PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2023
·Vol. 25
·期 19
·13716-13727
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IF 3.3
Caihong Wang,Yong Liu,Fengshen Han,Yongzhe Han,Tianyu Liu,Haitao Ren,Xu Han
Using metal-free catalysts is widely recognized as a promising approach toward wastewater remediation because of the absence of metal leaching. However, the oxidation products involved in the oxidation process and the corresponding mechanisms are still not clear. In this work, N-doped carbocatalysts (CN) were fabricated using as-prepared g-C3N4 and glucose solution, and the reactivity of the as-prepared catalysts was optimized by controlling calcination temperature. Correspondingly, increasing the calcination temperature promotes the catalytic oxidation of BPA. The positive correlations between the contents of pyridinic-N and graphitic-N and the kobs values of BPA oxidation, as well as XPS analysis indicate the important roles of pyridinic-N and graphitic-N in BPA oxidation. According to the series of characterizations of the oxidation products and Raman analysis of the reaction process, the moderately activated persulfate (PS) on the CN catalyst is the predominant species in BPA oxidation and BPA can be oxidized to BPA polymers with high selectivity by H-abstraction under alkaline conditions. This work highlights the important role of the moderate activation of PS in the polymerization of phenolic contaminants under alkaline conditions, which enriches our understanding of the oxidation of aromatic contaminants by PS under alkaline conditions.
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MICROCHIMICA ACTA
·
2023
·Vol. 190
·期 5
·1-10
·
IF 5.7
Teng Yuanjie,Li Xin,Chen Yingxin,Xu Pei,Pan Zaifa,Shao Kang,Sun Nan
The SERS intensity of analytes is primarily influenced by the density and distribution of hotspots, which are often difficult to manipulate or regulate. In this study, cucurbit[8]uril (CB[8]), a kind of rigid macrocyclic molecule, was introduced to achieve ~ 1-nm nanogap between gold nanoparticles to increase the density of SERS hotspots. Three kinds of estrogens (estrone (E1), bisphenol A (BPA), and hexestrol (DES)) which are molecules with weak SERS signals were targeted in the hotspots by CB[8] to further improve the sensitivity and selectivity of SERS. It was demonstrated that CB[8] can link gold nanoparticles together through carbonyl groups. In addition, the host–guest interaction of CB[8] and estrogens was proved from the nuclear magnetic resonance hydrogen and infrared spectra. In the presence of CB[8], the SERS intensities of E1, BPA, and DES were increased to 19-fold, 74-fold, and 4-fold, respectively, and the LOD is 3.75 µM, 1.19 µM, and 8.26 µM, respectively. Furthermore, the proposed SERS method was applied to actual milk sample analysis with recoveries of E1 (85.0 ~ 112.8%), BPA (83.0 ~ 103.7%), and DES (62.6 ~ 132.0%). It is expected that the proposed signal enlarging strategy can be applied to other analytes after further development. Graphical Abstract
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SENSORS AND ACTUATORS B-CHEMICAL
·
2023
·
IF 8.4
Lixia Lu,Bingchan Song,Jianwen Gao,Xinyu Shao
Different environmental estrogens (EEs) may coexist in the same foodstuff, necessitating the establishment of a simultaneous detection method. Although there are numerous studies on the detection of EEs, few was reported on the determination of two or more estrogens at the same time except HPLC . Our efforts have been made to develop a ratiometric aptasensor based on multicolor lanthanide-doped upconversion luminescence nanoparticles (UCNPs) to realize simultaneous and sensitive detection of two EEs (bisphenol A and 17β-estradiol). Three types of core-shell UCNPs with excellent luminous