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Journal of Cleaner Production · 2022 · IF 11.072

Degradation of iopamidol by silicate-based microfiltration membrane activated peroxymonosulfate in aqueous solution: Efficiency, mechanism and degradation pathway

Weiqiang Wang,Zhonglin Chen,Pengwei Yan,Bingyuan Wang,Yabin Li,Jing Kang,Jimin Shen,Yizhen Cheng,Shuyu Wang,Yue Liu,Zhe Wang,Xueyan Li

Iopamidol (IPM) was frequently detected in drinking water and effluents from wastewater treatment plants (WWTPs). A silicate-based microfiltration membrane (SFM) was successfully synthesized using silicate cement as raw material and pore-forming agent. In this study, peroxymonosulfate (PMS) was activated by SFM for the first time to effectively degrade and mineralize IPM. The removal efficiency and mineralization rate of IPM were 99.7% and 49.5% respectively within 30 min in the SFM/PMS process, which were higher than those obtained by PMS oxidation only (12.8% and 1.26%) and SFM adsorption (negligible). The effects of solution pH, PMS dosage, reaction temperature, natural organic matter (NOM), chloride ion (Cl − ), bicarbonate (HCO− 3), and water matrixes on the degradation of IPM were systematically evaluated. Based on radical inhibition examinations and X-ray photoelectron spectroscopy (XPS) analysis, the potential activation mechanism was elucidated. It was found that the Fe(II) and alkaline hydration products on the surface of SFM could promote the activation of PMS. Radical scavenging tests and electron spin resonance (ESR) experiments suggested that hydroxyl radicals ( • OH), sulfate radicals ( S O 4 · − ), singlet oxygen ( 1 O 2 ) and superoxide radicals ( O 2 · − ) generated in SFM/PMS system played a critical role for IPM degradation. Finally, eleven intermediates in the degradation process of IPM were identified and five degradation pathways were proposed, mainly including hydroxyl oxidation, amide hydrolysis, amino oxidation, hydroxyl substitution and dehydroxylation . The results show that the SFM/PMS process with its excellent catalytic activity is a promising strategy for effectively removing and mineralizing organic contaminants .

研究领域: 环境科学 · 水处理技术
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FUEL · 2025 · IF 7.5

Ultrahigh-efficiency mineralization of butyl xanthate via peroxydisulfate activation by carbon cobalt composite catalyst

Qiongqiong He,Zhaoyang Song,Libo Liu,Yuan Xu,Shaomeng Huang,Zhenyong Miao

Butyl xanthates (BX) are the most important agents utilized in the processing of metallic sulfide ores, and residual BX in beneficiation wastewater pollutes the mining environment. In this study, a cobalt carbon composite catalyst (Co@C800-1) was prepared to activate peroxydisulfate (PDS) for the degradation of BX, accompanied by a COD removal rate of up to 97.7% and an extremely high mineralization rate of 91.5%. After six cycles, Co@C800-1 still retained 96% of its catalytic performance. Moreover, this catalytic system demonstrated excellent degradation efficiency (>96 %) within a wide pH range (3–9) and exhibited good salt tolerance (SiO 3 2− and HCO 3 − ). Electron spin resonance analysis suggested that SO 4 − and OH are the main active species, while a small amount of 1 O 2 is present in the Co@C800–1/PDS system. The cobalt particles on the Co@C800-1 surface and the delocalized π-electrons from edge defects are the active sites for generating SO 4 − and OH. The C O groups on the Co@C800-1 surface are the active sites for producing 1 O 2 . Therefore, the synergistic effect of free radical and non-free radical reactions enables the Co@C800-1/PDS system to exhibit excellent degradation performance. The introduction of cobalt ions not only expedites the generation of SO 4 − and OH but also ensures the high stability of Co@C800-1 through cyclic reactions between cobalt ions. This provides a theoretical basis for the development of heterogeneous catalysts for BX degradation.

