RSC Advances
·
2017
·Vol. 7
·期 84
·53622-53630
·
IF 3.108
Changming Li,Hong Zeng,Pingle Liu,Jian Yu,Feng Guo,Guangwen Xu,Zhan-guo Zhang
The development of new routes for the utilization of red mud (RM) waste is very urgent due to its huge accumulation and potential environmental harm. By taking advantage of its Fe–Al–Si–Ti composition and excellent plasticity, we developed a ball milling and acid–base neutralization method to reuse the RM waste as Fe-based denitration catalysts. The resulting RM catalysts demonstrate excellent catalytic activity and stability with >90% NO conversion above 400 °C in the presence of SO2 and H2O, which is even much better than that of a commercial V–W–Ti catalyst. Characterization data reveal that our treatment eliminates poisonous alkaline metal elements and increases dispersion of RM particles, making the RM active for denitration reactions. The formation of ferric sulfate species with more reducible Fe3+/Fe2+ active sites by a SO2 activation method can further enhance the denitration activity. Moreover, NH3-TPD and in situ IR results demonstrate that the NH3-SCR reaction over the RM catalyst follows the Eley–Rideal mechanism at high temperature and the increased absorption of NH3 for alkaline metal-eliminated or SO2-activated samples accounts for its high DeNOx efficiency. The demonstrated feasibility for reusage of the RM as DeNOx catalyst has promising industrial prospects for its extremely low cost, no toxicity, and high efficiency.
研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2020
·Vol. 27
·期 22
·27663-27673
·
IF 3.056
Liu Yuan-zhen,Xu Qi-yan,Guo Rui-tang,Duan Chao-peng,Wu Gui-lin,Miao Yu-fang,Gu Jing-wen
The Cu/TiO 2 catalysts with the addition of Eu were developed by the sol-gel way for the selective catalytic reduction (SCR) of NO x by NH 3 . Activity tests revealed that CuEu/TiO 2 -0.15 catalyst showed the optimal de-NO x performance in a wide temperature range (150–300 °C), along with an admirable SO 2 tolerance. According to characterization analysis, the relationship between the NH 3 -SCR performance and physicochemical characters of samples was explored. The adjunction of Eu on Cu/TiO 2 catalyst can contribute to the formation of a large amount of Cu 2+ , adsorbed oxygen, and acid sites on the catalyst surface. Moreover, the Eu addition on Cu/TiO 2 is favorable to the generation of activated NO x and NH 3 substances adsorbed on the catalyst surface, which would conduce to the NH 3 -SCR process by Langmuir-Hinshelwood (L-H) mechanism effectively.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2020
·
IF 3.573
Guokai Cui,Shuzhen Lyu,Fengtao Zhang,Huiyong Wang,Zhiyong Li,Yanan Li,Jianji Wang
In this contribution, a series of ionic liquids (ILs) with tri-n-butylethyl-phosphonium cation ([P4442]) and functional anions are designed and prepared, including pyridinolate anion ([PyO]), pyridinecarboxylate anion ([PyCOO]), and pyridinesulfonate anion ([PySO3]). Each anion contains both N site and O site, which can react with SO2. It could be found that up to 4.71 mol SO2 mol–1 IL absorption capacity could be received by [P4442][PyO] at 20 °C and 1 bar. Compared to ILs with phenolate anion ([PhO]), benzoate anion ([PhCOO]), and benzenesulfonate anion ([PhSO3]), the pyridine-based counterparts in this work were found to significantly enhance SO2 capture capacity, especially for anions with high basicity. It was demonstrated from the combination of FT-IR and NMR spectroscopic investigations and DFT calculations that the simultaneous cooperative interaction of N···SO2 and O···SO2 between functional anion [PyO] and SO2 was the main reason for high absorption capacity of low-concentration SO2 by [P4442][PyO].