properties and distinct emitting colors were successfully synthesized via doping with various lanthanide ions , two of which were conjugated with specific aptamers and act as energy donors, while another one served as a reference. Because of their excellent luminescence quenching performance, ultra-thin metallic MoS 2 nanosheets were selected as the energy acceptor. Thus, a ratiometric luminescence aptasensor was established and successfully used for the simultaneous detection of two estrogens in tap water and milk samples, demonstrating its considerable practical application value.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2021
·
IF 7.46
Yuanxia Lv,Xiaohuan Qin,Kun Hu,Fanggui Ye,Shulin Zhao
This study proposes a surface-assisted laser desorption ionization time-of-flight mass spectrometry (SALDI-TOF MS) method using an ultrastable microporous hydrogen-bonded organic frameworks (MP-HOFs) for selective and sensitive analysis of two common organic pesticides: paraquat (PQ) and chlormequat (CQ) in real samples. MP-HOFs are formed by H-bonding self-assembly of co-planar π-conjugated large aromatic tectons with carboxylate groups. They can not only efficiently absorb and transfer laser energy, but also specifically capture and isolate target analytes from complicated systems. The proposed SALDI-TOF MS method exhibited high salt tolerance and low background. The selective enrichment performance of MP-HOFs was demonstrated by analyzing PQ and CQ in real samples. Simultaneous analysis results of PQ and CQ showed satisfactory reproducibility with relative standard deviations (RSDs) of 3.2–9.2% and 5.7–12.3% for spot-to-spot and sample-to-sample, good linearity (R 2 > 0.99), and high sensitivity with a limit of detection of 0.001 and 0.05 ng mL −1 , respectively. The detection limits of PQ and CQ test analytes were three and two orders of magnitude lower than those of non-enriched PQ and CQ, respectively. Furthermore, the possible ionization mechanism was discussed, and the presented approach was successfully applied for PQ and CQ detection in tap water, river water, and soil, confirming its potential in practical applications.
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MATERIALS CHEMISTRY AND PHYSICS
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2021
·
IF 4.094
Dedong Zeng,Jiangli Wang,Yu Xie,Yun Ling,Jinsheng Zhao,Hao Ye,Tongcai Chen
Designing and fabricating the double-capability photocatalysts with the capability of producing hydrogen from the splitting of water and degrading environmental organic pollutants under visible light irradiation are significant in environmental treatment and new energy preparation. As a proof of concept, TiO 2 @ZnFe 2 O 4 heterojunctions with high performance and stability were prepared by a one-step hydrothermal method , in which TiO 2 nanosheets successfully grew on the main body of ZnFe 2 O 4 nanorods . The microstructures and morphologies of the as-produced composites as well as their photocatalytic hydrogen generation rate and photocatalytic degradation performances towards humic acid, florfeniol, tetracyclines, and bisphenol A were investigated. The results indicate that TiO 2 @ZnFe 2 O 4 heterojunctions possessed the higher photocatalytic activities towards hydrogen production and contaminants degradation ability than that of only TiO 2 and ZnFe 2 O 4 . Especially, TiO 2 @ZnFe 2 O 4 heterojunctions with the molar ratio of 1:4 have the best activities and manifest good stability. Significant enhancement of visible light absorption and photogenerated charge separation of TiO 2 @ZnFe 2 O 4 were achieved. This work paves a way to construct a low-cost, environment-friendly, recyclable, and non-poisonous photocatalysts for hydrogen generation and the degradation of pollutants.