研究领域: 环境科学 · 催化化学
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Regulating the microenvironment of atomically dispersed cobalt to achieve the record-breaking mineralization and 100% removal of organic pollutant

Xue Zhao,Liangfei Duan,Mengshan Chen,Peizhi Yang,Qian Liu,Yuelong Liu,Haoran Zhang,Zhuang He,Guangzhi Hu,Yingtang Zhou

Advanced-oxidation-process (AOPs) based on peroxymonosulfate (PMS) can provide strong reactive oxygen species (ROS) for the elimination of persistent-organic-pollutants (POPs), but the input of highly active environmentally friendly catalysts is the key. Here, confined cobalt was in-situ deposited on natural mineral halloysite nanotubes by Coulomb interaction, which further realizes the introduction of atomically-dispersed cobalt sites in nitrogen-doped hollow-carbon-nanotubes with large specific surface area. The constructed CoNC/NHCNTs-900 material can effectively activate PMS, resulting in the removal rate of tetracycline probe pollutants close to 100%, and the mineralization rate reached a record of 89.07%. Combined with density functional theory calculations, it was proved that the enrichment of graphite nitrogen is beneficial to regulate the microenvironment of Co and promote the adsorption and activation of PMS. In-depth tracking of the formation of ROS and the mechanism of tetracycline mineralization proved that CoNC/NHCNTs-900-driven AOPs degradation of POPs into a low-toxic species has reliability and practical significance.

CAS / MDL: 80-05-7 71-00-1 66-71-7
研究领域: 环境科学 · 材料科学
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NEW JOURNAL OF CHEMISTRY · 2025 ·Vol. 49 ·期 9 ·3526-3535 · IF 2.5

Removal of volatile organic compounds using a membrane catalytic process involving a [BMIM]PF6 ionic liquid membrane and visible light-driven N–La–TiO2 photocatalysts

Shuang Meng,Yan Zhuang,Xue Yang,Dongxuan Guo,Jinlong Li

Volatile organic compounds (VOCs) emitted from industrial activities and transportation pose significant health risks to humans and contribute to environmental issues. As a result, there has been growing interest in developing effective technologies for VOC removal. This study investigates the removal of low-concentration VOCs from air using a membrane catalytic process that combines a supported ionic liquid membrane (SILM) with a novel visible light-driven photocatalyst. The system, consisting of a 1-butyl-3-methylimidazolium hexafluorophosphate ([BMIM]PF6) SILM and N-doped La–TiO2 photocatalysts, achieves a mineralization rate of 40%–60% and a removal efficiency of approximately 75% for VOCs under visible light exposure for 10 hours. The synergistic effects of membrane separation and photocatalytic degradation significantly enhance the overall VOC removal efficiency compared to using either method alone. The membrane catalytic system demonstrates particular applicability and stability for various organic compounds, including toluene, acetone, chloroform, benzene, and xylene. Overall, this work presents a promising approach for the removal and mineralization of VOCs.

CAS / MDL: 174501-64-5
研究领域: 环境科学 · 化学工程
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WATER AIR AND SOIL POLLUTION · 2024 ·Vol. 235 ·期 7 ·1-20 · IF 3.8

Synthesis of Co3O4/BiOBr/BiOI Ternary Heterostructure and its Photocatalytic Degradation of RhB

Wang Bo,Huang Lin,Li Silan,Qi Liqiang

Rhodamine B (RhB), an alkaline cationic organic dye, poses a significant threat to natural water environments. In this investigation, composites of Co 3 O 4 and BiOBr/BiOI were synthesized and evaluated for degradation of RhB under visible light irradiation. The photocatalyst (CBB-2) with a 10wt% Co 3 O 4 composite exhibited superior degradation efficiency, achieving 99.5% within 80 min and maintaining robust stability over four cycles. Meanwhile, after 90 min of light exposure, the mineralization rate of RhB reached 57.23%. A suite of characterization techniques verified the successful synthesis of the dual type-II heterojunction in the composite catalyst and the reinforced interactions among its components, thereby enhancing charge separation efficiency and photoresponsive performance. Free radical quenching experiments elucidated the critical role of •O 2 - and h + as radicals in the photocatalytic reaction process.

研究领域: 环境科学 · 材料科学
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Scientific Reports · 2024 ·Vol. 14 ·期 1 ·1-14 · IF 3.8

Synergistic oxidation of toluene through bimetal/cordierite monolithic catalysts with ozone

Wang Xiaojian,Peng Xiaomin,Zhao Quanzhong,Mi Jinxing,Jiang Huating,Li Shengli,Hu Hui,Huang Hao

