CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Yanke Yu,Desheng Wei,Zhaojian Tong,Jinxiu Wang,Jinsheng Chen,Chi He
Ammonia (NH 3 ) is a critical component causing environmental problems like haze and water pollution. Selective catalytic oxidation of ammonia (NH 3 -SCO) to N 2 and H 2 O is a promising method to abate NH 3 emission. However, inferior SO 2 tolerance is still a tremendous challenge to be conquered for present NH 3 -SCO catalysts regarding practical applications. Application of materials which was difficult to be sulfated by SO 2 should be an effective way to solve this problem. Here, a ReO x -CuSO 4 /TiO 2 catalyst which coupled the advantages of ReO x (Rhenium oxides, supplying highly active adsorbed surface oxygen enhancing NH 3 -SCO reaction) and CuSO 4 (providing Brønsted acid sites inhibiting the formation of N 2 O) was rationally fabricated. Results indicated that ReO x -CuSO 4 /TiO 2 catalyst exhibited excellent catalytic performance in NH 3 -SCO with almost 100% of NH 3 oxidized at 300 °C (N 2 selectivity as high as 96%). Crucially, the composite catalyst exhibited incredible activity and stability under harsh reaction conditions toward SO 2 (600 ppm) and H 2 O (4.0 vol%) owing to the superior inhibition capability for SO 2 adsorption. In situ DRIFTS, in situ Raman and in situ XPS demonstrated that the NH 3 -SCO reaction over ReO x -CuSO 4 /TiO 2 catalyst mainly obeyed a N 2 H 4 reaction mechanism and oxidation–reduction circle between Re 7+ and Re 6+ played a vital role. Moreover, SO 2 would not affect this reaction mechanism on ReO x -CuSO 4 /TiO 2 catalyst. The knowledge and understanding reported could provide critical insights for the design and optimization of efficient materials for industrial NH 3 oxidative elimination.
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高影响因子
JOURNAL OF CATALYSIS
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2021
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IF 7.92
Yonglong Li,Senyou Yang,Honggen Peng,Wenming Liu,Yangyang Mi,Zheng Wang,Changjin Tang,Daishe Wu,Taicheng An
Manganese (Mn)-based mixed oxides are considered the most efficient catalysts for low-temperature ammonia selective catalytic reduction of nitrogen oxides (NO x ) (NH 3 -SCR of NO x ). Water resistance and sulfur tolerance, especially the SO 2 tolerance of Mn-based catalysts, are the main obstacles preventing their practical application. Therefore, in this study, a series of cobalt (Co)-doped MnFeO x ternary mixed oxides catalysts with a hierarchically ordered structure (Hierc-MnFe 1-δ Co δ O x , δ = 0.2, 0.4 and 0.6) were developed and applied for NH 3 -SCR of NO x at low temperature. Compared with Hierc-MnFeO x , Hierc-MnFe 1-δ Co δ O x catalyst exhibited enhanced low-temperature activity and a broadened temperature window (NO x conversion above 80% was between 90 and 343 °C over Hierc-MnFe 0.6 Co 0.4 O x ), as well as better H 2 O resistance and SO 2 tolerance. The enhanced low-temperature activity was attributed to a larger amount of active oxygen species, a higher proportion of Mn 4+ , Fe 3+ and Co 3+ content, and the improvement of surface acidity, which can facilitate the adsorption and activation of NO and NH 3 . Additionally, the Hierc-MnFe 0.6 Co 0.4 O x catalyst exhibited superior soot tolerance due to its special hierarchically ordered architecture. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) revealed that the Co-modified Hierc-MnFe 1-δ Co δ O x ternary oxide catalyst could efficiently protect nitrate species on Hierc-MnFe 0.6 Co 0.4 O x from the poisoning effect of SO 2 , thereby boosting its SO 2 tolerance. This study provides a good candidate for low-temperature de NO x application with enhanced SO 2 and soot tolerance.
