SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Jie Zhong,Yong Feng,Bin Yang,Qian Xiong,Guang-Guo Ying
Modification using biochar as a carrier is a promising method to improve the activation of peroxymonosulfate (PMS) by magnetic nanoparticles. In this study, we provided an effective strategy to control the generation of oxygen vacancy to prepare N-doped magnetic biochar (NMB) by optimizing the heat treatment process of gas foaming. The NMB exhibited superior catalytic performance and stable recycling use in the activation of PMS to degrade sulfadiazine (SDZ). Through multiple characterization techniques and density functional theory (DFT) calculations, the mechanism of the reaction process about oxygen vacancy was explored for the first time in magnetic biochar. In addition, the degradation kinetics, recycling experiment, and removal of total organic carbon were carried out to evaluate the degradation performance of NMB/PMS system. After 15 min of reaction, the removal rate of SDZ reached 95.2%. After the fifth cycle of use, the removal rate of SDZ remained at 79.6%. In addition to SDZ, the NMB/PMS system could also efficiently remove ofloxacin, reactive brilliant red, and bisphenol A, suggesting excellent degradation reactivity for different types of pollutants. The oxygen vacancy was found to play an important role in the catalytic process probably through changing the electronic structure of the NMB catalyst and thereby activating the charge transfer to participate in the degradation. The results from this study might deepen the understanding of the activation mechanism driven by magnetic biochar and provide insights into the development of low-cost wastewater treatment technologies.
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Analytical Methods
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2022
·Vol. 14
·期 10
·1023-1030
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IF 3.532
Hanxing Yang,Zhongguang Ji,Yanbo Zeng,Jian Zhang,Lifen Chen,Hailong Wang,Yiwen Yang,Longhua Guo,Lei Li
An aggregation-induced emission monomer-based fluorescent molecularly imprinted poly(ionic liquid) (AIE-FMIPIL) was synthesized for the first time with an AIE probe 4-(1,2,2-triphenylvinyl)phenyl acrylate (TPE), and an ionic liquid as dual functional monomers, and an ionic liquid as cross-linker. AIE-FMIPIL displayed a sphere-like shape and its average diameter was 410 nm. The absolute quantum yields of TPE and AIE-FMIPIL were 9.23% and 12.61%, respectively. The synergetic effect of TPE in the AIE-FMIPIL framework contributed to the higher quantum yield of AIE-FMIPIL. 4-Nitrophenol (4-NP) efficiently quenched AIE-FMIPIL with high fluorescence based on the Förster resonance energy transfer mechanism. The synthesized AIE-FMIPIL sensor was highly sensitive for 4-NP detection (linear range, 0.02–1.5 μM) in the optimal detection condition, with a low detection limit of 10 nM (S/N = 3). AIE-FMIPIL showed increased sensitivity and quenching efficiency compared with AIE-FMIP comprising a traditional monomer and cross-linker. AIE-FMIPIL exhibited selective binding to 4-NP because of the imprinted sites. AIE-FMIPIL was adopted to detect 4-NP in environmental samples.
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WATER RESEARCH
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2022
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IF 13.4
Xu-Dan Yang,Bo Gong,Wei Chen,Chen Qian,Meng Du,Han-Qing Yu
Microplastics act as a source of organic contaminants in aquatic environments and thus affect their environmental fate and toxicity. Because of the weak and reversible interactions between microplastics and organic species, the organic coronas vary with their surrounding environments. Thus, in order to evaluate the possible environmental risks of microplastics, methods for evaluating the dynamic uptake of organic contaminants onto suspended microplastics in aquatic environments are greatly desired. In this work, a UV–vis spectroscopy-based approach was developed for in-situ monitoring organic contaminants uptake onto suspended microplastics after correcting the light scattering interference from microplastics suspensions and establishing the nonlinear relationship between concentration and light absorbance of organic species. The inverse adding-doubling method based on radiative transfer theory was adopted to correct the light scattering effect of suspensions. Then, the resulting mixed absorption spectra were decomposed to calculate the concentrations of the aqueous and adsorbed organic species simultaneously with a nonlinear calibration method. The uptake processes of bisphenol A and p-nitrophenol onto nylon 66 microparticles were monitored with this approach and confirmed by high-performance liquid chromatography analysis. The approach was validated by applying it to natural water samples, and the equilibrium adsorption capacity was found to be interfered mainly by the protein-like substances. This approach has high accuracy, good reproducibility, remarkable universality, and ease of handling, and also provides a potential tool for characterizing the corona formation process on suspended particles both in natural and artificial environments, such as eco-corona formation and engineering surface modification on nano/micro-particles.
