APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Yuxuan He,Jin Qian,Peifang Wang,Taiping Xie,Dionysios D. Dionysiou,Bianhe Lu,Sijing Tang
Advanced strategies for enhancing catalytic performance of catalysts include multi-metal active site exposure, vacancy growth and electronic structure optimization. Here, carbon nanotube-loaded CoSe 2 /FeSe 2 catalysts (Co/Fe-CNT) with multiphase boundaries and embedded selenium vacancies (V Se ) were prepared using a one-step hydrothermal method. The catalysts feature unique electronic structures and abundant active sites, and were found to exhibit unexpectedly high activity and stability in photocatalytic mediated sulphate radical (SR-photo) system, with impressive oxidation capacity for complex matrix polluted water. The spontaneously formed internal electric field strongly promoted charge transport and significantly enhanced the photocatalytic property. The V Se formed at the heterogeneous interface could modulate the surface electronic structure and accelerate the redox cycling of transition metals, thereby accelerating the production of reactive oxygen species and boosting the efficiency of contaminant degradation. This work provides guidance for the design of high-performance catalysts for V Se engineering and expands their potential for application in wastewater purification.
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WATER RESEARCH
·
2023
·
IF 12.8
Peng Xu,Rui Wei,Peng Wang,Xiang Li,Chunyan Yang,Tianyao Shen,Tong Zheng,Guangshan Zhang
Peroxymonosulfate (PMS) activation is a promising technology for water purification, but the removal performance of multiple pollutant matrices and the mechanism for reactive species transformation in the heterogeneous catalytic system remain ambiguous. Herein, a novel CuFe 2 O 4 /diatomite was fabricated for PMS activation to achieve efficient removal of typical pesticides. Uniform distribution of CuFe 2 O 4 on diatomite efficiently alleviated the agglomeration of CuFe 2 O 4 and increased specific surface area (57.20 m 2 g − 1 , 3.8-fold larger than CuFe 2 O 4 ). CuFe 2 O 4 /5% diatomite (5-CFD)/PMS system showed nearly 100% removal efficiency for mixed pesticide solution within 10 min (0.10 g L − 1 5-CFD and 0.40 g L − 1 PMS) and excellent anti-interference performance towards various coexisting substances (≥90% removal efficiency). The electrochemical measurements confirmed that the lower charge transfer resistance of 5-CFD significantly enhanced the electron-transfer capacity between 5-CFD and PMS, accelerating the reactions among Fe(III)/ Fe(II), Cu(II)/ Cu(I), and PMS, further generating •OH (261.3 μM), 1 O 2 (138.8 μM), SO 4 •– (11.8 μM), and O 2 •– . The O in reactive oxygen species didn't originate from dissolved oxygen (DO) but PMS, independent of the low solubility of DO and slow diffusion rate of O 2 in water. Furthermore, the production of 1 O 2 went through the process: PMS → O 2 •– → 1 O 2 , and SO 4 •– could rapidly convert into •OH. The degradation pathways and the evolution of intermediates were proposed by HPLC-QTOF-MS/MS and DFT calculations. QSAR analysis illustrated that the toxicity became lower with the reaction process. This study provides novel insights into the mechanism for pesticide degradation and active species transformation and the anti-interference capability of systems.
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Journal of Cleaner Production
·
2023
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IF 11.1
Tong Wen,Yunliang Zhao,Licai Chen,Yanhui Miao,Zixuan Zhang,Shaoxian Song,Tingting Zhang
The model of efficient, clean, and cheap collaborative governance has received considerable attention in the treatment of pollution such as wastewater and solid waste. The “waste control by waste” strategy is proposed and put into practice in this work, that is, the ferrosilicon from waste carbide slag is utilized for treating dyes wastewater via the advanced oxidation process (AOP) of ferrosilicon/PMS/light. The main component of ferrosilicon is FeSi and Fe 5 Si 3 , which are riched in Fe element and suitable for inducing the AOP reaction. When the ferrosilicon is used in the AOP system, 20 mg L −1 MB can be completely decolorized within 45 min. The excellent performance of the ferrosilicon/PMS/light system is also observed in various wastewater conditions such as solution pH (3–9) and dye types (MB, MO, MG , and CR), which is superior to common PMS/light and other reported system. In addition, the ferrosilicon catalyst can keep the MB removal at nearly 100% in five cycles, and the proportion of its leached iron is always less than 1%, which effectively solves the performance degradation and leaching loss of commonly used zero-valent iron (ZVI) catalyst. In the ferrosilicon/PMS/light system, the SO 4 ● ˉ and 1 O 2 radicals act as the main active species and their production is due to the redox of iron elements and the self-decomposition of PMS , respectively. Overall, this research progress provides a valuable reference for clean and cheap environmental governance.
