INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2020
·
IF 3.573
Xiangli Kong,Dawei Gong,Wei Ke,Minghui Qiu,Kaiyun Fu,Peng Xu,Xianfu Chen,Yiqun Fan
A ceramic membrane with multichannels generally has a higher specific area and larger throughput compared to that with a single channel, which is beneficial to the industrialization of ceramic membrane contactors for SO2 absorption. In this work, the mass transfer performance of SO2 absorption into NaOH solution was investigated at various gas and liquid operating conditions in a membrane contactor packed with a 19-channel hydrophilic membrane. The results showed that increasing the NaOH concentration can offset the effect of membrane thickness. To analyze the mass transfer process, a 3D mass transfer model was developed to simulate the concentration distribution of the components. The simulated SO2 fluxes were consistent with the experimental results. Additionally, the mass transfer model was applied to optimize the structure of channels in multichannel ceramic membranes. The operational mode of the multichannel ceramic membrane is optimized by blocking some inside channels to reduce the mass transfer resistance.
研究领域:
化学工程
·
环境工程
·
膜技术
·
传质
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Chang Liu,Xin Meng,Feng Hou,Fengming Ma,Yanchen Li,Ling Yin,Guoxiang Yue,Dongfang Guo,Hongwei Niu,Shiwang Gao,Huanjun Wang
Carbon dioxide (CO 2 ) chemisorption employing biphasic solvents is recognized as a method with substantial application potential. Nevertheless, under conditions of burning high-sulfur fuels or rapid load changes, SO 2 in the flue gas poses challenges to the stability and economic operation of biphasic CO 2 capture system. To tackle this, the impact of residual SO 2 on CO 2 capture performance was systematically investigated in a lab‑scale continuous absorption–desorption set-up using novel biphasic solvent. The system achieved steady CO 2 capture efficiencies of 97.8 % and 94.8 % over 20 days without SO 2 . In the presence of SO 2 , CO 2 capture efficiency declined from >90 % in the first 10 days to below 80 % after 13 days and 70 % after 17 days, owing to irreversible reactions between SO 2 and amine, pH drop, and amine loss. CO 2 loading and circulation capacity similarly decreased, while CO 2 desorption duty rose from 2.51 to over 5.0 GJ/t CO 2 , driven by increased solvent flow and amine degradation catalyzed by SO 4 2− . DFT calculations indicated that the dissolution of SO 2 formed SO 3 2− /SO 4 2− , which enhanced the hydration of CO 2 . However, SO 2 preferentially reacted with amines, acidifying the interface and hindering CO 2 absorption. Quantitative 13 C NMR indicated that the oxyanion produced by the dissolution of SO 2 reduced the concentrations of bicarbonates and carbonates in the rich phase. A mechanistic model based on film theory was proposed, delineating gas‑phase diffusion, liquid‑phase competition, and catalytic promotion by oxyanions. These findings guided recommendations for pretreatment and solvent‑management strategies to ensure stable biphasic CO 2 capture under real flue gas conditions.
研究领域:
碳捕集与封存
·
化学工程
·
环境科学
·
烟气处理
·
溶剂降解
·
反应机理
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Wenxiang Zhang,Yue Wu,Yinhui Li,Qingkuan Meng,Yongzheng Wang,Heping Ma
The deep removal of sulfur dioxide (SO2) from flue gas is of significant importance for environmental protection, yet developing adsorbents with high uptake capacity and selectivity, as well as excellent cycling stability, remains a formidable challenge. Herein, two porous aromatic frameworks (PAFs) with electron-rich conjugated structures (termed PAF-TrP and PAF-SBF) were prepared for the selective capture of SO2 from flue gas. A systematic investigation involving static gas adsorption, dynamic breakthrough experiments, stability tests, and molecular-level simulations demonstrated that both PAFs exhibit an exceptional SO2 capture performance. Under conditions of 298 K and 1 bar, the uptake capacities of SO2 in PAF-TrP and PAF-SBF reach 259.1 and 344.7 cm–3·g–1, respectively. The IAST (ideal adsorbed solution theory) selectivities of PAF-TrP and PAF-SBF toward SO2 in the SO2/N2 binary gas mixture are 4159.3 ∼ 902.8 and 3769.1 ∼ 844.3, respectively, at 298 K and 1 bar. Molecular-level simulation calculations based on density functional theory (DFT) revealed the intrinsic mechanism underlying the highly selective SO2 capture by the two PAFs. Specifically, the localized charge separation on the electron-rich aromatic conjugated frameworks of both PAFs generates a gradient electric field, which induces strong dipole–dipole and dipole−π interactions with polar SO2 molecules. Additionally, the construction mode of the two PAFs via strong covalent linkages endows them with remarkable stability and favorable regenerability. This study represents a meaningful endeavor toward developing high-performance adsorbents for flue gas desulfurization.