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JOURNAL OF MOLECULAR LIQUIDS
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2016
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IF 2.74
Tianxiang Zhao,Xi Feng,Wentao Zheng,Xingbang Hu,Jianbin Zhang,Youting Wu
In a previous work, the binary mixture of polyethylene glycol 200 (PEG) and dimethyl sulfoxide (DMSO) was used as a promising medium for absorption of SO 2 ( J. Chem. Eng. Data 2015 , 60 , 2135). As a continuation of the previous study, the solubility data of dilute SO 2 in the binary mixture of PEG + DMSO were measured by isothermal gas-liquid equilibrium experiments at 298.15 K and 122.66 kPa with SO 2 partial pressure below 128 Pa in the gas phase. The solubility of SO 2 decreased gradually with increasing mass fraction of PEG in the mixtures. We found that the absorption process, which obeyed Henry's law within the given experimental conditions, was physical absorption , and Henry's constants were further calculated from solubility data. Furthermore, to obtain important information about the absorption mechanism, the inter-molecular interactions among SO 2 , PEG, and DMSO were investigated by UV, FTIR, and 1 H NMR spectroscopic techniques. Spectral results showed that the interactions among SO 2 , PEG, and DMSO were resulted from both intermolecular hydrogen bonding and the O → S charge-transfer interaction.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Minghao Shi,Jihui Yang,Mingjia Zhang,Shule Zhang,Qin Zhong
The Ce-based catalysts show promising activity in the selective reduction of NO x with NH 3 (NH 3 -SCR) at medium and low temperatures, yet their limited sulfur tolerance hinders broader application. We have developed a catalyst by confining CeO 2 within the mesopores of ZSM-5 zeolite (CeO 2 @ZSM-5), resulting in uniform dispersion and ultra-small CeO 2 nanoparticles (<10 nm). This distinctive structure enhances the interaction between the carrier and active species, reducing the catalyst's surface basicity and its affinity for acidic SO 2 gas. Additionally, the small CeO 2 particle size leads to an increased Ce 3+ concentration, which inhibits the reaction between Ce active sites and SO 2 . Employing a dual strategy of reducing adsorption and inhibiting reactions, we significantly minimized the impact of SO 2 on NH 3 -SCR. Impressively, common Ce-based catalysts become deactivated due to the formation of corresponding sulfates through reaction with SO 2 , however, CeO 2 @ZSM-5 achieves NO x conversion above 98% and N 2 selectivity of 100% within the temperature range of 250 °C to 450 °C. The addition of 100 ppm SO 2 does not significantly affect NH 3 -SCR activity. This study provides an effective approach to mitigate SO 2 adsorption and reactions, offering a valuable strategy for the development of highly efficient sulfur-resistant catalysts.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Yu Zhang,Rui Wang
NH 3 ‑selective catalytic reduction as the fascinating technology for complete NO x removal, the key in practical applications is to explore advanced catalysts with high catalytic reactivity and stability at low temperature. Herein, a series of hollow spherical AMnO x (A = Ce, Cu, Ni) catalysts was fabricated by using carbon nanospheres as sacrificial template. Characterization analysis including XRD, ICP, BET, SEM, TEM, H 2 -TPR, NH 3 -TPD, XPS, in situ DRIFTS together with kinetic studies were applied to acquire knowledge of the morphological structure and surface features of the catalysts as-prepared. We also performed a comparative study on three samples with regard to their SCR activity at low temperatures. Notable, the catalytic activity of the NiMnO x catalyst (95.9 %) was vastly superior to that of the CeMnO x (85.4 %) and CuMnO x (30.5 %) at 100 °C. This enhanced low-temperature activity of NiMnO x are correlated against hollow structure with more active sites, wider pore distribution, higher surface Mn content and the enhancement in surface acidity and reducibility. Even with 5 vol% H 2 O in the reaction gas fraction, the catalytic performance of NiMnO x hollow spheres was superior to the other two catalysts. Besides, it can be used for six consecutive runs without suffering a substantial activity loss. Additionally, the impact of various crucial process variables, including space velocity, H 2 O, SO 2 , and metal poisons, on the denitrification efficiency of NH 3 -SCR was examined. The current researches have a positive guiding role in the development of high-efficiency low-temperature NH 3 -SCR denitrification catalysts to boost NO x degradation.
研究领域:
环境科学
·
催化化学
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高影响因子
FOOD CHEMISTRY
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2023
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IF 8.8
Di Zhang,Min Wang,Man Li,Lin Liu,Ran Duan,Nana Xue,He Chen,Lijun Shang,Tieliang Wang,Xujin Wu,Junfeng Zhang
Sulfur dioxide (SO 2 ) and viscosity play important physiological roles in organisms, and real-time detection of their content changes is critical for organisms and human health. Herein, we developed a fluorescence probe NPNB with aggregation-induced emission (AIE) performance and mitochondrial localization effect for simultaneous detection of viscosity and SO 2 . NPNB can realize the efficient and specific detection of SO 2 and viscosity at different emission wavelengths with a cross-talk-free effect, respectively. NPNB showed good sensing performance against SO 2 , including fast response (<7 min), and low detection limit (8.4 nM). Bioimaging experiments indicated that NPNB has good mitochondrial targeting and can achieve cellular imaging of both exogenous and endogenous SO 2 and viscosity. Importantly, NPNB enables real-time imaging of changes in SO 2 and viscosity during mitochondrial dysfunction. Moreover, the resulting probe has been applied to detect SO 2 in food and water samples with a satisfactory recovery (84.46–105.57 %), further demonstrating its compatibility and practicality.