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Journal of Environmental Chemical Engineering
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2022
·
IF 7.968
Abdul Latif,Ahsan Maqbool,Runzhan Zhou,Muhammad Arsalan,Kai Sun,Youbin Si
This study represents one of the first attempts towards bisphenol A (BPA) degradation by Trametes versicolor laccase immobilized on Ba-alginate beads. The effect of input variables including temperature (20–40 °C), BPA concentration (2–10 mg/L) and time (10–90 min) were studied using Box-Behnken design (BBD) and artificial neural network (ANN). The maximum BPA degradation of 84.34% was obtained when the temperature was 40 °C, BPA concentration 2 mg/L and time 50 min, which was accurately predicted by BBD (83.48%) and ANN (84.33%), proving the accuracy of prediction for both models. The values of R 2 and MSE for BBD were found to be 0.98, 9.88, while for ANN were 0.97, 38.25, respectively. Based on higher R 2 value and lower MSE, BBD was slightly better than ANN. The immobilized laccase showed higher storage stability than free laccase by retaining 68.64% and 44.62% of their activity at the same experimental conditions. Furthermore, BPA transformation was confirmed by Fourier-transform infrared spectroscopy (FTIR) analysis. GC-MS had detected the oxidative degradation products from BPA. Results showed that Ba-alginate immobilized laccase could be a promising biocatalyst in treating organic pollutants .
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Zizhao Qian,Yuanxiang Xiao,Xujun Zhang,Qing Li,Lujie Wang,Feiya Fu,Hongyan Diao,Xiangdong Liu
Bisphenol A (BPA) is the main precursor in the synthesis of epoxy resins. However, because of its toxic and nonrenewable nature, BPA is unsuitable in the sustainable preparation of epoxy resins. In contrast, Diphenolic acid (DPA) is renewable but its carboxyl group limits its applications in bio-based thermosets. In this study, we report a novel amidation route to tailor DPA to produce epoxide monomers that present epoxy resins with a high performance. The diphenolic amides exhibited very low toxicities when compared with that of BPA, and also provided an unexpected autocatalytic effect on the curing reactions when succinic anhydride (SA) was used as the hardener. Dynamic mechanical analyses (DMA) and tensile test results confirmed the remarkable thermomechanical properties of the cured epoxy resins, which may be attributed to the increased cross-linking density and enhanced hydrogen bonding by the amide groups. Among the SA-cured epoxy resins, diglycidyl ether of diphenolic ethylamide exhibited the best performance, which included a high T g of 114 °C, char yield (CY) of 20%, tensile strength of 60.2 MPa, and toughness value of 185 MPa. In addition, the DPA-derived epoxy resins have great potential in the preparation of bio-based composites because they act as excellent interfaces between the resin and cotton fibers (CoFs). Our study presents a new strategy to prepare bio-based epoxy resins with a high performance, emphasizing the greater potential of amidated DPA derivatives to replace BPA in the epoxy resin market.
