Environmental Science-Nano
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2022
·Vol. 9
·期 3
·1091-1105
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IF 9.473
Heng Shi,Yi He,Yubin Li,Teng He,Pingya Luo
Metal–organic frameworks (MOFs) for persulfate-based Fenton-like processes have attracted tremendous attention nowadays. However, the low utilization of active sites and poor stability of MOFs still impede their practical application. In this work, we demonstrate a unique photo Fenton-like catalyst with confined ultrasmall MOF nanoparticles anchored on a 3D-graphene network, which is fabricated through a simple confined thermal pulverization method. The ultrasmall Co–Fe MOF nanoparticles with confined structure endowed this catalyst with highly exposed active sites as well as excellent stability. It can maintain high degradation efficiency via visible light-assisted peroxymonosulfate (PMS) activation in a broad pH range from 1–13. Electron spin resonance (ESR) technology reveals that both radical and nonradical processes are involved in this process, and the broad pH adaptability of this system is due to the stable generation of ˙OH, SO4˙−, ˙O2−, and 1O2 under these pH conditions. This study provides new perspectives for the development of highly efficient and harsh environment-adaptive MOF-based Fenton-like catalysts.
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高影响因子
ENVIRONMENTAL RESEARCH
·
2022
·
IF 8.431
Yanqing Cong,Jiaxin Yi,Shengna Liang,Feng Zhang,Yi Zhang,Shi-Wen Lv
Bimetallic oxides with spinel structure show great prospects in the photocatalysis owing to many active sites. Herein, a novel 500NiCo 2 O 4 @CdS–5%Ag composite was fabricated via a feasible strategy. Interestingly, the combination with NiCo 2 O 4 could significantly enhance the absorption ability of CdS for visible light. Benefiting from the formation of heterojunction structure between NiCo 2 O 4 and CdS, the recombination of photogenerated electrons and holes was remarkably restrained. As an effective mediator, deposition of Ag could further promote the transfer of photogenerated charge carriers, thereby accelerating the reaction rate. Meanwhile, light absorption capacity of composite was also improved, owing to the surface plasmon resonance effect of metallic Ag. More importantly, 500NiCo 2 O 4 @CdS–5%Ag composite with great stability displayed an excellent performance in the photocatalytic degradation of OFX, and its highest removal efficiency was as high as 99.14%. Possible degradation pathways of OFX were given, and most of OFX could be degraded into CO 2 , H 2 O and other by-products with no toxicity. Significantly, the separation and transfer of photogenerated charge carriers followed indirect Z-scheme heterojunction mechanism. The O 2 − , OH and 1 O 2 were main active species in photocatalytic reaction system. All in all, current work inspired some new ideas for designing novel photocatalytic system in wastewater treatment .
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Kai Li,Shengjun Xu,Xiaobiao Liu,Huiji Li,Sihui Zhan,Shuanglong Ma,Yan Huang,Shiliang Liu,Xuliang Zhuang
A family of graphene-based activators including reduced graphene oxide (RGO), nitrogen doped reduced graphene oxide (NRGO), zero-valent manganese loaded reduced graphene oxide (Mn-RGO) and zero-valent manganese loaded N-doped reduced graphene oxide (Mn-NRGO) were fabricated to activate peroxymonosulfate (PMS) for bisphenol A (BPA) degradation. A significant synergistic effect between loaded manganese nano-particles (Mn-NPs) and doped N was revealed by comparing the apparent reaction rate constants with about 12.4, 7.6 and 10.5-folds enhancement when compared Mn-NRGO with RGO, NRGO, Mn-RGO, respectively. By integrating the results of chemical scavenger experiment, electron paramagnetic resonance test, galvanic oxidation process, PMS stoichiometric efficiency, linear sweep voltammetry and in-situ Raman spectrum, a predominant outer-sphere catalyst-PMS complexes mediated electron transfer pathway was uncovered. Based on kinetic studies, the specific contribution of synergistic effect was quantified to be at least 70%. The calculated Fermi level advanced by 0.03 eV in Mn-NG compared with that in NG, demonstrating that Mn-NG is more liable to donate electrons to PMS. The E ads and l O-O results pointed out that synergistic effect between Mn-NPs and doped N relied on the intimate affinity between Mn-NPs and HSO 5 – which triggered more uneven distribution of charge on the whole carbon sheets, and more adsorption of HSO 5 – on carbon framework. These newly created adsorption consequently reinforcing the formation of catalyst-PMS complexes and the elevation of mediated electron transfer pathway. Overall, this study firstly provides a comprehensive and definite insight of the synergistic effect between loaded Mn-NPs and doped-N on carbon materials for promoting PMS activation to degrade organics.