研究领域:
环境化学
·
材料科学
·
吸附技术
·
计算化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2019
·
IF 6.97
Qi Zhang,Yucui Hou,Shuhang Ren,Kai Zhang,Weize Wu
Functional ionic liquids (ILs), which have high absorption capacities of low-concentration SO2 through chemical interaction, have been widely studied. However, the absorbed SO2 in functional ILs is normally desorbed with high-temperature and steaming treatment, which is harmful to the stability of absorbents and causes high-energy consumption. In this work, functional ILs (monoethanolaminium lactate-[MEA]L, 1,1,3,3-tetramethylguanidinium lactate-[TMG]L, tetraethylammonium lactate-[N2222]L) mixed with ethylene glycol (EG) or H2O were used to capture low-concentration SO2, and then H2S was added to regenerate the absorbents via the liquid-phase Claus reaction. It was found that the reaction of H2S with SO2 in the absorbents proceeded fast and the absorbed SO2 was almost completely converted to solid sulfur (S8) under mild conditions without the addition of any catalysts. The effects of temperature, H2S initial pressure, and solvent on the Claus reaction in the functional ILs were investigated, and the optimal reaction conditions were obtained. The recycle experiments showed that the activity of the functional ILs for the Claus reaction was not decreased after being reused three times. The Claus reaction between H2S and SO2 in functional ILs provides a promising method for the efficient regeneration of functional ILs and SO2 resource utilization.
研究领域:
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2018
·
IF 4.908
Jian Liu,Rui-tang Guo,Ming-yuan Li,Peng Sun,Shu-ming Liu,Wei-guo Pan,Shuai-wei Liu,Xiao Sun
Mn/TiO 2 catalyst is a promising candidate for future utilization in low-temperature NH 3 -SCR reaction, but its bad resistance to SO 2 is still a great challenge for practical application. In this study, Eu was successfully used as the additive to improve its resistance to SO 2 under SCR conditions, while the pretreatment of Mn/TiO 2 and MnEu/TiO 2 catalyst by SO 2 + O 2 had a strong deactivation effect on them. In situ DRIFT study clarified that the deactivation of Mn/TiO 2 -S (SCR + SO 2 ), Mn/TiO 2 -S (SO 2 + O 2 ) and MnEu/TiO 2 -S (SO 2 +O 2 ) were mainly originated from the inhibited adsorption of NH 3 and NOx species, as well as the formation of a large amount surface sulfate species on them, which had a strong blacking effect on the SCR reactions over the three catalysts via both E-R and L-H routes. After the addition of Eu, SCR reaction over MnEu/TiO 2 catalyst with the existence of SO 2 took place through L-H pathway, accompanied by the generation of less surface sulfate species, which brought about the excellent SO 2 tolerance of MnEu/TiO 2 catalyst under SCR conditions.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
POLYMER
·
2021
·
IF 4.43
Zhen Li,Yunfei Zhi,Yonghao Ni,Hongying Su,Yingju Miao,Shaoyun Shan
Copolymerization of SO 2 with epoxide into the poly(cyclohexene sulfite) (PCS) is crucial due to the severe harm of SO 2 to the environment and the wide application need of the PCS product. However, the copolymerization tends to exhibit low conversion rate even under harsh conditions. The introduction of high-efficiency catalysts is an efficient way to solve the problem of limitation of SO 2 copolymerization. Herein, the novel and metal-free Schiff-base network (SNW) material, SNW-KUST1, was successfully designed and structurally characterized, which exhibits an excellent catalytic performance for the copolymerization of SO 2 and cyclohexene oxide with a record PCS selectivity of 93%. In comparison with the SNW-1, the catalytic activity of SNW-KUST1 is greatly improved, which can be attributed to the introduction of hydroxyl and increasing specific surface area. Moreover, the SNW-KUST1 can be reused more than 6 times without obvious decrease of the catalytic activity, and presents a wide applicability to various epoxides. A possible mechanism for the SO 2 copolymerization over SNW catalysts is proposed which includes the epoxide adsorption, ring-opening of epoxide, SO 2 insertion and the formation of PCS. It is an optimistic hope that this investigation can give a valuable guideline to design SNW materials with π-π conjugated and nitrogen-rich building blocks for the SO 2 copolymerization.