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JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Yantao Wan,Wei Zhang,Xiaolin Han,Lei Zhou,Huajun Zhen,Chengzi Wu,Qi Yu,Guangli Xiu
A novel B,N-decorated carbocatalyst (Fe@BPC-XBN) for peroxymonosulfate (PMS) activation was prepared by a simple pyrolysis method using the iron-based metal organic frameworks (Fe-MOF), boric acid and boron nitride (BN) as precursors. Fe@BPC-20BN removed 93.3% of bisphenol A (BPA) in 90 min compared to 64.9%, 82.1% and 83.5% with Fe@PC, Fe@BPC and Fe@PC-20BN, respectively, with 0.15 g/L catalyst and 1 mM PMS at initial pH of 7. The solo B-doping with boron acid on the Fe-MOF derived porous carbon enhanced its catalytic capacity; moreover, B, N co-doping with BN and boron acid as precursors further promoted the catalytic performance. The addition of BN not only provided more B, N catalytic centers but also improved the stability of the carbocatalyst. In addition, hydroxyl radicals , sulfate radicals, superoxide radicals, and singlet oxygen species were involved in the degradation of BPA. Fe species, –BCO 2 /–BC 2 O, pyridinic N, and pyrrolic N groups on the carbon matrix played the important roles in the BPA degradation. The outstanding catalytic performance of Fe@BPC-20BN could be attributed to the synergistic effects between iron nanoparticles and the B/N codoped carbon matrix. This study gives new insights into the design and preparation of high-efficient B,N-decorated carbocatalysts for environmental remediation.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Ying Lu,Fujian Yang,Siyuan Chen,Wenchao Shi,Chengdu Qi,Guilong Peng
In this work, Ni(II) was used as peroxymonosulfate (PMS) activator for decomplexation of Ni(II)-citrate, and subsequently applied for the decomplexation of chelated nickel in the electroless nickel plating wastewater. Effect of the co-existed substances (HCO 3 − , HPO 3 2− , H 2 PO 2 − , and P 2 O 7 4− ) on the decomplexation of Ni(II)-citrate were evaluated. Interestingly, except for H 2 PO 2 − , the presence of HCO 3 − , HPO 3 2− , and P 2 O 7 4− enhanced the decomplexation efficiency of Ni(II)-citrate via promoting the decomposition of PMS. Based on the radical quenching experiments and electron spinning resonance (ESR) spectra analysis, OH, SO 4 ‐ , and 1 O 2 were the primary reactive species involved in the decomplexation reaction process. Furthermore, after the decomplexation of the electroless nickel plating wastewater by PMS, the recovery of nickel was successfully achieved via adsorption coupled with electrodeposition , and 93.1% nickel recovery could be accomplished with initial Ni(II) eluent concentration of 32.5 g/L. Therefore, this study provides a green and promising approach for the application of advanced oxidation processes based on PMS activation, and has the potential to convert recoverable resources into value-added products from electroplating wastewater.
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JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Huiwang Dai,Wenjun Zhou,Wei Wang,Zhiqi Liu
In this study, three Co/N-C catalysts were prepared by pyrolysis of bimetallic zeolitic imidazole frameworks with different Co/Zn ratio, and the critical active Co species in peroxymonosulfate (PMS) activation was investigated. The three catalysts had distinct cobalt species but similar N configuration and graphitization degree. The Co species were distributed as single atoms (Co SAs) at a Co/Zn molar ratio of 1:8, while Co nanoclusters (Co NCs) and Co nanoparticles (NPs) would be formed with further increase in Co content. The degradation efficiency of BPA did not show correlation with the increasing of Co content in catalyst. Based on the catalytic performance comparison and reactive species detection, Co SAs was identified as active sites, which could interact with PMS to generate 1 O 2 via path of PMS→HOO*→O*→ 1 O 2 . However, the role of NCs and NPs in directly activating PMS was negligible. In addition, the increase of Co content in Co/N-C catalyst would result in mass cobalt leaching, which enhanced the BPA degradation via homogeneous catalytic reactions with Co IV as reactive species. It is an effective way to design the Co/N-C catalyst with high catalytic activity and stability via regulating the formation of Co SAs.
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RSC Advances
·
2021
·Vol. 11
·期 58
·36769-36776
·
IF 3.361
Qing Gao,Yang Zang,Ju Xie,Yongchuan Wu,Huaiguo Xue
In this work, an electrochemical sensor was designed for trace monitoring of bisphenol A (BPA) by decorating a hybrid bilayer molecularly imprinted membrane (MIM) on a multi-walled carbon nanotube-modified glassy carbon electrode. When BPA in the MIM was eluted, a composite molecularly imprinted electrochemical sensor was constructed. Under optimal conditions, the developed sensor showed two linear relationships between ΔIp and BPA concentration in the range of 0.04 μM to 8 μM, as well as good selectivity and stability, and was also applied to detect BPA in water samples with desirable recoveries ranging from 92.0% to 107.0%.
