APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Yue Yin,Ruolin Lv,Xiaoyang Li,Lu Lv,Weiming Zhang
Bimetallic Fenton catalyst has attracted widespread attention in refractory organics removal. Herein, we firstly investigated the influence of ZrO 2 structure features on H 2 O 2 activation in Zr-Fe bimetallic catalyst. The results show that the heterojunction structure will be formed after high temperature calcination , which makes the ability of Zr-Fe bimetallic catalyst to activate H 2 O 2 for bisphenol A degradation is 3.1 times higher than that of α-Fe 2 O 3 without Zr doping. Through characterization and density functional theory, it was identified that compared to (1 1 0) interface, the adsorption energy of H 2 O 2 on iron sites at (1 1 0)-(1 0 0) interface reduced by 1.27 kJ mol −1 , while the Fe–O bond length in the stable configuration of Fe-OOH increased by 0.16 Å, which was beneficial to the association and dissociation of H 2 O 2 on iron sites. Besides, the surface -OH of amorphous ZrO 2 in Zr-Fe bimetallic catalyst synthesized under low temperature conditions could promote HO 2 • /O 2 •- formation through the surface electron transfer, accelerating the Fe(III) reduction. In conclusion, this study reveals the influence of environment-friendly ZrO 2 structure features on H 2 O 2 activation, proposes a new insight into strengthening the synergistic effect between bimetals, and provides a reference for the structural optimization of bimetallic catalysts.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Biao Ma,Bin Li,Yang Li,Xiaobin Fan,Fengbao Zhang,Guoliang Zhang,Yuanzhi Zhu,Wenchao Peng
In this study, a facile atmospheric pressure chemical vapor deposition (CVD) method is used for the synthesis of nitrogen and sulfur co-doped hollow carbon sphere (NSC). Nano-CaCO 3 is used as template for the formation of hollow and highly hierarchical porous carbon structure. The doped percentages of N and S can be easily regulated by changing the ratio of N and S precursors and the deposition temperature. The obtained NSC is highly active for the catalytic oxidation of organic pollutants with peroxymonosulfate (PMS) as oxidant, and the reaction rate constant is 4.5 and 32.7 times faster than the single N or S doped samples, respectively. The PMS activation mechanism is comprehensively investigated by electron paramagnetic resonance (EPR) and radical quenching tests. Superoxide intermediate (O 2 •− ) and singlet oxygen ( 1 O 2 ) play the dominant role for phenol degradation. Moreover, with the introduction of secondary doped S atoms, more O 2 •− are generated for organics degradation. The excellent catalytic activity of NSC should be resulted from the optimized N and S doping percentages and large specific surface area (SSA). The synthesis strategy in this study provides a facile and low-cost synthetic method for heteroatom doped carbon materials and would expand the application of metal-free materials in the environmental remediation field.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Pijun Duan,Xinning Liu,Binhua Liu,Muhammad Akram,Yanwei Li,Jingwen Pan,Qinyan Yue,Baoyu Gao,Xing Xu
Effect of phosphate on pollutant removal was widely investigated in various peroxumonosulfate-based advanced oxidation processes (AOPs) but the role of phosphate was controversial. Many studies also used phosphate as buffer in PMS-based AOPs. This study shows that phosphate promoted PMS activation for pollutants removal. Therefore, PMS activation capacity of some strategies may be overestimated when conducted in the phosphate buffer. Importantly, the results of radical quenching tests, radical probes and reaction stoichiometries indicated that the yields of SO 4 − was elevated by the presence of phosphate and linearly depended on phosphate concentration, while the yields of OH remained constant. Density Functional Theory (DFT) calculation confirmed that PO 4 3− and HPO 4 2− could efficiently break O O bond of PMS, promoting the generation of SO 4 − for contaminants decomposition. These results illuminated the role of phosphate in AOPs utilizing PMS and uncovered the underlying mechanism of PMS activation by phosphate.
