ENERGY & FUELS
·
2017
·
IF 3.091
Yongli Sun,Yanling Zhang,Luhong Zhang,Bin Jiang,Wenhao Gu,Huawei Yang
In this work, a kind of aqueous solution of novel protic triamine-based ionic liquid was proposed for efficient SO2 capture. The mixed absorbents were prepared by blending 1,1,4,7,7-pentaethyldiethylene (PEDETA) with sulfuric acid and water, and their physicochemical properties were studied by various methods. Remarkably, the viscosities of the mixed absorbents are in the range of 1.44–1.85 mPa s at 293.2 K, which is as low as water. Detailed SO2 absorption experiments were carried out to investigate the influence of some important factors, including temperature (298.2, 313.2, and 328.2 K), SO2 partial pressure (0–1 bar), and sulfuric acid proportion. It is worth noting that the mixed absorbents showed excellent absorption capacity, especially at a low partial pressure. All absorbed SO2 could be released easily and completely by the method of heating reflux. More importantly, the absorbent could be reused for at least 5 cycles without noticeable changes in both absorption performance and chemical structure. A thermogravimetric analysis further confirmed its good thermal stability. The detailed absorption mechanism was proposed and demonstrated by an infrared spectrum. In the end, the pKa values and reaction enthalpy of the protonation reaction of PEDETA were determined by acid titration and parameter analysis based on the reaction equilibrium model. In summary, the mixed absorbents, which possess low viscosities, good resistance to sulfuric acid, excellent capacity, and reusability, may have a good perspective in industrial SO2 capture.
研究领域:
环境科学
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化学工程
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材料科学
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产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2025
·
IF 11.3
Wenjie Liao,Ling Zhou,Xiaoqiang Wang,Yue Liu,Zhongbiao Wu
Both improving the activity and reducing SO3 emissions during selective catalytic reduction of NOx by the NH3 (NH3–SCR) process over commercial V–Ti-based catalysts remain a challenge. Herein, Ce and P cooperatively modified the VMo/Ti catalyst to address this challenge. Within the temperature range of 250–350 °C, the optimal VMoCeP/Ti catalyst achieved a NO conversion of more than 95% and maintained a SO2 oxidation ratio below 1.0%. The enhanced SCR activity of the modified catalyst could be attributed to the improvement in surface acidity and redox capacity by the addition of Ce and P, which would promote NH3 adsorption and activation. Meanwhile, Ce and P coaddition could regulate the surface structure of vanadyl species from predominantly polymeric to a more dimeric form, which could also promote the SCR reaction. More importantly, except for the suppressed sulfation of vanadium species, both a lower proportion of polymeric vanadyl species and the strong interactions among V–Ce–P species could raise the energy barrier of the decomposition of sulfated vanadium species into SO3, thereby inhibiting SO2 oxidation. This work provided novel insights into developing efficient SCR catalysts with low SO2 oxidation ratios for both the academic and industrial fields.
