SO 2 loading. The phase-change mechanism was attributed to the polarity variation of DMCHA before and after absorption by forming the charge-transfer complex DMCHA·SO 2 . The viscosity of the lower phase reached a maximum value of 24.5 mPa s at the absorption capacity of 1 mol SO 2 /mol DMCHA, and the viscosity of the corresponding upper phase was 46.4 mPa s. Both are lower than the reported viscosity of most ionic liquids. This solution exhibited extremely high mass selectivity of SO 2 /CO 2 with a value of 626. The mass absorption capacity was founded to be 1.19 g SO 2 /g DMCHA at 1 atm, which is comparable with the highest reported mass absorption capacity. At low partial pressure, the absorption capacity still reached 0.78 g/g at 0.1 atm, 0.43 g/g at 0.02 atm and 0.27 g/g at 0.001 atm. Furthermore, DMCHA could be completely regenerated in 10 min via microwave heating. All the results indicated this phase-change solution is a promising candidate for SO 2 capture.

CAS / MDL: 98-94-2 7385-67-3
研究领域: 环境科学 · 化学工程
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ENERGY & FUELS · 2019 · IF 3.021

Highly Efficient and Reversible Absorption of SO2 from Flue Gas Using Diamino Polycarboxylate Protic Ionic Liquid Aqueous Solutions

Haiming Zhang,Bin Jiang,Na Yang,Na Zhang,Luhong Zhang,Zhaohe Huang,Xiaoming Xiao,Xiaowei Tantai

Ionic liquid (IL) aqueous solutions (aq) have emerged as promising candidates for SO2 absorption. In this work, a new series of diamino polycarboxylate protic ionic liquids (DPPILs) aq with low viscosities and high stabilities were developed and used for SO2 capture. All of the prepared absorbents could efficiently absorb low-concentration SO2 in simulated flue gas. Among them, DPPILs aq based on citric acid (CA) presented the most excellent SO2 desorption performance; nearly all absorbed SO2 could be easily desorbed under mild conditions. Particularly, N,N-dimethylethylenediamine citrate [DMEDA][CA] showed the highest available absorption capacity toward 0.2 vol % SO2 (up to 0.51 molSO2/molILs and 0.058 gSO2/gabs in 50 wt % aq at 20 °C), which also presented satisfactory SO2/CO2 selectivity, reusability, and SO2 removal efficiency. Fourier transform infrared and nuclear magnetic resonance spectroscopic analyses revealed that the protonation of [DMEDA]+ and [CA]− promoted SO2 absorption. Overall, the studied DPPILs aq with excellent physical properties, SO2 absorption–desorption performance, and stability may have a great perspective in industrial SO2 removal.

CAS / MDL: 108-00-9 109-55-7
研究领域: 化学工程 · 环境科学
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JOURNAL OF ALLOYS AND COMPOUNDS · 2017 · IF 3.133

Synthesis of SnO2 nano-dodecahedrons with high-energy facets and their sensing properties to SO2 at low temperature

Xiaohui Ma,Qixuan Qin,Nan Zhang,Chuan Chen,Xin Liu,Yu Chen,Chuannan Li,Shengping Ruan

Dodecahedron-like SnO 2 nanomaterial was synthesized via a solvothermal method under mild reaction condition. The morphological and structural characterization results indicated that the as-prepare dodecahedral SnO 2 nanocrystallines with the average length of 130 nm and width of 45 nm were partially surrounded by high surface-energy {221} facets. The gas-sensing performance of the sample was investigated and the experiment results showed that the sensor had a good sensitivity to sulfur dioxide (SO 2 ) at 183 °C. To 800 ppb SO 2 , the response could reach 1.32 and the response time was about 10 s. The good SO 2 -sensing performance of SnO 2 nanocrystallines was closely related to the high surface-energy {221} facets whose surface possessed more dangling bonds and the corresponding SO 2 -sensing mechanism was discussed.