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Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Xingyan Chen,Lifen Liu
In advanced oxidation processes (AOPs), organic pollutants are oxidized, but getting the most energy out of pollutant in reducing cost of AOPs is still a challenge. In this study, MoS 2 / Co 0.75 Mo 3 S 3.75 composite nano-catalyst with high density catalytic active sites was synthesized by homogeneous and dispersed doping of single Co atoms in MoS 2 by one-step hydrothermal method. The prepared catalyst was coated on stainless steel with silica sol for electrode application under visible light and activation of PMS (peroxymonosulfate) in Photocatalytic fuel cell (PFC) system. The synergy system at pH 6.5, visible light irradiation and 0.06 mM [PMS], was able to rapidly degrade RhB (50 mg·L −1 ) within 10 min and reach 98% degradation within 21 min (kinetic rate constant 0.261 min −1 ). The role of visible light contributes to RhB degradation more than oxidation by just PMS in PFC (Photocatalytic Fuel Cell). The dispersed Co sites have a significant effect of activating PMS, improving catalytic activity and enhancing reaction under closed circuit. The system has good stability, is also applicable to significant removal of tetracycline(TC, 76.35%) and bisphenol A (BPA, 53.76%). In MoS 2 / Co 0.75 Mo 3 S 3.75 -vis/PMS/PFC, species such as •OH, SO 4 •− , O 2 •− , h + and 1 O 2 jointly promote the degradation of RhB. This work provides a perspective for further study of two-dimensional metallic sulfide doped with transition metal ions and application of such vis/PMS/PFC system in removing other toxic pollutants .
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 29
·期 29
·44732-44745
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IF 5.19
Wang Zhijie,Bao Jianguo,Du Jiangkun,Luo Liting,Xiao Guangfeng,Zhou Ting
Pollutant degradation via periodate ( \({\text{IO}}_{4}^{-}\) ) and transitional metal oxides provides an economical, energy-efficient way for chemical oxidation process in environmental remediation. However, catalytic activation of periodate by manganese dioxide and the associated mechanism were barely investigated. In this study, four MnO 2 polymorphs (α-, β-, γ- and δ-MnO 2 ) were synthesized and tested to activate \({\text{IO}}_{4}^{-}\) for the degradation of sulfamethoxazole (SMX). The reactivity of different MnO 2 structures followed the order of α-MnO 2 > β-MnO 2 > γ-MnO 2 > δ-MnO 2 , suggesting that the particular crystalline structure in α-MnO 2 would exhibit higher activities via \({\text{IO}}_{4}^{-}\) activation. Herein, in α-MnO 2 / \({\text{IO}}_{4}^{-}\) system, 91.1% of SMX was eliminated within 30 min with degradation rate constant of 0.0649 min −1 , and the neutral pH exhibited higher efficiency in SMX degradation compared with acidic and alkaline conditions. Singlet oxygen ( 1 O 2 ) was unveiled to be the dominant ROS according to the results of electron paramagnetic resonance, chemical probes and radical quenching experiments, whereas \({\mathrm{O}}_{2}^{\bullet -}\) and • OH were mainly acted as a free-radical precursor. Six oxidation products were identified by LC–MS, and the elimination of sulfonamide bond, hydroxylation and direct oxidation were found to be the important oxidation pathways. The study dedicates to the mechanistic study into periodate activation over alpha-MnO 2 and provides a novel catalytic activation for selective removal in aqueous contaminants.
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Journal of Water Process Engineering
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2022
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IF 7.34
Yanzhuo Zhang,Shengxu Liang,Rui He,Jing Zhao,Jinghua Lv,Wei Kang,Jian Zhang
Antibiotics in the water environment pose harm to animals, plants, and humans. In this study, biochar doped with sulfur (S), nitrogen (N), and NS was used to adsorb and activate peroxymonosulfate (PMS) to degrade the antibiotics chlortetracycline, ofloxacin, and sulfadiazine in an aqueous solution. The adsorption capacity of the biochar doped with single atoms increased significantly, and the maximum saturated adsorption capacities of undoped, N-doped, S-doped, and NS-doped biochar were 40.7, 85.5, 63.3, and 40.7 mg/g, respectively. The increase in specific surface area and the number of functional groups was the main cause for the increase in the adsorption capacity of heteroatom-doped biochar. The antibiotic degradation process involved the use of biochar to activate PMS and produce reactive oxygen species (ROS) for complete removal. The concentration of environmentally persistent free radicals (EPFRs) increased in response to heteroatom-doped biochar, and the type of EPFRs changed, which enhanced the ability of biochar to degrade antibiotics. At the 500 °C preparation temperature, the degradation rates of antibiotics by the undoped, N-doped, S-doped, and NS-doped biochar were 73.83%, 84.32%, 79.60%, and 74.10%, respectively, whereas the degradation rates at 900 °C were 82.38%, 93.78%, 91.11%, and 81.55%, respectively. The sulfate radical was produced during the activation process and made the largest relative ROS contribution to the increased adsorption capacity, followed by singlet oxygen, hydroxyl radical , and superoxide radical. Recycling experiments confirmed that the heteroatom-doped biochar was highly reusable and that the removal rates of N-doped biochar and S-doped biochar were high (81.94% and 78.06%, respectively).
