NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 10
·4335-4345
·
IF 2.7
Jiali Zhang,Zhen Yan,Yanke Yu,Yanpeng Li
CuO/TiO2 catalysts with varying Sb doping ratios were synthesized and applied in the NH3-SCR process. The results of activity tests revealed that the addition of Sb effectively enhanced the performance of low-temperature SCR. Particularly, the CuSbTiOx-0.2 catalyst exhibited the highest activity, achieving over 91% conversion at 250 °C, along with the highest N2 selectivity and exceptional resistance to SO2. Comprehensive characterization analyses demonstrated that CuSbTiOx-0.2 possessed a significantly large specific surface area, the strongest surface acidity, and superior redox performance among the catalysts studied. In situ DRIFTS experiments provided further insights, indicating that Sb modification generated more active species, thereby enhancing the reactivity of ad-NH3 and ad-NOx species. The SCR reaction mechanism for CuSbTiOx-0.2 predominantly followed the Langmuir–Hinshelwood (L–H) and Eley–Rideal (E–R) mechanisms. These findings have the potential to advance the development of novel and effective non-vanadium SCR catalysts.
研究领域:
环境科学
·
催化材料
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Xinyu Han,Kaijie Liu,Mengyao Bian,Zhaoxu Yuan,Yannan Li,Yunlong Zhang,Xiangguang Yang,Yibo Zhang
Despite SO 2 being recognized as a catalyst poisoning substance, a trace amount can enhance the acidity of the NH 3 -SCR (selective catalytic reduction) catalyst, which facilitates NH 3 adsorption and accelerates the reaction rate according to the Eley-Rideal mechanism. In this study, monoatomically dispersed Ce atoms were doped into the MoTiO x lattice to regulate the quantity and distribution of sulfate. This regulation was achieved by leveraging the stronger affinity of SO 2 to Ce, thus maximizing the acidifying effect of SO 2 to boost the NH 3 -SCR performance of the catalyst. The catalyst demonstrated the ability to maintain over 80 % NO x conversion for at least 144 hours in the presence of high concentration SO 2 (250 ppm). A detailed examination of the surface dynamics after SO 2 introduction revealed that NH 4 (SO 4 ) 2 , formed on the surface, converted to NH 4 HSO 4 . The decomposition of NH 4 HSO 4 extracted lattice oxygen from the catalyst, leading to an increase in oxygen vacancies on the catalyst surface as the duration of SO 2 exposure increased. The surface-adsorbed oxygen, brought about by these oxygen vacancies, was readily activated, which promoted the dehydrogenation process of NH 3 and the progression of NH 3 -SCR. Further, based on the discovery of the unique phenomenon and mechanism of NH 4 HSO 4 decomposition that generates oxygen vacancies, gases containing poisonous SO 2 were utilized for the pretreatment of the catalyst to optimize its surface and enhance its sulfur resistance (fighting poison with poison). The results demonstrated that the pretreated catalyst rapidly achieved optimal NO x conversion and maintained catalytic stability for over 240 h even in the presence of 250 ppm SO 2 without any decrease in activity. This research innovatively leveraged the poisonous SO 2 to optimize the catalyst's surface, thereby achieving higher catalytic performance and sulfur resistance, which offers valuable insights into the design of novel sulfur-resistant catalysts.
研究领域:
催化化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
Environmental Chemistry
·
2023
·Vol. 20
·期 6
·235-248
·
IF 4.3
Hailiang Zhang,Long Jia,Yongfu Xu
Environmental context The process of ethylene ozonolysis is an essential source of CH2OO radicals, and the latter is an important oxidant for the atmospheric pollutant SO2. The accuracy of a widely used atmospheric chemistry model (Master Chemical Mechanism, MCM) in quantifying SO2 oxidation has not been evaluated. In this study, this accuracy was evaluated, and optimal parameters underpinned by data from smog chamber experiments.Rationale The oxidation of SO2 by CH2OO radicals in the ethylene-O3 system is one of the important pathways of sulfate aerosol formation, but the accuracy of Master Chemical Mechanism (MCM) simulation for this reaction was not evaluated, although the MCM has been widely used in previous studies.Methodology The oxidation of SO2 in the ethylene-O3 system was performed in detail under different conditions, which were used to evaluate the accuracy of MCM simulation for the reactions in this study.Results The experimental conditions of low RH and high initial SO2 concentration favour the SO2 oxidation in the ethylene ozonolysis, and the yield of CH2OO in the ethylene ozonolysis without irradiations was determined to be 0.43. The n-hexane (C6H14) oxidation intermediates can promote the SO2 oxidation rate by generating sulfur-containing organics in the aerosol water. The original MCM simulated SO2 consumption after 4-h reaction was more than 70% smaller than the measured results. By adjusting the yield of CH2OO and updating the reaction rate constants of CH2OO-related reactions (e.g. with SO2, H2O and organic acid), the difference between experiments and simulations decreased from 70% to 6.6%.Discussion The promotion effects of n-hexane on the oxidation of SO2 suggest that alkanes may be the precursors of sulfur-containing organics in the atmospheric environment. This study further confirms the effect of CH2OO on the oxidation of SO2 in the atmospheric environment and provides information on the performance of MCM simulation.