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CHEMOSPHERE
·
2021
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IF 7.086
Ran Ma,Sai Zhang,Xuewei Liu,Mingtai Sun,Jianzhong Cao,Jian Wang,Suhua Wang,Tao Wen,Xiangke Wang
Two-dimensional (2D) bismuth-based semiconductors have aroused intensive concern owing to their prominent photocatalytic activity for organic pollutants removal . In this work, a facile strategy for introducing oxygen vacancy in Bi-based oxyiodides (Bi x O y I z ) sheet-like architectures to activate molecular oxygen was proposed. The structure, photoelectric properties and visible light (λ > 420 nm) induced photocatalytic activities of these samples for decomposition of bisphenol A (BPA) were systematically characterized and evaluated. The as-prepared Bi 7 O 9 I 3 with a feeding Bi/I molar ratio of 1:1 exhibited the best photocatalytic activity comparable to those of similarly synthesized Bi 7 O 9 I 3 with other molar ratios and BiOIO 3 catalysts. The optimal Bi 7 O 9 I 3 achieved excellent photocatalytic activity with 99.6 % degradation efficiency of BPA within 20 min and superior structural stability with 95.1 % degradation retention over 5 cycling tests. In addition, the resulting Bi 7 O 9 I 3 sample displayed a high mineralization efficiency of BPA. Importantly, the plenty of oxygen vacancies (V o s) exsiting in Bi 7 O 9 I 3 played the dominant role in both accelerating electron transfer and activating molecular oxygen to facilitate the generation of superoxide radical (O 2 ·- ) and singlet oxygen ( 1 O 2 ), thereby proceeding oxidative degradation of BPA molecules during photoreactions. The efforts and attempts are also extendable to synthesis other 2D photocatalysts, providing potential for effective charge-carrier separation and molecular oxygen activation.
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Journal of Materials Chemistry A
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2021
·Vol. 9
·期 32
·17366-17379
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IF 12.732
Junjie Zhang,Wenran Gao,Yamei Yue,Wei Wang,Fatang Tan,Xinyun Wang,Xueliang Qiao,Po Keung Wong
Herein, biactive centers of Fe0-anchored graphitic N-rich graphene (Fe-GNG) were constructed via coordination and hydrogen bonding assemblies followed by calcination. The obtained Fe-GNG exhibited excellent peroxymonosulfate (PMS) activation ability to degrade diverse organic pollutants, accompanied by very low activation energy. Electron paramagnetic resonance and quenching experiments indicated that ˙OH and 1O2 were the predominant reactive species responsible for organics degradation, and were generated from PMS activation mainly at Fe0 and graphitic N sites, respectively. The degradation process had wide pH (2.2–10.3) and temperature (5–45 °C) application ranges, and a high tolerance to common matrix species, which enabled application to natural water systems. Furthermore, the magnetic Fe-GNG catalyst exhibited high stability and reusability, still degrading over 90% organics after five runs. This work provides a feasible strategy to construct multiple active sites for PMS activation, and clarifies the synergistic effect of metal and carbonaceous materials in radical and nonradical activation processes.
