NEW JOURNAL OF CHEMISTRY
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2023
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IF 3.3
Yujie Zhang,Yingjiang Wang,Zhaohui Li,Lingbo Qu,Lanlan Yu
Nanozymes, which possess similar catalytic activities to natural enzymes, are considered promising alternatives to natural enzymes. In the present study, a new bimetallic Fe/Mn metal–organic framework (MOF) nanomaterial was synthesized by doping Mn in MIL-101(Fe). Despite the low doping amount of Mn, the Fe/Mn MOF displayed remarkably enhanced peroxidase-like activity, catalyzing the conversion of chromogenic substrate ABTS to blue-green ABTS˙+. Subsequently, the addition of environmental pollutant aminophenol isomers induced different color changes in a solution, which provided a simple and feasible approach to differentiate them by the naked eyes. Based on the effect of aminophenol isomers on the absorption spectrum of ABTS˙+, colorimetric methods were developed to quantitatively determine m-AP and p-AP with detection limits of 0.13 μM and 0.20 μM, respectively. Furthermore, taking advantage of a smart phone software-color recognizer to analyze the RGB value, a rapid detection method for m-AP was proposed, offering a solution to detect m-AP in the absence of any analytical instruments. This work verified the essential role of doping Mn in enhancing the enzyme-like activity of nanozymes. Simultaneously, the proposed simple, rapid, and accurate sensing method provided a new option to differentiate and determine aminophenol isomers, which has great potential for environmental application.
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JOURNAL OF CHEMICAL THERMODYNAMICS
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2023
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IF 2.6
Chong Yang,Yuyao Xie,Shimin Xu,Hui Wang,Lihua Cheng,Xinping Ouyang
Liquid-liquid equilibrium (LLE) data for the ternary systems of phenol + toluene + solvent were determined at 298.2, 308.2, and 318.2 K under 101.3 kPa, in which 1,2-propanediol (1,2-PDO) or 1,3-propanediol (1,3-PDO) was screened as the extracting agent. Two important indicators (distribution coefficient and separation factor) were calculated to evaluate the extraction performance of solvent for separating phenol from coal tar containing toluene. The separation factor was all greater than one, indicating that it is feasible to select 1,2-PDO or 1,3-PDO as extractants for separating phenol from coal tar containing toluene. Meanwhile, solvation free energy and interaction energy among the components were calculated to investigate the separation mechanism of phenol from coal tar containing toluene using 1,2-PDO or 1,3-PDO at a molecular level. Furthermore, NRTL and UNIQUAC thermodynamic models were utilized to correlate experimentally determined LLE data for phenol + toluene + solvent (1,2-PDO or 1,3-PDO) ternary systems at (298.2–318.2) K under 101.3 kPa, and the root-mean-square deviation value was used to evaluate the discrepancy between correlated and experimental values, yielding corresponding binary interaction parameters. In addition, graphical user interface method for topological analysis developed by Marcilla was used to corroborate the reliability of obtained binary interaction parameters.
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Nano Research
·
2023
·
IF 9.9
Yue Meng,He Xun,Sun Shengjun,Sun Yuntong,Hamdy Mohamed S.,Benaissa Mhamed,Salih Alsamani A. M.,Liu Jun,Sun Xuping
Developing efficient and durable oxygen evolution reaction (OER) catalysts holds great promise for green hydrogen production via seawater electrolysis, but remains a challenge. Herein, we report a Co-doped Ni 3 S 2 nanosheet array on Ni foam (Co-Ni 3 S 2 /NF) as a high-efficiency OER electrocatalyst for seawater. In alkaline conditions, Co-Ni 3 S 2 /NF requires an overpotential of only 368 mV to drive 100 mA·cm −2 , superior to Ni 3 S 2 /NF (385 mV). Besides, it exhibits at least 50-h continuous electrolysis.
