NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 11
·5420-5430
·
IF 3.3
Qi Guo,Jihong Xu,Rui Tang,Yulin Min,Zhenhu Hu,Penghui Shi
In the degradation process of organic pollutants, compared with the free radical pathway, the non-radical pathway shows the advantages of mild oxidation ability, strong anti-interference, and adaptation to different pH values. In this study, a manganese–nitrogen co-doped porous carbon (Mn–N@C-1) with high nitrogen content was prepared to improve the contribution rate of non-radical pathways to the degradation process of organic pollutants. The high performance of Mn–N@C-1 is attributed to the formation of Mn–Nx sites between Pyridine N and Mn, which can effectively oxidize organic pollutants in water (phenol, bisphenol A, 2,4-dichlorophenol). In addition, the catalyst exhibits high catalytic activity over a wide pH range (pH = 3–9) and has good immunity to inorganic anions. Moreover, the Mn–Nx site and graphitic-N are considered to be the generation sites of singlet oxygen, and the role of metastable Mn–N@C-1/PMS* complexes in the electron transfer process is explored. Overall, this study explores the crucial role of non-radical pathways in the degradation of organic pollutants by carbon-based materials.
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高影响因子
Water
·
2023
·Vol. 15
·期 4
·830
·
IF 3.4
Shuaiguo Li,Kejian Tian,Qing Qiu,Yue Yu,Han Li,Menghan Chang,Xuejian Sun,Jinming Gu,Fenglin Zhang,Yibing Wang,Hongliang Huo
As a widespread pollutant, bisphenol A (BPA) has created a serious threat to ecosystem and human health. Therefore, expanding the available microbial resources used to screen highly efficient BPA-degrading bacteria with BPA as the sole carbon source is very important for the removal of this pollutant from the environment. In this study, the BPA degradation rate ofPseudomonassp. P1 to 30 mg/L was 96.89% within 120 h. Whole genome sequencing showed that the genome of strain P1 was composed of a single circular chromosome with a full length of 6.17 Mb, which contained 5636 predicted coding genes. Comparative genomic analysis showed that strain P1 contained 210 functional genes related to BPA degradation. It was confirmed that BPA degradation genes ferredoxin (bisdA), P450 (bisdB),CotAandLacin strain P1 were highly expressed under the induction of BPA. Combined with the identification of metabolites, the route of BPA degradation byPseudomonaswas proposed. A new metabolite, 4-vinylphenol, was detected for the first time in pathway Ⅰ. In pathway Ⅱ, BPA is directly oxidized to phenol and 4-isopropenyl phenol in the presence of laccase, which is rarely reported in the process of bacterial degradation of BPA. This study confirmed that strain P1 had good tolerance to various environmental factors at the gene level and enriched the degradation mechanism of BPA.Keywords:Bisphenol A;Pseudomonas;whole genome;biodegradation
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JOURNAL OF MATERIALS SCIENCE
·
2023
·Vol. 58
·期 8
·3551-3567
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IF 4.5
Yang Xia,Wei Songrui,Ma Xilong,Gao Zhuwei,Huang Wei,Wang Dun,Liu Zhongxin,Wang Jieqiong
The photothermal process exhibits the largest energy conversion efficiency among all solar energy utilization processes. In this study, a core–shell CoTiO 3 @MnO 2 (CTM) composite photothermal catalyst was synthesized by supporting MnO 2 on CoTiO 3 by hydrothermal synthesis. Binding to peroxymonosulfate (PMS) heterogeneous catalyst removed tetracycline in wastewater. The new catalyst was characterized by FT-IR, UV–Vis, XRD, BET, SEM, TEM, and so on. Kinetic analysis showed that CTM activated PMS at a rate of 3.2 and 3.5 times higher than that of pure light and heat conditions, with complete degradation of tetracycline (TC). Since the outer MnO 2 layer converted the absorbed solar energy into thermal energy, PMS was activated to generate active species while performing electron transfer, which resulted in a considerably improved catalytic efficiency. To prove the wide applicability of the catalyst, other pollutants were degraded, including bisphenol A (BPA), metronidazole (MNZ), and methyl orange (MO). The three pollutants were degraded within 40 min. Finally, our findings demonstrated the mechanism of the photothermal degradation process and provided a novel approach for environmental remediation using renewable solar energy.
Graphical Abstract In this paper, the degradation efficiency of CoTiO 3 was improved by loading MnO 2 on CoTiO 3 . Binding to peroxymonosulfate (PMS) heterogeneous catalyst activation for the catalytic degradation of tetracycline. It was found by experiments that the core-shell structure of the composite material CoTiO 3 @MnO 2 had better photothermal catalysis efficiency than photocatalysis and thermal catalysis.
