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A study on singlet oxygen generation for tetracycline degradation via modulating the size ofα-Fe_(2)O_(3)nanoparticle anchored on g-C_(3)N_(4) nanotube photocatalyst

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Nano Research 2023年第2期16卷 2236-2244页

作者： Hongjie Zhu Minghui Li Luning Zou Youyou Hu Hongguo Hao Jianmin Dou Junjie Mao Shandong Provincial Key Laboratory of Chemical Energy Storage and Novel Cell Technology School of Chemistry and Chemical EngineeringLiaocheng UniversityLiaocheng 252059China Key Laboratory of Functional Molecular Solids Ministry of EducationCollege of Chemistry and Materials ScienceAnhui Normal UniversityWuhu 241002China State Key Laboratory of Pollution Control and Resource Reuse School of the EnvironmentNanjing UniversityNanjing 210023China Gaotang liguo chemical plant Liaocheng 252059China

Photocatalysis is considered as an effective technique for mitigating ecological risks posed by residual tetracycline(TC).To improve the efficiency of this technique,it is necessary to enable photocatalysts to produce highly reactive species,such as singlet oxygen(1O2).However,due to the high activation energy of 1O2,photocatalysts can hardly produce 1O2 without assistance from external ***,we find that the size-reducedα-Fe_(2)O_(3)nanoparticles(~4 nm)that anchored on g-C_(3)N_(4)nanotube(α-Fe_(2)O_(3)@CNNT)can spontaneously generate ^(1)O_(2) for degradation of *** comparison,only hydroxyl radical(·OH)can be produced by g-C_(3)N_(4)nanotube loaded with~14 nmα-Fe_(2)O_(3)nanoparticles(α-Fe_(2)O_(3)/CNNT).Owing to the high reactivity of the ^(1)O_(2) species,the photocatalytic degradation rate(Kapp)of TC withα-Fe_(2)O_(3)@CNNT(0.056 min^(−1))was 1.8 times higher than that ofα-Fe_(2)O_(3)/*** experimental results and theoretical calculations suggested that reducing the size ofα-Fe_(2)O_(3)nanoparticles anchored on g-C_(3)N_(4)nanotube decreased the surface electron density ofα-Fe_(2)O_(3),which induces the generation of high-valent Fe(IV)active sites overα-Fe_(2)O_(3)@CNNT and turns the degradation pathway into a unique ^(1)O_(2) dominated *** study provides a new insight on the generation of ^(1)O_(2) for effective degradation of environmental pollutant.

关键词： singlet oxygen degradation pathway high-valent Fe(IV) tetracycline degradation

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Cadmium sulfide cage photocatalysis coupled electroactive biofilm for synergistic promotion of tetracycline degradation and electricity production

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Journal of Materials Science & Technology 2023年第35期166卷 86-97页

作者： Z.S.Yuan J.X.Zou X.L.Zhao J.Y.Shi C.S.Guo M.Yan School of Chemistry and Chemical Engineering Harbin Institute of TechnologyHarbin 150001China

tetracycline(TC)as a common broad-spectrum antibiotic,has been frequently detected in soil and sur-face *** becomes a great threat to the ecological ***,a device of photocatalysis as-sisted microbial fuel cell(photo-MFC)was constructed for TC degradation and energy *** this photo-MFC,cadmium sulfide(CdS)cage photocatalysis can degrade most of TC in a short *** the Co_(3)O_(4)@C-CC(carbonization and calcination of the ZIF-67 precursor in-situ grown on the carbon cloth(CC))bioanode degrades the rest of TC as well as the photocatalytic products,thus improving the *** co-existence of photocatalysis with bioanode changes the microbial community structure of the *** dominant phylum is Geobacter(60.2%)in normal MFC while that in photo-MFC are Pro-teobacteria(43.5%)and Geobacter(33.2%).Therefore,the synergistic effect of photocatalytic degradation and biodegradation achieves a chemical oxygen demand(COD)removal of 98.6%,which is higher than that of normal MFC(77.6%)or single CdS cage photocatalysis(23.8%).In addition,the photogenerated electrons can be transferred to the cathode,which reduces their combination with holes and increases the electricity generation of MFC,achieving a maximum power density of 3.37 W/m^(2).After degradation,the effluent with 200 mg L^(−1) TC exhibits no visible ***,electrochemical test,finite-difference time-domain(FDTD),density functional theory(DFT)calculation and the free radical trapping experiments verify the possible mechanisms of photocatalytic degradation in this *** strat-egy paves a new way for low energy consumption removal and energy recovery of organic pollutants.

