ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2023
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IF 11.4
Wenjun Sun,Yuanna Zhang,Zedong Lu,Yanchu Ke,Xuelin Wang,Jing Wu
Organic pollutants are toxic and are present in drinking water. The conventional processes of most water plants can basically meet the discharge standard. However, based on the improvement of the objective of organic pollutants control and the constant change of water characteristics, the results may not be ideal. This study evaluates the effectiveness of different treatments such as microfiltration, nanofiltration, reverse osmosis, activated carbon, and ultraviolet irradiation/H2O2 in terms of the removal of organic pollutants. Among the DOM results, nanofiltration, reverse osmosis, and activated carbon showed optimal performance due to the characteristics of processes and the compound properties. However, the risks of low-molecular-weight organic residue and byproduct formation are still present. Thirty-nine species of synthetic organic compounds (SOC) were qualitatively and semiquantitatively analyzed. Different technologies showed varying removal capabilities for SOC based on their properties and many substances coexisted leading to abnormal removal performances. These residual organics showed the characteristics of lower molecular weight, more hydrophilicity, further unknown impacts, and with risk of DBPs. Based on the above insights, possible methods can be rationally chosen for on-demand decontamination of organics in unconfined aquatic environment and long-time impact on water characteristics and human health also should be considered.
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高影响因子
Journal of Environmental Chemical Engineering
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2023
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IF 7.7
Xinyu Li,Fei Ye,Hui Zhang,Munir Ahmad,Zhenxing Zeng,Shuaijie Wang,Sufeng Wang,Dawei Gao,Qingrui Zhang
Integrating g-C 3 N 4 with narrow-band semiconductor to construct a Z-scheme structured heterojunction has been regarded as a common strategy to improve the photocatalytic performance of g-C 3 N 4 . However, limited catalytic activity increment is achieved due to the contradiction of expanding the light absorption scope of traditional photo-oxidation semiconductors (PS II) and preserving their valance band oxidative abilities. Herein, to extend the light absorption range of g-C 3 N 4 based Z-scheme photocatalyst to the whole solar spectra while without losing the high oxidative ability of this system, we select the heavy doped W 18 O 49 as PS II and provide a facile in situ hydrothermal method to elaborately fabricate an rGO decorated W 18 O 49 @g-C 3 N 4 (r-CNW) Z-scheme photocatalyst. The prepared r-CNW-2 (with optimal W 18 O 49 to g-C 3 N 4 weight ratio of 1:2) exhibits improved photocatalytic performance with H 2 O 2 generation rates of 71, 58.5 and 6.3 μmol g −1 h −1 obtained under the simulated solar light, visible light (>400 nm) and NIR light (>800 nm) irradiation, respectively, which is 1.3 and 2 times higher than those of the g-C 3 N 4 counterparts (54, 29 μmol g −1 h −1 and even not detected).such outstanding performance of r-CNW-2 could be associated with the broader light absorption, fast charge separation, and rapid redox reactions. Moreover, the r-CNW-2 also displays an excellent E-coli inactivation activity, comparable to most g-C 3 N 4 -based photocatalysts. Our work gives a new insight through trading off light absorption and redox ability to fabricate efficient Z-scheme photocatalyst for photocatalytic H 2 O 2 generation and environmental remediation.
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WATER RESEARCH
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2022
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IF 13.4
Chaozhi Kuang,Guoshen Zeng,Yangjian Zhou,Yaoyao Wu,Dexuan Li,Yingfei Wang,Chuanhao Li
Conventional electrocatalytic degradation of pollutants involves either cathodic reduction or anodic oxidation process, which caused the low energy utilization efficiency. In this study, we successfully couple the anodic activation of sulfates with the cathodic H 2 O 2 production/activation to boost the generation of sulfate radical (SO 4 ·− ) and hydroxyl radical (·OH) for the efficient degradation of emerging contaminants. The electrocatalysis reactor is composed of a modified-graphite-felt (GF) cathode, in-situ prepared by the carbonization of polyaniline (PANI) electrodeposited on a GF substrate, and a boron-doped diamond (BDD) anode. In the presence of sulfates, the electrocatalysis system shows superior activities towards the degradation of pharmaceutical and personal care products (PPCPs), with the optimal performance of completely degrading the representative pollutant carbamazepine (CBZ, 0.2 mg L −1 ) within 150 s. Radicals quenching experiments indicated that ·OH and SO 4 ·− act as the main reactive oxygen species for CBZ decomposition. Results from the electron paramagnetic resonance (EPR) and chronoamperometry studies verified that the sulfate ions were oxidized to SO 4 ·− radicals at the anode, while the dissolve oxygen molecules were reduced to H 2 O 2 molecules which were further activated to produce ·OH radicals at the cathode. It was also found that during the catalytic reactions SO 4 ·− radicals could spontaneously convert into peroxydisulfate (PDS) which were subsequently reduced back to SO 4 ·− at the cathodes. The quasi-steady-state concentrations of ·OH and SO 4 ·− were estimated to be 0.51×10 −12 M and 0.56×10 −12 M, respectively. This study provides insight into the synergistic generation of ·OH/SO 4 ·− from the integrated electrochemical anode oxidation of sulfate and cathode reduction of dissolved oxygen, which indicates a potential practical approach to efficiently degrade the emerging organic water contaminants.