研究领域:
化学工程
·
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Omega
·
2022
·
IF 4.132
Yucui Hou,Qi Zhang,Minjie Gao,Shuhang Ren,Weize Wu
The absorption of SO2 from flue gas and its conversion to chemicals is important in the industry. Functional ionic liquids (ILs) have been broadly used to absorb SO2 in flue gas, but seldom convert it to chemicals. As we know, water is inevitable in a desulfurization process. In this work, three functional ILs (monoethanolaminium lactate-[MEA][Lac], 1,1,3,3-tetramethylguanidinium lactate-[TMG][Lac], tetraethylammonium lactate-[N2222][Lac]) with or without water were used as absorbents to absorb SO2 in flue gas, and then the absorbed SO2 in the absorbents was converted to sulfur via a Claus reaction. The result shows that the three ILs can efficiently absorb SO2 and convert it to sulfur. But the addition of water in the ILs can reduce the conversion of absorbed SO2, and the conversion increases with increasing the acidity of absorbents. To explain this phenomenon, we studied the Claus reaction in H2SO3, NaHSO3 and Na2SO3 aqueous solutions. It turns out that the conversion of the Claus reaction is related to the species of S (IV) in the order of the oxidability: H2SO3 > HSO3– > SO32–, and their proportions dependent on the pH of solutions. On the basis of the absorption mechanism of SO2 in functional ILs aqueous solution, H2S reacts with HSO3– and SO32– with weaker oxidability, resulting in the lower conversion. Importantly, we found that the addition of lactic acid could increase the conversion of SO2 via the Claus reaction.
研究领域:
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
TRANSACTIONS OF TIANJIN UNIVERSITY
·
2018
·Vol. 25
·期 3
·226-236
·
IF 0
Feng Wei,Gu Wenhao,Zhang Lühong,Tantai Xiaowei,Jiang Bin,Yang Huawei,Zhang Hongjie
An organic macromolecule, poly(1-vinylimidazole), with an appropriate polymerization degree was proposed and mixed with water to form a novel aqueous absorbent for SO 2 capture. This aqueous solution absorbent has the advantages of simple preparation, good physicochemical properties, environment-friendliness, high ability in deep removal of SO 2 , and excellent reusability. Moreover, pH-responsive behavior, pH buffering absorption mechanism, and their synergistic effect on absorption performance were revealed. The solubilities of SO 2 in the absorbent were measured in detail, and the results demonstrated excellent absorption capacity and recyclability. Then, mathematic models that describe SO 2 absorption equilibrium were established, and the corresponding parameters were estimated. More importantly, on the basis of model and experimental data, the absorption and desorption could maintain high efficiency within a wide operating region. In summary, this work provided a low-cost, efficient, and unique absorbent for SO 2 capture and verified its technical feasibility in industrial application.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2017
·
IF 2.843
Dongshun Deng,Xiaobang Liu,Bao Gao
Four azole-based DESs from acetyl choline chloride (ACC) and azoles (imidazole, Im, and 1,2,4-triazole, Tri) were prepared and utilized for SO2 capture. Their physicochemical properties, including density, viscosity, TGA, freezing point, and pH, were determined. The influences of temperature and pressure on the SO2 absorption performance of the DESs were systematically conducted. The results showed that all the DESs exhibited efficient and reversible absorption for SO2, and ACC-Im possessed higher absorption capacity than ACC-Tri, with the maximum value of 0.381 g of SO2 per g of ACC-Im (1:2) DES at 303.15 K and 0.1 bar. The possible absorption mechanism was investigated using 1H NMR and FTIR spectroscopy. Furthermore, the ACC-Tri (1:2) was used to capture SO2 at low partial pressure, showing high available capacity of 0.116 g of SO2 per g of DES for 3300 ppm of SO2. Present DESs emerge as promising absorbents for SO2 due to easy preparation, high absorption capacity, and good reversibility.