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WATER RESEARCH
·
2021
·
IF 11.236
Chenying Zhou,Peng Zhou,Minglu Sun,Yang Liu,Heng Zhang,Zhaokun Xiong,Juan Liang,Xiaoguang Duan,Bo Lai
The sluggish kinetics of Fe(II) recovery strongly impedes the scientific progress of Fenton reaction (Fe(II)/H 2 O 2 ) towards practical application. Here, we propose a novel mechanism that metal-free nitrogen-doped carbon nanotubes (NCNT) can enhance Fenton chemistry with H 2 O 2 as electron donors by elevating the oxidation potential of Fe(III). NCNT remarkably promotes the circulation of Fe(III)/Fe(II) to produce hydroxyl radical ( • OH) with excellent stability for multiple usages (more than 10 cycles) in the NCNT/Fe(III)/H 2 O 2 system. Although carbonyl on NCNT can act as the electron supplier for Fe(III) reduction, the behavior of NCNT is distinct from common reductants such as hydroxylamine and boron. Electrochemical analysis and density functional theory calculation unveil that nitrogen sites of NCNT can weakly bind with Fe(III) to elevate the oxidation potential of Fe(III) (named near-free Fe(III), primarily FeOH 2+ ) at pH ranging from 2.0 to 4.0. Without inputs of external stimulations or electron sacrificers, near-free Fe(III) can promote H 2 O 2 induced reduction of Fe(III) to initiate Fenton chain reactions for long-lasting generation of • OH. To our delight, it is a common property of N-doped carbon materials (e.g., graphene, carbon nanofibers, and acetylene black), our research thus provides a novel, sustainable, and green strategy for promoting Fenton chemistry.
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ENVIRONMENTAL TECHNOLOGY
·
2021
·
IF 3.247
Dong Yang,Peng Gao,Xin Ren,Yifan Niu,Zhenfen Wu,Zhenggang Gu,Hongbo Peng
The wide application of endocrine disruptors (EDs) has recently created great public concerns because of their toxicities. Previous studies have stated that the effect of oxygen-containing functional groups of carbon nanotubes (CNTs) for Bisphenol A (BPA) sorption, but no study has been quantified the exact contribution of the oxygen-containing functional groups. Moreover, the role of solvents on the adsorption of BPA should be considered. Considering the well properties of CNTs, graphitized (MG), carboxylated (MC) and hydroxylated (MH) multi-walled CNTs were selected as model adsorbents, BPA was used as model adsorbate. Solubility and single point adsorption coefficient (logKd) of BPA were n-hexadecane > water > methanol, suggesting that hydrophobic interaction was the main mechanism for BPA sorption on CNTs. For different functional groups of CNTs, π-π interaction between MH and BPA may be stronger than that of MC, and thus the sorption of BPA on MH was higher than that of MC. Moreover, hydrogen bond resulted in the higher adsorption of BPA on MH when compared with MC. The oxygen-containing functional groups of CNTs played a key role for BPA sorption in methanol because the values of contribution were 20%–45% for -OH and were 5%–25% for -COOH. In n-hexadecane, other factors such as hydrophobic interactions should be considered because the contribution percentages of -OH were ca.15% and the values for -COOH were ca.10%. The results are expected to provide important information on the interaction of EDs and CNTs.
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FOOD CHEMISTRY
·
2021
·
IF 7.514
Jie Liu,Qian Liu,Liulin Wei,Xiaomei Chen,Zhiqiang Li,Yidong Xu,Xueyun Gao,Xiaoxiao Lu,Jingchan Zhao
An on-line in-tube solid-phase microextraction (in-tube SPME) coupled with high-performance liquid chromatography (HPLC) method was proposed based on a novel polyhedral oligomeric silsesquioxane (POSS)-hybrid monolith for the determination of four bisphenols (BPs) in milk. The monolith was synthesized using acrylamide (AM) and monomethacrylate-functionalized POSS (mono-MA-POSS) as functional monomers to copolymerize with ethylene dimethacrylate (EDMA). Due to the abundant hydrogen bonding, π-π and hydrophobic interaction sites, the synthetic monolith displayed satisfying extraction performance for target BPs. Under the optimized conditions, the developed on-line in-tube SPME-HPLC method exhibited low limits of detection (LODs) (0.030–0.055 ng mL −1 ). The spiked recoveries were between 85.4 % and 111.8 %, and the relative standard deviations (RSDs) were less than 3.5 % for all the analytes. The results showed that the proposed method provided alternative for the analysis of BPs in complex samples.
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