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CATALYSIS LETTERS
·
2022
·Vol. 152
·期 12
·3537-3547
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IF 2.936
Liu Zonghui,Zhang Zhongze,Wen Zhe,Xue Bing
Development of simple and high performance solid catalysts for the utilization of biomass has become an important research topic in heterogeneous catalysis and sustainable chemistry. Herein, a highly efficient catalytic system was studied for the catalytic transfer hydrogenation of furfural to high value furfuryl alcohol over a series of acidic or basic oxides catalysts. Among those oxides, acidic Al 2 O 3 is identified as the most effective for FAL production, giving a FUR conversion as high as 40% (FUR consumption rate was 186 mmol g cat −1 h −1 ) and FAL selectivity of 99% after only 5 min at 150 °C using 2-propanol as the H-donor and solvent. Furthermore, the as prepared Al 2 O 3 give an Ea value of 15.2 kJ/mol, which is much lower than other complex catalysts in the literatures. Correlating the catalyst performance with its physical and chemical properties uncovers that the large specific surface area and high acidity of Al 2 O 3 would be the key to the catalyst performance. Graphical Abstract
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高影响因子
CHEMOSPHERE
·
2022
·
IF 8.943
Zhuyu Sun,Dan Geng,Xiuling Wu,Luxiang Zhu,Jin Wen,Le Wang,Xiaoxiang Zhao
As an emerging class of organic contaminants , polyhalogenated carbazoles (PHCZs) have been increasingly detected all over the world since 1980s. Due to the environmental persistence, bioaccumulation, and dioxin-like toxicity, PHCZs have aroused widespread concerns in recent years. However, efficient approach for the degradation of PHCZs is quite limited so far. Therefore, in this study, an advanced oxidation process (AOP), sulfidated zero-valent iron/peroxymonosulfate (S-ZVI/PMS) system was used to degrade 3-chlorocarbazole (3-CCZ), which is one of the mostly detected PHCZs congeners. The degradation of 3-CCZ was systematically studied under different conditions by varying the molar ratio of S/Fe, the dosage of S-ZVI or PMS, pH and temperature. The results indicated that S-ZVI/PMS was an effective strategy for PHCZs treatment. The 20-min degradation efficiency of 3-CZZ was up to 96.6% with the pseudo-first-order rate constant of 0.168 min −1 under the conditions of 5 mg/L 3-CZZ, 0.3 g/L S-ZVI (S/Fe = 0.2), 1.0 mM PMS, pH 5.8 and 25 °C. HCO 3 − , Cl − and humic acid (HA) showed inhibitory effects to different degrees. Results of the electron paramagnetic resonance (EPR) and scavenging experiments clarified the dominant role of •OH, followed by 1 O 2 and SO 4 •─ . The product analysis and DFT calculation revealed three degradation pathways of 3-CCZ, namely hydroxylation, dechlorination and C–N bond cleavage, which largely alleviated the toxicity of the parent compound. This study showed the effectiveness of S-ZVI/PMS system in PHCZs treatment and provided a comprehensive investigation on the degradation behaviors of PHCZs in AOPs.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 29
·期 27
·40734-40744
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IF 5.19
Zhu Bo,Xu Jiangyan,Xu Zhihui,Wu Meisheng,Jiang Hongmei
A facile soft-template solvent thermal strategy was developed to prepare mesoporous carbon–silica composite (MMCS) by using furfuryl alcohol (FA) as carbon precursor, Pluronic copolymer P123 as template, hydrated iron nitrate as iron source, and teraethylorthosilicate as silicon source and it was applied for the removal of methyl orange (MO). The as-synthesized MMCS with abound of hydrophilic groups processed a high specific surface area, large pore volume, and good magnetic response. With the increased amount of FA, the surface area and functional groups increased, promoting the adsorption effect. The maximum adsorption capacity of MO on MMCS can be high to 113.1 mg g −1 at pH 4 with 150 mg L −1 initial MO concentration. The adsorption isotherm, kinetic, and thermodynamics were all studied and the results showed the adsorption process well fitted Langmuir adsorption isotherm and pseudo-second-order model. Additionally, it was shown that the adsorption process could not be interfered by the co-existence of PO 4 3− , NO 3 − , CO 3 2− , SO 4 2− , and real water matrix. And the proposed adsorbent can remove MO in three practical water samples with satisfied removal rates ranging from 92.8 to 99.8%. Thus, the MMCS prepared in this study could be utilized as an alternative adsorbent for the removal of methyl orange from practical aqueous solution.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Yu Li,Jiemin Chen,Jie Zhong,Bin Yang,Zequn Yang,Kaimin Shih,Yong Feng