研究领域:
生物化学
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医学检测
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材料科学
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2018
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IF 6.653
Jianliang Sun,Lianghai Li,Guangying Zhou,Xue Wang,Liang Zhang,Yueping Liu,Jierui Yang,Xianghong Lü,Feng Jiang
The conventional flue gas treatment technologies require high capital investments and chemical costs, which limit their application in industrial sectors. This study developed a sulfur-cycling technology to integrate sulfide production by biological sulfur reduction and simultaneous catalytic desulfurization and denitrification with H2S (H2S-SCDD) for flue gas treatment and sulfur recovery. In a packed bed reactor, high-rate sulfide production (1.63 ± 0.16 kg S/m3-d) from biological sulfur reduction was achieved using organics in wastewater as electron donors at pH around 5.8. 93% of sulfide in wastewater was stripped out as H2Sg, which can be a low-cost reducing agent in the H2S-SCDD process. Over 90% of both SO2 and NO were removed by the H2S-SCDD process under the test conditions, resulting in the formation of sulfur. 88% of the input S (H2Sg and SO2) were recovered as octasulfur with high purity. Besides partial recycling to produce biogenic sulfide, excessive sulfur can be obtained as a sellable product. The integrated sulfur-cycling technology is a chemical-saving and even profitable solution to the flue gas treatment in industrial sectors with wastewater available.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2022
·Vol. 29
·期 47
·71721-71730
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IF 5.19
Huang Wenjun,Li Sichao,Wang Hongbin,Cui Peng,Xu Haomiao,Cheng Can,Qu Zan,Yan Naiqiang
Oxidation–reduction-absorption based on sulfite is a promising process for simultaneous removal of NO x and SO 2 . However, excessive oxidation of sulfite and competitive absorption between NO x and SO 2 limit its application. A matching strategy between antioxidants and alkaline agents has been proposed to solve these problems and enhance the absorption process. The comparison results of inhibitors showed that hydroquinone exhibited long-term high-efficiency inhibition of S(IV) (SO 3 2- /HSO 3 - ) oxidation. The comparison of alkaline agents showed that the Na 2 SO 3 solution with heterogeneous mixture of MgO and hydroquinone exhibited better absorption performance than that with other combinations. The absorption amounts of NO x in 0.15 mol/L Na 2 SO 3 50 mL solution added 0.1% hydroquinone (HQ) with 0.09 mol/L MgO were 2.24 mmol, which improved 5 times than that without additives. In addition, studies on the influence of pH showed that the pH of MgO mixture could be stabilized at 9–10 for a long time, while the pH of Na 2 CO 3 mixture decreased faster. Further studies suggested that the hydration of MgO resulted in the solution with MgO keeping high pH. This is also the main reason why the combination of MgO and hydroquinone is superior to the combination of Na 2 CO 3 and hydroquinone in desulfurization and denitration performance.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2019
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IF 8.355
Zijian Song,Ben Wang,Wu Yang,Tao Chen,Chuan Ma,Lushi Sun
Fe 2.5 M 0.5 O 4 (M = Mn, Ti and Cu) were investigated for the first time as the catalyst for simultaneous removal of NO and SO 2 through catalytic oxidation-absorption with vaporized H 2 O 2 . The physicochemical properties of as-prepared catalysts were comprehensively characterized by XRD, SEM, TEM, BET, XPS, TPR, VSM, TG and PL analyses. Activity test results showed that SO 2 can be completely removed under most conditions. However, NO removal was affected by catalyst, H 2 O 2 consumption, reaction temperature, GHSV and coexistence gases (i.e., H 2 O, O 2 , NO and SO 2 ). Mn, Ti and Cu doping in the magnetite can remarkably enhance NO removal. Redox pairs and oxygen vacancy of catalysts were considered as vital factors affecting OH generation. Base on the catalyst characterization and DFT calculation results, the main mechanism of Mn, Ti and Cu doping on the catalytic activity improvement was explained as follows: (a) Mn, Ti and Cu doping can increase the catalyst surface area; (b) Ti on the surface can directly promote the catalytic decomposition of H 2 O 2 ; and (c) Mn and Cu doping can promote the generation of oxygen vacancy and indirectly increase the activity. Moreover, two arrangement forms of an industrial simultaneous removal system for NO, SO 2 and Hg 0 were proposed.
