Journal of Water Process Engineering
·
2025
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IF 6.7
Haoran Xv,Qian Zhang,Thiquynhxuan Le,Duclenh Phan,Libo Zhang
Ammonium persulfate has been proven to be effective in purifying thiosulfate (S 2 O 3 2− ) and sulfite (SO 3 2− ) impurities in desulfurization solutions. However, the sole use of ammonium persulfate as an oxidant faces the challenge of high oxidant consumption. In this study, a novel approach was proposed to enhance the oxidation efficiency of ammonium persulfate on sulfur-containing ions through ultrasonic activation. The results indicate that this technology has the advantages of high purification efficiency and low usage of ammonium persulfate. Specifically, the concentrations of S 2 O 3 2− and SO 3 2− decreased from 16.26 g/L and 38.30 g/L to 1.09 g/L and 8.89 g/L, respectively, meeting the actual production requirements; and the usage of ammonium persulfate could be reduced by 10–30 g per liter of solution compared with the case of ammonium persulfate alone. The introduction of ultrasound increased the generation of free radicals (SO 4 · − and ·OH), enhancing their oxidative capacity. The contribution of free radicals to the oxidation of S₂O₃ 2− and SO₃ 2− increased from 11.1 % and 9.8 % to 50.0 % and 25.8 %, respectively. This study reveals that the ultrasonic activated ammonium persulfate is expected to achieve efficient purification of the desulfurization mother liquor and reduce the addition of ammonium persulfate.
研究领域:
环境科学
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化学工程
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DOI
高影响因子
Catalysts
·
2025
·Vol. 15
·期 3
·255
·
IF 4
Changhui Zhu,Xudong Zhang,Wenling Xu,Yanni Zheng,Baohe Tian,Xi Chen,Wenchao Zhu
To overcome the limitations of conventional catalysts in sterically hindered esterification reactions, a radio frequency (RF) plasma-modifiedSO42−/S2O82−/SnO2-Al2O₃ solid superacid catalyst was synthesized via sol-gel and impregnation, followed by RF plasma treatment and calcination. Comprehensive characterization revealed that the RF plasma modification endowed the catalyst with a uniform particle distribution (4.32 nm average size), larger specific surface area (104.44 m2·g−1), elevated total acid content (142.86 μmol·g−1), and increased oxygen vacancy concentration (16.4%), compared to the conventional sol-gel–impregnation–calcination-prepared catalyst. The RF plasma-modifiedSO42−-S2O82−/SnO2-Al2O3was subsequently applied to perform the esterification reaction of Tyr, with a higher steric hindrance. Mechanistic studies indicated that the plasma-induced surface etching and electronic redistribution/intensified electron-withdrawing capability ofSO42−/S2O82−groups synergistically strengthened Brønsted/Lewis acidity. For the esterification of tyrosine—a sterically demanding substrate—the modified catalyst achieved a 92.1% methyl tyrosine yield under the optimized conditions (180 °C, 0.8 MPa N2, 6 h), where the catalyst exhibited a better mechanical strength and better lifetime with five cycles. This work not only provides a scalable plasma-assisted strategy for tuning solid superacids but also establishes an eco-friendly alternative to traditional catalysts, and was applied to the esterification reactions of some high-steric-hindrance substrates.