研究领域:
催化化学
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环境化学
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2025
·
IF 4.8
Xiao Yang,Heying Zhao,Aiyong Wang,Wangcheng Zhan,Yanglong Guo,Li Wang,Xuan Tang,Yun Guo
SO 2 in the sintering flue gas severely inhibits the CO oxidation performance of commercial Pt/Al 2 O 3 catalysts. However, the major poisoning mechanism of SO 2 on Pt/Al 2 O 3 in CO oxidation in the presence of H 2 O remains to be elucidated. Here, Pt/Al 2 O 3 was pretreated with different reducing atmospheres at high temperatures. Among these, the catalyst pretreated with a CO atmosphere at 600 °C (denoted as Pt/Al 2 O 3 -CO-600) exhibited superior CO oxidation performance and enhanced sulfur resistance in the presence of both H 2 O and SO 2 . The combination of XPS, HAADF-STEM, TG-MS, SO 2 oxidation test, and in-situ DRIFTS reveal that the Pt species on Pt/Al 2 O 3 -CO-600 transformed from Pt oxide clusters to metallic Pt nanoparticles. This transformation enhanced SO 2 adsorption and reactivity, leading to increased sulfate accumulation. Despite the high SO 2 reactivity and sulfate content, in-situ DRIFTS revealed that the CO reaction of Pt/Al 2 O 3 -CO-600 was less hindered by SO 2 and the sulfated Al 2 O 3 . This is attributed to the high ratio of the under-coordinated (UC) Pt sites in Pt/Al 2 O 3 -CO-600, which promotes the reaction intermediates spillover from Pt site to Al 2 O 3 compared to the Pt/Al 2 O 3 . This phenomenon was positively correlated with the sulfur resistance of reduced catalysts. Accordingly, the UC site contributes to the spillover of sulfate intermediate (H 2 SO 4 ), reducing the CO reactivity loss of Pt/Al 2 O 3 due to the intermediate coverage. This study elucidates that the primary poisoning pathway of Pt/Al 2 O 3 in the presence of H 2 O and SO 2 is the difficulty of sulfate intermediate spillover.
研究领域:
催化化学
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环境化学
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材料科学
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表面科学
✓ 已验证
产品关联
DOI
高影响因子
Small
·
2024
·
IF 13
Guanqing Zhang,Fengqing Liu,Qiliang Zhu,Hao Qian,Shouchao Zhong,Jingze Tan,Anmin Zheng,Fujian Liu,Lilong Jiang
Herein, a variety of 2,6-diaminopyridine (DAP) derived nitrogen-doped hierarchically porous carbon (DAP-NHPC-T) prepared from carbonization-induced structure transformation of DAP-Zn-SiO 2 -P123 nanocomposites are reported, which are facilely prepared from solvent-free co-assembly of block copolymer templates P123 with pyridine-rich monomer of DAP, Zn(NO 3 ) 2 and tetramethoxysilane. In the pyrolysis process, P123 and SiO 2 templates promote the formation of mesoporous and supermicroporous structures in the DAP-NHPC-T, while high-temperature volatilization of Zn contributed to generation of micropores. The DAP-NHPC-T possess large BET surface areas (≈956–1126 m 2 g −1 ), hierarchical porosity with micro-supermicro-mesoporous feature and high nitrogen contents (≈10.44–5.99 at%) with tunable density of pyridine-based nitrogen sites (≈5.99–3.32 at%), exhibiting good accessibility and reinforced interaction with SO 2 . Consequently, the DAP-NHPC-T show high SO 2 capacity (14.7 mmol g −1 , 25 °C and 1.0 bar) and SO 2 /CO 2 /N 2 IAST selectivities, extraordinary dynamic breakthrough separation efficiency and cycling stability, far beyond any other reported nitrogen-doped metal-free carbon. As verified by in situ spectroscopy and theoretical calculations, the pyridine-based nitrogen sites of the DAP-NHPC-T boost SO 2 adsorption via the unique charge transfer, the adsorption mechanism and reaction model have been finally clarified.
研究领域:
材料科学
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化学工程
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环境科学
✓ 已验证
DOI
PubMed
高影响因子
RSC Advances
·
2018
·Vol. 8
·期 7
·3858-3868
·
IF 2.936
Shuohan Yu,Sheng Xu,Bowen Sun,Yiyang Lu,Lulu Li,Weixin Zou,Peng Wang,Fei Gao,Changjin Tang,Lin Dong
Chromium oxide nano-particles with an average diameter of 3 nm covered by amorphous carbon (CrOx/C) were successfully synthesized. The synthesized CrOx/C materials were used for the selective catalytic reduction of NOx by NH3 (NH3-SCR), which shows superb NH3-SCR activity and in particular, satisfactory regeneration ability in the presence of SO2 compared with Mn-based catalysts. The as-prepared catalysts were characterized by XRD, HRTEM, Raman, FTIR, BET, TPD, TPR, XPS and in situ FTIR techniques. The results indicated presence of certain amounts of unstable lattice oxygen exposed on the surface of CrOx nano-particles with an average size of 3 nm in the CrOx/C samples, which led to NO being conveniently oxidized to NO2. The formed NO2 participated in NH3-SCR activity, reacting with catalysts via a “fast NH3-SCR” pathway, which enhanced th NH3-SCR performance of the CrOx/C catalysts. Furthermore, the stable lattice of the CrOx species made the catalyst immune to the sulfation process, which was inferred to be the cause of its superior regeneration ability in the presence of SO2. This study provides a simple way to synthesize stable CrOx nano-particles with active oxygen, and sheds light on designing NH3-SCR catalysts with highly efficient low temperature activity, SO2 tolerance, and regeneration ability.
