ENVIRONMENTAL TECHNOLOGY
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2022
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IF 3.475
Sheng Sheng,Jingjing Fu,Siyuan Song,Yuxuan He,Jin Qian,Ziyang Yi
The increasing use of fluoroquinolone antibiotics, which are found in various environmental media, is a constant threat to ecological safety and human health. In this paper, SrFeO3@MoS2 heterogeneous catalyst was prepared to activate peroxymonosulfate (PMS) for the degradation of levofloxacin (LVO). The characteristics of SrFeO3@MoS2 samples were studied and the optimum conditions for the removal of LVO by SrFeO3@MoS2/PMS system were investigated. The removal of LVO by the SrFeO3@MoS2-0.3/PMS system could reach 96.06% within 20 min of reaction. The effect of inorganic anions (SO42−, Cl−, NO3− and H2PO4−) commonly found in actual water bodies on catalytic reaction was explored. The reusability investigation revealed that the catalyst could still remove 88.06% of LVO within 20 min after four cycles. Moreover, SO4•−, •OH and 1O2 were identified by Electron Paramagnetic Resonance (EPR) tests and scavenger experiments, where the SO4•− and •OH were dominant reactive species. Combining with the XPS characterisation, the activation mechanism of SrFeO3@MoS2-0.3/PMS was proposed, and the oxygen vacancies and transition metals on the sample surface were active sites of PMS activation. Furthermore, the possible degradation pathways of LVO were well-established based on the detected intermediates.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Yin Li,Jiahui Hu,Yubin Zou,Lin Lin,Hebin Liang,Huaxin Lei,Bing Li,Xiao-yan Li
High-valent iron–oxo species (Fe V =O) generated through peroxide activation by Fe-based catalysts can realize the selective and efficient degradation of organic pollutants in water treatment. However, the rapid and efficient generation of Fe V =O for the selective degradation of pollutants over a wide pH range with high stability is challenging. In this study, a N, P, and S co-doped Fe-single atom (SA) catalyst (Fe SA -NPS@C) with FeN 4 active center was synthesized as a highly efficient catalyst for the peroxymonosulfate (PMS)-based oxidation. The Fe SA -NPS@C catalyst exhibited an excellent catalytic performance at low dosages of both the catalyst and PMS for the degradation of pollutants over a wide pH range with high stability. For the degradation of ofloxacin (OFX), the rate constant pertaining to PMS with Fe SA -NPS@C was 1.68 min −1 , considerably higher than those obtained using the N -doped and N and P co-doped Fe-SA catalysts. The degradation pathway of OFX revealed that the electrostatic effect was of significance in its degradation by Fe V N 4 =O with Fe V N 4 =O being the dominant reactive species. Density functional theory calculations revealed that the heteroatom doping effectively altered the electronic structure of the FeN 4 site of Fe SA -NPS@C, which strengthen its coordination with PMS, promote the electron transfer to PMS, and facilitate the interaction between Fe V N 4 = O and OFX, and thus significantly enhanced its catalytic activity. These findings provide new insights into the oxidation mechanism of Fe V =O in heterogeneous systems and the catalytic ability enhancement through heteroatom doping.