研究领域:
大气化学
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环境科学
✓ 已验证
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2020
·
IF 3.573
Bin Jiang,Shuai Hou,Luhong Zhang,Na Yang,Na Zhang,Xiaoming Xiao,Xiaodong Yang,Yongli Sun,Xiaowei Tantai
Ionic liquids (ILs) as promising absorbents for SO2 capture in flue gas desulfurization have been extensively studied. In this work, a multisite absorption strategy was used to synthesize ether-linked diamine protic ionic liquids (EDPILs) for efficient SO2 capture. The prepared EDPILs containing ether-linkage chain exhibited superior SO2 absorption relative to conventional protic ionic liquids (PILs). Density functional theory calculations demonstrated that the ether-linkage chain intensified the physical interaction between EDPILs and SO2. In a subsequent experiment, bis(2-dimethylaminoethyl) ether dilactate [BDMAEE][L]2, which possessed outstanding SO2 capture capacities, was used to prepare aqueous solutions (aq), which reduced viscosity of PILs and improved their applicability. An in-depth assessment of the desulfurization performance of [BDMAEE][L]2 aq revealed that effective SO2 absorption can be achieved even at relatively low concentrations. Specifically, 50 wt % [BDMAEE][L]2 aq exhibited a high absorption capacity (1.04 molSO2/molILs, 0.097 gSO2/gabsorbents) as well as a high SO2/CO2 selectivity at 0.2 vol % SO2 and 40 °C. Overall, ether-linked absorbents with improved desulfurization performance (high SO2 absorption capacity, satisfactory SO2 removal efficiency, and excellent reusability) possess good application prospects in flue gas desulfurization.
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
ACS Catalysis
·
2022
·
IF 13.7
Yongjun Ji,Shaomian Liu,Shaojia Song,Wenqing Xu,Liang Li,Yu Zhang,Wenxing Chen,Huifang Li,Jingang Jiang,Tingyu Zhu,Zhenxing Li,Ziyi Zhong,Dingsheng Wang,Guangwen Xu,Fabing Su
Pt-based catalysts are promising for the selective catalytic reduction of NOx by CO (CO-SCR), but some technical issues hinder their practical application, including the high Pt loading needed, high reduction temperature, and the low tolerance toward SO2. Here, we report a novel Pt catalyst for CO-SCR, which has negatively charged single-atom Pt embedded on CuO squares, and the latter is supported on CoAlO nanosheets. This Pt–CuO/CoAlO catalyst with an ultra-low Pt loading (0.02 wt %) exhibited 91% NO conversion and 80% N2 selectivity in 3% O2 at 200 °C. More importantly, it showed almost no activity loss in 200 ppm SO2 over a 15 h test. The theoretical calculations reveal that the negatively charged Pt has a stronger NO adsorption ability than the positively charged Pt, and Cu serves as the CO adsorption site. The much-weakened SO2 adsorption on Pt–CuO/CoAlO relative to the NO and CO adsorption effectively avoids the catalyst poisoning by SO2.
研究领域:
催化化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2019
·
IF 6.97
Shuaiqi Gao,Pengling Zhang,Zhenzhen Wang,Guokai Cui,Jikuan Qiu,Jianji Wang
The emission of SO2 from the combustion of fossil fuels leads to many environmental issues. The incorporation of ionic liquids (ILs) on porous supports to produce supported ionic liquids is an effective technology for SO2 capture. However, blockage of pore channels is one of the main problems of this technology, which results in a substantial decrease of absorption capacity. Herein, a novel type of ionic liquid, 1-methyl-3-(3-triethoxysilylpropyl) imidazolium tetrazolate, functionalized large pore sized 3D mesoporous FDU-12 sorbents has been synthesized through a chemical grafting method. The as-prepared materials are characterized using SAXS, N2 adsorption, TEM, XPS, elements analysis, EDS mapping, and TGA and then the performance of these materials to capture SO2 is studied. The IL@FDU-12 materials are found to exhibit a high absorption capacity of SO2 up to 8.19 mmol SO2/g-sorbent (i.e., 524.2 mg/g) and a fast absorption rate (ca. 6 min is needed to reach equilibrium) at 25 °C and 1 bar since blockage of pore channels is effectively avoided and the IL is highly dispersed in the channels. These materials can also be used for the effective capture of CO2 (1 bar) and low content of SO2 (10%). Moreover, they have excellent thermal stability and can be reused in many absorption/desorption cycles without loss of the high absorption capacity and fast sorption/desorption rate.
