APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
·
IF 24.319
Lanlan Liang,Peike Cao,Xin Qin,Shuai Wu,Haokun Bai,Shuo Chen,Hongtao Yu,Yan Su,Xie Quan
Developing catalysts with high efficiency and excellent interference tolerance for practical application remains a challenge in catalytic ozonation process. Herein, the surface Vo-rich catalyst was successfully prepared by lattice-doping Co into zinc ferrite spinel, which exhibited efficient mineralization of recalcitrant organic pollutants . The contaminants removal was mainly attributed to the nonradical-based oxygen species of surface atomic oxygen (*O) rather than traditional hydroxyl radical ( · OH). The experiments and DFT calculation results revealed that Vo was the main active sites for adsorption of ozone and production of *O. The O-O in ozone was dissociated at Vo, trigging the formation of *O. In addition, the Vo-driven nonradical catalysis showed high resistance to the coexisting ions (200 mM Cl - , SO 4 2- and NO 3 - ) and exhibited excellent performance for actual wastewater treatment . This work provides a novel strategy to regulate the oxidation pathways in catalytic ozonation process for efficient mineralization of pollutants in complicated water matrices.
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ANALYTICA CHIMICA ACTA
·
2022
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IF 6.911
Xiqing Liu,Tao Wang,Yongqing Wang
In this study, a conversion method and molecular imprinting technology were used to design molecularly imprinted polymers (MIP)-based ratiometric fluorescence test papers. The ZnO quantum dots (ZnO QDs) acted as the background quantum dots and ZIF-8 raw material. Carbon dots (CDs) were used as the identification signals. The imprinting layer achieved a selective function. Therefore, a ZnO@ZIF-8/CDs@MIPs sensor was designed for the detection of Bisphenol A (BPA). The sensor exhibited a fast response time for BPA detection. In addition, the sensor demonstrated that effective detection of BPA can still be achieved in complex environments. The detection limit of this sensor was 0.778 nM with a linear range of 0–60 nM. The corresponding test solutions exhibited clear changes from blue to yellow. The selectivity experiments results demonstrated that ZnO@ZIF-8/CDs@MIPs only exhibit excellent selective recognition effect for BPA. ZnO@ZIF-8/CDs@MIPs-2 was used for the detection of BPA in canned food and compared with the results of HPLC detection of BPA. The two spiked recovery ranges were 96.58–102.04% and 97.43–103.82%, respectively. In addition, the prepared ZnO@ZIF-8/CDs@MIPs-2 test paper visually recognized BPA under ultraviolet light. This study provides guidelines for the design and application of fluorescent test papers for quick detection in practical applications.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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IF 5.2
Xuelian Chen,Tong Zhou,Xiqiang Pan,Hong Li
We demonstrate a simple approach for fabricating polydopamine microcapsules decorated with silver nanoparticles (Ag@PDA MCs) as highly efficient catalysts for water purification . Polydopamine microcapsules (PDA MCs) were formed on the MnCO 3 template from self-polymerization and the removal of template under mild EDTA solution, followed by in situ reduction of Ag + by PDA and growth of monodispersed Ag nanoparticles . Under optimized conditions, the Ag@PDA MCs exhibits 41.56 wt% of Ag loading contents and superior catalytic performance for the degradation of organic pollutants with rate constant of 2.93 min -1 for methylene blue and 1.03 min -1 for 4-nitrophenol. The excellent catalytic activity can mainly be ascribed to high surface roughness of microcapsules, high Ag loading ratio, and uniform distribution of Ag nanoparticles . In addition, this catalyst can be recycled for five times with degradation efficiency higher than 98%. The Ag@PDA MCs possessed fast reduction rate, high catalytic activity, and good recyclability as well as facile preparation and easy separation, showing great potential for the application in wastewater treatment .