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Frontiers in Environmental Science
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2022
·
IF 5.411
Wang Qinghong,Ji Yuanyuan,Hu Jingze,Ye Huangfan,Liu Ya,Wang Yuxian,Chen Chunmao,Li Zhuoyu
Cerium oxides loaded silica catalysts were synthesized by an impregnation method by simply mixing Ce precursor with silica spherule (Ce/SS) and ordered MCM-41 zeolites (Ce/MCM-41), followed by a mild calcination. Compared with pure SS and MCM-41, Ce modified Ce/SS and Ce/MCM-41 demonstrate much improved catalytic ozonation activities for mineralization of recalcitrant nitrobenzene (NB). At solution pH of 6, 86 and 97% TOC mineralization rates were achieved within 60 min for Ce/MCM-41 and Ce/SS, respectively. Characterization results suggest that Ce loading significantly increases the surface Lewis acidic sites, which would synergize with Ce3+/Ce4+ redox cycle for the activity improvement. With the aid of in situ electron paramagnetic resonance (EPR) spectra and quenching tests, hydroxyl radical (·OH), superoxide radical (O2•–), and singlet oxygen (1O2) are identified as the O3 catalytic decomposition products, while ·OH mainly accounts for NB mineralization. The detailed degradation route of NB was further investigated by the multi-chromatography analysis. NB is firstly oxidized into polyhydroxy compounds, followed by small molecular organic acids, and finally being mineralized into CO2 and H2O. This study established a facile strategy to synthesize highly active and stable Ce/SiO2 catalysts for catalytic ozonation, and elucidated the in-depth mechanisms for the activity origins of the Ce loaded silica-based materials in catalytic ozonation processes (COP).
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
·
IF 9.136
Meng Xie,Mingya Yao,Shiyong Zhang,Lingshuai Kong,Lingxi Zhao,Jinhua Zhan,Ru-Song Zhao
Carbon-based single-atom cobalt catalysts exhibit high catalytic activity for the removal of novel pollutants in advanced oxidation processes. Here, atomically dispersed Co species with five-coordinated nitrogen atoms on carbon nanotubes (CNT) catalyst (Co-N 5 /CNT) was successfully fabricated via a low-temperature solvothermal reaction. The obtained Co-N 5 /CNT catalyst exhibited superior catalytic performance for PMS activation for sulfamerazine degradation. Its apparent rate constant k obs was 1.6 times higher than that of the Co-N 4 /CNT catalyst with four-coordinated nitrogen atoms prepared by the same method. Electron transfer non-radical mechanism was the main pathway for Co-N 5 /CNT to activate PMS. Higher single-atom cobalt metal loading (1.39 wt% vs 1.08 wt% in Co-N 4 /CNT) and significantly enhanced electron transfer ability (0.82 e vs 0.77 e in Co-N 4 /CNT) were the key factors for its superior catalytic performance. This work demonstrates a novel carbon-based single-atom cobalt catalyst for the removal of novel antibiotic contaminants by activating PMS in environmental catalysis applications.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
·
IF 6.371
Chaojie Lyu,Jiarun Cheng,Kaili Wu,Jiwen Wu,Ju Hao,Yuanyuan Chen,Huichao Wang,Yunguo Yang,Ning Wang,Woon-Ming Lau,Jinlong Zheng
Transition metal-based electrocatalysts are the promising candidates to substitute noble metal-based catalysts for water electrolysis, owing to its abundant earth reserves and inexpensive fabrication costs. Interface engineering and cation doping engineering are verified as the effective methods to improve the sluggish electrocatalytic performance of transition metal-based electrocatalysts. Here, we synthesized a self-supported heterostructure of Ce doped Co(OH) 2 nanosheets/CoP nanowires on the support of nickel foam (Ce-Co(OH) 2 /CoP/NF) by simple hydrothermal method , low-temperature phosphorization method. The Ce atom doping can lead to lattice distortion and abundant superficial defects on crystal surface, which will generate more active sites and faster charges transformation. The heterointerface between Ce-Co(OH) 2 and CoP also can lead to electronic structure modulation at interface domain, which not can induce much fresh active sites in this area, but can optimize the active sites to the optimal state for superior catalytic activity. Benefitting from these, it only needs the overpotentials of 253 and 56 mV to realize 10 mA/cm 2 for OER and HER under 1 M KOH solution, which is much enhance than single-phased samples. As the bifunctional electrocatalyst for two-electrode system, it merely requires 1.53 V to attain 10 mA/cm 2 in 1 M KOH, and it also exhibits outstanding overall water splitting performance in alkaline natural electrolyte, along with excellent catalytic long-time durability. In addition, the Ce-Co(OH) 2 /CoP/NF-based electrolyzer also could achieve energy-saving hydrogen production, and simultaneously oxidative degradation of organic materials or biomass upgrading at anode under lower voltages. This work paves a novel idea to fabricate high-efficient bifunctional electrocatalysts for energy-saving H 2 production.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Qirui Wang,Pengfei Xiao