研究领域:
环境科学
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材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
Catalysis Science & Technology
·
2021
·Vol. 11
·期 15
·5125-5134
·
IF 6.119
Yanke Yu,Xianfang Yi,Jiali Zhang,Zhaojian Tong,Changwei Chen,Mudi Ma,Chi He,Jinxiu Wang,Jinsheng Chen,Bingbing Chen
Non-vanadium-based catalysts with high SO2 tolerance are still interesting in selective catalytic reduction of NO by NH3 (NH3-SCR) and SO2 adsorption is the foremost step for the deactivation of catalysts. In order to alleviate the adsorption of SO2, we fabricated a series of rhenium (Re; without stable sulfate) supported TiO2 catalysts and studied their SO2 tolerance for the first time. Owing to suitable surface acidity and reducibility, ReOx/TiO2 catalysts exhibited satisfactory activity in a wide temperature range of 250–350 °C. As expected, experimental results and DFT calculations indicated that SO2 adsorption on ReOx/TiO2 catalysts was rather weak, thus the catalysts performed excellent SO2 tolerance in the NH3-SCR reaction. Moreover, in situ DRIFTS indicated that the NH3-SCR reaction on ReOx/TiO2 catalysts followed the Eley–Rideal mechanism and SO2 had little effect on the reaction mechanism. Our findings should provide new insights into the development of SCR catalysts with high SO2 tolerance.
研究领域:
催化化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
Catalysts
·
2019
·Vol. 9
·期 6
·519
·
IF 3.444
Jiaming Shao,Fawei Lin,Yan Li,Hairong Tang,Zhihua Wang,Peixi Liu,Guanyi Chen
NO oxidation was conducted over MnOx-CeO2catalysts, which were synthesized by the co-precipitation method. The calcination temperature and third metal doping were the main considerations. MnCe catalysts calcined at 350 °C and 450 °C attained the highest NO conversion efficiency, compared to 550 °C. XRD results suggested that the higher the calcination temperature, the higher the crystallization degree, which led to a negative effect on catalytic activity. Subsequently, Sn, Fe, Co, Cr, and Cu were separately doped into MnCe composites, but no improvement was observed for these trimetallic catalysts in NO conversion. Nevertheless, MnCeSn, MnCeFe, and MnCeCo still exhibited a desirable NO conversion efficiency, so they were tested under SO2addition together with MnCe catalyst. Among them, MnCeFe exhibited the highest NO conversion after whole poisoning testing. XPS results indicated that Fe could protect Mn and Ce metal oxides from being reduced during SO2poisoning process. Furthermore, in in-situ DRIFTS measurement, part of nitrate species maintained undestroyed on the MnCeFe catalyst surface after SO2poisoning. These characteristics reinforced that Fe dropping would achieve better performance under SO2atmosphere.Keywords:MnOx-CeO2;co-precipitation;NO oxidation;SO2resistance;metal addition
研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
ChemistrySelect
·
2024
·Vol. 9
·期 28
·e202401039
·
IF 1.9
Xueqi Wang,Kai Li,Fei Wang,Lei Shi,Shuangyou Bao,Jiacheng Bao,Xin Sun
Graphical In this study, we prepared the thermally modified copper slag catalyst CS-CaO-900 and applied it to a pilot-scale Fenton-like denitrification system. In single-factor experiments, the effects of six factors, namely inlet NO concentration, H 2 O 2 concentration, catalyst dosage, reaction temperature, L/G ratio, and pH value, on desulfurization and denitrification were investigated. Through analysis of the experimental results, the three factors that had the greatest impact on the maximum denitrification efficiency, namely pH value, H 2 O 2 concentration, and reaction temperature, were selected. The response surface methodology was employed to investigate the significance of the three factors and optimize the parameters, and it was finally determined that the initial pH of the slurry had the greatest impact on the maximum denitrification efficiency, followed by the H 2 O 2 concentration. At the same time, the combination of initial slurry pH and reaction temperature, initial slurry pH and H 2 O 2 concentration also had a large impact on the maximum denitrification efficiency, and the combination of reaction temperature and H 2 O 2 concentration had a non-significant impact on the denitrification efficiency. And through the model optimization to get the best parameters, denitrification experiments under this parameter to achieve the maximum denitrification efficiency of 91.5 %, for further industrial application to provide reference and guidance. In this study, Response Surface Methodology (RSM) was employed to optimize the experimental factors influencing the simultaneous removal of NOx and SO 2 in a spray tower wet scrubbing experiment. Thermally modified copper slag (CS-CaO-900) was prepared by heat treating the original copper slag. The performance of CS-CaO-900 in the synchronized removal of NOx and SO 2 was then evaluated in an expanded experimental setup. Based on single-factor experimental results, the Box-Behnken design of RSM was used to optimize the reaction parameters in a two-stage sequential reactor (bubbling reactor + spray tower). NOx removal efficiency was modeled as a function of reaction temperature, pH, and H 2 O 2 concentration. Regression curves provided a visual representation of the interaction effects among these parameters on NOx removal efficiency in the thermally modified copper slag/H 2 O 2 composite slurry. This study elucidates the characteristics of each parameter under wet scrubbing conditions and provides essential data for industrial applications.