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Molecular Catalysis
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2023
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IF 4.6
Jing Li,Suxia Ma,Ke Ren,Nuo Xu
SSZ-13 zeolite was synthesized from fly ash using a combined alkali fusion hydrothermal method. The optimal synthesis parameters are as follows: NaOH/FA=1.4, SiO 2 /Al 2 O 3 =50, H 2 O/SiO 2 =1800, TMAda-OH/Al 2 O 3 =7, the amount of SSZ-13-seed=10%, and crystallization time and temperature were 160 °C and 40 h. Based on this, a series of fly ash-based Fe-SSZ-13 catalysts were prepared using three different methods and tested in catalytic oxidation with H 2 O 2 for NO removal. The experiment results showed that the NO removal efficiency catalyzed by Fe-SSZ-13-SSIE, Fe-SSZ-13-LIE and Fe-SSZ-13-IM were 78%, 87% and 84%, respectively. ESR was used to detect hydroxyl radicals, UV-vis, XPS and H 2 -TPR were applied to test the composition, state and distribution of iron species, while NH 3 -TPD and Py-FTIR were performed to analyze the intensity and type of acidic sites, and finally to determine the relationship between catalyst structure, active species and catalytic performance in combination with NO removal experiments. The catalytic oxidation mechanism analysis revealed that the excellent catalytic performance can be attributed to the dual function of strong Brønsted acidity on the surface and isolated Fe 3+ with high dispersion, which can rapidly decompose H 2 O 2 into ·OH and efficiently achieve NO oxidation. In conclusion, the preparation of fly ash catalysts has great potential for achieving the dual function of waste utilization and pollutant removal.
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Journal of the Taiwan Institute of Chemical Engineers
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2022
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IF 5.477
Ping Song,Zhongping Yao,Xiao Zhang,Yanjing Liu,Yunsong Xu,Jiankang Wang
Background Fenton-like technology based on in situ formation of H 2 O 2 by activated molecular oxygen has a promising application prospect in the degradation of organic pollutants, which can reduce the environmental and security problems caused by excessive use of H 2 O 2 in traditional Fenton technology. Methods We constructed a micro-nano dendritic zero-valent copper catalyst (mnZVC) by the simple electrochemical reduction, and studied the performance, mechanism and degradation pathway of mnZVC-activated molecular oxygen for the degradation of metronidazole (MNZ). Significant Findings In mnZVC/air system, metronidazole (MNZ) removal efficiency reaches 92.39% within 120 min under pH 3, much higher than that of commercial micron zero-valent copper. In addition, mnZVC has versatility to degrade phenol, methyl orange (MO), rhodamine B (RhB) and tetracycline hydrochloride (TCH). The continuous high-volume generation of H 2 O 2 is the main reason for the high efficient removal of MNZ, which is attributed to the micro-sized dispersibility and nano-sized activity of the mnZVC. Besides, •OH and •O 2 − are proved to be the main active species directly causing MNZ degradation by free radical scavenging experiments and other analysis. Based on the results of LC-MS, the primary degradation intermediates of metronidazole were identified, and three possible degradation pathways were proposed. This work provides a new idea for the design of catalyst with in situ generated H 2 O 2 for degradation of organic contaminants.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2022
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IF 4.831
Xue-Liang Liu,Mengdi Yan,Zhi-guo Chen,Bingxin Zhang,Ningcong Yao,Shan Zhao,Xiaoxia Zhao,Tao Zhang,Guangfan Hai
In this paper, we reported a coumarin-based fluorescent probe for selective detection of H 2 O 2 /SO 2 derivatives via ICT process. To the best of our knowledge, it was few reported with the same probe to enable visual detection of H 2 O 2 /SO 2 derivatives in vivo and in vitro. H 2 O 2 and SO 3 2− were selectively sensed over other analytes, and the probe displayed 20-fold and 220-fold relative fluorescence intensity respectively, as well as the good linear relationship and the excellent detection limits of 2.7 * 10 3 nM and 19.3 nM. Furthermore, the probe was successfully used for fluorescence imaging of the HeLa cells and the mice to monitor exogenous and endogenous H 2 O 2 and SO 3 2− , suggesting its potential biomedical application for investigation and detection the intermediate indicator of oxidative stress in vitro and in vivo.
