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NEW JOURNAL OF CHEMISTRY · 2024 · IF 2.7

Facile synthesis of an α-Bi2O3/BiO2 heterojunction for enhanced piezoelectric catalytic degradation of dye wastewater

Yuanwen Hou,Jia Tang,Li Jiang,Ning Xie,Hongquan Fu,Juan Zhang,Hejun Gao,Bin Xu,Yunwen Liao

Piezocatalytic technology represents an innovative form of advanced oxidation technology for degradation of organic pollutants. Piezoelectric catalysis technology combines electrochemistry and piezoelectric properties, and promotes charge transfer through a piezoelectric field, thus promoting catalytic reactions. This study employed a one-step microwave method to fabricate an α-Bi2O3/BiO2 heterojunction with a narrow bandgap. This catalyst exhibited a high efficiency in the degradation of methyl orange dye, achieving a removal rate of 93% in 60 minutes, with a reaction rate constant of 0.0324 min−1. The investigation of the catalytic mechanism demonstrates that the construction of the α-Bi2O3/BiO2 heterojunction facilitates the separation of charge carriers, increases the degree of polarization, and consequently enhances the efficiency of piezoelectric catalytic degradation. This work opens the way for the design and development of high-performance piezoelectric catalysts.

CAS / MDL: 56-81-5
研究领域: 环境科学 · 材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2021 · IF 7.312

Efficient degradation of phenolic wastewaters by a novel Ti/PbO2-Cr-PEDOT electrode with enhanced electrocatalytic activity and chemical stability

Qian Zhou,Derong Liu,Guoyuan Yuan,Yi Tang,Kuncheng Cui,Songshan Jiang,Yongde Xia,Wei Xiong

Novel Ti/PbO 2 -Cr-PEDOT electrodes were prepared by electrodeposition for electrochemical degradation of phenolic wastewater. The electrodes were characterized by XRD, SEM-EDS, XPS, and FT-IR to study the crystalline, surface morphology, elements distribution, and microstructure of the electrodes. A flat and compact interface was obtained with Cr and PEDOT doping into β-PbO 2 plate by electrodeposition method. The linear sweep voltammetry (LSV) and electrochemical impedance spectroscopy (EIS) were conducted to explore the electrochemical performance of the prepared electrodes. The Ti/PbO 2 -Cr-PEDOT electrode exhibited a higher oxygen evolution potential (OEP, 2.53 V vs SCE) and a lower charge transfer resistance compared with Ti/PbO 2 . Phenol degradation efficiency of 100% and TOC removal rate of 95.02% were achieved in the electrochemical degradation of phenol within 120 min. The optimal process parameters (phenol concentration = 1000 mg·L -1 , electrolyte concentration = 4.0 g·L -1 , current density = 15 mA·cm −2 and electrode distance = 3 cm) in the process of electrochemical oxidation of phenol wastewater were explored. Active species trapping experiments proved that ·OH radicals played an important role in the electrochemical system. Furthermore, the electrode also showed high activity for the degradation of other phenolic wastewaters such as phloroglucinol (η DEP  = 100%), bisphenol A (η DEP  = 97.17%) and p-chlorophenol (η DEP  = 89.77%) within 60 min. A possible degradation pathway was proposed based on the intermediate products determined by HPCL. The Ti/PbO 2 -Cr-PEDOT electrode showed excellent stability with only 3% loss of degradation efficiency (η DEP  = 96.95%) after recycling tests for 5 times. These results suggest that Ti/PbO 2 -Cr-PEDOT is a promising electrode for electrochemical degradation of phenolic wastewaters.

研究领域: 环境科学 · 电化学工程
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COLORATION TECHNOLOGY · 2023 · IF 1.8

Iron(III) complexes promote hydrogen peroxide activation for efficient degradation of dyeing wastewater

Shouying Wu,Linping Zhang,Jianing Fan,Wei Wu,Bolin Ji,Xueling Feng,Bijia Wang,Yimeng Ma,Yi Zhong,Hong Xu,Zhiping Mao