Toluene treatment has received extensive attention, and ozone synergistic catalytic oxidation was thought to be a potential method to degrade VOCs (violate organic compounds) due to its low reaction temperature and high catalytic efficiency. A series of bimetal/Cord monolithic catalysts were prepared by impregnation with cordierite, including Mn x Cu 5−x /Cord, Mn x Co 5−x /Cord and Cu x Co 5−x /Cord (x = 1, 2, 3, 4). Analysis of textural properties, structures and morphology characteristics on the prepared catalysts were conducted to evaluate their performance on toluene conversion. Effects of active component ratio, ozone addition and space velocity on the catalytic oxidation of toluene were investigated. Results showed that Mn x Co 5−x /Cord was the best among the three bimetal catalysts, and toluene conversion and mineralization rates reached 100 and 96% under the condition of Mn 2 Co 3 /Cord with 3.0 g/m 3 O 3 at the space velocity of 12,000 h −1 . Ozone addition in the catalytic oxidation of toluene by Mn x Co 5−x /Cord could efficiently avoid the 40% reduction of the specific surface area of catalysts, because it could lower the optimal temperature from 300 to 100 °C. (Co/Mn)(Co/Mn) 2 O 4 diffraction peaks in XRD spectra indicated all the four Mn x Co 1−x /Cord catalysts had a spinel structure, and diffraction peak intensity of spinel reached the largest at the ratio of Mn:Co = 2:3. Toluene conversion rate increased with rising ozone concentration because intermediate products generated by toluene degradation might react with excess ozone to generate free radicals like ·OH, which would improve the toluene mineralization rate of Mn 2 Co 3 /Cord catalyst. This study would provide a theoretical support for its industrial application.

CAS / MDL: 10026-22-9 10377-66-9
研究领域: 环境科学 · 催化化学
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Journal of Cleaner Production · 2020 · IF 7.246

Visible-light-driven AgBr–TiO2-Palygorskite photocatalyst with excellent photocatalytic activity for tetracycline hydrochloride

Yingying Shi,Zhuan Yan,Yingtao Xu,Tian Tian,Jing Zhang,Jianfeng Pang,Xihua Peng,Qianghua Zhang,Mingli Shao,Wenyi Tan,Hailun Li,Qingping Xiong

Tetracycline hydrochloride (TC) wastewater has complex components, high concentration of organic matter and certain biological toxicity. Photocatalytic degradation is of great application prospect due to its green, thorough and efficient removal of TC. In this study, heterojunction photocatalyst supported on Palygorskite (Pal) AgBr–TiO 2 -Pal with visible light response was successfully prepared via sol-gel and liquid deposition method successfully. Taking TC as the target pollutant, the photocatalytic performance of AgBr–TiO 2 -Pal photocatalys excited by visible light was studied. The spreading/grafting of AgBr–TiO 2 on the surface of Pal was improved by a series of structural characterization and composition analysis. The results also demonstrated that the specific surface area of AgBr–TiO 2 -Pal was about 48.06 m 2 ⋅g −1 with uniform mesoporous slit. The AgBr–TiO 2 -Pal catalyst was very effective for the degradation of TC, and it still retained its high stability and reusability after five cycles. The results showed that under the best reaction conditions (initial concentration of tetracycline 10 mg⋅L −1 , catalyst dosage 0.5 g⋅L −1 , pH value 9), with the excitation of visible light, the maximum removal ratio of TC was 90%, and the mineralization ratio was 67%. The removal efficiency and degradation rate of TC by AgBr–TiO 2 -Pal catalyst were 2.17 and 4.75 times as much as those of TiO 2 respectively. The outstanding photocatalytic performance of heterogeneous AgBr–TiO 2 -Pal catalyst was obtained by fully participate in the reaction by photoinduced charge. This study could be expected to be used in photocatalytic degradation of antibiotic pollutants in wastewater treatment .

研究领域: 环境科学 · 化学 · 材料科学 · 废水处理
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SEPARATION AND PURIFICATION TECHNOLOGY · 2022 · IF 9.136

Effective removal of tetracycline from water by catalytic peroxymonosulfate oxidation over Co@MoS2: Catalytic performance and degradation mechanism

Xi Li,Wenwen Zhang,Zhenxue Liu,Shiwen Wang,Xiao Zhang,Baokang Xu,Peng Yu,Yanhua Xu,Yongjun Sun

