CHEMOSPHERE
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2023
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IF 8.8
Yudan Liu,Jingke Wu,Nanchunxiao Cheng,Pengfei Gan,Yunyi Li,Wen Liu,Jiangyu Ye,Meiping Tong,Jialiang Liang
Vacuum ultraviolet (VUV) based advanced oxidation processes (AOPs) recently attracted widespread interests. However, the role of UV 185 in VUV is only considered to be generating a series of active species, while the effect of photoexcitation has long been overlooked. In this work, the role of UV 185 induced high-energy excited state for the dephosphorization of organophosphorus pesticides was studied using malathion as a model. Results showed malathion degradation was highly related to radical yield, while its dephosphorization was not. It was UV 185 rather than UV 254 or radical yield that was responsible for malathion dephosphorization by VUV/persulfate. DFT calculation results demonstrated that the polarity of P-S bond was further increased during UV 185 excitation, favoring dephosphorization while UV 254 did not. The conclusion was further supported by degradation path identification. Moreover, despite the fact that anions (Cl - , SO 4 2 - and NO 3 - ) considerably affected radical yield, only Cl - and NO 3 - with high molar extinction coefficient at 185 nm significantly affected dephosphorization. This study shed light on the crucial role of excited states in VUV based AOPs and provided a new idea for the development of mineralization technology of organophosphorus pesticides.
研究领域:
环境科学
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化学
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DOI
PubMed
高影响因子
WATER RESEARCH
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2023
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IF 12.8
Jialiang Liang,Jingke Wu,Pengfei Gan,Yudan Liu,Peng Zhen,Yunyi Li,Zhiwei Zhao,Wen Liu,Meiping Tong
Organophosphorus pesticides are extensively utilized worldwide, but their incomplete dephosphorization poses significant environmental risks. This study investigates the dephosphorization of dimethoate (DMT), a representative organophosphorus pesticide, using a vacuum ultraviolet system. Surprisingly, in addition to hydroxyl radicals ( • OH), non-radical processes such as photoexcitation and singlet oxygen atoms (O( 1 D)) exert more significant effects on DMT dephosphorization. The degradation kinetics of DMT demonstrate a perfect linear correlation with the radical yield in both UV-based and VUV-based advanced oxidation processes (AOPs), with greater efficacy of radical attack observed in the VUV system. This heightened efficiency is attributed to the excitation of DMT to a high-energy excited state induced by UV 185 radiation. Additionally, • OH alone is inadequate for achieving complete dephosphorization of DMT. The Fukui index and singly occupied orbital (SOMO) analysis reveal that the O( 1 D) generated by UV 185 -induced photolysis of O 2 exhibits exceptional selectivity towards P=S bonds, thereby playing an indispensable role in the dephosphorization process of DMT. This study highlights the significant contribution of non-radical pathways in DMT dephosphorization by VUV, which holds great implications for the advancement of photochemical-based AOPs.
研究领域:
环境科学
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农药化学
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DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
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2025
·Vol. 49
·期 35
·15448-15456
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IF 2.5
Dalong Zheng,Yuchun Tan,Xin Song
Chemical modification is a critical method to improve the properties and structures of catalysts, which remains challenging. In this study, a series of Cu–Al catalysts were prepared by a hydrothermal synthesis method for hydrogen sulphide (H2S) and phosphine (PH3) removal at 80 °C, and the role of metal complexes and acid were discussed in detail. Results showed that the HCl-treated CuAlOx catalyst with the molar ratio of Cu : Al : HCl = 5 : 5 : 1 exhibited the highest performance among all the materials tested, corresponding to capacities of 37.25 mgS g−1 for sulfur and 64.15 mgP g−1 for phosphorus. The catalysts were characterized by X-ray diffraction, Brunauer–Emmett–Teller analysis, X-ray photo electron spectroscopy, scanning electron microscopy, transmission electron microscopy, inductively coupled plasma, and in situ IR. Results showed that HCl was able to expose more active sites and expand the catalyst channel by speciation generation and structural corrosion. Cu+ species was the most important constituent in the catalyst. It was derived from the reduction of Cu2+ species, facilitated by the provision of additional electrons from Cl ions and H2 in the thermal treatment process. Metal coordination promoted the interaction of metal crystal faces, which offered more advantages in pollutant removal than single copper or aluminum. Pollutant molecules were vertically adsorbed on the Cu+ species to generate sulfur species and phosphorus species with the help of oxygen species and active sites. Subsequently, the products rapidly shifted to the surface of the catalyst and occupied the active sites and vacancies, resulting in inactivation. The strategy of metal coordination and acid treatment is an important approach that provides possibilities for enhanced catalytic performance in various applications.