Coordination complexes were widely used in advanced oxidation processes. The ligands with various substituents could lead to differences in the catalytic properties and mechanisms. In this work, the iron(III)–N,N′-dipicolinamide (FeL) complexes (the iron(III) complexes with substituents –CH 3 , –H, –Cl and –NO 2 named as FeL1, FeL2, FeL3 and FeL4, respectively) were used to activate hydrogen peroxide (H 2 O 2 ) for degrading dyes wastewater. Mechanism studies indicated that the FeL4/H 2 O 2 system contains the Fe V =O in addition to the same • OH and O 2 •− as the other systems, which made it exhibit more excellent performance than others. The results of the performance tests showed that the FeL4/H 2 O 2 system could remove 97%, 89%, 100%, 83%, 100%, and 99% of RR195, RY145, RB194, RB19, MB, and RhB, respectively, which proved the good application performance of the FeL4/H 2 O 2 system. In addition, the performance of the FeL4/H 2 O 2 system was not influenced by anions and natural organics. This study verified the feasibility of modulating the catalytic performance of the complexes by changing the substituents and provided an efficient catalytic system for dyeing wastewater treatment.

研究领域: 环境科学 · 化学
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APPLIED SURFACE SCIENCE · 2020 · IF 6.182

The favourable synergistic operation of photocatalysis and catalytic oxygen reduction reaction by a novel heterogeneous CoFe2O4-TiO2 nanocomposite

Qiong Sun,Songhao Wu,Kaijing Li,Bing Han,Yingjie Chen,Beili Pang,Liyan Yu,Lifeng Dong

The improved photocatalytic activity of TiO 2 with the addition of spinel CoFe 2 O 4 as an effective catalyst for O 2 reduction reaction (ORR) is studied and proved in this study. CoFe 2 O 4 -TiO 2 heterostructure nanoparticles are prepared by a reflux condensation and two-step hydrolysis-hydrothermal method. The addition of trace CoFe 2 O 4 onto TiO 2 can improve its affinity to O 2 , generate a faster transportation of photo-induced carriers, but hardly affect band structure. With an appropriate amount of CoFe 2 O 4 to TiO 2 , a remarkable acceleration occurs in photocatalytic decolorization of dye wastewater, and the calculated apparent kinetic constant ( k app ) of the composite (0.020 min −1 ) is 2.4 and 5.6 times of pure TiO 2 (0.0085 min −1 ) and CoFe 2 O 4 (0.0036 min −1 ), respectively. Quenching experiments with different radical scavengers show that O 2 –∙ is the key oxidative radical in all photocatalytical reactions. Meanwhile, the rapid growth of O 2 –∙ production by CoFe 2 O 4 -TiO 2 is proved to be a major cause for photocatalytic performance improvement. Furthermore, an improved electrochemical ORR catalytic ability by CoFe 2 O 4 -TiO 2 is verified and the 2-plus-2 electron route generates the same product (H 2 O 2 ) as the photocatalytic process. Therefore, the synergistic operation of photocatalytic and catalytic ORR process by CoFe 2 O 4 -TiO 2 resulted in a rapid degradation of dye wastewater.

CAS / MDL: 101-84-8 112-90-3
研究领域: 材料科学 · 环境科学
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH · 2023 ·Vol. 31 ·期 4 ·6511-6526 · IF 5.8

Efficient degradation of cellulosic ethanol wastewater by perovskite activation of Sr element A-site doped lanthanide copper chalcogenide materials

Huang Likun,Wang Huixian,Wang Guangzhi,Mu Deying,Hou Yue,Di Xinyi,Zhou Simin,Wang Dongdong,Wang Dandan

The degradation of cellulosic ethanol wastewater by peroxymonosulfate (PMS) is one of the important methods to solve the environmental problems caused by it. In order to improve the degradation efficiency of cellulosic ethanol wastewater, the design of more catalytically active and stable chalcogenide catalysts has become a problem that needs to be solved nowadays. The application of foreign cations to replace the A- or B-site to increase the oxygen vacancy of the chalcocite catalyst to improve the efficiency of chalcocite catalytic degradation of wastewater has received much attention. In this work, the perovskite material LaCuO 3 was synthesized using a citric acid-sol–gel method, and the novel material La 1-x Sr x CuO 3 was prepared by doping of Sr element at the A position. In order to prepare catalytic materials with better performance, this study carried out performance-optimized degradation experiments on the prepared materials and determined that the catalytic efficiency of La 0.5 Sr 0.5 CuO 3 prepared under the conditions of the complexing agent dosage of 1:2, the gel temperature of 80 °C, and the calcination temperature of 700 °C was better than that of the catalytic materials prepared under other conditions. The prepared material has good recycling function; after four times recycling, the removal rate of pollutant COD is still more than 85%. This work provides a new synthesis method of perovskite material with good recycling function and high catalytic efficiency for the degradation technology of cellulosic ethanol wastewater. Graphical Abstract