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Journal of Environmental Chemical Engineering
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2022
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IF 7.968
Pengkai Jin,Liu Yang,Zhongyi Sheng,Xinyue Chu,Dianhui Chen
An indium and copper-doped mordenite catalyst (InCu/MOR) was prepared and tested as a potential catalyst for high temperature NH 3 selective catalytic reduction (NH 3 -SCR) of NO x in the gas turbine . The InCu/MOR catalyst exhibited excellent catalytic activity (over 83 % NO x conversion) in the presence of 5 % H 2 O and 100 ppm SO 2 above 550 °C. A series of characterization (XRD, Py-TR, XPS, NH 3 -TPD, H 2 -TPR and in-situ DRIFTS) were applied to analyze the catalyst. The obtained results showed that the addition of indium promoted the formation of isolated Cu 2+ and more Brønsted acid sites, which could improve the tolerance to sulfur dioxide and inhibit the occurrence of high temperature ammonia oxidation side reactions. Meanwhile, the ammonia on InO + /In 2 O 3 sites was activated and reacted with the nitrate/nitrite species on the catalyst surface to form nitroammonium (NH 4 NO 3 /NH 4 NO 2 ), which was a short lived intermediate for NH 3 -SCR. The superior catalytic performance of InCu/MOR could attribute to these comprehensive effects.
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高影响因子
APPLIED SURFACE SCIENCE
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2018
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IF 4.439
Weiyuan Yao,Yue Liu,Zhongbiao Wu
A series of CeO 2 @Ce-O-P “multi-core@shell” catalysts were synthesized in this paper for selective catalytic reduction (SCR) of NO with NH 3 . The experimental results had showed that CeO 2 @Ce-O-P-30:3 yielded best SO 2 tolerance of an over 70% deNO x efficiency at 250 °C in the presence of 100 ppm SO 2 for 20 h, which was much higher compared to pure Ce-O-P and CeO 2 samples. Further characterization results indicated that Ce-O-P coating layer could somewhat inhibit sulfur depositing on the catalysts during SCR reaction in the presence of SO 2 , thereby protecting the active sites from SO 2 poisoning. Especially, O 2 -TPD results illustrated that a great amount of active oxygen species were retained on used CeO 2 @Ce-O-P catalyst after a long term reaction. The synergetic effect of “multi-core@shell” structure could be attributed to such enhanced performances. The “core” CeO 2 devoted abundant active oxygen sites to fulfill the SCR reaction. And the “shell” Ce-O-P could not only provide acid sites, but also protect the active oxygen species by avoiding the over-adsorption of SO 2 on the catalyst. This work could provide a new way to increase the sulfur resistance for low temperature SCR catalysts.
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高影响因子
Journal of Natural Gas Chemistry
·
2012
·
IF 1.348
Lincai Peng,Junping Zhuang,Lu Lin
Effects of Zr/Ti molar ratio in SO 2− 4 /ZrO 2 -TiO 2 solid acid catalyst calcined at different temperatures on its surface properties and catalytic activity were thoroughly investigated in this paper. The physicochemical characteristics of prepared samples were determined by N2 adsorptiondesorption, XRD, NH3-TPD and XPS techniques, respectively. It was found that the crystallization temperature of the samples increased after the combination of ZrO 2 and TiO 2 ; and phase transformations from the anatase to the rutile of TiO 2 species and the tetragonal to the monoclinic of ZrO 2 species were effectively suppressed at higher temperature. The sample with a Zr/Ti molar ratio of 3/1 calcined at 450 °C showed the highest surface area and the most acid sites among all the tested samples. The acid site densities of samples were relatively closed to each other if they were calcined at the same temperature, however, decreased with the calcination temperature. The result indicates that the sulfur content in samples is a crucial factor to control the acid site density. Calcining the sample at 650 °C and higher temperatures resulted in a significant desorption of sulfate ion on the samples. The synthesized samples were evaluated as a potential catalyst for glucose conversion under the near-critical methanol conditions (200 °C/4 MPa). The results suggested that the relatively weaker acid sites of the catalyst were more favorable for the accumulation of methyl glucosides, while the moderate acid sites were responsible for the formation of methyl levulinate. The catalytic activity for methyl levulinate production almost increases linearly with the catalyst acid site density. The catalyst deactivation is due to the loss of sulfate ion and the two catalysts with Zr/Ti molar ratios of 3/1 and 1/3 could effectively alleviate the deactivation caused by sulfate solution in the reaction medium and can be reused after calcination with the reuse rate of over 90% in terms of the methyl levulinate selectivity.
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