Transition metal compounds are often used as activators in advanced oxidation processes for the treatment of refractory organics. However, the problems of inter-particle agglomeration, metal ion leaching and difficulty in recycling frequently occurred, resulting in reduced activation performance and secondary pollution. In this study, biochar (BC) was prepared from agricultural waste pine cone shells, and then a self-synthesized heterogeneous CuFe 2 O 4 -MoS 2 @BC composite was prepared for the first time, which can be used as an activator of peroxymonosulfate (PMS) for the oxidative degradation of tetracycline (TC). Analysis techniques such as XRD, SEM, BET, FT-IR, Raman, XPS, and VSM indicated that the heterogeneous catalyst with good surface properties and catalytic stability has been successfully prepared. When different concentrations of TC were treated with 0.5 g/L CuFe 2 O 4 -MoS 2 @BC and 1 mmol/L PMS, the highest degradation rate could reach 99.66 % after 60 min. Under the interference of pH, common anions and humic acid in the water environment, the degradation system can still achieve high degradation efficiency, showing excellent anti-interference ability and practical applicability. The analysis of activation mechanism reveals that the three redox ion pairs Cu + /Cu 2+ , Fe 2+ /Fe 3+ and Mo 4+ /Mo 6+ simultaneously participated in the activation of PMS, realizing multi-path electron transfer . And MoS 2 played an excellent co-catalysis role in promoting the cycling of the valence states of the ions. A total of 24 intermediate products was detected in the degradation process using LC-MS technology, and the possible degradation pathways for TC degradation were proposed. The self-synthesized CuFe 2 O 4 -MoS 2 @BC composite with high catalytic performance, stability, recyclability and low ion leaching rate has broad application prospects in the treatment of tetracycline antibiotic wastewater by activated PMS.
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BIOMASS & BIOENERGY
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2023
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IF 6
Jirui Yang,Yanwei Zhang,Feng Shen,Xinhua Qi
Meerwein-Ponndorf-Verley (MPV) reaction has been widely acknowledged to be a mild catalytic transfer hydrogenation method for selective reduction of biomass-derived furfural to furfuryl alcohol . Herein zirconium-containing mesoporous composite catalyst was developed through the combination of sol-gel process and soft templating method, in which naturally abundant glucose and F127 triblock copolymer were used as the ligand and pore-forming agent, respectively. The hydroxyl groups in glucose molecules were demonstrated to be coordinated with zirconium ion during hydrolysis-condensation of zirconium precursor, leading to the even dispersion of zirconia nanoparticles in the composite catalyst. The composite catalyst was proven to be highly efficient for catalyzing MPV reduction of furfural with the maximum furfuryl alcohol yield of 93.4% at 180 °C within 180 min in 2-propanol, which served as both solvent and reductant . The composite also showed a good reusability . After five consecutive reaction cycles, furfuryl alcohol yield was slightly reduced from 93.4% to 77.7%, but it could be recovered to 92.8% after the reused composite was regenerated with dilute alkali solution. Batch experiments and systematic characterizations demonstrated that the excellent catalytic performance of composite catalyst was determined by multiple factors mainly including the stronger Lewis acidity, a considerable amount of basic site and the rich mesoporous structure. This study provides a facile strategy to prepare multifunctional composite catalysts using naturally abundant carbohydrates as the feedstocks for lignocellulosic biorefinery .