研究领域: 环境科学 · 材料科学
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Materials Today Communications · 2024 · IF 3.7

Construction of Z-scheme ZnO/g-C3N4 photocatalytic systems for degradation of dyeing wastewater

Lijuan Wang,Yinghan Li,Jun Cai,Shuqing Liu,Zifan Yuan,Depeng Gao

A novel heterogeneous nanocomposite photocatalyst ZnO/g-C 3 N 4 was fabricated by secondary high-temperature calcination using g-C 3 N 4 and ZnO as raw materials and characterized by XRD , SEM , TEM, EDS , FT-IR, Zeta potential , UV-Vis and XPS . The results displayed that the ZnO/g-C 3 N 4 components were tightly bound, evenly distributed and significantly reduced in size, which could provide more active sites. The heterogeneous types, photocatalytic performance, degradation mechanism of ZnO/g-C 3 N 4 for dyeing wastewater were speculated by REDOX potential, heterojunction , and quenching experiments. The degradation efficiency of ZnO/g-C 3 N 4 on MB was much higher compared with that of single ZnO, g-C 3 N 4 and the mechanical mixture of ZnO and g-C 3 N 4 , which can reach more than 95% at 60 min. The degradation rate was also significantly improved, with the degradation rate exceeding 50% at 20 min. The composite ZnO/g-C 3 N 4 could degraded 90% MB after 5 cycles. The quenching experiment showed that hydroxyl (·OH) and photogenerated hole (h + ) played the main role in the reaction process. It was confirmed that the prepared ZnO/g-C 3 N 4 formed a Z-scheme photocatalytic system by examining the transfer paths of e - and h + in various types of heterojunction and contrasting the CB and VB energy levels with the REDOX potentials of ZnO and g-C 3 N 4 . The Z-Scheme ZnO/g-C 3 N 4 photocatalyst has the characteristics of stability, reusability, and no by-product, making it an ideal choice for environmental purification.

CAS / MDL: 64-17-5
研究领域: 环境科学 · 材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Degradation of pyrazole wastewater by electro-peroxone with fluidized N-doped electrodes: Dual-zone synergistic catalytic reaction

Hongwei Zhu,Yijie Cheng,Jingjing Zhu,Weiqing Han,Xu Yin,Wei Li,Liankai Gu,Zhifeng Gao,Haoming Chen,Kajia Wei

The electro-peroxone (E-P) technology exploits in-situ generated H 2 O 2 to drive the peroxone reaction, which not only improves degradation efficiency but also utilizes wasted O 2 in the process of O 3 generation. However, limited by the cathodic interface reaction, a quantity of O 3 diffused into the bulk solution could not be effectively utilized. To address this problem, a dual-zone E-P process was proposed in combination with nitrogen-doped granular activated carbon (GAC (N) ) and a 2 electron-oxygen reduction reaction (2e-ORR) system, i.e., the E-GAC (N) -P system. Combining EPR and quenching experiments, the addition of GAC (N) was proven to alter the ·OH-dominated reaction routine of E-P to the ·OH and ·O 2 – synergistic routine, which achieved a high pollutant removal efficiency of up to 98.75 % and a reaction rate constant of 0.3838 min −1 (3.5 times that of the traditional E-P system). In terms of the mineralization mechanism, the E-GAC (N) -P system not only effectively inhibited the accumulation of intermediate products but also increased the total organic removal by 63.94 %. Moreover, the efficient removal of COD in actual wastewater also confirmed that the E-GAC (N) -P system had excellent mass transfer efficiency and 36.9 % lower electric energy consumption than did the traditional E-P system, indicating good practical application prospects.