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CHEMICAL ENGINEERING JOURNAL
·
2023
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IF 15.1
Juan Zhang,Yulong Ma,Yonggang Sun,Lei Wang,Liqiong Wang,Zhen Wang,Bolong Zhao,Jingdan Gao,Min Xu
The application of heterogeneous advanced oxidation processes (AOPs) in the removal of refractory pollutants has been hindered by several drawbacks, such as difficult recovery of the powder catalyst, the low yields and inefficient utilization of reactive oxygen species (ROS). We developed a novel catalytic membrane named 2D CoO@MoS 2 membrane, its catalytic active layer was a composite material formed by MoS 2 nanosheets wrapped and intercalated between 2D CoO porous nanoplates, providing abundant active sites and oxygen vacancies (O v ). 2D CoO@MoS 2 membrane was applied to activate peroxymonosulfate (PMS) for benzotriazole (BTA) degradation. DFT calculations and series characterizations demonstrated that electron transfer occurred at the contact interface between 2D CoO and MoS 2 phase, while the 2D CoO@MoS 2 composite could act as an effective electron donor for PMS. The redox cycles of Mo(IV)/ Mo(VI) and O v /O 2− could synergistically enhance the regeneration of Co(II), thereby maintaining the cycle of catalytic active center, which facilitated the spontaneous dissociation of PMS to generate various ROS, including SO 4 − (30.2 μM), 1 O 2 (8.6 μM) and OH (5.8 μM). These ROS rapidly degraded 99.7% of BTA (20 mg/L) through the nanoconfined layer of hydrophilic membrane with an ultra-high flux of 2172 L m −2 h −1 in a super-fast time (∼195 ms). Surprisingly, the degradation rate constant k exhibited 3 to 5 orders of magnitude higher compared to conventional heterogeneous AOPs. Furthermore, the catalytic stability, degradation pathways and biological toxicity of BTA degradation were also evaluated. This membrane-based AOPs technique provides a new approach to overcome the limitations of conventional heterogeneous catalysis.
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ANALYTICA CHIMICA ACTA
·
2023
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IF 6.2
Yang Liu,Xueping Dang,Huaixia Chen
A molecularly imprinted polymer (MIP) monolithic column was prepared in situ in a pipette tip using phenol and bisphenol A as dual templates, 4-vinyl pyridine and β -cyclodextrin as bifunctional monomers . It was used for the selective and simultaneous solid phase extraction of eight phenolics, including phenol, m-cresol, p-tert-butylphenol, bisphenol A, bisphenol B, bisphenol E, bisphenol Z, and bisphenol AP. The MIP monolithic column was characterized by scanning electron microscopy, Fourier transform infrared spectroscopy , thermogravimetric analysis and nitrogen adsorption experiment. The results of selective adsorption experiments showed that the MIP monolithic column can selective recognize the phenolics and have excellent adsorption property. The imprinting factor for bisphenol A can be as high as 4.31, and the maximum adsorption capacity for bisphenol Z can reach 201.66 mg g −1 . Under the optimal extraction conditions, a selective and simultaneous extraction and determination method for eight phenolics was established based on the MIP monolithic column and high-performance liquid chromatography with ultraviolet detection. The linear ranges (LRs) of the eight phenolics were 0.5–200 μg L −1 , the limits of quantification (LOQs) and detection (LODs) were 0.5–2.0 μg L −1 and 0.15–0.67 μg L −1 . The method was applied to detect the migration quantity of the eight phenolics from polycarbonate cups and had satisfactory recovery. The method has the advantages of simple synthesis, short extraction time, as well as good repeatability and reproducibility, which provides a sensitive and reliable strategy for extracting and detecting phenolics from food contact material.