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
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IF 9.136
Sheng Liu,Yujuan Guo,Shunmin Yi,Shijing Yan,Chaoliu Ouyang,Fei Deng,Chunxue Li,Guangfu Liao,Qing Li
Supported noble metal heterogeneous catalysts have been proven to be effective for the treatment of toxic organic pollutants. Herein, ultrafine Ag nanoparticles (NPs) with an average size of approximately 4.37 nm was decorated on the surface of pure silicon zeolite nanoparticle (PSZN) and confined in pore channels through a low-cost and environmentally friendly in-situ reduction strategy. The prepared Ag/PSZN nanocomposites showed ultrahigh catalytic activity for the reduction of 4-nitrophenol (4-NP) (∼200 s, 17.29 × 10 -3 s −1 ) and methylene blue (MB) (∼4 min, 76.53 × 10 -2 min −1 ), which outperforms the majority of the previously reported Ag-based catalysts. The excellent catalytic performance is due to the large loading amount (W t = 16.8 %) and ultrasmall size of Ag NPs, which provides abundant active sites. Moreover, it showed outstanding recyclability of 93 % and 86 % removal of 4-NP and MB, respectively, after 10 cycle reactions, and stability after 300 days of storage at room temperature. This work offers new insights into the fabrication of Ag-based catalysts for efficiently removing organic pollutants from aqueous solutions.
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RSC Advances
·
2023
·Vol. 13
·期 37
·25828-25835
·
IF 3.9
Xia Xu,Liming Yang,Yanjun Cui,Bing Hu
The successful development of efficient and stable catalysts for 4-NP reduction reactions is beneficial to the environment and ecology. Fe3O4@Pt exhibits excellent catalytic performance for 4-NP reduction reaction due to the synergistic effect between Fe and Pt. But its structure and catalytic performance are extremely unstable. Here, we utilized the small-scale organic compound 2-hydroxyethylamine as surfactant to construct a stable composite nanomaterial. Then investigated the influence of monochromatic light (650 nm, 808 nm and 980 nm) and temperature on the kinetics of 4-NP reduction reaction by 2-hydroxyethylamine stabilized Fe3O4@Pt. The results indicate that both temperature and monochromatic light radiation can affect kinetic regulation. Increasing temperature can promote the catalytic rate, while monochromatic light radiation can induce agglomeration and inhibit the catalytic rate. This study opens up a new way for developing and regulating catalysts for heterogeneous catalysis reactions.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Hui-Shan Meng,Shu-Zhen He,Mei-Mei Wang,Jia-Rui Xi,Jia-Tai Wen,Hong-Wei Luo,Wei-Kang Wang,Juan Xu
The activation of persulfate by heterogeneous catalysts is susceptible to background matrices present in wastewater, resulting in reduced catalytic efficiency during practical applications. Herein, a persulfate activation cell (PAC) is developed by spatially separating pollutants and persulfate into two independent chambers. The CuCoNi-NF catalyst is fabricated and utilized as the electrode of the PAC. The performance of the PAC is compared with a mixed persulfate activation system (PAM) concerning cyclic degradation of various phenolic pollutants and in the presence of different environmental matrices. The results indicate that phenol pollutants such as bisphenol A (BPA) can be degraded in the PAC via transferring electrons to persulfate. The PAC exhibits superior stability compared to the PAM during six cyclic BPA degradation experiments, with BPA degradation rate constant decreasing by 16.7% for PAC and 81.9% for PAM. Over the 192-hour continuous operation period, the PAC attains a BPA removal efficiency of 88.8 ± 5.6%, a TOC removal efficiency of 74.0 ± 4.6%., and a current output of 0.24 ± 0.04 mA. Furthermore, environmental matrices such as cations, anions, humic acid, and natural water environments demonstrate a slight enhancing effect on BPA degradation in the PAC while conversely displaying inhibition in the PAM. High solution conductivity benefits BPA degradation in the PAC by reducing internal resistance. The pH level of the environment (pH 6–9) has minimal impact on the degradation of BPA in the PAC. The pollutants begin to degrade in PAC when the anode potential reaches their oxidation potential, and the stable potential difference between the anode and cathode ensures the continuous oxidation of the pollutants. Our work proposes a novel persulfate activation strategy that can effectively degrade target pollutants by resisting environmental interferences.