研究领域:
催化化学
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生物有机化学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
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IF 8.1
Yongchao Wang,Yahui Liu,Fancheng Meng,Jian Zhang,Shuai Zhao,Xile Tian,Lina Wang,Desheng Chen,Tao Qi
The significant chemical similarity between vanadium and chromium complicates the process of efficient extracting V(Ⅳ) from the solution containing Cr(Ⅲ) to prepare high-purity vanadyl sulfate electrolyte. In this study, the separation of vanadium and chromium with 2-ethylhexyl phosphoric acid-2-ethylhexyl ester (EHEHPA) was enhanced by increasing the concentration of SO 4 2− . Under the extraction equilibrium pH of 2.5, the extraction of Cr(III) was suppressed by increasing the concentration of SO 4 2− anions, which hardly affected the extraction efficiency of V(IV), achieving a separation factor as high as 5780.6 at SO 4 2− concentration of 1.75 mol·L −1 . Furthermore, after pretreatment of the water-leaching solution of sodium-roasted vanadium slag, extraction was carried out under the conditions of equilibrium pH of 1.8 and SO 4 2− concentration of about 2.00 mol·L −1 , and after stripping, the vanadyl sulfate electrolyte containing 2.12 mol·L −1 of vanadium and only 0.11 mg·L −1 of chromium was obtained. It was proved that Cr(Ⅲ) mainly extracted in the form of CrSO 4 + into organic phase by one EHEHPA dimer as [CrSO 4 (H 2 O)] + under higher SO 4 2− concentrations (e.g., ≥1.50 mol·L −1 ), while Cr(Ⅲ) was extracted by two EHEHPA dimers as Cr 3+ without SO 4 2− in the solution. Based on the density functional theory, the complex structures of Cr(III) were optimized and the energy changes of Cr(III) extraction reactions were calculated, indicating the complexation between SO 4 2− and Cr(III) under higher SO 4 2− concentrations resulting in the inhibition of Cr(III) extraction, and thus enhancing the separation of vanadium and chromium.
研究领域:
化学工程
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材料科学
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DOI
高影响因子
Minerals
·
2024
·Vol. 15
·期 1
·9
·
IF 2.2
Ke Yang,Li Zhou,Zhengshan Chen,Wei Zhang,Wenge Zhou
The dissolution of dolomite can not only provide the chemical components in hot springs but also provide a high-quality reservoir for geothermal resources. However, there is still debate about the main controlling factors and mechanisms of the dissolution process of dolomite. The Shuijing hot springs in Guizhou Province are rich in SO42−and the geothermal reservoir is dolomite, which provides an excellent opportunity to understand the role of SO42−in the dissolution process of dolomite. In this paper, water–rock interaction experiments were conducted at different temperatures to study the effects of SO42−, pH, and CO2on the dissolution of dolomite from the Shuijing hot springs geothermal reservoir. The results indicate that temperature is a significant factor affecting the chemical composition of hot springs water, with higher temperatures having a more pronounced effect on the dissolution of dolomite. At lower temperatures of 25 °C and 90 °C, the molar ratio of the released Ca2+and Mg2+during the dissolution of dolomite in the initial reaction stage generally approaches the Ca/Mg molar ratio of dolomite, exhibiting congruent dissolution. However, at elevated temperatures of 150 °C, the released Ca/Mg molar ratio surpasses the Ca/Mg molar ratio of dolomite, demonstrating an incongruent dissolution characteristic with Ca2+being preferentially released over Mg2+. Additionally, the relative importance of CO2, SO42−and pH on the dissolution degree of dolomite is CO2> SO42−> pH = 4 > pH = 7 > pH = 10. The promotion effect of SO42−on dolomite dissolution indicates that the greater the SO42−concentration, the stronger the dissolution of dolomite, and its dissolution ability is enhanced with the increase in temperature. Furthermore, the effect of CO2on the dissolution of dolomite is stronger than that of SO42−, leading to the oscillating fluctuation trend of the released Ca2+and Mg2+.