研究领域:
催化
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环境工程
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2025
·
IF 7.7
Lingnan Kong,Quanhua Xie,Yuanyuan He,Shiyu Dong,Yang Liu,Wenliang Fan,Haiyan Yao,Mingfu Zhao,Nianbing Zhong
This paper proposes a polyvinyl alcohol/AlFFIVE-1-Ni (PVA/KAUST-8)-coated long-period fiber grating (LPFG) SO 2 concentration sensor to accurately monitor SO 2 concentrations online. To enhance the adhesion strength between the fiber and a SO 2 -sensitive film, the etched LPFG surface was silanized using 3-aminopropyltriethoxysilane, and then coated with a PVA/KAUST-8 SO 2 -sensitive sol using the doctor blading method. A fluorosilane hydrophobic coating was deposited on the SO 2 -sensitive membrane surface and integrated with a LPFG temperature sensor, thereby effectively eliminating measurement interference caused by ambient temperature and humidity fluctuations during SO 2 concentration detection. The morphology and composition of the SO 2 -sensitive films were characterized using optical microscopy, field-emission scanning electron microscopy, X-ray diffraction analysis, and X-ray photoelectron spectroscopy. Furthermore, the working principle of the sensors for the detection of SO 2 was established. Under optimized parameters (LPFG diameter: 60 μm; PVA doping in PVA/KAUST-8: 12 wt%; SO 2 -sensitive film: 45 μm; fluorosilane composite layers: 12) within a humidity range of 0–60 % RH and a temperature range of 25–45 °C, the sensor demonstrated a good selective SO 2 detection with 2.79 pm/ppm sensitivity, 1.07 ppm detection limit, 390 s response time, and 8.89 % maximum relative error.
研究领域:
传感器
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光纤技术
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分析化学
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材料科学
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环境监测
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表面工程
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Beilei Li,Xiaoxiang Wang,Yaqing Wang,Weijia Wang,Shuguang Zhou,Shihan Zhang,Wei Li,Sujing Li
Elimination of NO x from the non-electric industrial boilers has become priority under the effective implementation of ultra-low emissions. A series of Ce-promoted FeVO 4 catalysts with improved acidity and reducibility have been synthesized in this work. Thereinto, 10Ce/FeVO 4 exhibited an optimum low-temperature performance with 90% of NO x conversion and 95% of N 2 selectivity at 200–300 °C which was kept nearly unchanged with different concentrations of SO 2 ranging from 50 ppm to 200 ppm, showing a superior sulfur tolerance. An array of well-designed experiments has demonstrated that Ce mainly existed as CeVO 4 under a low doping content (1 wt%) on FeVO 4 , which could efficiently increase the amount of acid sites. With more cerium (5–12 wt%) loading on FeVO 4 , the appearance of CeO 2 further resulted in a strong interaction between cerium species and ion species, thus significantly improving the low-temperature catalytic activity . Therefore, the optimum coexistence of CeVO 4 and CeO 2 over 10Ce/FeVO 4 modulated its Brønsted acid and enhanced its redox circulation of Fe 3+ species. Moreover, the NH 3 -SCR reaction pathways of 10Ce/FeVO 4 were broadened from only Eley-Rideal to both Eley-Rideal and Langmiur-Hinshelwood mechanisms after Ce loading on FeVO 4 catalyst. With the presence of SO 2 , the S O/S-O deriving from the generated Ce 2 (SO 4 ) 3 and NH 4 HSO 4 increased the Brønsted acid sites, inducing a satisfying SO 2 tolerance of 10Ce/FeVO 4 catalyst, although the Langmiur-Hinshelwood pathway of 10Ce/FeVO 4 was immediately cut off due to the competitive adsorption of gaseous SO 2 and NO x . This work exemplifies a promising strategy for developing an ideal low-temperature NH 3 -SCR catalyst with good SO 2 resistance.