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高影响因子
INORGANIC CHEMISTRY
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2022
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IF 5.436
Chengyu Zhang,Zhaodong Nan
Metal–organic frameworks (MOFs) can be used as ideal artificial nanozymes for an open structure to transfer substances and products. The nanozymic mechanism of MOFs needs further investigation for wide application. In this manuscript, no peroxidase-like activity was found for ZIF-67 (a kind of MOF), however, it enhanced the peroxidase-like activity of the Fe0.8Ni0.2S2/ZIF-67 composite, in which Fe0.8Ni0.2S2 was the active composition. The catalytic constant (Kcat) is higher at 1.98 (for TMB) and 2.08 (for H2O2) times and the catalytic efficiency (Kcat/Km) is higher at 3.13 (for TMB) and 2.67 (for H2O2) times, than those of Fe0.8Ni0.2S2. The Km value decreased about 85 times (for H2O2) for Fe0.8Ni0.2S2/ZIF-67 than that of horseradish peroxidase (natural enzyme). The mechanism was proposed. The limit of detection of H2O2 for Fe0.8Ni0.2S2/ZIF-67 is 0.039 μM, which is lower by about 18.2 times than that of Fe0.8Ni0.2S2. Simultaneously, Fe0.8Ni0.2S2/ZIF-67 was used to rapidly detect ascorbic acid for only 1.0 min in food monitoring. This study may be important to design a new kind of nanozyme.
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CHEMOSPHERE
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2022
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IF 8.943
Yanchao Li,Can Wang,Shuang Pan,Xin Zhao,Ning Liu
Fe/Mn@carbon cloth (CC) was successfully fabricated through high-temperature shock (HTS) technique and used as cathode modification in heterogeneous electro-Fenton (hetero-EF) process for methylisothiazolinone (MIT) degradation. The nanocrystalline on Fe/Mn@CC electrode is doped with Fe and Mn oxides and coated with carbon layer, which could markedly enhance the electrocatalysis with high electro-chemical active area and low resistance. Fe/Mn@CC modified cathode can efficiently in-situ produce and activate H 2 O 2 , showing high electrocatalytic activity to MIT degradation. The 95.2% MIT degradation with in 100 min were achieved under the condition of 30 mA current, 0.75 L min −1 aeration intensity and initial pH = 3. Based on the CV curves and stability test, the high degradation activity revealed the kinetically beneficial regeneration of Fe II /Mn II in Fe/Mn@CC and activation of H 2 O 2 . The electron transfer between Fe II/III and Mn II/III , together with the direct Fe II /Mn II regeneration on the cathode, could markedly promote the H 2 O 2 utilization, and eventually lead to MIT degradation.
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高影响因子
Materials Chemistry Frontiers
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2022
·Vol. 6
·期 19
·2848-2858
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IF 8.683
Dan Zhao,Rui Zhang,Mengyu Xu,Xiaoyun Li,Yan Jiao,Xincai Xiao
Since biofilm infections could cause chronic diseases and drug resistance, posing a serious threat to human health, the development of antibiofilm nanomaterials has attracted the interest of researchers. In this study, a quaternized carbon dot–papain complex (qCD–P) was prepared, and the complex exhibited inhibiting and eliminating abilities against internal resident bacteria and external matrix biofilms, with a minimum inhibitory concentration against Staphylococcus aureus biofilms at 20 μg mL−1. The morphology, particle size, surface potential, and groups of the prepared qCD–P were characterized through multiple characterization means, and the target and antibiofilm mechanisms were explored from the perspective of its two components qCDs and papain. Meanwhile, based on the optical properties of qCDs and catalytic properties of papain, a dual-channel detection platform (naked-eye visualization and ratio fluorescence) of hydrogen peroxide has been realized with o-phenylenediamine as the substrate. The multifunctional qCD–P would provide a foundation for research on the potential applications of nanomaterials for in-clinic treatment and biochemical detection.