Co-based heterogeneous catalysts exhibit relatively high performance on peroxymonosulfate (PMS) activation for antibiotic pollution control in water. But the aggregation and loss of active components limit their expanded application. In this study, a 3D rose-like MoS 2 was designed and synthesized to anchor Co in its special lamellar structure and achieve its high dispersion. 98.9% of tetracycline (TC) was removed within 60 min with a mineralization rate of 50.5% under neutral condition. The accelerated valence cycle between Co 2+ and Co 3+ was the key to PMS activation and TC degradation. And the lamellar structure of MoS 2 endowed the catalyst with better stability and inhibited Co leaching. The influences of common anions (Cl − , HCO 3 − , H 2 PO 4 − , and SO 4 2− ) and humic acid in aqueous solution on TC degradation were systematically investigated. The catalytic mechanism of PMS activation and the generation of reactive oxygen species (ROS) over Co@MoS 2 were deeply investigated. The reduced biotoxicity of the intermediates indicated the potential of Co@MoS 2 /PMS system for the control of environmental risks caused by TC. This work provided a new insight for the design of metal-doped heterogeneous catalyst with high stability and a new direction for the remediation of antibiotic contamination in water.

研究领域: 环境科学 · 催化 · 水处理 · 材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2019 · IF 5.107

Study on catalytic performances and reaction mechanisms of graphene electroactive membrane in wastewater treatment

Yu Bai,Lu Zhou,Keke Ma,Hongjie Zhou,Yiying Xin

This study was conducted to access the catalytic performances and reaction mechanisms of Graphene Electroactive Membrane (GEM). The GEM was prepared by vacuum-pressing method, and characterized by FESEM and FTIR. Catalytic performances were measured in the index of decolorization ratio and mineralization rate. Active species were recognized by scavengers for investigating reaction mechanisms. The impacts of current intensity and water flux on catalytic performances were presented to illustrate the mechanisms of GEM electro-catalysis deeply. According to the results, the method of GEM preparation was reliable and Graphene was an appropriate material for Electroactive Membrane (EM). Compared with EM electro-catalysis and GEM with no electro-catalysis (GEM-NEC), the mineralization rate increased by 56.1% and 28.8% respectively, and the decolorization rate increased by 45.5% and 29.8% respectively. The decolorization rate of GEM electro-catalysis with 0.2 M Ammonium Oxalate (Scavenger of electron hole) decreased 32.7% more than GEM electro-catalysis with no scavenger. Thus, direct oxidation was the main mechanism of GEM electro-catalysis, which was very different from traditional electro-catalysis. When current intensity was less than 20 mA and water flux was higher than 3 mL/min, decolorization ratio increased dramatically. Thus, electro-catalytic process and adsorption-diffusion process played important roles in GEM electro-catalysis process. The GEM electro-catalysis was an effective and stable advanced wastewater treatment for removal of organic pollutants.

CAS / MDL: 7220-79-3 61-73-4
研究领域: 环境工程 · 化学工程 · 材料科学
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RESEARCH ON CHEMICAL INTERMEDIATES · 2025 · IF 3.5

Enhancement of the photocatalytic degradation performance for tetracycline of magnetic Fe3O4/ZnO/g-C3N4 composites by strengthening the bonding effect

Han Lijuan,Chai Keyi,Du Xinyu,Wang Xiangtong,Zhang Ping,Wang Xiaotian

Tetracycline poses a serious threat to the ecosystems even if the concentration is very low due to its structural stability. In this work, a series of magnetic separable Fe 3 O 4 /ZnO/g-C 3 N 4 composite with excellent degrading tetracycline performance were prepared. And, repeated calcination method was used to strengthen the bonding effect of single component improving the formation of heterojunction. Electrochemical analysis confirmed that the ZnO/g-C 3 N 4 and Fe 3 O 4 /ZnO/g-C 3 N 4 heterojunctions were generated, effectively accelerating the electron separation and transfer in photocatalytic process. The characterization results also showed that ZnO and Fe 3 O 4 nanoparticles are evenly distributed on the surface of g-C 3 N 4 . With the increase of the loading mass concentration of ZnO/g-C 3 N 4 , the degradation rate of tetracycline on Fe 3 O 4 /ZnO/g-C 3 N 4 composite increased and then decreased. The degradation rate of tetracycline on optimal Fe 3 O 4 /ZnO/g-C 3 N 4 composite reached to 94.50% while the TC mineralization rate reached to 61.61% under visible light irradiation for 120 min, exhibiting excellent photocatalytic performance. Due to the effect of Fe 3 O 4 , Fe 3 O 4 /ZnO/g-C 3 N 4 materials exhibited good magnetic property, which is beneficial to separation and recovery of photocatalysts. The reusability experiment showed that the degradation rate of tetracycline was 80.66% after five cycles, displaying good reusability.