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ACS ES&T Water
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2022
·
IF 0
Yibing Sun,Hongchao Li,Shengli Zhang,Ming Hua,Jieshu Qian,Bingcai Pan
Heterogeneous peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs) are under extensive investigation for their great potential in water remediation. The understanding of the PMS activation mechanism is crucial but still debatable. Here, we describe a thorough investigation of the mechanism involved in PMS activation by using molybdenum disulfide (MoS2) as a catalyst. This MoS2/PMS system exhibited intriguing target-dependent reactivity. Further comprehensive experimental results excluded the major contributions of various possible species, including HO•, SO4•–, O2•–, 1O2, homogeneous Mo(VI), and heterogeneous Mo(VI). We then proposed a surface ≡Mo–OOSO3– complex as the major reactive species, while SO4•– derived from the decomposition of ≡Mo–OOSO3– acted as the secondary reactive species for pollutant removal. This complex could oxidize pollutants through the oxygen-atom-transfer mechanism and perform both nucleophilic and electrophilic attacks. This work provides novel perspectives for the mechanistic understanding of heterogeneous PMS-based AOPs for water remediation.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
·
IF 9.965
Wenwu Zhou,Bing Yang,Guo Liu,Chenmin Xu,Qiuyi Ji,Weiming Xiang,Dunyu Sun,Qiang Zhong,Huan He,Liu Yazi,Zhe Xu,Chengdu Qi,Shiyin Li,Shaogui Yang
Employing perylene diimide supermolecule (PDI) as metal-free cocatalyst, a novel PDI/g-C 3 N 4 /Bi 2 WO 6 (PCB) photocatalyst was constructed for the effective degradation of antibiotics. Both the photocatalytic activity and photostability of g-C 3 N 4 /Bi 2 WO 6 (gCB) were further improved after loading PDI. Under simulated sunlight illumination, the apparent rate constant of tetracycline (TC) degradation by PCB reached 2.6 times that of gCB. The photocatalytic activity of PCB still kept over 80% after 4 cycle experiments, while gCB only remained around 21%. The superior activity of PCB was ascribed to the synergism between the extended visible light absorption range through the participation of PDI cocatalyst and facilitated gCB-to-PDI photoelectron transfer. TC would finally be transformed into non-toxic ring opening products and mineralized. This work demonstrated that PDI was an excellent metal-free cocatalyst and exhibited great potential to boost the activity of photocatalysts.
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RSC Advances
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2022
·Vol. 12
·期 8
·4550-4561
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IF 4.036
Yun Liu,Haihua Yang,Tao Chen
It is highly desirable to explore efficient catalysts for reducing toxic Cr6+ to benign Cr3+ under mild and eco-friendly conditions. This article describes a facile fabrication of nitrogen doped carbon (N@C-g-C3N4) as a metal-free catalyst for Cr6+ reduction using lignin as a carbon source and g-C3N4 nanosheets as a nitrogen source. The structural properties of the N@C-g-C3N4 catalyst are characterized by TEM, HR-TEM, XRD, TGA, Raman, EDS-mapping, XPS and BET techniques. The summation of these analyses sheds light on the high surface area (903 m2 g−1), mesopore size (17.3 nm) and defects (ID/IG = 0.97) of N@C-g-C3N4, which contribute to its excellent catalytic activity in HCOOH-mediated reduction of Cr6+ to Cr3+ with high rate constant (2.98 min−1) and turnover frequency (2.21 molK2Cr2O7 gcatalyst−1 min−1) and complete degradation (100%) within 5 min. The catalytic performance of the catalyst reveals that the reduction activity is significantly dependent on the concentration of Cr6+ and HCOOH, catalyst loading, pH, temperature, and foreign ions. Particularly, the N@C-g-C3N4 catalyst shows superior stability and renewability with little loss of activity (≥95%) after 8 months storage and five repeated uses. Furthermore, N@C-g-C3N4 can be applied in other hydrogenation reactions involving K3[Fe(CN)6], 4-NP and BPA using NaBH4 as a hydrogen donor, and the removal of organic dyes. These findings illustrate that N@C-g-C3N4 as a metal-free catalyst is effective, versatile and eco-friendly for the reduction of Cr6+ from contaminated environments.