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CHEMOSPHERE
·
2023
·
IF 8.8
Qinghong Wang,Yayan Tong,Yalin Wu,Shuangying Li,Huahua Bai,Qingxiang Zhou
Bisphenols (BPs) are typical endocrine disruptors , which can cause great effects on environmental, organisms and human health. In this study, β-Cyclodextrin (β-CD) functionalized polyamidoamine dendrimers-modified Fe 3 O 4 nanomaterials (MNPs@PAMAM (G3.0)@β-CD) were facilely synthesized. It exhibited good adsorption capacities for BPs, which was utilized to construct a sensitive tool in combination with high performance liquid chromatography for monitoring BPs such as bisphenol A (BPA), tetrabromobisphenol A (TBBPA), bisphenol S (BPS), bisphenol AF (BPAF) and bisphenol AP (BPAP) in beverage samples. The factors affecting the enrichment were examined such as generation of adsorbent, dosage of adsorbent, type and volume of eluting solvent, elution time and pH value of sample solution. The optimal parameters for enrichment was as follows: dosage of adsorbent, 60 mg; adsorption time, 50min; sample pH, pH7; elutent, 9 mL mixture of methanol and acetone(1:1); elution time, 6min; sample volume, 60 mL. The experimental results demonstrated that the adsorption conformed to pseudo-second-order kinetic model and Langmuir adsorption isotherm model. The results showed the maximum adsorption capacities of BPS, TBBPA, BPA, BPAF and BPAP were 131.80 μgg −1 , 139.84 μgg −1 , 157.08 μgg −1 , 142.11 μgg −1 and 134.23 μgg −1 , respectively. Under optimal conditions, BPS had good linear relationship over range from of 0.5–300 μgL −1 , and the linear ranges of BPA, TBBPA, BPAF and BPAP ranged from 0.1 to 300 μgL −1 . The limits of detection (S/N = 3) for BPs were good in range of 0.016–0.039 μgL −1 . The spiked recoveries of target bisphenols (BPs) in beverages were approving over range from 92.3% to 99.2%. The established method possessed merits of easy to operate, good sensitivity, rapidness as well as environmental friendliness, and which earned great application potential for the enrichment and detection of trace BPs in practical samples.
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PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Qingru Xie,Yanping Zhu,Haiyang Xian,Qingze Chen,Chengshuai Liu,Fei Wu,Xiaoliang Liang,Runliang Zhu
Doping transition metal into ferrihydrite (Fh) may significantly affect its structure and Fenton reactivity. The comparative study of Fh and M(II)-Fh (M = Cu, Co, or Mn), for the first time, reveals that doping metal ions can alter the property and content of oxygen vacancy (OVs) and the oxidation potential of Fh, which subsequently affects H 2 O 2 decomposition, HO . generation, and Fenton reactivity of the catalysts. The overall Fenton activity of the samples in decomposing bisphenol A decreases in the order Cu-Fh > Fh > Co-Fh > Mn-Fh. In specific, Cu-Fh is the most efficient catalyst as it has the lowest energy barrier for decomposing H 2 O 2 into HO . at OVs sites and the highest oxidation potential (benefiting the reduction of Fe(III) to Fe(II) by H 2 O 2 ). Our findings show the complex heterogeneous Fenton reactivity of M-Fh, and doping can be an efficient strategy for achieving highly efficient Fenton catalysts.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Jingxuan Yang,Dongxu Qu,Jue Wang,Yangtao Wu,Lingjun Bu,Yuanxi Huang,Shiqing Zhou
The N-Br bond in monobromoamine (NH 2 Br) can be cleaved by UV irradiation to generate Br • and subsequently HO • , resulting in an advanced oxidation condition (i.e., UV/NH 2 Br). This study investigated the degradation of six contaminants of emerging concern (CECs) in the UV/NH 2 Br process, including the phenolic hydrocarbons phenol and bisphenol A (BPA), the amines aniline and sulfadiazine (SDZ), and the persistent organic pollutants ibuprofen (IBP) and carbamazepine (CBZ). The results showed that UV/NH 2 Br process significantly improved the degradation of CECs following pseudo-first order kinetics, and the degradation of CECs was enhanced with the increase of NH 2 Br dosage. UV/NH 2 Br was more efficient in degrading CECs containing phenolic hydroxyl groups (100 %), followed by those containing amine groups (> 95 %). The degradation efficiency was influenced by the pH value and was highest at pH 7. It was found that low concentrations of Cl − (< 0.5 mM ) and HCO 3 − (< 0.5 mM) promoted the degradation of SDZ and IBP, but further increases in Cl − and HCO 3 − (0.5 ∼ 5.0 mM) resulted in inhibition. SDZ and IBP degradation was inhibited by photo absorption competition and free radical depletion in natural organic matter and actual water. Probe experiments showed that reactive bromine species (RBS), reactive nitrogen species (RNS), and hydroxyl radical (HO • ) played a dominant role in CEC degradation. During the degradation of IBP by UV/NH 2 Br, hydroxylation, bromination , and quinylation were proposed as the primary reaction mechanisms. As compared to HOCl disinfection, NH 2 Cl disinfection after the UV/NH 2 Br process produced lower concentrations of disinfection by-products (DBPs).