关键词： Photo-MFC CdS cage tetracycline degradation Mineralization Electricity production

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Mesoporous amorphous FeOOH-encapsulated BiO_(2–x) photocatalyst with harnessing broad spectrum toward activation of persulfate for tetracycline degradation

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Chinese Journal of Chemical Engineering 2024年第7期71卷 235-248页

作者： Pengfei Wu Zhaolong Liu Li Wu Yingkun Zhang Bing Wang Zhanghao Cheng Wenquan Cui Xiangyang Lv Qingling Liu Tianjin Key Laboratory of Indoor Air Environmental Quality Control School of Environmental Science and EngineeringTianjin UniversityTianjin 300350China Hebei Pollution Control Technology Innovation Center of Steel and Coking Industry Department of Environmental and Chemical EngineeringHebei College of Industry and TechnologyShijiazhuang 050091China Hebei Key Laboratory of Environmental Photocatalytic and Electrocatalytic Materials College of Chemical EngineeringNorth China University of Science and TechnologyTangshan 063210China Hebei Academy of Product Quality Supervision&Inspection Shijiazhuang 050227China

With the growing concern about the water environment,the advanced oxidation process of persulfate activation assisted by photocatalysis has attracted considerable attention to decompose dissolved organic *** this work,to overcome the drawbacks of the photocatalytic activity reduction caused by the photo-corrosion of non-stoichiometric BiO_(2–x),a novel material with amorphous FeOOH in situ grown on layered BiO_(2–x) to form a core-shell structure similar to popcorn chicken-like morphology was produced in two simple and environmentally beneficial *** a series of degradation activity tests of hybrid materials under different conditions,the as-prepared materials exhibited remarkable degradation activity and stability toward tetracycline in the FeOOH@BiO_(2–x)/Vis/PS system due to the synergism of photocatalysis and persulfate *** results of XRD,SEM,TEM,XPS,FTIR,and BET show that the loading of FeOOH increases the specific surface area and active sites appreciably;the heterogeneous structure formed by FeOOH and BiO_(2–x) is more favorable to the effective separation of photogenerated *** optimal degradation conditions were at a catalyst addition of 0.7 g·L^(–1),a persulfate concentration of 1.0 g·L^(–1),and an initial pH of 4.5,at which the degradation rate could reach 94.7%after 90 *** influence of typical inorganic anions on degradation was also *** studies and radical quenching experiments revealed that·OH,SO_(4)^(-)·,and·O_(2)^(-)were the principal active species generated during the degradation of *** results of the 1,10-phenanthroline approach proved that the effect of dissolved iron ions on the tetracycline degradation was limited,and the interfacial reaction that occurs on the active sites on the material's surface was a critical *** work provides a novel method for producing efficient broad-spectrum Bismuth-based composite photocatalysts and photocatalytic-activated persulfate synerg

关键词： Amorphous FeOOH BiO_(2–x) Activated persulfate Photocatalytic tetracycline degradation

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Synergistic CO_(2)reduction and tetracycline degradation by CuInZnS-Ti_(3)C_(2)T_(x)in one photoredox cycle

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Nano Research 2022年第9期15卷 8010-8018页

作者： Lijing Wang Zhan Zhang Renquan Guan Dandan Wu Weilong Shi Limin Yu Pan Li Wei Wei Zhao Zhao Zaicheng Sun Henan Engineering Center of New Energy Battery Materials Henan D&A Engineering Center of Advanced Battery MaterialsCollege of Chemistry and Chemical EngineeringInstitute of Architectural EngineeringShangqiu Normal UniversityShangqiu 476000China Faculty of Physics Faculty of ChemistryNortheast Normal UniversityChangchun 130024China Center of excellence for environmental safety and biological effects Beijing Key Lab for Green Catalysis and SeparationDepartment of Chemistry and Chemical EngineeringCollege of Environmental and Energy EngineeringBeijing University of TechnologyBeijing 100124China School of Material Science and Engineering Jiangsu University of Science and TechnologyZhenjiang 212003China