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PubMed
高影响因子
Water
·
2023
·Vol. 15
·期 12
·2243
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IF 3.4
Jing Wang,Quanfeng Wang,Pei Gao,Da Sun,Libo Jin,Li Ma,Lan Yang,Jujiao Zhao
Peroxymonosulfate (PMS) activation is an intriguing technology for refractory organic pollutant removal in wastewater treatment. Herein, a highly dispersed Mn-Ce bimetallic oxide on carbon nanotubes (MCC) was synthesized and applied to catalyze PMS for the degradation of phenol. The material was well characterized using a transmission electron microscope (TEM), N2adsorption–desorption isotherms, X-ray powder diffraction (XRD), and X-ray photoelectron spectroscopy (XPS). The synthesized MCC showed superior activity for PMS activation. Thekvalue of phenol removal with MCC is 0.135 min−1, which is greatly superior to that of CNT (6.17 × 10−5min−1) and Mn-Ce bimetallic oxide (3.18 × 10−4min−1). Electron paramagnetic resonance (EPR), along with radical quenching experiments, revealed that the activation of PMS by MCC for phenol degradation involves both radical and non-radical reaction pathways. Moreover, a synergic effect between Mn-Ce bimetallic oxide and CNT was identified to be responsible for the outstanding catalytic activity.Keywords:PMS activation;Mn-Ce bimetallic oxide;CNT;synergic effect
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MICROPOROUS AND MESOPOROUS MATERIALS
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2023
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IF 5.2
Zi-Wen Zhou,Zhe-Ning Wu,Chun-Xian Cai,Ru-De Lin,Xiao-Qi Yu,Kun Li,Na Wang
Covalent Organic Frameworks (COFs) with uniform aperture size, high surface area and tunable structure have been proposed as a potential material in water treatment. In this work, we utilized methoxy based covalent organic frameworks (COF–OMe) at room temperature as a dual-role smart material. For one thing, it can respond to the pH of solutions by visual, colorimetric change. Due to the protonation effect of methoxy groups in its pore skeleton, the fluorescent intensity of COF–OMe went down and the color changed from yellow to black as the pH decreased reversibly. For another, the abundant pores and ordered conjugated structure endowed it with a large surface area and light absorption ability. Therefore, the light-triggered oxidase-mimic porous COF–OMe can be applied in the synergistic removal of organic pollutants with synergistic physical absorption and light degradation. The outstanding and sensitive response to pH, great removal efficiency and dual function made it applied in water treatment with great potential, achieving killing two birds with one stone.
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RENEWABLE ENERGY
·
2023
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IF 8.7
Shanshuai Chen,Puxiang Yan,Xiaona Yu,Wanbin Zhu,Hongliang Wang
The development of a highly active and robust catalyst for the conversion of lignin, the largest volume of renewable aromatic resource in nature, to value-added aromatics is of great importance in sustainable chemistry. However, the condensation of lignin depolymerization intermediates into recalcitrant macromolecules restricts high yields of desired products, and this remains a great challenge in lignin valorization. Here, a serious of bifunctional Ru–ZnO/SBA-15 catalysts were synthesized for lignin conversion to aromatics. Roles of Ru and ZnO in these catalysts for lignin conversion were in-depth analyzed. The effect of the ratio of Ru to ZnO was studied. Other reaction conditions including temperature and time were systematically optimized. More than 51.3% yields of aromatics were obtained over Ru–10ZnO/SBA-15 at 240 °C for 4 h. Structure-activity relationship research of the catalyst revealed that the high yield of product could be attributed to the following three reasons: 1) the Lewis acidic sites on Ru/SBA-15 are significantly improved after ZnO modification, and thus promotes the C–O bond cleavage ; 2) the oxophilic ZnO is beneficial to absorb the substrate and reaction intermediates, and therefore enhances the hydrodeoxygenation activity of the adjacent Ru; 3). The interaction between Zn and Ru in Ru–ZnO/SBA-15 changes Ru electronic properties and leads to the formation of highly active catalytic sites with high electron density. These results indicated that the bifunctional Ru–ZnO/SBA-15 catalyst with high catalytic activity could be a good choice for lignin conversion to high-yield aromatics.
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Advanced Healthcare Materials
·
2023
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IF 10
Yutong Shao,Miaomiao Chen,Wenlong Chen,Zehui Wang,Mengzhang Sui,Mingyu Tian,Yingnan Wu,Jitao Song,Debin Ji,Fengling Song
Photodynamic therapy (PDT) uses photosensitizers to convert oxygen (O 2 ) to reactive oxygen species (ROS) under irradiation to induce DNA damage and kill cancer cells. However, the effect of PDT is usually alleviated by apoptosis resistance mechanism of tumor living cells. MTH1 enzyme is known to be such an apoptosis-resistance enzyme which is over expressed as a scavenger to repair the damaged DNA. In this work, a hypoxia-activated nanosystem FTPA, which can be degraded to release the encapsulated PDT photosensitizer 4-DCF-MPYM and an inhibitor TH588 is proposed. The inhibitor TH588 can inhibit the DNA repair process by reducing the activity of MTH1 enzyme, and achieve the purpose of amplifying the therapeutic effect of PDT. This work demonstrates that a precise and augmented tumor PDT is achieved by integration of hypoxia-activation and inhibition resistance of tumor cells to apoptosis.