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ACS Applied Polymer Materials
·
2023
·
IF 5
Xiaoqiu Yao,Runxin Teng,Ming Jin,Decheng Wan
Uniform gold nanoclusters (AuNCs) are hardly available unless through abundant strong ligands (at the cost of low catalytic activity and narrow catalytic spectrum) or through well-defined (but expensive) templates, and it appears a tougher challenge for direct preparing supported and uniform AuNCs. Here, we show that with an amphiphilic and dendritic molecular template in hand, highly catalytically active, uniform, and supported AuNCs are one-pot achievable. Branched polyethylenimine (PEI) is modified with a few thioether groups and alkylated with hydrophobic acetyls and polystyrene chains to afford reverse micelle-like dendritic polymers. The structurally optimized dendritic polymer can act as a surfactant to mediate very stable water-in-oil high internal phase emulsion (HIPE) within a wide pH spectrum. Moreover, the dendritic polymer switches into the unimolecular state along the interface of the HIPE when pH is below 6, which is critical to the formation of uniform AuNCs. Experimentally, upon the transformation of HIPE into an open-cellular polyHIPE, the gold ions are simultaneously transformed into AuNCs. Direct preparation of the supported and uniform AuNCs (1.8 ± 0.2 nm) are feasible because the dendritic polymer can simultaneously act as a surfactant, a polymer ligand, and a unimolecular template. Meanwhile, the trace thioether groups in the PEI core reduce the size of AuNCs by enhancing nucleation of AuNCs since in the absence of thioether groups, larger particles are obtained. The supported AuNCs are catalytically active because they are stabilized by weak coligands. For the model reaction of the catalyzed reduction of 4-nitrophenol, the catalyst shows a turnover frequency of 112.5 h–1, which is very high. The catalyst is durable and well recyclable.
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FOOD CHEMISTRY
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2023
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IF 8.8
Guoqiang Guo,Tingting Li,Ziyi Liu,Xinyu Luo,Ting Zhang,Siyuan Tang,Xu Wang,Da Chen
Recently, converting bio-waste into bio-asset and implementing a portable sensing instrument for pollutant monitoring has been highly desirable and challenging. Herein, biomass-derived nitrogen-doped carbon dots (CDs) are prepared hydrothermally and emit blue fluorescence (470 nm) with a high quantum yield of 23.2%. Significantly, CDs can serve as a pH-modulated fluorescence switching nano-sensor to detect 4-NP from 0.054 to 68 μM with low detection limit (LOD, 54 nM) and limit of quantification (LOQ, 181 nM) based on inner filter effect. Moreover, the satisfactory recovery of 101.8–107.5% is gained in practical sample monitoring. Furthermore, a smartphone-integrated optosensing device with CDs-based film is developed for detecting 4-NP with LOD and LOQ of 0.110 μM and 0.350 μM. Concomitantly, the practicability of this device is further validated in several crop samples with satisfactory recovery rates of 101.6–108.6%. Therefore, this work provides a reliable way and a prospective application for on-site 4-NP monitoring in food.
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ACS Applied Polymer Materials
·
2023
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IF 5
Siyuan Zhang,Jiao He,Xinjian Cheng
Amphiphilic hyperbranched polymers (AHBPs) possess important characteristics, such as high solubility, low viscosity, and multiple functional groups, making them of significant scientific interest. In this work, a chain transfer agent (CTA) with a styrene unit was synthesized at first. Subsequently, the CTA was polymerized with a coumarin derivative containing a −C=C bond through reversible addition-fragmentation chain transfer-self-condensing vinyl polymerization (RAFT-SCVP) to obtain the hyperbranched polymer HP-1. Finally, using HP-1 as a macromolecular CTA, amphiphilic hyperbranched fluorescent probes AHP-2 and AHP-3 were synthesized via RAFT polymerization of hydrophilic monomers poly[oligo(ethylene glycol) methacrylate] (PEGMA) and 2-(dimethylamino)ethyl methacrylate (DMAEMA). The as-prepared AHP-2 and AHP-3 were characterized and confirmed. These macromolecular fluorescent probes enable highly sensitive and specific recognition of 4-nitrophenol (4-NP) with detection limit as 0.59 μM. A unique fluorescence quenching effect, termed “enriching inner filter effect (IFE)”, was revealed through the study of the recognition mechanism of the probes for 4-NP in hyperbranched polymers. This effect has the potential to expand the preparation methods of both fluorescent probes and functional hyperbranched polymers. This work investigates the synthesis methodology of amphiphilic hyperbranched polymers and the performance of fluorescent probes, providing a valuable approach for the development of highly sensitive polymer fluorescent probes in the future.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Fengliang Cao,Qingshan Zhao,Debin Kong,Xiaojie Tan,Xinxin Li,Tengfei Liu,Linjie Zhi,Mingbo Wu
Atomically dispersed metal-nitrogen-carbon (M-N-C) catalysts show great potential for heterogeneous catalysis. However, recognizing and engineering the microenvironment of M-N x sites to achieve satisfactory catalytic performance remains challenging. Herein, we propose a facile g-C 3 N 4 -assisted template strategy to anchor atomic Fe-N 4 sites on highly nitrogen-doped carbon nanosheets. Through regulating the ratio and type of peripheral nitrogen species by carbonization temperature, the optimal Fe-N-C-800 catalyst showed significantly boosted catalytic activities (overall turnover frequency of 13.43 min −1 and activation energy of 19.44 kJ mol −1 ) for nitroarene reduction with extremely low reductant dosage, exceeding most reported metal catalysts. Experimental and theoretical results reveal appropriate graphitic- and pyrrolic-N dopants surrounding the Fe-N 4 center can tailor the local electronic structure and contribute to obvious upshift of the d-band center, which dramatically promotes the adsorption and conversion of reactant substrates, eventually delivering the unprecedented catalytic performance. This work provides a guide for rational coordination environment regulation of single-atom catalysts for efficient chemical transformations.