CAS / MDL: 9002-84-0
研究领域: 环境科学 · 化学工程
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ACS Sustainable Chemistry & Engineering · 2021 · IF 8.198

Experimental and Theoretical Study on Glycolic Acid Provided Fast Bio/Seawater-Degradable Poly(Butylene Succinate-co-Glycolate)

Han Hu,Jiayi Li,Ying Tian,Chao Chen,Fenglong Li,Wu Bin Ying,Ruoyu Zhang,Jin Zhu

The very slow degradation of biodegradable polymers in the marine environment is due to the lack of dedicated degradation enzymes in open seas. As a result, introducing monomers that have a fast hydrolysis process is required to accelerate seawater degradation. Poly(butylene succinate-co-glycolate) (PBSGA) copolyesters with glycolic acid (GA) units ranging from 5 to 40% were synthesized by our newly developed polymerizing method based on oligo(glycolic acid). The results of 1H-NMR and GPC revealed that short GA segments were evenly distributed between BS segments, obtaining random copolyesters with a weight-average molecular weight over 6.24 * 104 g/mol. The copolymerized GA units hinder its crystallization capability and increase hydrophilicity of the PBSGAs, which still displayed mechanical properties comparable or even better than most biodegradable polymers. Fast degradation in seawater and enzymatic environments (Candida antarctica lipase B enzymes) is proved experimentally. The quick decomposition in seawater was originated from accelerated hydrolysis. For instance, the weight loss of PBSGA40 (compositions of GA units) exceeded 22% after 49 days. Possible degradation mechanisms were proposed based on Fukui function analysis and frontier molecular orbital calculation. Additionally, the energy barrier for hydrolysis was calculated by the density functional theory method, indicating that the hydrolysis of the polymer chain became more and more easy with the increase in GA units. At last, the addition of GA units only had a mild effect on the shelf life of the PBSGAs.

研究领域: 材料科学 · 环境科学 · 生物学
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Small · 2024 · IF 13

Simultaneous Efficient Photocatalytic Hydrogen Evolution and Degradation of Dye Wastewater without Cocatalysts and Sacrificial Agents Based on g-C3N5 and Hybridized Ni-MOF Derivative-CdS-DETA

Yongzhuo Yu,Wei Li,Yuxin Huang,Huixing Yang,Chaoyu Lv,Hui xiang Yan,Di Lin,Shichao Jiao,Linlin Hou,Zhiliang Wu

Inspired by energy conversion and waste reuse, hybridized Ni-MOF derivative-CdS-DETA/g-C 3 N 5 , a type-II heterojunction photocatalyst, is synthesized by a hydrothermal method for simultaneous and highly efficient photocatalytic degradation and hydrogen evolution in dye wastewater. Without the addition of cocatalysts and sacrificial agents, the optimal MOF-CD(2)/CN5 (i.e. Ni-MOF derivative-CdS-DETA (20 wt.%)/g-C 3 N 5 ) exhibit good bifunctional catalytic activity, with a H 2 evolution rate of 2974.4 µmol g −1 h −1 during the degradation of rhodamine B (RhB), and a removal rate of 99.97% for RhB. In the process of H 2 -evolution-only, triethanolamine is used as a sacrificial agent, exhibiting a high H 2 evolution rate (19663.1 µmol g −1 h −1 ) in the absence of a cocatalyst, and outperforming most similar related materials (such as MOF/g-C 3 N 5 , MOF-CdS, CdS/g-C 3 N 5 ). With the help of type-II heterojunction, holes are scavenged for the oxidative degradation of RhB, and electrons are used in the decomposition of water for H 2 evolution during illumination. This work opens a new path for photocatalysts with dual functions of simultaneous efficient degradation and hydrogen evolution.

研究领域: 材料科学 · 环境科学 · 化学
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RSC Advances · 2023 ·Vol. 13 ·期 5 ·2993-3003 · IF 3.9

Bi2O3 modified TiO2 nanotube arrays and their application towards unsymmetrical dimethylhydrazine degradation in wastewater by electroassisted photocatalysis

YiZhi Zeng,Feng Zhou,Yuan Gao

In the present research, the preparation process parameters of TiO2 nanotube arrays (TNAs) prepared by anodic oxidation were systematically studied by the orthogonal experimental method for the first time. Herein, the parameters of nine factors were optimized; the optimal parameters were: the electrolyte was a 0.2 mol L−1 NaF solution with 3% vol H2O at pH 7, the anodic oxidation voltage was 40 V, the electrode spacing was 4 cm and the reaction was carried out for 60 minutes. The physicochemical properties of the materials were characterized by SEM, XRD, EDS, UV-vis, and PL spectroscopy. By electrodeposition of Bi2O3 modified TNAs, the degradation rate of unsymmetrical dimethylhydrazine (UDMH) wastewater on the TNAs-10 was 89.14% within 10 h, which was 2.69 times that on pure TNAs. A bias potential of +0.3 V (vs. open circuit potential) was applied to the modified TNAs-10. The degradation rate of UDMH was significantly enhanced on the TNAs-10 (bias) process as compared to the TNAs-10 process. The degradation rate of UDMH wastewater on TNAs-10 (bias) exhibited an exponential distribution. UDMH and its toxic by-products FDMH, NDMA were completely degraded after 8 h.