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Xinhao Wang,Zhaokun Xiong,Hongle Shi,Zelin Wu,Bingkun Huang,Heng Zhang,Peng Zhou,Zhicheng Pan,Wen Liu,Bo Lai
Rationally regulating reaction mechanisms in Fenton-like reactions by tuning the properties of catalysts is of great significance, but still challenging. Herein, we synthesized various active center size-dependent catalysts to realize the switching of reaction mechanisms and pollutant degradation routes in peroxymonosulfate (PMS) activation systems. The results illustrated that the reaction mechanism transformed from radical oxidation (51.64%) to nonradical oxidation (89.92%) with the decrease of active center size from nanoparticle (Co NP -NC) to single atom (Co SA -NC). The evolution of reactive species switched the degradation intermediates and pathway of sulfisoxazole (SIZ). The generation of singlet oxygen ( 1 O 2 ) in Co SA -NC/PMS tends to selectively attack electron-rich site of SIZ, while reaction between radicals and SIZ prefers non-selective oxidation in Co NP -NC/PMS system. Besides, the toxicity tests indicated that the conversion from non-selective to selective oxidation resulted in lower toxicity of effluent after reaction, which can further reduce environmental risks of effluent.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2023
·
IF 8.7
Haijian Xie,Jiawei Wu,Mengzhen Yu,Huaxiang Yan,Shakil Masum,Peifu Cai,Yun Chen
Bisphenol A (BPA) is a toxic endocrine disruptor often found in landfill leachate . Adsorption behaviors and mechanisms of BPA onto organo-bentonites amended loess , e.g., Hexadecyltrimethylammonium chloride-bentonite (HTMAC-B) and Carboxymethylcellulose-bentonite (CMC-B) were experimentally investigated. The adsorption capacity of loess amended by HTMAC-B (LHB) and CMC-B (LCB) is 4.2 and 4 times greater than that of loess (L), respectively. It is attributed to the increase of hydrogen bonds and hydrophobic lateral interactions between the adsorbent and the adsorbate. The binary (Pb 2+ -BPA) systems may enhance BPA adsorption onto the samples by the formation of coordination bonds between the hydroxyl group of BPA and Pb 2+ ions. A cycled column test was used for investigating the transport behavior of BPA in LHB and LCB samples. The hydraulic conductivity of loess amended by the organo-bentonite (e.g., HTMAC-B, CMC-B) is generally lower than 1 × 10 −9 m/s. Especially for CMC-B amended loess, the hydraulic conductivity can be reduced to 1 × 10 −12 m/s. This guarantees the hydraulic performance of the liner system. Transport behavior of BPA in cycled column test is explained by the mobile-immobile model (MIM). Modelling results showed that loess amended by organo-bentonites can increase the breakthrough time of BPA. In comparison to loess-based liner, the breakthrough time of BPA for LHB and LCB can be increased by a factor of 10.4 and 7.5, respectively. These results indicate that organo-bentonites can serve as a potentially effective amendment for improving the adsorption of loess-based liners.
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高影响因子
CHEMOSPHERE
·
2023
·
IF 8.8
Yongli Liu,Yue Zhang,Jingwen Niu,Linchun Nie,Shiyu Huang,Huanhuan Liu,Shuai Yuan,Qingxiang Zhou
Bisphenol A (BPA) is an endocrine disrupting chemical and poses a grave threat to the human health. Herein, a fluorescent probe constructed with molecularly imprinted polymers decorated carbon dots (CDs@MIPs) was proposed for determination of BPA with high selectivity . The CDs@MIPs were constructed using BPA, 4-vinylpyridine and ethylene glycol dimethacrylate as template, functional monomer and cross linker, respectively. The obtained fluorescent probe not only owned a highly selective recognition function derived from MIPs but also displayed an excellent sensitivity for sensing BPA stemmed from CDs. The fluorescence intensity of CDs@MIPs was varied before and after the removal of BPA templates. The fluorescent decrease fraction of the fluorescent probe demonstrates a nice linearity in BPA concentration range of 10–2000 nM (r 2 = 0.9998) and the detection limit is as low as 1.5 nM. The fluorescent probe was triumphantly utilized to sense the level of BPA in real aqueous and plastic samples with good results. Moreover, the fluorescent probe offered a wonderful means for fast identification and sensitive detection of BPA from environmental aqueous samples.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Kexin Yin,Ruixian Wu,Yanan Shang,Dongdong Chen,Zelin Wu,Xinhao Wang,Baoyu Gao,Xing Xu
Two coordination structures (Co-N 4 or Co-N 3 ) of cobalt single-atom catalysts (Co-SACs) were prepared by using the chitosan as starting precursor to evaluate the modulated coordination microenvironment of Co-SACs for organics degradation. The degradation performances for carbamazepine (CBZ) as well as the radical/nonradical pathways in Co-N 4 /PMS and Co-N 3 /PMS systems was evaluated. Results showed that more radicals could be produced by the Co-N 3 catalyst via stronger PMS adsorption as well as the subsequent peroxide bond cleavage of PMS. In addition, a lower energy gap between the CBZ and Co-N 3 /PMS complex was endowed for the Co-N 3 coordination to boost stronger electron-transfer process for CBZ. As a result, both radical and electron-transfer process was boosted by the coordinated Co-N 3 sites than those of Co-N 4 coordination. This work provides a new insight on the versatile catalytic pathways with modulated coordination microenvironment of carbon-based SACs for high-efficiency PMS activation.