研究领域:
化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
KOREAN JOURNAL OF CHEMICAL ENGINEERING
·
2020
·Vol. 37
·期 4
·623-632
·
IF 2.69
Yan Zhinan,Kang Yong,Li Dan,Liu Yu Chun
Hematite (α-Fe 2 O 3 ) is a promising alternative to the catalysts currently used due to its low cost, fairly good activity and environmentally friendly properties. In this study, α-Fe 2 O 3 /SiO 2 nanocatalysts promoted with cobalt and cerium (Co 3 O 4 -CeO 2 -α-Fe 2 O 3 /SiO 2 ) were prepared via wet co-impregnation method, and the effects of promoters on catalytic performances for SO 2 oxidation at different temperatures, SO 2 concentrations, cycle numbers, catalytic stability as well as catalyst charging were investigated. The results indicated that SO 2 conversion rose with the increasing of catalyst charging and SO 2 concentration. Also, the as-prepared catalyst had the maximum SO 2 conversion at the reaction temperature of 500 °C, excellent catalytic recyclability and activity stability. Its physicochemical and redox properties were characterized by XRD, BET, SEM, FT-IR and XPS. The results of XRD and FT-IR spectra confirmed that the formation of Ce 2 FeO 4 network in the Co-Ce co-doped catalysts proved the promoting effect of cerium on higher valence state of the active ingredient. The N2 adsorption/desorption results evidenced that cerium could increase the proportion of mesoporous, and the XPS spectra indicated that cobalt and cerium in the catalysts could increase the available oxygen (O β /O α ) for the redox reaction. Due to its excellent low onset temperature, fairly good activity and environmentally friendly properties, the as-prepared catalyst of Co 3 O 4 -CeO 2 -α-Fe 2 O 3 /SiO 2 appeared to be more efficient for the SO 2 conversion in a large concentration range.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2013
·
IF 2.004
Chao Chen,Xiao-Sen Li,Zhao-Yang Chen,Zhi-Ming Xia,Ke-Feng Yan,Jing Cai
The equilibrium hydrate formation conditions for ternary simulated flue gas [CO2 (0.1368) + N2 (0.8547) + SO2 (0.0085)] with SO2 aqueous solutions, and SO2 + tetra-n-butyl ammonium bromide (TBAB) aqueous solutions were measured using the temperature search method, over the temperature and pressure range of (272.85 to 283.15) K and (1.20 to 5.09) MPa, respectively. The corresponding equilibrium gas compositions were analyzed. The effects of SO2 concentration and TBAB additive on the hydrate phase equilibrium were studied. For the flue gas and SO2 aqueous solution, the presence of SO2 reduces the hydrate formation pressure. The higher is the SO2 concentration in aqueous solution, the easier the hydrate forms, and the higher the SO2 concentration in equilibrium gas phase is. N2 mole fractions in equilibrium gas phase are higher than that in the feed flue gas, while CO2 is lower due to its relative high solubility. For a given system, the equilibrium hydrates formation pressure increases with the increase in temperature. Both SO2 and N2 mole fractions in equilibrium gas phase decrease with the increase in pressure, while the CO2 mole fraction increases. TBAB solution with w4 = 0.050 not only reduces the equilibrium hydrates formation pressure markedly, but also helps the dissolution of SO2 in aqueous solution. The SO2 concentrations in equilibrium gas phase for the TBAB addition system are much smaller than those without TBAB addition. The pressure reducing effect of the TBAB promoter for SO2 containing flue gas is dependent on the SO2 concentration and smaller than that for flue gas without SO2. A small amount of SO2 produces a synergy with TBAB to promote the hydrate formation, but the high SO2 concentration produces an inhibition on the hydrate formation, and causes the hydrate equilibrium pressure increase. The optimum SO2 mass fraction in solution is lower than 0.010.
研究领域:
化学工程
·
环境科学
✓ 已验证
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2019
·
IF 6.393
Haili Yu,Faqin Dong,Bowen Li,Frank S. Riehle
Rapid, reliable, and highly selective detection of SO 2 and its derivatives has an especially important practical significance in terms of environmental monitoring and human health. In this study, we describe a novel Co 2+ triggered radical reaction pathway for visual colorimetric detection of SO 2 and SO 3 2− . The reaction between Co 2+ and SO 2 or SO 3 2− with the assistance of dissolved oxygen produces highly active sulfate radical, leading to the oxidation of o-phenylenediamine (OPD). The oxidation products containing 2,3-dinitro-phenazinemethane, OPD dimer, and OPD trimer show strong UV–vis absorption. Consequently, SO 2 and SO 3 2− are quantitatively determined using the Co 2+ -OPD colorimetric detection system. This colorimetric assay exhibits a 60–650 μM and 30–70 ppm linear ranges for detection of SO 3 2− and SO 2 , respectively. The corresponding limit of detection is calculated to be 4.07 μM and 1.26 ppm for SO 3 2− and SO 2 . What is more, a distinct color change can be found at a SO 3 2− concentration of 50 μM by the naked-eye observation. The specific radical detection guarantees that the present colorimetric assay has a good anti-interference ability over common inorganic ions and gases.