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Catalysts
·
2022
·Vol. 12
·期 10
·1164
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IF 4.501
Haiqin Lu,Lu Gan
A series of biochar materials was prepared through pyrolyzing poplar wood powder waste under different pyrolyzing temperatures, which were afterwards characterized in detail. Then, the poplar powder biochar (PPB) was used to degrade bisphenol A (BPA) in water via activating peroxymonosulfate (PMS). The results indicate that the activation efficiency of the prepared PPB was correlated with its surface functional groups, which were regulated by its pyrolyzing temperature. Specifically, the biochar pyrolyzed at 600 °C (PPB-600) exhibited the optimal BPA removal activity, in which 0.5 g/L of PPB-600 could remove 0.02 mM of BPA within 120 min. From the results of scavenging tests, ESR analysis and probe pollutant degradation tests, it was inferred that the BPA was degraded by non-radical singlet oxygen in the PPB/PMS system. Since PPB consumed its surface oxygen functional groups and structural defects to activate PMS, the catalytic performance of PPB was gradually reduced after several cycles. This study can provide new insight for the design and preparation of metal-free biochar catalysts from waste wood precursor for the highly-efficient removal of refractory organic pollutants in water.Keywords:persulfate activation;biochar;wood powder waste;organic pollutant degradation;non-radical pathway
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Minxian Zhang,Xuecong Lin,Ziran Yi,Xiang Xu,Jingling Yang,Mingshan Zhu
Through visible light driven ligand-to-metal charge transfer (LMCT) with organic pollutant-semiconductor is a new method to promote reactive oxygen species (ROS) generation in water treatment. This study is the first time to use ciprofloxacin (CIP) pollutants induced LMCT on ZnO mesocrystal with rich oxygen vacancies (M-ZnO-OV) to improve ROS generation for CIP self-degradation. The results show an obviously increased intensity of HO • and O 2 •− through the LMCT process, leading to the optimal kinetic rate constant of 0.043 min –1 for CIP degradation, which is 7.5 times that of ZnO non-LMCT process. The presence of oxygen vacancies (OVs) in M-ZnO-OV leads to an electron-deficient Zn atom nearby OVs, promoting the formation of LMCT complex, and then resulting in rapid electron transfer from OVs to oxygen in water to generate ROS. The present investigation provides a new OVs-enhanced LMCT process to improve the concentration of ROS for water treatments.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Hao Du,Ningyi Li,Lingxuan Yang,Qiang Li,Guoxiang Yang,Qi Wang
Environmental crisis caused by Cr(VI) pollution has gained remarkable attention. Developing efficient photocatalysts for Cr(VI) remediation remains a great challenge. Herein, the Ag@Ag 3 VO 4 /Ag 3 PMo 12 O 40 (Ag@Ag 3 VO 4 /AgPMo) S-scheme heterojunctions were prepared via the combination of hydrothermal and photodeposition methods for Cr(VI) reduction. The resultant S-scheme heterojunctions were characterized to investigate their morphological, structural, photoelectrochemical and optical properties. The synergy of surface plasmon resonance (SPR) effect of Ag and S-scheme hetero-structure improved their photo(electro)chemical performance. Upon visible light irradiation, the optimized Ag@Ag 3 VO 4 /AgPMo delivered superior photoreduction efficiency (94.8%) of Cr(VI) and stability with a slight loss of the performance (92.8% after 6 cycles). The enhancement of Cr(VI) reduction performance may be ascribed to the extended light absorption range and separation and migration pathway of photo-induced electron-hole pairs confirmed by the proposed photoreduction mechanism. This work not only confirms a highly active catalytic system for the light-driven environmental application, but pave a way for the construction of S-scheme heterojunction photocatalysts.
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