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
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IF 13.6
Wen Song,Xinyu Xiao,Guanlong Wang,Xiaoli Dong,Xiufang Zhang
Supporting Fe catalysts on N doped carbon (Fe-N-C) renders a promising way towards peroxymonosulfate (PMS) activation for water decontamination , but constructing high-efficiency Fe-N-C remains challenging due to the insufficient understanding of the structure-performance relationship. Herein, the N doped carbon nanotube supported Fe catalysts (Fe-NCNT) were prepared towards PMS activation for organic pollutants removal, in which the Fe-N coordination number and Fe species were tuned through changing the pyrolysis temperature to study their roles in PMS activation. Results showed increasing the pyrolysis temperature converted the Fe-N 4 structure in Fe-NCNT to low-coordinated Fe-N 3 structure and produced Fe nanoparticles (FeNP, encapsulated in carbon). The Fe-NCNT with Fe-N 3 and FeNP exhibited a remarkably high specific activity (0.119 L min −1 m −2 ), which was 1.8 times higher than that of Fe-NCNT with only Fe-N 4 and obviously outperformed those of the state-of-the-art PMS activators. The low-coordinated structure and FeNP promoted the PMS reduction on Fe 2+ of Fe-N x for •OH and SO 4 •− production, which served as major oxidants for pollutants degradation . The experimental results and theoretical calculation corroborated the low-coordinated structure and FeNP jointly enhanced the PMS adsorption and electron density on Fe center, which accelerated electron transfer from Fe center to PMS for radical production.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
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IF 22.1
Yi Yang,Jingjing Liu,Miaoli Gu,Bei Cheng,Linxi Wang,Jiaguo Yu
Coupling photocatalytic H 2 O 2 evolution with simultaneous furfuryl alcohol oxidation can avoid the slow water oxidation reaction and fully utilize photogenerated carriers to produce valuable chemicals. Herein, a COF (denoted as BTTA) was synthesized by the Schiff-base condensation and in-situ grown on the surface of TiO 2 nanofibers. The resultant TiO 2 /BTTA composite has a large interface and a short carrier migration distance. Furthermore, the porous and ultrathin BTTA layers endow the composites abundant active sites and excellent light absorption ability. Remarkably, a H 2 O 2 -evolution rate of 740 μmol L −1 h −1 and a furoic alcohol conversion of 96 % are achieved. In-situ irradiated X-ray photoelectron spectroscopy and electron spin resonance confirm the S-scheme carrier transfer mechanism, which spatially separates photogenerated carriers with strong redox power. This work opens a new door to the rational design of S-scheme photocatalysts for economic and green photosynthesis of H 2 O 2 and organic compounds.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2023
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IF 9.8
Zhansheng Li,Baocheng Qu,Jingqiu Jiang,Tadiyose Girma Bekele,Hongxia Zhao
The photoactivity of dissolved organic matter (DOM) has a great impact on the photodegradation of organic pollutants in natural waters. In this study, the photodegradation of TBBPA was investigated under simulated sunlight irradiation in the presence of copper ion (Cu 2+ ), dissolved organic matter (DOM) and Cu-DOM complexation (Cu-DOM) to illustrate the effect of Cu 2+ on photoactivity of DOM. The rate of photodegradation of TBBPA in the presence of Cu-DOM complex was 3.2 times higher than that in pure water. The effects of Cu 2+ , DOM and Cu-DOM on the photodegradation of TBBPA were highly pH dependent and hydroxyl radical(·OH) responded for the acceleration effect. Spectral and radical experiments indicated that Cu 2+ had high affinity to fluorescence components of DOM, and acted as both the cation bridge and electron shuttle, resulting the aggregation of DOM and increasing of steady-state concentration of ·OH (·OH ss ). Simultaneously, Cu 2+ also inhibited intramolecular energy transfer leading to the decrease of steady-state concentration singlet oxygen ( 1 O 2ss ) and triplet of DOM ( 3 DOM ⁎ ss ). The interaction between Cu 2+ and DOM followed the order of conjugated carbonyl C O, COO − or C O stretching in phenolic groups and carbohydrate or alcoholic C O groups. With these results, a comprehensive investigation on the photodegradation of TBBPA in the presence of Cu-DOM was conducted, and the effect of Cu 2+ on the photoactivity of DOM was illustrated. These findings helped to understanding the potential mechanism of interaction among metal cation, DOM and organic pollutants in sunlit surface water, especially for the DOM-induced photodegradation of organic pollutants.