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高影响因子
METALLURGICAL AND MATERIALS TRANSACTIONS B-PROCESS METALLURGY AND MATERIALS PROCESSING SCIENCE
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2025
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IF 3.1
Zhang Ningyu,Zhang Yang,Xiang Junyi,Xue Yuxiao,Yu Wenhao,Lv Xuewei
The conventional vanadium extraction and dephosphorization processes in the converter are carried out separately, which results in high energy consumption and operational complexity. Calcium ferrates possess the dual function of oxidizing agents and alkaline sources, which provides a novel approach for integrating vanadium extraction and dephosphorization processes. Accordingly, the simultaneous extraction of vanadium and dephosphorization from V-bearing hot metal by the addition of calcium ferrates was proposed in this study for the first time. The experiments were conducted in a low-frequency induction furnace at 1523 K to 1673 K in an inert atmosphere. Thermodynamic calculations and experimental studies demonstrate the potential of calcium ferrates to facilitate vanadium extraction and dephosphorization simultaneously. Especially CaFe 4 O 7 and CaFe 2 O 4 , due to their low melting point and high Oxidizing ability, can reduce the vanadium and phosphorus contents in hot metal to below 0.024 and 0.010 wt pct at 1623 K for 6 minutes of reaction. Correspondingly, the lg L V are 2.42 and 2.37, whereas the lg L P are 2.13 and 2.14, respectively. In the slag, vanadium is oxidized from V 3+ to V 5+ by Fe 2 O 3 with the CaO content increases. A shift from spinel to calcium vanadium silicate is observed. Phosphorus is always present in calcium silicate. The simultaneous vanadium extraction and dephosphorization are achieved only by adding calcium ferrate, effectively recovering vanadium resources and improving semi-steel purity.
研究领域:
冶金学
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材料科学
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化学工程
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提取冶金
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DOI
高影响因子
Journal of Water Process Engineering
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2023
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IF 7
Zijun Xie,Bo Sun,Hongying Lin,Meng Fu,Yi Zhang,Zequn Ma,Xiangming Li
Dephosphorylation that separates phosphate groups from substrates is a significant reaction for both living organisms and environmental protection. Meanwhile, 4-nitrophenol (4-NP) is known to be a popular organic compound used for pesticides production, which is genotoxic and carcinogenic to humans and animals. Herein, we have developed a bifunctional catalyst that can be used for simultaneous dephosphorylation and 4-nitrophenol (4-NP) reduction when para-nitrophenyl phosphate (p-NPP) serves as the model compound. This bifunctional catalyst was obtained by in-situ growth of NiFe layered double hydroxide on the reduced graphene oxide/polyelectrolytes assembly nanolayers (denoted as rGP 3.5 /NiFe LDH). The results demonstrate that the rGP 3.5 /NiFe LDH can activate dephosphorylation of p-NPP at 20 °C and the catalytic efficiency increases significantly with increasing temperature in the range of 20 °C to 90 °C. Moreover, by-product 4-NP formed through p-NPP dephosphorylation is further fully converted to 4-aminophenol by the rGP 3.5 /NiFe LDH within 15 min. As far as we know, this is the first example for both dephosphorylation and 4-NP reduction through NiFe LDH as bifunctional catalysts, which paves the way for the development of multiple potential applications for NiFe LDH.
研究领域:
催化
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环境化学
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材料科学
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纳米技术
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高影响因子
KOREAN JOURNAL OF CHEMICAL ENGINEERING
·
2021
·Vol. 38
·期 1
·135-143
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IF 3.309
Ma Chenghui,Zhang Xiaoting,Wen Kang,Wang Rong,Han Runping
Coating superparamagnetic iron oxide particles, i.e., Fe 3 O 4 , as adsorbents have major advantages over bare adsorbents for water treatment. As a versatile material, zirconium has been extensively studied for phosphate removal. In this study, the Fe 3 O 4 core was pre-coated with branched polyethyleneimine (PEI) first, and then loaded with zirconium to result in a highly selective adsorbent (i.e., Zr-PEI@Fe 3 O 4 ) for phosphate with a greatly broadened pH range. Scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), BET surface area, and magnetization were used to characterize the resulting adsorbent and to explore the underlying adsorption mechanism. The adsorption performance of Zr-PEI@Fe 3 O 4 toward phosphate was performed by batch experiment. The results showed that Freundlich model better fit the adsorption isotherms, while the Elovich equation better described the kinetic process. The maximum adsorption capacity of dephosphorization 32.2 mg·g −1 (according to P element) emerged in the condition of 1.0 g·L −1 and pH at 2 with 303 K. The process was spontaneous and endothermic. Zr-PEI@Fe 3 O 4 has the potential to remove phosphate from solution due to its easy separation and some good adsorption property.
研究领域:
环境科学
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材料科学
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水处理
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DOI
高影响因子
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