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Symmetry-Basel
·
2023
·Vol. 15
·期 3
·629
·
IF 2.7
Fuchong Li,Wei Liu,Li Tian,Wei Cao,Xu Li,Junhong Guo,Jinfeng Cui,Baoping Yang
Because of easy functionalization, low cost, and large-scale fabrication, pure organic fluorescent polymers are widely applied in light-emitting display, bio-fluorescence-enhanced imaging, explosive detection, and other fields. Among these applications, due to their unique optical rotation characteristics, chiral fluorescent polymer materials are part of fluorescent polymers which could be used in chiral molecular detection and separation, biological target detection, etc. In this work, we designed and synthesized the first chiral organic fluorescent polysulfate materials through sulfur fluoride exchange polymerization (new click chemistry) by asymmetric binaphthol molecular. The chiral fluorescent polysulfate were synthesized by R/S [1,1′-binaphthalene]-2,2′-diol(Binol.), propane-2,2-diylbis(4,1-phenylene) bis(sulfurofluoridate) (FO2S–BA–SO2F) and 4,4′-(propane-2,2-diyl)diphenol(BA.) through step-by-step polymerization reaction under alkali present. It was found that the local crystallization of pure bisphenol A polysulfate was broken by the asymmetric axial chiral BINOL molecule inserted in it and let the polymer into the amorphous state. Fluorescent chiral molecules are uniformly dispersed in the polymer; the 120 µm film prepared by the film scraper was transparent and had good luminescence characteristics under ultraviolet light. After fluorescence detection, the excitation wavelength is 450 nm, and the emission wavelength is 480 and 517 nm.Keywords:polysulfate material;fluorescence;polymer;chiral binaphthol
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Applied Sciences-Basel
·
2023
·Vol. 13
·期 5
·3182
·
IF 2.7
Chuning Zhang,Huaqiang Chu,Qian Ma,Yanyan Chen,Jianwei Fan
It is important to further enhance the performance of green and efficient non-homogeneous catalysts for advanced oxidation process of Peroxymonosulfate (PMS-AOP) for green treatment of industrial wastewater. In this paper, nitrogen–sulfur co-doped MOFs-derived carbon material (CoSN@C) was prepared by one-pot synthesis followed by carbonization, and its morphological structure was characterized by XRD and SEM. After pyrolysis, the CoSN@C still maintained the dodecahedral morphology and structure of ZIF-67. The synergistic effects of S and N significantly elevated the activation of PMS. The results show that the CoSN@C + PMS system can effectively activate PMS to degrade Rhodamine B (RhB), with a rate constant (1.85 min−1) four times higher than that of the CoN@C + PMS system (0.44 min−1). The optimal catalytic process parameters of material dosage, PMS concentration, temperature, pH, and other parameters were also investigated for the activation of PMS to remove Rhodamine B. The cyclic experiment shows that the CoSN@C has excellent recyclability and the degradation rate of RhB still reached 88.9% after four cycles. Radical capture experiments and EPR tests showed that the CoSN@C + PMS system generated a large amount of SO4·−and ·OH radicals adsorbed on the catalyst surface and a certain amount of singlet oxygen, and the free radical pathway and non-radical pathway worked together to degrade RhB efficiently and rapidly. While non-radical pathway with singlet oxygen as main reactive oxygen species played a key role in the CoN@C + PMS system. This work provides a new idea for the rational design of non-homogeneous catalysts for PMS-AOP system.Keywords:advanced oxidation process;peroxymonosulfate (PMS);non-homogeneous catalyst;MOFs
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