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2023
·Vol. 30
·期 16
·48088-48106
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IF 5.8
Musajan Zulhumar,Xiao Pengfei
Herein, mesoporous carbon-anchored cobalt ferrite nanocomposites (nano-CoFe 2 O 4 @MC) were fabricated using a hydrothermal method for application as heterogeneous catalysts to activate peroxymonosulfate (PMS), in order to solve the problems of low activation performance and secondary pollution caused by the inter-particle agglomeration, metal ion leaching, and difficult recovery of nano metal catalysts. Analysis techniques such as SEM, TEM, XRD, BET, FTIR, VSM, TGA, and Raman spectroscopy indicated that the prepared nanocomposites have excellent surface properties, structural stability, and magnetic properties. The performance of nano-CoFe 2 O 4 @MC for Congo red (CR) degradation was evaluated by comparison with other treatment systems and study of the influence of experimental parameters, including the anchoring ratios, catalyst dosage, PMS concentration, initial pH, CR concentration, coexisting anions, and humic acid. Both radical and nonradical pathways were observed in the activation process of PMS by nano-CoFe 2 O 4 @MC. The analysis results of the element composition and ionic state of the catalyst show that the redox cycle of two ion pairs, Co 3+ /Co 2+ and Fe 2+ /Fe 3+ , could enhance the multipath electron transfer on the catalyst surface to promote the generation of reactive oxygen species. Identification of the intermediate products revealed CR was transformed into 12 intermediates through two branch pathways in the nano-CoFe 2 O 4 @MC/PMS system. After five cycles of use, the catalytic efficiency of the catalyst did not decrease significantly. Nanocomposites with high catalytic performance, stability, recyclability, and a low ion leaching rate have broad application prospects in the treatment of antibiotic wastewater.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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IF 5.2
Rui Zhou,Tong Wang,Fei Wang,Dongnian Zhang,Zhihong Hu,Huaizhu Li,Na Huang,Sa Ban,Chuncai Kong,Zhimao Yang,Xiaojun Jia,Hao Zhu
The citrate sol-gel method was used to synthesize LaNi 0.6 Co 0.4 O 3 anchored at ZnO (LaNi 0.6 Co 0.4 O 3 /ZnO) for activation of peroxymonosulfate to degrade ofloxacin in simulated wastewater. LaNi 0.6 Co 0.4 O 3 nanoparticles were uniformly and firmly dispersed on ZnO support during the synthesis process. LaNi 0.6 Co 0.4 O 3 /ZnO had a rapid catalytic rate with an efficiency of 90% in 10 min, which was higher than that of LaNi 0.6 Co 0.4 O 3 (87.7%). Meanwhile, LaNi 0.6 Co 0.4 O 3 /ZnO significantly inhibited metal ion leaching compared to LaNi 0.6 Co 0.4 O 3 (Ni leaching: 0.128 mg/L to 0.022 mg/L, Co leaching: 0.083 mg/L to 0.012 mg/L). The composite material maintained great cyclic stability with efficiency of 93% after 5 cycles. Based on electron paramagnetic resonance studies and the quenching experiments, SO 4 ·− 、 · OH、 · O 2 − and 1 O 2 were the main reactive oxygen species involved in the reaction. The degradation intermediates of ofloxacin were detected by ICP-MS to propose the possible degradation pathways. This work provides an insight for perovskite catalyst for the activation of PMS to treat pharmaceutical wastewater.