研究领域:
环境化学
·
分析化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Zhong-yi Wang,Rui-tang Guo,Zhen-zhen Guan,Xu Shi,Wei-guo Pan,Zai-guo Fu,Hao Qin,Xing-yu Liu
A sequence of Cr-modified CeZr 2 O x catalysts were synthesized through the co-precipitation way and applied in selective catalytic reduction (SCR) of NO x with ammonia. The optimal catalyst (Cr 1 CeZr 2 O x ) exhibited the excellent NH 3 -SCR activity and high SO 2 resistance. From the characterization results, Cr species in Cr 1 CeZr 2 O x could suppress the formation of ZrO 2 crystals, which could also contribute to stronger surface acidity and reducibility . Besides, more Ce 3+ and surface adsorbed oxygen species were observed on Cr 1 CeZr 2 O x catalyst. On the basis of in situ DRIFT experiments, it could be confirmed that the NH 3 -SCR process on Cr 1 CeZr 2 O x was promoted through Langmuir-Hinshelwood (L-H) mechanism. Besides, the improved NO oxidation and more ad-NO x and ad-NH 3 also played a vital role for the superior low-temperature SCR activity of Cr 1 CeZr 2 O x .
研究领域:
催化化学
·
环境科学
✓ 已验证
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2019
·
IF 0
Limei Cao,Qian Wang,Ji Yang
A novel ultrafine Pt/Beta catalyst supported on carbon paper was prepared and applied to selective catalytic reduction of NO x by H 2 at a low temperature below 90 °C. Here, 0.8 wt.% Pt/Beta reached approximately 100 % NO conversion at 90 °C under oxygen-rich conditions (1000 ppm NO, 1 % H 2 , and 4 % O 2 ). The influence of the dispersion and particle size of Pt on the catalytic performance was investigated using Polyvinylpyrrolidone (PVP) as a structure directing agent to regulate the Pt particles. The feeding amount of PVP significantly influenced the catalytic activity of the catalysts. When the feeding amount was less than 50 mg, the Pt particle size was smaller, and the dispersion was higher, providing a higher NO conversion. However, when the feeding amount exceeded 50 mg, the dispersion no longer increased, and the activity slightly decreased. N 2 physisorption (BET) confirmed that excessive PVP decreased the specific surface area, which suppressed the catalytic activity of Pt/Beta. Moreover, the NO conversion efficiency was dependent on the dispersion and particle size of Pt and was minimally affected by the surface area of the catalysts. The Pt/Beta catalyst system was deactivated, and an irreversible poisoning phenomenon for SO 2 was observed. Zr, Ce, and V were introduced into the catalyst system as metal auxiliaries . The Ce-modified Pt-Ce/Beta catalyst prepared in this study showed resistance to SO 2 .
研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
RARE METALS
·
2021
·Vol. 41
·期 1
·37-44
·
IF 4.003
Shi Ze-Di,Zhang Le,Ma Yue-Long,Zhou Tian-Yuan,Sun Bing-Heng,Shao Cen,Huang Guo-Can,Yin Shi-Tong,Hou Su-Dan,Yang Zeng-Wang,Chen Hao
银作为一种功能性材料, 由于其优良的导电性而用作于汽车电子的电接触材料。但是, 这种材料极易遭受大气腐蚀问题, 并导致结构的损坏和器件的失效。本文研究了应用于印刷电路板中导电银的腐蚀行为, 并从动力学和机理方面发现了影响材料结构损害最主要的环境因素(SO 2 污染物、温度和相对湿度(RH, Relative humidity))。相较于其他因素, 温度(55 °C)是运行环境中引起导电材料结构变化的最主要因素, 并且表面的腐蚀层厚度达到了最大值, 即 d film =15.56× 10 -5 μm。然而, 在腐蚀过程中, SO 2 污染物和RH促进了腐蚀物质的扩散, 并也会增加腐蚀产物层(Ag 2 S和Ag 2 SO 4 )的厚度。因此, 本文不仅大大增强了人们对于不同环境因素下导电材料结构损害的认识, 同时也为实际生产中的防腐设计和材料选择提供了重要的指导。 Graphical abstract
研究领域:
材料科学
·
环境科学
✓ 已验证
DOI
高影响因子
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2016
·Vol. 92
·期 4
·767-774
·
IF 2.738
Xiaocai Meng,Jianying Wang,Haichao Jiang,Xiangjing Zhang,Shuolei Liu,Yongqi Hu