Optimizing photocatalytic CO_(2)reduction with simultaneous pollutant degradation is highly ***,the photocatalytic efficiency is restricted by the unmatched redox ability,high carriers’recombination rate,and lack of reactive sites of the present ***,the CuInZnS-Ti_(3)C_(2)T_(x)hybrid with matched redox ability and suitable CO_(2)adsorption property was rationally *** nucleation and growth process of CuInZnS was interfered by the addition of Ti_(3)C_(2)T_(x)with a negative charge,resulting in thinner nanosheets and richer reactive ***,the Schottky heterojunction built in the hybrid simultaneously improved the photoexcited charge transfer property,sunlight absorption range,and CO_(2)adsorption ***,upon exposure to sunlight,CuInZnS-Ti_(3)C_(2)T_(x)exhibited an efficient photocatalytic CO_(2)reduction performance(10.2μmol·h^(−1)·g^(−1))with synergetic tetracycline degradation,obviously higher than that of pure *** on the combination of theoretical calculation and experimental characterization,the photocatalytic mechanism was investigated *** work offers a reference for the remission of worldwide energy shortage and environmental pollution problems.

关键词： CuInZnS-Ti_(3)C_(2)T_(x) photocatalysis CO_(2)reduction tetracycline degradation

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Nonradical-dominated peroxymonosulfate activation through bimetallic Fe/Mn-loaded hydroxyl-rich biochar for efficient degradation of tetracycline

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Nano Research 2023年第1期16卷 155-165页

作者： Yihui Li Deying Lin Yongfu Li Peikun Jiang Xiaobo Fang Bing Yu State Key Laboratory of Subtropical Silviculture Zhejiang Agriculture and Forestry UniversityHangzhou 311300China School of Environment and Resources Zhejiang Agriculture and Forestry UniversityHangzhou 311300China

Biochar-based transition metal catalysts have been identified as excellent peroxymonosulfate(PMS)activators for producing radicals used to degrade organic ***,the radical-dominated pathways for PMS activation severely limit their practical applications in the degradation of organic pollutants from wastewater due to side reactions between radicals and the coexisting ***,bimetallic Fe/Mn-loaded hydroxyl-rich biochar(FeMn-OH-BC)is synthesized to activate PMS through nonradical-dominated *** as-prepared FeMn-OH-BC exhibits excellent catalytic activity for degrading tetracycline at broad pH conditions ranging from 5 to 9,and about 85.0%of tetracycline is removed in 40 *** on studying the influences of various anions(HCO_(3)^(−),NO_(3)^(−),and H_(2)PO_(4)^(−))show that the inhibiting effect is negligible,suggesting that the FeMn-OHBC based PMS activation is dominated by nonradical *** paramagnetic resonance measurements and quenching tests provide direct evidence to confirm that 1O2 is the major reactive oxygen species generated from FeMn-OH-BC based PMS *** calculations further reveal that the FeMn-OH sites in FeMn-OH-BC are dominant active sites for PMS activation,which have higher adsorption energy and stronger oxidative activity towards PMS than OH-BC *** work provides a new route for driving PMS activation by biochar-based transition metal catalysts through nonradical pathways.

关键词： biochar peroxymonosulfate activation tetracycline degradation advanced oxidation nonradical pathways

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Achieving high-efficient photocatalytic persulfate-activated degradation of tetracycline via carbon dots modified MIL-101(Fe)octahedrons

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Chinese Journal of Chemical Engineering 2024年第2期66卷 298-309页

作者： Hao Yuan Xinhai Sun Shuai Zhang Weilong Shi Feng Guo School of Material Science and Engineering Jiangsu University of Science and TechnologyZhenjiang 212003China School of Energy and Power Jiangsu University of Science and TechnologyZhenjiang 212003China