CAS / MDL: 25249-54-1 9003-39-8
研究领域: 材料科学 · 传感器技术
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NEW JOURNAL OF CHEMISTRY · 2021 ·Vol. 45 ·期 42 ·19812-19817 · IF 3.591

A single small molecule fluorescent probe for imaging RNA distribution and detecting endogenous SO2 through distinct fluorescence channels

Zhaomin Wang,Yong Liu,Weishan Wang,Chang Zhao,Weiying Lin

Fluorescent probes are a powerful tool in biological and biochemical fields. Herein, we prepared a new small molecule fluorescent probe PYQU as a robust tool that can explore the interaction between RNA and SO2 in biological environments. The probe PYQU could detect SO2 and RNA by a change in green and red fluorescence, respectively. Besides, the probe PYQU has excellent properties, such as low biological toxicity, good membrane permeability, and high selectivity. PYQU was used to detect SO2 in living cells and zebrafish in the green channel and visualize endogenous RNA of cells with a deep red fluorescence signal. Therefore, we believe that the probe PYQU is a valuable, robust, and reliable tool for studies of RNA and SO2.

CAS / MDL: 75-03-6
研究领域: 生物化学 · 分子生物学
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2023 · IF 4.2

Capture and Catalytic Reduction of SO2 with H2 to Elemental Sulfur by Novel Guanidinium-Based Deep Eutectic Solvents

Yan Wang,Shuhang Ren,Yucui Hou,Yuanyuan Zhang,Yaling Li,Wanxiang Zhang,Weize Wu

In this work, a series of novel functionalized deep eutectic solvents (DESs) using 1,1,3,3-tetramethylguanidinium tetrazolate ([TMG][Tetz]) as a hydrogen-bond acceptor (HBA) and azole derivatives as hydrogen-bond donors (HBDs) were synthesized for the capture and catalytic reduction of SO2. [TMG][Tetz]:imidazole (Im) (1:2) DES with favorable stability and reversibility could effectively capture 2000 ppm of SO2. The absorption capacity of [TMG][Tetz]:Im (1:2) DES for 2000 ppm of SO2 was high up to 2.0 mol SO2/mol DES (0.40 g SO2/g DES) at 293.15 K. The results of the UV–vis and FTIR spectra revealed that two kinds of combination existed between SO2 and the DES: charge transfer interaction and chemical interaction. Surprisingly, the absorbed SO2, which was found to form charge transfer complexes with the DES, can be reduced by H2 to elemental sulfur under mild conditions without byproduct and additional catalysts. The yield of elemental sulfur could reach up to 37% at 373.15 K.

研究领域: 化学工程 · 环境科学
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JOURNAL OF MOLECULAR LIQUIDS · 2023 · IF 6

Efficient SO2 capture at ultra-low concentration using a hybrid absorbent of deep eutectic solvent and ethylene glycol

Fuliu Yang,Jixue Fan,Lingqiang Meng,Jian Wu,Jun Li,Zhuhong Yang,Yifeng Chen,Xiaoyan Ji

Deep eutectic solvents (DESs) are considered as the highly effective absorbents for sulfur dioxide (SO 2 ) capture. However, the high viscosity of DESs and the resulting slow absorption rate as well as low absorption capacity at low SO 2 concentration seriously hinder their industrial application. In this study, DES of N-methyldiethanolamine (MDEA) and imidazole (Im) is simply blended with ethylene glycol (EG) forming a hybrid absorbent, namely MDEA/Im-EG, which exhibits extremely high SO 2 capture capacity at low concentration. In particular, SO 2 capture capacity in MDEA/Im-EG (molar ratio = 1:1) reaches 0.446 g SO 2 /g absorbent at 293.2 K with SO 2 concentration of 2000 ppm. Moreover, the corresponding desorption enthalpy is only −40.67 kJ/mol. To well understand the results, thermodynamic analysis of SO 2 capture is performed and the SO 2 capture mechanism is speculated by nuclear magnetic resonance and Fourier transform infrared spectroscopy.