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WATER AIR AND SOIL POLLUTION
·
2023
·Vol. 234
·期 7
·1-17
·
IF 2.9
Xiao Sihua,Wan Jinquan,Wang Yan,Yan Zhicheng,Ma Yongwen,Sun Jian,Tang Min,Cao Jianye,Chen Jinxin
The large-scale wastewater treatment plants (WWTPs) in developed regions collect volumes of wastewater containing various emerging contaminants (ECs) every day, but without any effective process to eliminate them. Therefore, it is of vital importance to study the occurrence of ECs in the effluents from WWTPs. In this study, the concentration levels and pollution characteristics of typical ECs in effluents were investigated for source identification and risk assessment. In total, 13 of 39 analyzed ECs were detected in the effluents, with the highest detection concentration at 706 µg/L (oxolinic acid). Sulfaphenazole showed the highest detection frequency at 100%, while Liede WWTP (1.2 million m 3 /day), located at Tianhe District, was with the highest detection concentration (899 µg/L) among all sampling sites. Parallel factor analysis was applied to identify the dissolved organic matters (DOMs) of excitation–emission matrix spectroscopy (EEMS) first. Based on previous research data, the connection between DOMs and pollution sources could be built. Then, principal component analysis (PCA) and Pearson’s correlation analysis were used to determine the correlation between ECs and DOMs. Finally, ecological and health risk quotients were calculated for the risk assessment of ECs. The results illustrated that oxolinic acid, sulfaphenazole, sulfaquinoxaline, sulfadimethoxypyrimidine, penicillin V, and flumequine were potentially discharged from human activities and livestock, poultry, and aquaculture industry; the possible sources of sulfadoxine and nafcillin were agricultural activities, food production, and catering industry; sulfapyridine and erythromycin were believed to come from hospital wastewater; and the discharges of lincomycin, sulfameter, and sulfamerazine were related to petrochemical industry or chemical production activities. Except for sulfadoxine, all detected ECs posed a high or median risk on aquatic ecosystem, which is enough to threaten aquatic organisms. Even though only oxolinic acid, sulfaquinoxaline, and sulfadimethoxypyrimidine presented a potential risk on humans’ health, the cumulative effect of ECs in the human body still needs attention. The threats of ECs from large-scale WWTPs in China’s developed regions are pointed out for the first time, which could possibly bring widespread attention on emerging pollution from WWTP effluents, potentially advance the introduction of relevant policies, and provide the direction and target pollutants for follow-up mitigation actions.
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JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS
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2023
·
IF 4
Baogang Su,Yao Li,Yijun Du,Linjun Shao,Hongyu Tao,Chenze Qi,Shujing Zhou,Jinjing Li
Supported transition metal catalysts have played a critical role in the modern synthetic chemical industry. Herein, MCM-41 was chemically modified with amino groups and then used as the support of six transition metal cations . The chemical structures , microstructures and dispersions of these supported transition metal cations were carefully characterized by XRD , TEM and BET. The chelations of modified MCM-41 support with these transition metal cations were confirmed by FT-IR and XPS . The reduction reaction of 4-nitrophenol into 4-aminophenol was employed to evaluate the catalytic activities and recyclabilities of these supported transition metal catalysts. Meanwhile, their reactivities with o -Ps species were assessed by positron annihilation lifetime spectroscopy (PALS). It was found that the reduced o -Ps annihilation intensities (ΔI 3 ) were well associated with their catalytic activities while the o -Ps annihilation lifetime values (τ 3 ) were related to their catalytic recyclabilities. In all, the catalytic activities and recyclabilities of supported transition metal cations can be conveniently evaluated by their o -Ps annihilation properties. This method holds great potential in the design and preparation of highly active and stable supported transition metal catalysts.
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