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ANALYTICA CHIMICA ACTA
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2021
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IF 6.558
Qi Zhou,Yuanyuan Zhang,Ting Zeng,Qijin Wan,Nianjun Yang
The morphology of nanomaterials affects their properties and further their applications. Herein, CuO nanomaterials with different morphologies are synthesized, including CuO nanostrips, nanowires and microspheres . After their characterization by means of electron microscopy and X-ray powder diffraction, these CuO nanomaterials are further mixed with graphene nanoplates (GNP) to explore their performance towards electrochemical detection of glucose and tetrabromobisphenol A (TBBPA). Among three composites, the composite of CuO nanostrips and GNP exhibits the largest active surface area, the lowest charge transfer resistance, and the highest accumulation efficiency toward TBBPA. Meanwhile, this composite based non-enzymatic sensor shows superior performance for the glucose monitoring. Since these sensors for the monitoring of both glucose and TBBPA possesses long-term stability, high reproducibility, and wide linear ranges and low detection limits, this work provides a strategy to tune the sensing performance of nanomaterials by means of tailoring the morphologies of nanomaterials.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Xiaohui Fan,Heng Lin,Jinjin Zhao,Yican Mao,Jiaxing Zhang,Hui Zhang
Activation of peroxymonosulfate (PMS) for organic-contaminated water remediation is a promising strategy. In this study, a sludge-derived biochar (SBC) was prepared as an efficient and low-cost metal-free catalyst to activate PMS for the abatement of bisphenol A (BPA) in water. The results demonstrate that BPA could be rapidly oxidized by the combination of SBC and PMS. Compared with the slight adsorption (8.1%) by SBC alone and limited direct oxidation (2.4%) by sole PMS, the removal efficiency of BPA was boosted to 94.5% within 60 min in the presence of both SBC and PMS. Active species participating in the rapid elimination of BPA were investigated via both chemical quenching experiment and electron paramagnetic resonance (EPR) technique. The results indicate that non-radical rather than radical process plays an important role in BPA abatement in the SBC/PMS system. The electron-transfer non-radical process was further verified by the open circuit potential test. It is proposed that PMS is bound to SBC to form a surface reactive complex (SBC-PMS*), which would abstract the electrons from the adsorbed BPA through the conductive carbon tunnel. The present work provides an alternative of controlling waste by waste.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Chuanyi Guo,Chaofa Chen,Jiaying Lu,Du Fu,Cheng-Zong Yuan,Xi-Lin Wu,Kwun Nam Hui,Jianrong Chen
Stable and recyclable catalysts are crucial to the peroxymonosulfate (PMS) based advanced oxidation process (AOPs) for wastewater treatment . Herein, nitrogen-rich carbon wrapped Fe 3 C (Fe 3 C@CN) on carbon felt (CF) substrate was synthesized by using Prussian blue (PB) loaded CF as the precursors. The obtained Fe 3 C@CN/CF catalyst was applied for degradation of bisphenol A (BPA) via the heterogeneous catalytic activation of PMS. Results showed that ~91.7%, 95.2%, 98.1% and 99.1% of BPA (20 mg/L) were eliminated in the Fe 3 C@CN/CF + PMS system within 4, 10, 20 and 30 min, respectively. The fast degradation kinetics is attributed to the production of abundant reactive species ( OH, SO 4 − and 1 O 2 ) in the Fe 3 C@CN/CF + PMS system, as demonstrated by the electron paramagnetic resonance spectroscopy and quench experiments. The Fe 3 C@CN/CF catalyst was stable and can be easily recycled by using an external magnet. The results indicated that the nanoconfined Fe 3 C endowed Fe 3 C@CN/CF with high stability and magnetic property and enabled the efficient electron transfer for PMS activation. This study provides a cost-effective approach for the fabrication of stable and recyclable Fe 3 C@CN/CF catalyst, and shed a new light on the rational design of multifunctional catalyst for advanced water remediation.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Wei Miao,Ying Liu,Dandan Wang,Ningjie Du,Ziwei Ye,Yang Hou,Shun Mao,Kostya (Ken) Ostrikov
Transition-metal and nitrogen co-doped carbon-based catalysts receive much attention in peroxymonosulfate (PMS) activation. However, the contribution of doped metal and the kinetic mechanisms of the emerging nonradical pathways especially enabled by reactive singlet oxygen species remain unclear. Herein, we report Fe-N-co-doped carbon-based catalysts (FeCNx) for peroxymonosulfate activation. The catalysts achieve fast removal of a broad spectrum of organic pollutants in a wide pH range without the common Fe leaching. Both catalyst surface-activated PMS complex (catalyst-PMS*), surface-bound radicals, and singlet oxygen are identified. The new mechanism is enabled by the Fe-Nx single-atomic-site that enhances the adsorption of PMS and facilitates the formation of catalyst-PMS*. The formation route of singlet oxygen species is elucidated for the first time for Fe, N-co-doped carbon-based catalysts with density functional theory simulation. This study reveals the intrinsic role of Fe-Nx site in catalysts and provides new insights into the origin and kinetics of non-radical pathways for peroxymonosulfate activation.