BACKGROUND Ionic liquids (ILs) have been widely used in the field of SO 2 separation for gases. In this study, two kinds of guanidinium-based dicarboxylic acid ionic liquids including [1,1,3,3-tetramethylguanidinium][Poly(ethylene glycol) bis(carboxymethyl) ether] ([TMG][PBE]) and [1,1,3,3-tetramethylguanidinium] [Suberic acid] ([TMG][SUB]) were synthesized, and their absorption and desorption performance of SO 2 were investigated. RESULTS The saturated molar ratio of SO 2 to [TMG][PBE] and [TMG][SUB] were 8.74 and 5.96 mol SO 2 per mole ILs at 25 °C, respectively. [TMG][PBE] saturated with SO 2 was easier to desorb and could be recycled at least 5 times without loss of initial performance, while the ability to absorb SO 2 by [TMG][SUB] was gradually weakened after desorption. The absorption mechanism is discussed. Results showed that SO 2 could interact not only with the amino group on the cation but also with the methylene bonded to the carbonyl carbon on the anion for [TMG][SUB]. As for [TMG][PBE], SO 2 could interact with the ether group by S-O ligand interaction, instead of interacting with the methylene group bonded to the carbonyl carbon on the anion. [TMG][PBE] show good performance for SO 2 capture. CONCLUSION The anion of dicarboxylic acid-based ILs plays an important role in absorption/desorption of SO 2 on the basis of the experimental results. © 2016 Society of Chemical Industry
研究领域:
化学工程
·
环境科学
·
绿色化学
·
气体分离技术
✓ 已验证
DOI
高影响因子
CHEMICAL PHYSICS LETTERS
·
2019
·
IF 1.901
Liang Wei,Yilin Wang,Zhongjiao Fan,Rujia Wang,Yuan Wang,Jianqiu Chen,Yun Xu
Solubility of SO 2 in [N 2224 ][Met] was measured at temperature from 313.2 to 333.2 K and pressure up to 1.8 bar. The [N 2224 ][Met] absorbed SO 2 at high speed and could be recycled for four times. The Reaction Equilibrium Thermodynamic Model (RETM) was used to correlate the experimental data, Henry’s constant ( H ), reaction equilibrium constant ( K 0 ), and thermodynamic properties ( Δ r H m 0 , Δ r G m 0 , Δ r S m 0 , Δ H phy a n d Δ H chem ) were derived. Considering the absorption capacity and low absorption enthalpy, as well as the fast absorption process, [N 2224 ][Met] is thought to be a promising absorbent to ordinary solvent as a desulfurizer.
研究领域:
化学工程
·
环境科学
·
绿色化学
·
热力学
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Zhihao Zhao,Chao Ma,Lingyun Xu,Zhenwei Yu,Dong Wang,Lei Jiang,Xiangyu Jiang,Guangcheng Gao
Polyaniline-based conductive polymers are promising electrochemical sensor materials due to their unique physical and chemical properties, such as good gas absorption, low dielectric loss, and chemical and thermal stabilities. The sensing performance is highly dependent on the structure and dimensions of the polyaniline-based conductive polymers. Although in situ oxidative polymerization combined with the self-assembly process has become one of the main processes for the preparation of flexible polyaniline-based gas sensors, how to prepare polyaniline materials into uniformly arranged microwire arrays is still an urgent problem. In this paper, an in-depth study was conducted on the preparation of polyaniline microwire arrays by combining a wettability interface dewetting process and a liquid-film-induced capillary bridges method. The factors influencing the preparation of polyaniline microwire arrays, including solution concentration, template width, evaporation temperature, and evaporation time, were investigated in detail. The wire formation rates were recorded from the results of SEM images. 100% microwires formation rate can be obtained by using a 1.0 mg mL–1 concentration of polyaniline solution and a 10 μm silicon template at an evaporation temperature of 80 °C for 18 h. The prepared microwire arrays can realize sulfur dioxide sensing at room temperature with a response speed of about 20 s and can detect sulfur dioxide gas as low as 1 ppm. Thus, the liquid-film-induced capillary bridge method shows a new possibility to prepare gas sensor devices for insoluble polymers.
研究领域:
材料科学
·
化学传感器
·
纳米技术
·
环境监测
✓ 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）