研究领域:
催化
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环境科学
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化学工程
✓ 已验证
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Weiyang Yuan,Shuzhen Chen,Changlei Qin,Dawid Piotr Hanak,Xu Zhou
CO2 adsorption is an important approach to control the excessive CO2 emission from energy and industrial plants and mitigating the greenhouse effect. As an acknowledged high-temperature adsorbent, Li4SiO4 shows advantages in capturing a large amount of CO2 with a fast reaction rate and excellent cyclic stability. However, its CO2 adsorption capacity would be significantly affected by the flue gas impurities, such as SO2 and O2. The underlying reaction mechanism of such impurities and Li4SiO4 is still unclear. For this reason, this work studied the reaction path and kinetics between Li4SiO4 and SO2 through experiments, thermodynamic calculations, and characterizations. The results showed that Li4SiO4 reacts with SO2 to produce Li2SiO3 and Li2SO4 in the presence of O2 at 500–700 °C and forms Li2SiO3 and Li2SO3 in the absence of O2 at 500–682 °C. Furthermore, this study revealed a very low activation energy of 7.47 kJ/mol for Li4SiO4 sulfation in the presence of O2 in the kinetic-controlled stage, and the value goes up to 249.7 kJ/mol in the diffusion-controlled stage. These results will provide valuable references for the industrial applications of CO2 adsorption by Li4SiO4.
研究领域:
化学工程
·
环境科学
✓ 已验证
DOI
高影响因子
Molecular Catalysis
·
2025
·
IF 4.9
Qiuju Qin,Chaolian Zhu,Donghai Mo,Zhengjun Chen,Lihui Dong,Bin Li,Liya Zhou
MnO x exhibits excellent low temperature activity for degradation NO x , but its poor SO 2 tolerance restrains its application. Herein, an in situ construction method for MnO x loading on Mn-doped ZrO 2 carrier with carbon (MnO x /Mn-ZrO 2 -C) derived from Mn(NO 3 ) 2 /UIO-66 by in situ doped pyrolysis–oxidation, in which Mn replaces Zr to modify the electronic structure of the ZrO 2 . The MnO x /Mn-ZrO 2 -C with abundant surface oxygen and acid sites showed excellent activity and better SO 2 resistance. A series of characterization results indicated that Mn doping modulates the electron structure of carrier ZrO 2 and enhances the interactions among MnO x , carbon, and Mn-ZrO 2 , resulting in increasing the electron cloud density around Mn and Zr, and consequently, the Mn and Zr on the MnO x /Mn-ZrO 2 -C exhibit poorer sulfiphilic. These findings emphasize the benefits of utilizing a multipronged effect to fabricate highly active and sulfur-resistant NH 3 -SCR catalysts.
研究领域:
催化化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2013
·
IF 2.145
Wei-guo Pan,Jie-nan Hong,Rui-tang Guo,Wen-long Zhen,Hong-lei Ding,Qiang Jin,Cheng-gang Ding,Shi-yi Guo
MnO x –CuO x /TiO 2 and MnO x –CuO x /Al 2 O 3 catalysts were prepared by sol–gel method and used for low temperature selective catalytic reduction of NO with NH 3 . The results showed that MnO x –CuO x /TiO 2 had better catalytic activity and SO 2 resistance than MnO x –CuO x /Al 2 O 3 in the temperature range of 100–250 °C. The properties of the catalysts were characterized by using XRD, N 2 adsorption, temperature programmed reduction (H 2 -TPR) and temperature programmed desorption (NH 3 -TPD). It was found that the support has a great impact on the acidity of catalyst; TiO 2 and Al 2 O 3 can promote the formation of Lewis acid sites and Brönsted acid sites respectively.