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Journal of Environmental Chemical Engineering
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2021
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IF 5.909
Latif Abdul,Xiongyuan Si,Kai Sun,Youbin Si
In the current study, bisphenol A (BPA) removal in water environment by carbonate-activated peroxymonosulfate (CO 3 2- /PMS) oxidation process is reported for the first time. The CO 3 2- /PMS system showed excellent catalytic activity by degrading 100% BPA within 40 min reaction time. BPA degradation showed pseudo-first-order kinetics with rate constant ( k ) value of 0.0918 min −1 . The effects of initial concentration of CO 3 2- , PMS, BPA, pH, and inorganic anions, including nitrate (NO 3 - ), sulfate (SO 4 2- ), chloride (Cl - ), phosphate (PO 4 - ), and humic acid (HA) were studied. The addition of NO 3 - , SO 4 2- , and PO 4 - in the CO 3 2- /PMS system decreased BPA degradation %, whereas a high concentration of Cl − and HA addition promoted BPA degradation %. Electron paramagnetic resonance and radical scavenging experiments verified that both the SO 4 •– and HO • were generated in the CO 3 2- /PMS system. According to liquid chromatography-mass spectrometry results, the possible degradation pathways for BPA were suggested. Toxicity experiments revealed that BPA metabolites were not toxic. It could be concluded that the CO 3 2- /PMS system is a promising process for removing BPA in different types of water (ultrapure, lake, and wastewater)
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CHEMOSPHERE
·
2021
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IF 7.086
Jiaxin Mu,Shangyi Li,Jing Wang,Xukai Li,Weirui Chen,Xinyuan Tong,Yiming Tang,Laisheng Li
Herein, we demonstrated the construction of three-dimensional (3D) cerium oxide (CeO x )/SBA-16 nanocomposites for efficient removal of bisphenol A (BPA) via a catalytic ozonation , with a high BPA mineralization up to 60.9% in 90 min. On one hand, the CeO x /SBA-16 mesoporous structured materials presented large surface area and uniform pore distribution, which was conducive to the adsorption of transformation by-products (TBPs) and then, the mass transfer. On the other hand, CeO x /SBA-16 could enhance the ozone utilization efficiency and meanwhile facilitate the formation of OH, the main reactive oxygen species . Through the exploration of dissoluble organic matters and the identification of the reaction intermediates, two BPA degradation pathways were proposed. This approach reported here will benefit the design and construction of mesoporous structured materials for catalytic elimination of hazards to remediate the environment.
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ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
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2021
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IF 6.291
Guomin Geng,Yanhui Gao,Zhitong Zhang,Kangqi Gao,Wenyu Zhang,Jianjun Song
Developing monolithic carbon-based catalyst with low cost, easy separation and high performance to degrade pollutants via PMS activation is crucial. In this work, a series of novel monolithic Me-CA catalysts based on biomass derived carbon aerogel were prepared by hydrothermal method using waste watermelon peel as raw material. Co-CA catalyst showed excellent performance to activate PMS for 2, 4-DCP degradation in different temperature and different water matrices. Different pollutants, such as ciprofloxacin (CIP), bisphenol A (BPA), and 2, 4-dichlorophenoxyacetic acid (2, 4-D) could also be removed in the Co-CA/PMS system. As expected, Co-CA could be easily separated from degraded solution, and show high stability and reusability for PMS activation with a lower cobalt leaching. Based on the results of the quenching tests, electron paramagnetic resonance (EPR) spectra, Chronoamperometric test (i-t curves) and electro-chemical impedance spectroscopy (EIS), the PMS activation mechanism was proposed. The phytotoxicity assessment determined by germination situation of mung bean indicated that PMS activation could eliminate the hazards of 2, 4-D. Therefore, this study provides a low cost, efficient and environmental-friendly monolithic biomass carbon aerogel catalyst for different pollutants degradation , which further advances monolithic catalyst for practical wastewater treatment .
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