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CHEMICAL ENGINEERING JOURNAL
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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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JOURNAL OF HAZARDOUS MATERIALS
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2022
·
IF 14.224
Xingxing Peng,Qihang Zheng,Lei Liu,Yuzhe He,Tianyu Li,Xiaoshan Jia
T2, a gram-positive bacterium capable of rapidly degrading tetrabromobisphenol A (TBBPA), and affiliated with the genus Enterobacter , was isolated for the first time from sludge that had been contaminated for several years. The TBBPA degradation data fitted the first-order model well. Under optimal conditions (pH of 7, temperature of 31 °C, TBBPA concentration of 5 mg L −1 , and inoculum size of 5%), 99.4% of the initially added TBBPA was degraded after 48 h. TBBPA degradation fitted the first-order model with the half-life of 3.3 h. These results illustrated that the TBBPA degradation capability of strain T2 was significantly better than that of previously reported bacteria. A total of 17 intermediates were detected, among which five were reported for the first time. Whole-genome sequencing revealed that strain T2 had a chromosome with the total length of 4 854 376 bp and a plasmid with the total length of 21 444 bp. It harbored essential genes responsible for debromination, such as cyp450 , gstB , gstA , and HADH, and genes responsible for subsequent complete mineralization , such as bioC , yrrM , Tam , and Ubil . A key protein of haloacid dehalogenases responsible for the biodegradation of TBBPA may also be involved in the regulation of TBBPA degradation in natural environment. In soil bioremediation experiments, strain T2 showed excellent environmental adaptation. It was able to biodegrade TBBPA and its typical intermediate bisphenol A efficiently. Therefore, it could potentially be applied to treat TBBPA-contaminated sites.
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ELECTROCHIMICA ACTA
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2022
·
IF 7.336
Mengfan Cao,Yanjiao Zou,Yuanyuan Zhang,Ting Zeng,Qijin Wan,Guosong Lai,Nianjun Yang
Here we present a facile, rapid and reliable electrochemical sensor for quantitative analysis of hazardous photographic developing agents, including metol (MT), hydroquinone (HQ) and catechol (CC). They have been identified as usual contaminants in environment and water samples. This sensor is based on a nanocomposite of three-dimensional (3D) porous flower-like Co 3 O 4 @C hybrid and graphene nanoplates (Co 3 O 4 @C/GNP). The Co 3 O 4 @C/GNP compoiste is prepared by a two-steps procedure, consisting of the composite synthesis of a Co-MOF precursor and GNPs in the first step and subsequently direct calcination process in the N 2 atmosphere. The morphology, composition, and electrochemical behavior of the Co 3 O 4 @C/GNP composite is characterized by using microscopic methods and electrochemical techniques, revealing its 3D porous structure, abundant pores, a large electrode active area, a high conductivity, outstanding electrocatalytic and sensing performance toward MT, HQ, and CC. Taking advantages of a huge electroactive surface area and a fast electron transfer rate of GNPs and strong electrical catalytic ability of the Co 3 O 4 @C hybrid, the fabricated Co 3 O 4 @C/GNP sensor displays high sensitivity for quantitative analysis of MT, HQ and CC. Their detection limits are as low as 5.1, 14.7 and 169 nM (S/ N = 3), respectively. Beyond that, the proposed Co 3 O 4 @C/GNP electrochemical sensor shows strong reproducibility, good stability and selectivity in the voltammetric quantitation of these analytes. It has been also successfully applied in measuring these photographic developing agents in water environment. Consequently, the fabricated Co 3 O 4 @C/GNP composite is expected to be an excellent electrode material in the applications of electrochemical sensing.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Hailan Qin,Jingyu Sun,Dongsheng Xia,Haiming Xu,Qilin Yu,Yi Zheng,Yintao Shi
Boosting nonradical ( 1 O 2 , e − and h + ) process to enhance the selective degradation for electrophilicity contaminants is an ingenious strategy. Herein, BiOI/BiOCl heterojunction with rational interface oxygen vacancies (IOVs) concentration was successfully synthesized by ultrasonic method. Moreover, multi-characterization and interference experimental unveiled that the appropriate IOVs concentration can not only effectively reduce the transport resistance of photo-induced carriers but also boost the nonradical process. Thus, BOC-5 can remove 84% (20 mg/L) tetracycline hydrochloride (TC-HCl) in 1 h and present wonderful insecticidal performance for rotifers. Simultaneously, the quantitative methods of IOVs concentration, the contribution of the active species to the catalytic performance and the contribution of different 1 O 2 source to the total 1 O 2 were established for the first time. Furthermore, the structure–activity relationship between the IOVs concentration and the catalytic properties was firstly constructed. This work provides an inventive idea to purify water pollutants and disinfestation by boost nonradical process via interface defect engineering.
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