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2020
·
IF 5.774
Qingping Xin,Chao Zhang,Yu Zhang,Qingqing Liang,Lei Zhang,Shaofei Wang,Hui Ye,Xiaoli Ding,Yuzhong Zhang
Obtaining high SO 2 absorption flux for membrane contactor is noticeably vital for fule gas desulfurization, and superhydrophobic surface is essential to reach excellent desulfurization performance. The development of a generic and low budget strategy for membrane contactors preparation is important in indisturial application. In this study, a superhydrophobic polyethersulfone-silica (PES/PES-SiO 2 ) gas-liquid membrane contactor is fabricated using a facile spin coating method. PES substrate is prepared by a facile non-solvent induced phase separation (NIPS), and then the superhydrophobic surface of PES/PES-SiO 2 is formed on the PES substrate by spin coating method. The solubility parameters of mixed solvent, PES concentration, and SiO 2 content are regulated to investigate the morphology of membrane contactors. On one hand, the surface structure of MMMCs is regulated, and constructs lotus-leaf like morphology, which noticeably elevate surface roughness. On the other hand, SiO 2 nanoparticles enhance hydrophobic characteristic with water contact angle 159° and anti wetting resistance with liquid entry pressure of water (LEP w ) 1.389 bar. Moreover, the SiO 2 nanoparticles help to significantly improve the stability of desulfurization performance, which is much higher than PES control membrane after 12 h test. The SO 2 absorption fluxes and SO 2 removal efficiencies are 1.24 × 10 −3 mol·m −2 ·s −1 and 63.8%, respectively. Besides, the membrane phase transfer coefficient ( K m ) and membrane phase transfer resistance ( H / K m ) are explored.
研究领域:
化学工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
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
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOM
·
2023
·Vol. 75
·期 2
·268-278
·
IF 2.6
Li Yan-Chun,Zhao Fei-Ping,Liu Hui,Peng Bing,Min Xiao-Bo,Lin Zhang
It is critical to recycle valuable elements such as zinc and iron from smelting waste containing zinc ferrite because of the resource crisis and environmental sustainability. Sulfating roasting followed by water leaching has been considered a promising approach. In this study, a novel sulfating roasting method using SO 2 has been developed to treat zinc ferrite for the efficient separation of zinc and iron. Moreover, the conversion mechanism of zinc ferrite and SO 2 was investigated in detail. The results showed that the transformation rate of zinc ferrite reached 95.47% at 600°C for 30 min under SO 2 /SO 2 + O 2 of 60% (v/v). The mechanism studies revealed that O in SO 2 combined with the O vacancy of \( {\text{Zn}}_{{{\text{A}} - {\text{site}}}}^{{2 + }} - {\text{O}} - {\text{Fe}}_{{{\text{B}} - {\text{site}}}}^{{3 + }} \) , while the S in SO 2 combined with the \( {\text{Fe}}_{{{\text{B}} - {\text{site}}}}^{{3 + }} \) of \( {\text{Zn}}_{{{\text{A}} - {\text{site}}}}^{{2 + }} - {\text{O}} - {\text{Fe}}_{{{\text{B}} - {\text{site}}}}^{{3 + }} \) for electron migration. S (IV) was oxidized to S (VI) while Fe 3+ was reduced to Fe 2+ . Importantly, zinc ferrite transformed into zinc-deficient magnetite intermediate ( \( {\text{Zn}}^{{2 + }} ({\text{Fe}}^{{2 + }} )_{{{\text{A}} - {\text{site}}}} - {\text{O}} - {\text{Fe}}^{{3 + }} ({\text{Fe}}^{{2 + }} )_{{{\text{B}} - {\text{site}}}} \) ) via reduction of Fe 3+ and migration of Fe 2+ . The transformation of zinc ferrite was a catalyst-free redox reaction. This study provided a new insight into the utilization of smelting waste and a theoretical basis for the efficient separation of zinc and iron from smelting waste containing zinc ferrite.
研究领域:
冶金工程
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环境科学
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材料科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）