研究领域:
地质学
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水文学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2017
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IF 6.216
Yuefei Ji,Yuanyuan Shi,Lu Wang,Junhe Lu
Nitrobenzene (NB) is a recalcitrant organic compound caused great environmental concerns. Sulfate radical-based advanced oxidation processes (SR-AOPs) are promising environmental remediation and wastewater treatment technologies. In this contribution, we observed that degradation of NB by thermally activated persulfate oxidation process resulted in the formation of a suite of intermediates including 2-nitrophenol (2-NP), 3-nitrophenol (3-NP), 4-nitrophenol (4-NP), 2,4-dinitrophenol (2,4-DNP), 2,6-dinitrophenol (2,6-DNP), and 2,4,6-trinitrophenol (2,4,6-TNP) as well as coupling products. The formation of the nitrophenols was suggested to follow the sequence of mononitrophenols → dinitrophenols → trinitrophenol. Time-dependent evolutions of mononitrophenols and dinitrophenols were illustrated and their formation mechanisms were proposed. The evolution patterns of mononitrophenols were fitted by sequential reaction kinetic model. The formation of polynitrated phenolic compounds suggests that both denitration and nitration processes occurred during SO 4 − -based oxidation of NB. Nitration agent (i.e., NO 2 ) arising from the conversion of nitro group upon SO 4 − /HO attack is proposed to play an important role in the formation of polynitrated compounds. TOC measurement revealed that mineralization was less efficient as compared with NB degradation. The presence of NO 2 − was found to inhibit the degradation of NB but promote the formation of 2,4-DNP. Temperature played an important role in both the degradation of NB and the distribution of products. Since polynitrated aromatics are more persistent and mutagenic, the results of this contribution suggest that particular attention should be paid to their formation during SO 4 − -based oxidation processes.
研究领域:
环境科学
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化学工程
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DOI
高影响因子
Environmental Science-Nano
·
2024
·Vol. 11
·期 3
·881-888
·
IF 5.8
Yingkang Chen,Cheng-Wei Kao,Tao Luo,Hang Zhang,Yan Long,Junwei Fu,Zhang Lin,Liyuan Chai,Ting-Shan Chan,Min Liu
Tetrafluoromethane (CF4), as the simplest and most abundant perfluorocarbon in the atmosphere, is listed in the ‘United Nations Framework Convention on Gases’ for its strong greenhouse potential. With its increasing atmospheric emissions, catalytic hydrolysis of CF4 as a non-toxic by-product method has been extensively studied. However, the highly symmetric and inert structure of CF4 makes it hard to be adsorbed on the catalyst surface. Herein, we developed a protonated sulfate (–HSO4) modified ZrO2 (S-ZrO2) to enhance CF4 adsorption and achieve its complete decomposition at 650 °C, which was superior to common γ-Al2O3. Combining the surface acidity test, in situ infrared spectroscopy and density function theory simulations, we demonstrated that the introduced –HSO4 effectively enhances the Lewis acidity of adjacent Zr sites, which shows strong CF4 adsorption ability and promotes its decomposition.
研究领域:
催化化学
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环境科学
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产品关联
DOI
高影响因子
APPLIED CLAY SCIENCE
·
2022
·
IF 5.907
Qiubei Gu,Jing Liu,Yixuan Yang,Runliang Zhu,Lingya Ma,Xiaoliang Liang,Shiqin Long,Jianxi Zhu,Hongping He
Ion-adsorption rare earth deposits (IAREDs) are important source for rare earth elements (REEs). The transportation, accumulation, fractionation, and leaching of REEs in IAREDs are mainly controlled by the interactions between REEs and mineral geosorbents. The coexisting ions can significantly affect the mineral-REEs interactions, which, however, are not currently well studied. This work investigated the effects of sulfate (SO 4 2− ) on the adsorption of REEs on kaolinite and ferrihydrite, two typical mineral geosorbents in IAREDs with distinct surface properties. The obtained results indicate that, with increasing SO 4 2− concentration, the adsorption of REEs is hardly changed on kaolinite but remarkably enhanced on ferrihydrite. Additionally, SO 4 2− can particularly improve the adsorption of middle REEs on ferrihydrite. The in situ ATR-FTIR spectra results, coupled with 2D correlation spectroscopic analysis, indicate that the promoted adsorption of REEs by SO 4 2− on Fh is attributed to both the electrostatic attraction and the formation of Fe-REE-SO 4 ternary complexes. However, the negatively charged kaolinite can hardly adsorb SO 4 2− because of the strong electrostatic repulsion between them. Desorption experiments reveal that REEs can be more efficiently desorbed by NH 4 Cl from kaolinite than from ferrihydrite. The obtained results suggest that coexisting oxyanions have profound effects on the mineral-REEs interactions, which should be taken into consideration while exploring the transportation, accumulation, and fractionation of REEs in IARED.