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
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IF 13.6
Liwei Yang,Fashan Yang,Heng Zhang,Hongyu Zhou,Mengfan Luo,Yunmei Liu,Chuanliang Zhao,Lu Zheng,Bo Lai
At present, the potential mechanism of manganese oxide (MnO 2 ) activation of PI and the key active sites of PI activation are still unclear and controversial. To this end, three different crystal forms of MnO 2 were prepared in this study and used to activate PI to degrade pollutants. The results showed that different crystal types of MnO 2 showed different catalytic abilities, and the order was γ-MnO 2 > α-MnO 2 > β-MnO 2 . Through quenching experiments, EPR tests, Raman experiments and in situ electrochemical experiments, it has been confirmed that electron transfer-mediated non-free radical process is the main mechanism of pollutant degradation , in which the active substance is the highly active metastable intermediate complex (MnO 2 /PI*). Hydroxyl radical (HO • ), superoxide radical (O 2 •− ), singlet oxygen ( 1 O 2 ) and iodine radical (IO 3 • ) did not participate in pollutant degradation. The quantitative structure-activity relationship analysis confirmed that the catalytic performance of MnO 2 was highly positively correlated with the surface Mn(IV) content, which indicated that the surface Mn(IV) site was the main active site. Overall, this study will be of great help to the design and application of manganese dioxide activation for periodate degradation of pollutants.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Baokang Xu,Xiao Zhang,Yue Zhang,Shiwen Wang,Peng Yu,Yongjun Sun,Xi Li,Yanhua Xu
The nonradical pathway selectively oxidizes pollutants with less interference from environmental factors, which can effectively improve the environmental suitability of peroxymonosulfate (PMS) activation. Herein, a Co-doped nanotubular carbon nitride catalyst (Co-CNNT) based on CoN x sites was constructed for stable and efficient PMS activation with a better specific surface area, number of CoN x sites, and electron transfer capability than Co-doped lamellar carbon nitride catalyst (Co-CN). Co-CNNT improved PMS utilization efficiency (∼50%) and enhanced the contribution of the electron transfer pathway to tetracycline (TET) degradation. The enhanced ability of Co-CNNT to adsorb PMS leads to Co-CNNT–PMS* generated by PMS at the CoN x site, which raises the Co-CNNT surface potential and allows PMS to be activated in a manner that captured electrons. Thus, the Co-CNNT/PMS system could effectively destroy electron-rich or low-potential pollutants within 24 min. The stronger environmental adaptability allows it to maintain catalytic activity in complex aqueous matrices, achieving effective oxidation of diluted tetracycline-based pharmaceutical wastewater. This paper reveals the effects of carbon nitride morphology control strategies on the properties of CoN x active sites and PMS activation mechanisms, providing new insights into the induction of nonradical PMS activation pathways.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jian Ke,Hailun Zhao,Shangkun Zhu,Zixuan Zheng,Qiulian Yang,Yanhua Liu,Ruixin Guo,Jianqiu Chen
The safe disposal of excess sludge generated from chemical wastewater treatment processes has attracted worldwide concern because of its high yield and toxicity. In our work, purified terephthalic acid excess sludge-derived biochar (PTABC) was prepared via one-step pyrolysis without additives. The prepared catalyst was demonstrated to degrade sulfamethoxazole (SMX) via the activation of peroxymonosulfate (PMS). The inhibitory effects of anions were negligible. The reactive oxygen species were investigated based on the radical scavenging experiments and electron paramagnetic resonance technique. Additionally, the electron transfer process was investigated via electrochemical measurements. The results show that the non-radical pathways take a leading role in the degradation of SMX and the corresponding contributions of sulfate radical (SO 4 •– ), hydroxyl radical (•OH) and non-radical pathways in PTABC-700/PMS system for SMX degradation were 12.59%, 3.28%, and 84.13%, respectively. Active sites of PTABC-700 responsible for SMX degradation were also proposed. Overall, this study provides a promising strategy for converting excess sludge into functional catalysts and achieving treatment of SMX-contaminated wastewater.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jingyun Zhang,Zhen Jia,Shitao Yu,Shiwei Liu,Lu Li,Congxia Xie,Qiong Wu,Youzheng Zhang,Hailong Yu,Yuxiang Liu,Jinhui Pang,Yue Liu
Controllable carbonyl group (C O) hydrogenation is the key to the transformation of furfural molecules into high-value furfuryl alcohol chemicals. Herein, a non-noble copper metal catalyst (Cu/MgO) was prepared for the efficient hydrogenation of furfural to furfuryl alcohol under mild conditions. At 383 K and 2 MPa H 2 , 99.9% conversion of furfural with 99.9% selectivity to furfuryl alcohol was achieved within 80 min while the turnover frequency (TOF) was 56.87 h −1 . The temperature of a reductive pretreatment can be used to tune the nature of the interfaces between reduced copper and the metal oxides present in copper-magnesium oxide catalysts. The valence copper species exhibited unique catalytic properties in the hydrogenation of furfural to furfuryl alcohol. Besides, the Cu/MgO-350 exhibited excellent stability and reusability without significant activity loss. These results were accounted for by the MgO alkaline interface contributing to the effective formation and high dispersion of different valence Cu species. The active site had strong adaptability to the adsorption of reactants and desorption of products, thus avoiding excessive hydrogenation of furfural. According to the analysis of the characterization data, furfural adsorption mainly existed in η 1 (O)-aldehyde binding mode which was consistent with the density functional theory (DFT) calculation. DFT calculations of the reaction process showed that the theoretical results favored the hydrogenation of furfural through a hydroxyalkyl intermediate rather than of an alkoxide intermediate.