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
CHEMICAL ENGINEERING SCIENCE
·
2026
·
IF 5.1
Xiao-Ya Wang,Wen-Qiang Gong,Fei-Feng Mao,Wei Hui,Xian-Lu Wu,Tiao Zhang,Yan Zhou,Jia-Yin Zhang,Duan-Jian Tao
The high-purity separation of gases with similar properties (e.g., SO 2 vs. CO 2 ) remains a major challenge for ionic liquid (IL) absorbents. In this work, we report the highly efficient and selective capture of SO 2 via SO 2 -triggered reversible solid–liquid phase transition in a series of tunable alkyl quaternary ammonium hydrogen sulfate ionic liquids (AQA-HSO 4 ). The results show that AQA-HSO 4 achieve ultrahigh IAST SO 2 /CO 2 selectivities (up to 855) and high uptake capacity (7.1 mmol g −1 ) at 293.2 K and 100 kPa. This superior performance is rooted in a rationally designed phase transition mechanism, where the modulation of alkyl chain lengths (from ethyl to hexyl) finely tunes the ionic microenvironment by balancing electron-donating and steric effects. Systematic investigations, including SO 2 absorption and kinetic analyses, in-situ FT-IR, DFT and COSMOtherm calculations, reveal that the [HSO 4 ] − anion serves as the primary active site, forming suitable cooperative hydrogen bonding and Coulombic interactions specifically with SO 2 , while remaining inert to CO 2 /N 2 . Kinetic analysis confirms that the spontaneous phase transition of AQA-HSO 4 drastically lowers the mass transfer energy barrier, enabling [N 4444 ][HSO 4 ] to reach 67% of its saturation capacity within 5 min. Additionally, [N 4444 ][HSO 4 ] exhibits outstanding stability and recyclability, with negligible capacity loss (<0.1%) after 20 absorption–desorption cycles, and can be fully regenerated under mild, energy-efficient conditions (depressurization to ∼20 kPa) without external heating. This work provides a promising strategy for developing next-generation, phase-transition-responsive absorbents for high-purity gas separation processes.
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产品关联
DOI
高影响因子
ENVIRONMENTAL RESEARCH
·
2025
·
IF 7.7
Huasheng Wang,Shuang Deng,Hongyun Hu,Can Fang,Guangqian Luo,Ze Wang,Songgeng Li
Excessive ClO 2 tends to be produced and escape, causing secondary pollution when wet oxidation of NO with NaClO 2 is conducted under acidic conditions. NaClO 2 alkaline oxidation has accordingly received a wide attention. In this work, NaClO 2 alkaline oxidation of NO has been systematically studied in a self-built spray tower. Focus has been placed on the effects of acidic components contained in flue gas such as CO 2 , HCl and SO 2 . ClO 2 and HClO 2 are considered more effective for NO oxidation, which tend to be produced in an acidic environment. HCO 3 − has a relatively higher hydrolysis coefficient than ClO 2 − , leading to more HClO 2 formation. Similarity is found with HCl although the effect is not as significant as CO 2 due to its low concentration in flue gas. SO 2 exhibits a negative effect on NO removal since HClO 2 can be consumed by SO 2 . Nearly 100 % NO removal efficiency can be achieved although there is an initial time delay necessary for the neutralization of alkaline environment. A similar performance has been observed for HCl. On the contrary, SO 2 exhibits a negative effect on NO removal due to the competition with NO in the consumption of NaClO 2 . Additives such as NaClO and CTAC were also used to enhance NaClO 2 alkaline oxidation performance. Interesting to note that CTAC can nearly eliminate the time delay by intensifying the gas-liquid mass transfer.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）