研究领域: 化学工程 · 环境科学
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Sulfur transformation and thermogravimetric analysis of model compounds in oxygen carrier aided pyrolysis/gasification process

Lulu Wang,Chenyang Zhou,Laihong Shen,Yuyang Long,Dongsheng Shen

Sulfur impurity in solid fuel should be paid attention to in the thermal process from the perspective of environment and sulfur recovery, especially the auto-thermal oxygen carrier aided pyrolysis/gasification (OCAP). To uncouple the complex sulfur transformation during OCAP of solid fuel and elucidate the main mechanism, several typical model compounds of various functional groups were used to investigate the kinetic analysis and sulfur transformation through temperature-programmed method. The OCAP process consisted of devolatilization and partial gasification. The activation energy of sulfur models devolatilization was less than that of partial gasification, because the required energy was much more to release lattice oxygen from oxygen carrier. Furthermore, the actual oxygen transport capacity of oxygen carrier (OC) redistributed the sulfurous gases. It was found that H 2 S was released earlier than SO 2 . H 2 S release was ascribed to the devolatilization including the reactions between radicals and hydrogen abstracted from base at low temperature (200–300 °C). The different contact modes between sulfur compounds and OC proved that S could be absorbed in the form of iron sulfide and incorporated into char at low temperature but released in the form of SO 2 by OC oxidation at the elevated temperature (400–600 °C), which was in accordance with the kinetic analysis. The migration of sulfur from disulfide had priority over that from monosulfide, and the sulfur connecting with dialkyl (benzyl) was easier to escape than that with diaryl (phenyl) in OCAP process. The fate of sulfur model compounds was conducive to reveal the complex behaviors of solid fuel with different sulfur species, and this work provides evidence to implement the desulfurization and sulfur recovery strategy.

研究领域: 化学工程 · 环境科学 · 能源技术
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JOURNAL OF MOLECULAR LIQUIDS · 2021 · IF 6.165

Dual effects of long-chain alcohols in phase change capture of SO2: Increasing mutual solubility and decreasing product viscosity

Shengchao Xu,Wenbo Zhao,Xuhao Xie,Bo Hao,Xuefei Li,Yuan Chen

To realize the goal of energy-saving SO 2 capture process, a series of novel SO 2 phase change absorbents (SPCAs) composed of 2-[2-(Dimethylamino)ethoxy]ethanol (DMEE)/long-chain alcohols/hexadecane were investigated in this work. The long-chain alcohols had dual effects in SPCAs, i.e., increasing mutual solubility of DMEE and hexadecane , and decreasing viscosity of the absorption products. Three alcohols, including butyl, hexyl and decyl alcohol, could turn the immiscible mixture of DMEE and hexadecane into homogeneous solution to form SPCAs. The decyl alcohol in absorption product could efficiently decrease the viscosity from 2338.1 mPa·s to 362.02 mPa·s, which is beneficial to gas-liquid mass transfer and fluid transport process. Meanwhile, the NMR and FTIR results indicated that DMEE chemically absorbed SO 2 , forming a zwitterionic alkyl sulfite compound. The long-chain alcohol formed hydrogen bonds with the alkyl sulfite and it didn't change the reaction mechanism. Noteworthy, the SPCA can absorb 0.823 mol SO 2 /mol DMEE (0.396 g SO 2 /g DMEE) at 293.15 K and 0.002 atm, which was exceptionally attractive. Furthermore, the absorbed SO 2 could be partly released under vacuum at 110 °C and the net cycle capacity can reach 73% ~ 74% of the maximum capacity, which indicated the SPCAs have a promising application prospect.

研究领域: 环境科学 · 化学工程 · 材料科学
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DYES AND PIGMENTS · 2017 · IF 3.473

A far-red ratiometric fluorescent probe for SO2 derivatives based on the ESIPT enhanced FRET platform with improved performance

Dong-Peng Li,Xian-Jing Han,Ze-Quan Yan,Yun Cui,Jun-Ying Miao,Bao-Xiang Zhao

A ratiometric fluorescent probe (L-HF3) based on an efficient FRET platform constructed by 2-dicyanomethylene-3-cyano-4,5,5-trimethyl-2,5-dihydrofuran (TCF) and 3-hydroxyflavone (HF) fluorophores for detection of sulfur dioxide derivatives (HSO 3 − /SO 3 2− ) was developed. The probe featured very large (pseudo) Stokes shifts , good selectivity and high sensitivity, high FRET efficiency and high resolution of the emission bands. The probe was also mitochondria-targeted and could detect exogenous and endogenous bisulfite in living cells.

研究领域: 生物化学 · 分子生物学 · 细胞生物学
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