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Journal of Environmental Sciences
·
2023
·
IF 6.9
Xiuying Liu,Qianna Xia,Jiao Zhou,Bowen Li,Shuaiqi Zhao,Long Chen,Aimal Khan,Xiaoxia Li,Aihua Xu
The design of efficient heterogeneous catalysts in bicarbonate-activated hydrogen peroxide systems (BAP) is a hot topic in wastewater treatment. In this work, Cu 2 O nanoparticles with different morphologies including cubic shape (c-Cu 2 O), octahedron shape (o-Cu 2 O) and spherical shape (s-Cu 2 O), were applied in BAP for the first time to degrade tetracycline hydrochloride (TC). Compared with Cu 2+ ions and CuO, TC degradation was boosted in the presence of Cu 2 O in the BAP system, with the degradation rate following the order c-Cu 2 O > o-Cu 2 O > s-Cu 2 O. The morphology-dependent effects could be linearly correlated with the ratio of surface oxygen species (O S ), but not with the surface area or Cu(I) ratio. The c-Cu 2 O catalyst with exposure of (100) facets contained 76.6% O S as the active site for H 2 O 2 adsorption and activation, while the value was much lower for o-Cu 2 O and s-Cu 2 O with dominant (111) facets. The presence of HCO 3 − enhanced the interactions among Cu 2 O, H 2 O 2 and TC, leading to facile oxidation of Cu(I) to Cu(II) by H 2 O 2 , and the formation of various reactive species such as hydroxyl radicals and Cu(III) contributed to TC degradation. This work provides a new method for enhancing H 2 O 2 activation with heterogeneous catalysts by crystal facet engineering.
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2023
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IF 4.3
Shijie Wei,Hongcen Zheng,Jia-Jia Zhao,Shouyun Yu,Bingdang Wu,Guoyang Zhang,Shujuan Zhang
Self-sensitized degradation is a typical fate of azo dyes in aquatic systems but its kinetics is far too slow to meet the requirement for a thorough decolorization. Small diketones were found being able to enhance the degradation of dyes under UV irradiation and the introduction of an electron-denoting group at the α -position of the simplest β -diketone (acetylacetone, AA) had a further enhancement effect on the degradation. However, it is unclear whether such enhancement effects exist in the solar-irradiated systems. To clarify this question, the effects of three AA derivatives were investigated with Acid Orange 7 (AO7) as a representative azo dye. Compared with the AA derivatives with a methyl or an ethyl group at the central carbon (AA-CH 3 and AA-CH 2 CH 3 ), 3,5-diacetylheptane-2,6-dione (AA-CH 2 -AA, which is a condensed combination of AA and AA-CH 3 ) showed a >2-fold stronger enhancement effect. The nonstoichiometric enhancement effect of AA-CH 2 -AA on AO7 photodegradation disclosed a novel pathway for dye degradation: AA-CH 2 -AA could enhance the degradation of AO7 by reacting with the photo-sensitized 1 O 2 , whereas AA led to an inhibitory effect on the self-sensitized degradation of AO7 by quenching the excited state of the azo dye. These results demonstrate that small diketones could be designed to regulate the photodegradation of azo dyes in multiple pathways.
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Journal of Water Process Engineering
·
2023
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IF 7
Hao-Liang Jiang,Ming-Hui Li,Ling-Xi Zhao,Zhao-Xing Yan,Meng Xie,Jin-Ming Lin,Ru-Song Zhao
Flower-like Co Ni layered double oxide (LDO) was successfully synthesized and applied to activate peroxymonosulfate (PMS) to degrade tetracycline (TC). Co Ni LDO was rich in oxygen vacancies (O V ) and had a high specific surface area. 30 mg/L TC was 100 % degraded in 60 min under the condition of 0.1 g/L Co Ni LDO, 1.6 mM PMS, and unadjusted pH (5.45). A reaction mechanism dominated by O V was proposed in the TC removal system. Superoxide radical and singlet oxygen played major role in the reaction system, while sulfate radical and hydroxyl radical played minor role. The anti-interference ability of the Co Ni LDO/PMS system to anions was relatively strong. At the same time, Co Ni LDO showed high recovery efficiency. The degradation efficiency of TC was still higher than 92 % after five cycles. Through the detection of degradation intermediates, a possible degradation path was proposed. This study provided an efficient approach for TC degradation and provided a new clue for improving catalytic performance by introducing O V into the catalysts in PMS-based advanced oxidation processes systems.
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