研究领域:
矿物学
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环境科学
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DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Zhaochang Wu,Sijie Ge,Ying Han,Mengchen Zong,Shilong He,Jie Zhang
Heterogeneous catalytic ozonation is widely used in advanced treatment for the removal of refractory organics from bio-treated coking wastewater. However, the effect of inorganic anions on quinoline removal by catalytic ozonation remains unclear. In this study, the effect of three inorganic anions including Cl - , Br - , SO 4 2- on performance and mechanism for quinoline removal by TiO 2 catalyst was investigated. Results indicated that all three anions have inhibitory effects on quinoline removal; meanwhile Br - exhibited the strongest inhibition. Furthermore, the effect of factors including initial solution pH, ozone concentration, catalyst dosage and coexistence of anions on Br - inhibition was explored. The Br - inhibition mechanism was further systematically analyzed by characterizing the physicochemical properties of catalysts and investigating free radicals and quinoline degradation pathways. The inhibition caused by Br - became stronger with the coexistence of SO 4 2- . The presence of Br - reduced the amount of oxygen vacancies and active sites on catalysts. Also, the activity and stability of catalysts decreased because of the Ti ions leaching, which was obviously exacerbated as the coexistence of SO 4 2- . Moreover, the Br - and SO 4 2- both could react with •OH to form abundant RHS (BrOH •- , Br• and Br 2 •- ) with low oxidative activity to further inhibit quinoline removal. The radical scavenging tests demonstrated that the main reactive oxygen species (ROS) was changed from •OH to O 2 •- and 1 O 2 in the catalytic ozonation system by the introduction of Br - and SO 4 2- . Meanwhile, brominated byproducts were found to be generated during the degradation of quinoline by GC-MS analysis.
研究领域:
环境科学
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化学工程
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产品关联
DOI
高影响因子
JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2021
·
IF 6.789
Tao Huang,Shu-wen Zhang,Lulu Zhou,Hui Tao,Aiyin Li
Ultrasonication has been mechanically applied widely in the recycling of spent lithium-ion (SLI) batteries while its influence on chemical pathways has barely been reported. In this study, ultrasonication and sulfate radicals were used in a coupling system to obtain efficient recoveries of Co and Li from SLI batteries. The synergistic effect of ultrasonication and sulfate radicals on recycling was quantitatively analysed by significance analysis and surface responses in a central composite design . The employment of persulfate significantly affected the whole recycling process during the sonication . Factors including acoustic time, operating powers, and temperature all had a significant effect on the recoveries of Co and Li. The maximum recovery efficiencies of Co and Li of 97.33% and 99.25%, respectively, and the minimum loss rate of Al of 4.13% were simultaneously obtained by the fitting predictor. The optimal combination of factors for the sonication system included an acoustic time (min) of 5.5, an operating power (W) of 168, a temperature (°C) of 86, and a ratio of cathode foil to S-solution (mg/mL) of 1:60. A moiety of cathode active material was directly separated from the aluminium collector by sulfate radical-related reactions. Co and Li cations dissolved from LiCoO 2 by carbon dioxide radicals were reprecipitated by excess oxalate. The research demonstrated the positively synergistic influence caused by ultrasonication and sulfate radicals on achieving efficient recoveries of Co and Li from SLI batteries, explicitly expanding the technical choices for the recycling procedure.
研究领域:
环境科学
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化学工程
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DOI
高影响因子
CRYSTENGCOMM
·
2025
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IF 2.6
Feng Jiao,Jinzhao Huang,Zehui Liu,Yu Zhang,Xiaolong Deng,Ke Zhang,Guixin Zhao
In this paper, sodium sulfite (Na₂SO₃) and cerium nitrate (Ce(NO₃)₃) were added in the hydrothermal method for the preparation of FeCo LDH, and needle-like Ce-FeCo LDH (NS) catalysts were grown in situ on a carbon cloth.The additions of Na₂SO₃ and Ce(NO₃)₃ regulated the electron transfer of the metal cations in the LDH, and significantly improved the performance of the catalysts. The prepared Ce-FeCo LDH (NS) catalysts exhibited excellent electrochemical properties. The overpotential of OER was 221 mV at a current density of 10 mA/cm² in 1 M KOH. The surface structure and catalytic performance of the catalysts were maintained well after 100 h stability test. This study provides a new idea for the improvement and design of OER catalysts based on FeCo LDH, which is an important reference for clean energy research.