研究领域: 环境科学 · 材料科学
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2024 · IF 7.7

Construction of mechanically robust and recyclable catalytic hydrogel based on hydroxypropyl cellulose-supported by montmorillonite/ionic liquid with different anions for pollutants(4-NP, MB, CR, Rhb) degradation

Xikun Zhang,He Zhang,Xue Lv,Ting Xie,Junzheng Chen,Di Fang,Shurui Yi

Dye wastewater poses a serious threat to the environment and human health, necessitating sustainable degradation methods. In this study, Na-based Montmorillonite (MMT) was exfoliated using different ionic liquids ([C16MIM][Cl], [C16MIM][BF 4 ], [C16MIM][PF 6 ]), and silver nanoparticles (Ag NPs) were green-synthesized using hydroxypropyl cellulose (HPC). The HPC significantly enhanced the dispersion of MMT in the hydrogel. By introducing lauryl methacrylate (LMA), a hydrophobic associative network was constructed in PAM/LMA/HPC/MMT@ILs&Ag NPs hydrogel. This hydrogel demonstrated outstanding mechanical properties, with a stress of 833.21 kPa, strain of 3300 %, and toughness of 14.36 MJ/m 3 . It also exhibited excellent catalytic activity, with a rate constant of 0.83 min −1 for 4-nitrophenol degradation at 28 °C. The effects of temperature and catalyst concentration on the catalytic reaction were systematically investigated. This study presents a simple green synthesis approach for Ag NPs using HPC, achieving superior mechanical performance and stable MMT dispersion in aqueous solutions.

研究领域: 材料科学 · 环境科学 · 纳米技术
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Journal of Environmental Chemical Engineering · 2022 · IF 7.968

Deactivation characteristics of Ce-modified Cu-based carbon materials for catalytic wet air oxidation of phenol wastewater

Guoqiang Li,Siqi Chai,Guojie Zhang,Jun Liu,Yongfa Zhang,Yongkang Lv,Ying Wang,Yuqiong Zhao

In this paper, Ce-modified Cu-based carbon materials (Cu-Ce/AC) were prepared by impregnation method using walnut shell as the carbon precursor, Cu-ammonia solution as Cu source and Ce as modifier. The catalytic wet air oxidation (CWAO) degradation of phenol wastewater was carried out in a self-assembled fixed-bed reactor. The stability of Cu-Ce/AC catalyst under different pH conditions was studied. This study combines XRD, BET, FT-IR, ICP-OES and XPS characterization techniques to study the main reasons for the deactivation of Cu-Ce/AC catalysts. The reaction mechanism of Cu-Ce/AC catalytic wet air oxidation degradation of phenol was clarified. The result indicates that although phenol was completely converted in the CWAO process, the acidic intermediate product produced were difficult to completely degraded. Therefore, the pH of the solution gradually decreased. In acidic environment, the interaction between active component Cu and carbon carrier is weak, resulting in a large amount of metal leaching into the solution. As a result, the COD conversion gradually decreases. The alkaline environment can effectively slow down the leaching of catalyst Cu while maintaining its high catalytic activity . In addition, the incompletely degraded intermediate products are easy to accumulate and deposit on the Cu-Ce/AC surface, block the micropores and cover the surface-active sites, which reduces the catalyst activity. The study also found that there is a redox cycle between Cu + , Cu 2+ Ce 3+ and Ce 4+ during phenol degradation, which enables Cu and Ce to form a strong interaction. The redox cycle can also promote the formation of oxygen vacancy (h + ), O 2 − ·, and HO·, making the degradation of phenol more thorough. At the same time, the mutual conversion between metal lattice oxygen and surface chemisorbed oxygen can generate high concentration of oxygen defect sites, which can improve the oxygen storage capacity of Cu-Ce/AC. These oxygen vacancies also provide more reactive sites to further promote adsorption and catalytic oxidation degradation of phenol and intermediate products.

研究领域: 环境科学 · 催化材料
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