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JOURNAL OF MEMBRANE SCIENCE
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2022
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IF 10.53
Xuemei Bao,Qianqian Liu,Jiahui Yang,Furong Wang,Fengjiao Yu,Jian Yu,Yang Yang
Fouling control is of great significance for polymeric membrane-based wastewater purification and reclamation. Herein, we designed a reactive polysulfone (PSF) ultrafiltration (UF) membrane integrating resorcinol–formaldehyde (RF) resin nanospheres and β -FeOOH nanoparticles ( [email protected] /PSF) with unique self-cleaning performance. The [email protected] /PSF membrane with an optimal RF resin and β -FeOOH loading showed a reasonable water flux (376.3 L m −2 h −1 bar −1 ) and high rejection (97.5%) to bovine serum albumin. Besides, the membrane could capture trace amount of cationic dyes in the feed solution via electrostatic attraction. After organic fouling, the permeation flux of the membrane was effectively recovered under visible-light irradiation at neutral pH. We confirmed that the low-bandgap RF resin nanospheres blended in the PSF matrix produced H 2 O 2 in-situ upon absorption of visible light. Then the adjacent β -FeOOH nanoparticles catalyzed the conversion of the self-supplied H 2 O 2 to •OH radicals. The [email protected] /PSF membrane provided a unique platform to perform cascade reaction for production of •OH radicals concentrated in restricted space, which effectively degraded the adsorbed organic foulants. The proposed self-cleaning mechanism that can work under sunlight and ambient condition is expected to simplify and economize the cleaning operations of polymeric UF composite membranes in complex wastewater purification.
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FOOD CHEMISTRY
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2022
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IF 9.231
Dong Li,Ran Tian,Shiyu Kang,Xue-Qiang Chu,Danhua Ge,Xiaojun Chen
Ag nanoparticles (Ag NPs) with high electrocatalytic activity are of great significance for electrochemical sensors. Nanostructures as scaffold can solve aggregation problem of Ag NPs so that to ensure the stability. In this work, Ag NPs immobilized on FeS 2 nanoprisms (Ag/FeS 2 ) were prepared via an in-situ photocatalytic reduction approach. The enlarged electrode effective surface area, enhanced electron transfer and the synergic impact between Ag NPs and FeS 2 lead to an enhanced catalytic activity. The electrochemical detection method exhibited great performance of low detection limit (0.6 μM), wide linear range and high sensitivity (244.4 μA mM −1 cm −2 ) for H 2 O 2 . Moreover, Ag/FeS 2 as a peroxidase mimic can catalyze oxidation of colorless 3,3′,5,5′-tetramethylbenzidine (TMB) to blue product (oxTMB) by H 2 O 2 , which achieved effective detection of H 2 O 2 with a 3.0 μM detection limit. A promising way was successfully eatablished to perform the quantitation of H 2 O 2 in serum and beverage.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2022
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IF 4.831
Xin Zhan,Xiaoxiao Yu,Benmengyang Li,Rui Zhou,Qingyu Fang,Yiwei Wu
In the presence of thioglycolic acid (TGA) and under the catalysis of Fe 3+ , a simple, rapid, sensitive, selective and effective ratiometric fluorescence sensor platform based on the mixed physically blue nitrogen-doped graphene quantum dots (N-GQDs) as probe signals and orange rhodamine B as internal standard signals has been constructed for analysis of H 2 O 2 in human serum. TGA is the key factor for fluorescence response toward H 2 O 2 by N-GQDs and the mechanism is H 2 O 2 reacts speedily with TGA under the catalysis of Fe 3+ , and produces intermediate of superoxide anions ( O 2 − ), which accepts electrons from N-GQDs, and generates graphene oxide, causing the fluorescence quench of N-GQDs. Compared with N-GQDs probe, the sensitivity of the ratiometric fluorescence sensor platform of N-GQDs/rhodamine B for analysis of H 2 O 2 has been improved by nearly 5-folds. Under the optimum conditions, F λ=580nm / F λ=440nm has a good linear relationship with the concentration of H 2 O 2 and the detection limit of H 2 O 2 is 0.46 μmol/L with 3.5% RSD. The established sensor platform has been successfully used for probing H 2 O 2 in human serum with satisfactory results. The superior performance of the probe lies in its high selectivity and can be directly employed in detecting H 2 O 2 in serum samples without any sample pretreatment procedures.
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