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
SEPARATION SCIENCE AND TECHNOLOGY
·
2021
·
IF 2.475
Chunyao Zheng,Ke Li,Chao Zhang,Dongshun Deng
Weak basic guanidinium acetylacetonate ([TMG][acac]) was synthesized and blended with PEG200 to construct hybrid absorbent for SO2. The composition was optimized on the basis of viscosity and SO2 absorption performance. For the preferred 20% [TMG][acac]-PEG200 mixture, the effect of various parameters were systematically investigated. Results showed that the maximum mass ratio of SO2 to [TMG][acac] was 0.838 and 0.331 at 30°C for pure and 10% SO2, respectively. The mixture was easily recycled five times. The present SO2 capture process using [TMG][acac]-PEG200 mixtures was a promising method for SO2 removal with both good reversibility and high absorption capacity.
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
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Zhang-Min Li,Shu-Xian Zhu,Fei-Feng Mao,Yan Zhou,Wenshuai Zhu,Duan-Jian Tao
Currently available aerogels as effective adsorption materials for capture of trace sulfur dioxide (SO 2 ) are unfavorable from the perspective of deep desulfurization technologies. Herein, four phenolic resin-based aerogels with controlled structures varying from spherical (∼1 μm) to nanofiber (∼20 nm) were prepared and characterized using hexadecyl trimethyl ammonium bromide (CATB) as a soft template. It is demonstrated that adjusting the usage amount of CTAB from 0.00 to 0.15 g could effectively regulate SO 2 adsorption capacities of phenolic resin-based aerogels. AG-0.15 nanofiber aerogel exhibited an outstanding SO 2 uptake through a swelling mechanism (10.58 mmol g −1 at 298.2 K, 1.0 bar), and displayed a very high SO 2 /N 2 selectivity (7271 at 298.2 K). Moreover, AG-0.15 nanofiber aerogel also had excellent performance for selective capture of 2000 ppm SO 2 in the mixed SO 2 /N 2 /CO 2 gases through dynamic column breakthrough experiments. Overall, phenolic resin-based nanofiber aerogels are perceived as a promising adsorbent for effective removal of trace SO 2 from flue gas.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2022
·
IF 10.53
Qingping Xin,Xinghui Zhang,Wei Shao,Hong Li,Yuzhong Zhang
The purification of sulfur dioxide (SO 2 ) from the flue gas is an urgent problem given its toxicity to humans and organisms and attendant environmental concerns. In this study, aiming at the separation of SO 2 , mixed matrix membranes (MMMs) are fabricated by incorporating covalent organic framework (COF) into Pebax 1657 polymer matrix . By strengthening the solubility-diffusion mechanism of SO 2 gas molecules, SO 2 /N 2 gas separation performance is investigated. Firstly, MMMs are fabricated by incorporating a porous framework material (TpPa-1) containing SO 2 affinity groups into the Pebax 1657 matrix as a filler. Then the azo group (Azo) is introduced into the MMMs by the method of physical blending. The MMMs with light-responsive characteristic are fabricated by introducing TpPa-1 blended with pAAB into the Pebax 1657 polymer matrix. Secondly, the SO 2 /N 2 separation performance of Pebax/TpPa-1 MMMs is improved with the increasing of filler loading. Specially, the Pebax/TpPa-1 membrane with 5 wt% exhibits the most excellent SO 2 /N 2 separation performance with SO 2 permeability of 1709 Barrer and SO 2 /N 2 selectivity of 811. The MMMs overcome the trade-off effect and achieve enhancement of SO 2 permeability and SO 2 /N 2 selectivity simultaneously. Thirdly, both the SO 2 permeabilities and SO 2 /N 2 selectivities of Pebax/pAAB@TpPa-1-5% membrane exhibit regular and reversible changes under UV–Vis light-conversion conditions, indicating that MMMs containing Azo possesses dynamic light-responsive properties. Furthermore, TpPa-1 and pAAB repel each other in the membrane because both have negative charges, resulting in the forced surface segregation of COF in the Pebax/pAAB@TpPa-1 MMMs.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）