Environmental Science-Nano
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2023
·Vol. 10
·期 10
·2744-2753
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IF 7.3
Jiaxin Lv,Ruixin Chen,Zhen Wu,Yang Bai,Han Song,Chen Tian,Mengye Wang,Zhang Lin
The enrichment of microplastics in polar ice is a typical phenomenon discovered in recent years. Thus, it is worthwhile to explore the degradation behavior of microplastics in frozen environments, which is crucial to evaluate their impact on polar ecosystems. Here, taking polystyrene (PS) as an example, the degradation behaviors of MPs in frozen anoxic Fe(II)-containing solutions were investigated. The results revealed that PS degradation rate in frozen solution was 14.6-fold higher than that in water. Mechanism study showed that freezing-induced aggregation and extrusion of PS enhanced the generation of environmentally persistent free radicals (EPFRs), which in turn contributed to the formation of H2O2. Moreover, freezing-induced enrichment of Fe(II) further interreacted with H2O2 to form Fe(IV) and OH free radicals at a pH of ∼6.5, and thus accelerated the degradation of PS. Such reaction was accompanied by the formation of Fe(III)-containing products, which would further react with aged PS to produce new EPFRs and Fe(II). Such cycles of aged PS/EPFRs and Fe(III)/Fe(II) continued to accelerate the degradation of PS in the frozen solution. This study provides an overlooked pathway for microplastic degradation in frozen Fe(II)-containing solutions, which would be of key importance to understand the degradation behaviors of microplastics in frozen environments.
研究领域:
环境科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2017
·
IF 6.216
Hongya Liu,Shuxiang Bao,Zutong Cai,Tiefeng Xu,Nan Li,Lulin Wang,Haixiang Chen,Wangyang Lu,Wenxing Chen
A biomimetic catalytic system composed of iron hexadecachlorophthalocyanine (FePcCl 16 ), hydrogen peroxide (H 2 O 2 ), H 2 O and pyridine exhibited high activity for ultra-deep removal of dibenzothiophene (DBT) in model oil containing n-octane. The conversion of DBT was up to 100% after 60 min operation at room temperature. In addition, the FePcCl 16 catalyst could be recycled for more than 23 times without noticeable decrease on the conversion of DBT. Moreover, the activation energy evaluated through Arrhenius’ equation was found to be equal to 25.5 kJ/mol. Nitrogen-containing compounds such as pyridine, quinoline, and acridine, naturally existing in many kinds of fuel oil, had previously been considered to inhibit the oxidative desulfurization (ODS) process. Surprisingly, these organonitrogen compounds could actually accelerate the conversion rate of DBT in this catalytic system. Mechanistic studies revealed that the high-valent iron(IV)-oxo species were the main active intermediate via the heterolytic O–O bond cleavage of the putative iron(II)-hydroperoxo species. Pyridine binding to iron(II)-hydroperoxo complexes was demonstrated to facilitate the generation of high-valent iron(IV)-oxo species and enhance the reactivity of high-valent iron(IV)-oxo species in ODS.
研究领域:
化学工程
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催化科学
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环境科学
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Yunxiao Zheng,Xiaohui Wu,Yongchun Zhao,Tao Zhou,Mingjie Huang
Polymerization transfer (PT) technology is highly advantageous for treating high-salinity wastewater due to its high tolerance to coexisting anions and superior electron utilization efficiency. Here, we report the unusual simultaneous achievement of rapid pollutant removal (pseudo-first-order rate constant of 0.15 min −1 , 56.0-fold higher than unmodified counterparts) and high PT ratio (>65 %) in a peroxymonosulfate (PMS) activation system. This was achieved by simply tuning the Fe content within a rationally designed Fe/N engineered pine sawdust biochar catalyst. Performance enhancement stems from Fe-induced graphitization improving electron transfer, coupled with N-induced moderate orbital hybridization between Fe 3 d (Fe/N biochar) and O 2 p (PMS) atomic states, optimizing PMS adsorption-desorption and yielding the lowest energy barrier for Fe(IV) O formation. Remarkably, the system maintains robust performance under high salinity conditions (500 mM Cl − , HCO 3 − , NO 3 − , and SO 4 2− ) and achieves 67.5–77.3 % chemical oxygen demand (COD) removal during 17-day continuous-flow treatment of real coking wastewater, where polymerization-mediated organic removal through C C/C O coupling. Furthermore, residual oligomers are efficiently removed by subsequent activated carbon (AC) adsorption or poly-ferric sulfate (PFS) coagulation, establishing an integrated “catalytic polymerization-AC/PFS polishing” paradigm for sustainable treatment of refractory organics in high salinity coking wastewater.
研究领域:
环境工程
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催化化学
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水污染控制
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材料科学
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环境功能材料
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高级氧化技术
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2023
·
IF 11.4
Shuang Meng,Minglu Sun,Peng Zhang,Chenying Zhou,Chuanshu He,Heng Zhang,Yang Liu,Zhaokun Xiong,Peng Zhou,Bo Lai
The continuous electron supply for oxidant decomposition-induced reactive oxygen species (ROS) generation is the main contributor for the long-standing micropollutant oxidation in the iron-based advanced oxidation processes (AOPs). Herein, as a new class of co-catalysts, metal borides with dual active sites and preeminent conductive performance can effectively overcome the inherent drawback of Fenton-like reactions by steadily donating electrons to inactive Fe(III). Among the metal borides, tungsten boride (WB) exhibits a significant co-catalytic performance run ahead of common heterogeneous co-catalysts and exceptionally high stability. Based on qualitative and semi-quantitative tests, the hydroxyl radical, sulfate radical, and iron(IV)-oxo complex are all produced in the WB/Fe(III)/PDS system and Fe(IV)-induced methyl phenyl sulfoxide decomposition is up to 72%. Moreover, the production efficiency of ROS and relative proportions of radical and nonradical pathways change with various experimental conditions (dosages of PDS, WB, and solution pH) and water matrices. The rate-determining step of Fe(II) regeneration is greatly accelerated resulting from the synergetic effect between exposed metallic reactive sites and nonmetallic boron with reductive properties of WB. In addition, the self-dissolution of surface tungsten oxide and boron oxide leads to a renovated surface for sustainable Fe(III) reduction in long-term operations. Our discovery provides an efficient and sustainable strategy in the field of enhanced AOPs for water remediation.
研究领域:
环境科学
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材料科学
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化学工程
·
水处理
✓ 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）