CAS / MDL: 144-62-7 60-54-8
研究领域: 材料科学 · 环境化学 · 光催化 · 纳米复合材料 · 水处理
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Environmental Progress & Sustainable Energy · 2020 ·Vol. 39 ·期 5 ·e13404 · IF 1.989

Two-step method for the construction and start-up of a fungal–bacterial biofilter for treating gaseous toluene

Jian Zhai,Chunhua Jiang,Chao Long

In this study, a two-step method was applied to build and start up a fungal–bacterial biofilter. The reactor was built by controlling pH and adding an antibiotic based on a conventional biofilter. A low pH (5.9) and the addition of chloramphenicol were favorable for the construction of the fungal–bacterial biofilter. The results illustrated that it took only 15 days to complete the start-up of the fungal–bacterial biofilter. The removal efficiency (RE) and the mineralization rate (MR) were 93.0% and 77.6%, respectively, at a toluene concentration of 1,000 ± 112 mg m −3 and an empty bed residence time (EBRT) of 45 s. The new method effectively overcomes the unstable performance and nonuniversality of such a reactor, which was constructed by inoculating a pure fungal culture into a bacterial biofilter. Removal performance comparison and PICRUSt analysis showed that the higher the relative abundance of benzoate degradation-related genes in activated sludge is, the more suitable the sludge is for inoculation. The increase in toluene MR and the apparent morphology and scanning electron microscopy (SEM) results of biofilms in the top layer of the fungal–bacterial biofilter suggest that the biofilter performance enhancement can be attributed to the ability of fungi to distribute toluene-degrading bacteria.

研究领域: 环境工程 · 微生物学 · 生物技术
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CHEMOSPHERE · 2022 · IF 8.943

Effect of pyrolysis temperature on the activated permonosulfate degradation of antibiotics in nitrogen and sulfur-doping biochar: Key role of environmentally persistent free radicals

Yanzhuo Zhang,Mengqi Xu,Rui He,Jing Zhao,Wei Kang,Jinghua Lv

Because of the increasingly widespread contamination of antibiotics, the preparation of biochar by heteroatom doping to further improve the catalytic degradation efficiency of antibiotics has become a major focus of research. In this study, N-doped (NBC), S-doped (SBC), and NS-doped (NSBC) moso bamboo biochar were obtained at preparation temperatures of 300–700 °C. The concentration of environmentally persistent free radicals (EPFRs) in all biochars peaked when the preparation temperature was 500 °C: 2.45 × 10 19 spins·g −1 (BC), 9.23 × 10 19 spins·g −1 (NBC), 6.10 × 10 19 spins·g −1 (SBC), and 4.36 × 10 19 spins·g −1 (NSBC). After heteroatom doping, EPFR species were more abundant, and the distribution of three types of EPFRs (oxygen-centered (g > 2.0040), carbon-centered (g < 2.0030), and carbon-centered radicals with oxygen atom free radicals (2.0030 < g < 2.0040) varied with the preparation temperature. In the process of antibiotic degradation, both NBC and SBC increased the degradation rate of antibiotics, whereas NSBC reduced the degradation rate. Compared with the degradation rate of antibiotics of biochar (79.86%), the degradation rate of antibiotics by NBC, SBC, and NSBC via PMS activation was 92.23%, 88.86%, and 70.97% on average in 30 min, respectively. The greatest contributors to the catalytic degradation were SO 4 •- , followed by 1 O 2 , •OH, and O 2 •- . EPFRs and 1 O 2 might be the main contributors to the free radical and non-free radical pathways. The enhancement of EPFRs following the N doping or S doping of biochar is the key factor underlying PMS activation. Therefore, changes in the structure of biochar can better activate PMS to produce reactive oxygen species-degrading antibiotics. The mineralization rate of antibiotics by BC, NBC, SBC, and NSBC was 42.12%, 47.06%, 44.99%, and 39.01%, respectively. This means that a small portion of the antibiotics was completely decomposed into CO 2 , H 2 O, and inorganic substances after degradation. Cyclic experiments showed that heteroatom-doped biochar had higher reusability, and the degradation rate decreased less than 15%.

研究领域: 环境科学 · 化学工程 · 材料科学
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