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WATER RESEARCH
·
2023
·
IF 12.8
Mengfan Luo,Heng Zhang,Yang Shi,Jia Zhao,Can Feng,Jialong Yin,Yang Liu,Peng Zhou,Zhaokun Xiong,Bo Lai
Advanced oxidation technologies based on periodate (PI, IO 4 − ) have garnered significant attention in water decontamination. In this work, we found that electrochemical activation using graphite electrodes (E-GP) can significantly accelerate the degradation of micropollutants by PI. The E-GP/PI system achieved almost complete removal of bisphenol A (BPA) within 15 min, exhibited unprecedented pH tolerance ranging from pH 3.0 to 9.0, and showed more than 90% BPA depletion after 20 h of continuous operation. Additionally, the E-GP/PI system can realize the stoichiometric transformation of PI into iodate, dramatically decreasing the formation of iodinated disinfection by-products. Mechanistic studies confirmed that singlet oxygen ( 1 O 2 ) is the primary reactive oxygen species in the E-GP/PI system. A comprehensive evaluation of the oxidation kinetics of 1 O 2 with 15 phenolic compounds revealed a dual descriptor model based on quantitative structure−activity relationship (QSAR) analysis. The model corroborates that pollutants exhibiting strong electron-donating capabilities and high p K a values are more susceptible to attack by 1 O 2 through a proton transfer mechanism. The unique selectivity induced by 1 O 2 in the E-GP/PI system allows it to exhibit strong resistance to aqueous matrices. Thus, this study demonstrates a green system for the sustainable and effective elimination of pollutants, while providing mechanistic insights into the selective oxidation behaviour of 1 O 2 .
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RSC Advances
·
2023
·Vol. 13
·期 22
·15063-15076
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IF 3.9
Song Wang,Yonggang Zhang
Advanced oxidation processes are frequently applied to a variety of refractory organic wastewater, but rarely is electro-Fenton combined with activated persulfate technology applied to the removal of refractory pollutants. In this work, the electro-Fenton process was combined with zero-valent iron (ZVI) activated peroxymonosulfate (PMS), two advanced oxidation processes based on different radicals, to form the ZVI-E-Fenton-PMS process to treat wastewater, whose main advantages are the generation of more reactive oxygen species and the reduction of oxidant cost to achieve rapid removal of pollutants. This process can not only produce H2O2 and activate PMS at the cathode, but also reduce Fe(III) to realize the sustainable Fe(III)/Fe(II) redox cycle. The main reactive oxygen species in the ZVI-E-Fenton-PMS process were found to be ˙OH, SO4˙− and 1O2 by radical scavenging experiments and electron paramagnetic resonance (EPR), and the relative contributions of the three reactive oxygen species for the degradation of MB were estimated to 30.77%, 39.62% and 15.38%, respectively. Then, by calculating the ratio of the relative contributions of each component to the removal of pollutants at different PMS doses, it was found that the synergistic effect of the process was better when the proportion of ˙OH in the oxidation of reactive oxygen species (ROS) was higher and the proportion of non-ROS oxidation increased year-on-year. This study provides a new perspective on the combination of different advanced oxidation processes and reveals the advantages and potential of this process for application.
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