研究领域:
材料科学
·
清洁能源研究
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DOI
高影响因子
Materials
·
2024
·Vol. 17
·期 21
·5145
·
IF 3.1
Siqi Lv,Yujian Liang,Xuezhen Zhang,Xiaomei Tan,Zuotan Huang,Xuan Guan,Chongmin Liu,Zhihong Tu
Pyrite is one of the most abundant metal sulfide tailings and is susceptible to oxidation, yielding acidic mine drainage (AMD) that poses significant environmental risks. Consequently, the exploration of pyrite surface oxidation and the kinetic influencing factors remains a pivotal research area. Despite the oxidation of pyrite producing a significant amount of sulfate (SO42−), a comprehensive investigation into its influence on the oxidation process is lacking. Leveraging pyrite’s semiconducting nature and the electrochemical intricacies of its surface oxidation, this study employs electrochemical techniques—cyclic voltammetry (CV), Tafel polarization, and electrochemical impedance spectroscopy (EIS)—to assess the effect of SO42⁻ on pyrite surface oxidation. The CV curve shows that SO42−does not change the fundamental surface oxidation mechanism of pyrite, but its redox peak current density decreases with the increase in SO42−, and the surface oxidation rate of pyrite decreases. The possible reason is attributed to SO42−adsorption onto pyrite surfaces, blocking active sites and impeding the oxidation process. Furthermore, Tafel polarization curves indicate an augmentation in polarization resistance with elevated SO42−concentrations, signifying heightened difficulty in pyrite surface reactions. EIS analysis underscores an increase in Weber diffusion resistance with increasing SO42⁻, indicating that the diffusion of Fe3+to the pyrite surface and the diffusion of oxidized products to the solution becomes more difficult. These findings will improve our understanding of the influence of SO42−on pyrite oxidation and have important implications for deepening the understanding of surface oxidation of pyrite in the natural environment.
研究领域:
环境科学
·
电化学
·
矿物学
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产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Yang Liu,Hailong Feng,Weiyi Li,Xueping Wang,Guoxiang Huang,Longxia Wang,Xingqiu Li,Yuxing Xie,Chenglu Liang
Catalysts in-situ reconstructed from transition metal sulfides for oxygen evolution reaction (OER) have been regarded as potential alternatives for the noble metal catalysts . Intriguingly, it was found that the self-optimized SO 4 2− @Cu doped Co(OH) 2 catalyst was reconstructed from bimetallic sulfide of CuCo 2 S 4 . During the OER process, the copper was partially leached and meantime doped into the in-situ generated Co(OH) 2 with SO 4 2− adsorption, while only oxides were discovered in counterparts of mono-metal sulfides. As a result, the SO 4 2− @Cu doped Co(OH) 2 catalyst exhibited superior OER performances, with low overpotentials of 211/272 mV to achieve the current densities of 10/100 mA cm −2 , exceeding the counterparts reconstructed from mono-metal sulfides. Experimental and theoretical results suggested that the in situ generated Cu doped Co(OH) 2 possessed thin and loosely layered structure with expanded lattice spacing (lattice spacing expanded from 0.28 nm to 0.46 nm) due to the SO 4 2− adsorption, making the intermediates more accessible to the active centers. In addition, the catalyst surface changed from hydrophobicity to super hydrophilicity , which greatly accelerated the mass transfer. This work indicated that the in-situ reconstruction process was greatly influenced by the interactions between metal sites and sulfide species, directly influencing the OER performances of the reconstructed catalysts.
研究领域:
材料科学
·
电化学
✓ 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）