The use of cocatalyst in Fenton-like reactions has been demonstrated as a reliable approach to improve their efficiency via accelerating the circulation of Fe 3+ /Fe 2+ . In this study, we for the first time used natural pyrite (FeS 2 ) as a Fenton-like cocatalyst to improve the reactivity of Fe 3+ instead of the widely investigated molybdenum disulfide that releases potential harmful molybdenum ions. The presence of FeS 2 significantly improved the degradation of sulfamethoxazole (SMX) by Fe 3+ -peroxymonosulfate (PMS); near complete removal of SMX by FeS 2 -Fe 3+ -PMS was achieved, while no obvious removal of SMX by Fe 3+ -PMS was noticed. Meanwhile, the surface area-normalized rate constant of SMX degradation by FeS 2 -Fe 3+ -PMS was more than 18 times higher than that by MoS 2 -Fe 3+ -PMS. FeS 2 -Fe 3+ -PMS worked effectively in a wide range of pH values from 3.0 to 10.0. Although hydroxyl radicals, sulfate radicals, superoxide anion radicals, and singlet oxygen were recorded by electron paramagnetic resonance spectroscopy, only sulfate radicals were mainly responsible for the degradation. Sulfide ions were identified as one of the intermediates, but the reactive species generated by their interaction with PMS did not contribute to the degradation. FeS 2 had a good stability by continually accelerating the circulation of Fe 3+ /Fe 2+ . The findings from this study reveal a highly efficient cocatalyst for Fenton-like reactions.
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高影响因子
ENVIRONMENTAL RESEARCH
·
2022
·
IF 8.431
Yong Cheng,Han-Qing Zhao,Aqiang Ding,Fei Chen,Jun Liu,Dazhi Fang,Chenglong Li,Yongkui Huang,Peili Lu
The widespread application of quaternary ammonium compounds (QAC) has posed a serious hazard to the environment and human being, and high concentration of Cl − in QAC wastewater may further increase the difficulty of pollutants elimination . In this study, such a QAC wastewater under high salinity conditions was chosen as the target, the prepared Ti/(Ru x Ir y )O 2 anode exhibited favorable catalytic performance for the oxidation and mineralization of QAC under high salinity conditions. Increasing the Ru/Ir ratio of Ti-based electrode coating also slightly promoted the inner catalytic capacity. The combination of electron paramagnetic resonance (EPR) and quenching experiments indicates that 1 O 2 served as a main reactive specie in the Ti/(Ru x Ir y )O 2 electrooxidation system. The increase of pH could decrease the removal efficiency of QAC for the reduced 1 O 2 yield, and the rise of Cl − concentration could favor the QAC oxidation, and Cl − was a better electrolyte to promote the oxidation of organic contaminants when compared to Na 2 SO 4 or Na 2 CO 3 . Additionally, the conversion pathway of the model pollutant was tentatively investigated, the results demonstrated that there were almost no halogenated final products residual by electrocatalytic oxidation with Ti/(Ru x Ir y )O 2 anode. This study not only elucidate the reaction mechanism of Ti/(Ru x Ir y )O 2 anode electrocatalytic oxidation of high salinity QAC wastewater, but also may provide an efficacious and eco-friendly method for the treatment of high salinity QAC wastewater.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Linjie Wang,Qing Jin,Youlin Xiang,Lu Gan,Lijie Xu,Ying Wu,Xingyu Fang,Haiqin Lu,Shuguang Han,Juqing Cui
Spinel structured Co x Mn 3-x O 4 nanoparticles embedded carbon composites (Co x Mn 3-x O 4 -C) were rationally designed and prepared using Co/Mn bimetallic metal organic frameworks (MOFs) as the template. The Co x Mn 3-x O 4 -C represented prominent bisphenol A (BPA) degradation capability by activating peroxymonosulfate (PMS), in which Co 1.5 Mn 1.5 O 4 -C exhibited the highest BPA degradation efficiency. Specifically, Co 1.5 Mn 1.5 O 4 -C (0.1 g/L) could completely degrade 0.1 mM of BPA within 3 min, which was better than many previous reported catalysts. Moreover, the Co 2+ leaching was limited in the Co 1.5 Mn 1.5 O 4 -C/PMS system. It was revealed that hydroxyl radical (•OH) and singlet oxygen ( 1 O 2 ) were the main active species in the reaction system, which dominated a dual pathway mechanism for BPA degradation. Furthermore, the Co 1.5 Mn 1.5 O 4 -C could maintain its performance in a variety of water matrices with promising recyclability. This study encourages the rational design and preparation of high-efficient catalysts by employing tunable MOFs precursors for refractory organic pollutant degradation.
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高影响因子
危险品化学品经营许可证（带存储）