The synergistic reaction of photocatalysis and advanced oxidation is a valid strategy for the degradation of harmful antibiotic ***,carbon dots(CDs)modified MIL-101(Fe)octahedrons to form CDs/MIL-101(Fe)composite photocatalyst was synthesized for visible light-driven photocatalytic/persulfate(PS)-activated tetracycline(TC)*** electron spin resonance(ESR)spectra,scavenging experiment and electrochemical analysis were carried out to reveal that the high visible light-driven photocatalytic degradation activity of TC over CDs/MIL-101(Fe)photocatalysts is not only ascribed to the production of free active radicals in the CDs/MIL-101(Fe)/PS system(·OH,·SO_(4-),^(1)O_(2),h^(+)and·O_(2)^(-))but also attributed to the consumption of electrons caused by the PS,which can suppress the recombination of photo-generated carriers as well as strong light scattering and electron trapping effects of ***,the possible degradation pathways were proposed by analyzing intermediates via liquid chromatography-mass spectrometry *** research presents a rational design conception to construct a CDs/PS-based photocatalysis/advanced oxidation technology with high-efficient degradation activity for the remediation of organic antibiotic pollutant wastewater and for the improvement of carrier transport kinetics of photocatalysts.

关键词： Carbon dots MIL-101(Fe) Photocatalytic Persulfate activation tetracycline degradation

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Combination tanning mechanism inspired environmentally benign catalyst for efficient degradation of tetracycline

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Collagen and Leather 2023年第4期5卷 131-140页

作者： Meng Xiao Shuangmei Liu Wenqian Qi Yu Peng Qingyu Yan Hui Mao College of Chemical Engineering Sichuan UniversityChengdu 610065People's Republic of China College of Chemistry and Materials Science Sichuan Normal UniversityChengdu 610066People's Republic of China School of Materials Science and Engineering Nanyang Technological UniversitySingapore 639798Singapore

The utilization of chelation reaction between metals and tannins is a common tanning method in leather ***,a novel combination tanning mechanism inspired environmentally benign catalyst(CMBT-Fe^(0))was synthesized by immobilizing Fe nanoparticles onto bayberry tannin(BT)grafted chitosan microfibers(CM).The obtained catalyst featured a well-defined microfibrous structure,on which Fe^(0)nanoparticles were highly dispersed to exhibit exceptional catalytic activity for the degradation of tetracycline(TC).The catalytic activity of CMBT-Fe^(0)was 1.72 times higher than that of the commercial Fe^(0)nanoparticles without immobilization,with 95.03%of TC degraded within 90.0 *** CMBT-Fe^(0)catalysts were recycled 6 times,with the removal rate of TC maintained at 82.56%.Furthermore,a possible mechanism responsible for the catalytic removal of TC was provided by analyzing the catalytic degradation products via liquid chromatography-mass ***,our investigation successfully developed efficient catalysts to address the concerned environmental issue of antibiotic pollution.

关键词： Vegetable tannin Combination tanning Environmental catalyst tetracycline degradation

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Nitrogen-doped hollow mesoporous carbon spheres modified MnO2 with enhanced photocatalytic activity for the degradation of tetracycline

Nitrogen-doped hollow mesoporous carbon spheres modified MnO...

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中国化学会第十届全国无机化学学术会议

作者： Lan Ding Xiaojing Wang Inner Mongolia Key Laboratory of Chemistry and Physics of Rare Earth Materials School of Chemistry and Chemical EngineeringInner Mongolia University

Herein, the nitrogen-doped hollow mesoporous carbon spheres(N-HMCs) modified MnO was prepared by one-pot hydrothermal reaction. The nanocomposite was characterized by X-ray diffraction, scanning electron microscopy, transmission electron microscopy and X-ray photoelectron spectroscopy to study its micromorphology, structure, and chemical composition/states. The results revealed that N-HMCs play three vital roles in improving photocatalytic efficiency. First, N-HMCs could serve as a photosensitizer to enhance visible-light absorption. Second, N-HMCs is an excellent conductive material to transfer the photoexcited electrons quickly to hinder the electron-hole pairs recombination. Third, N-HMCs could provide more active sites in the photocatalytic process. Additionally, the N-HMCs@MnO composite exhibited high adsorption activity, high visible-light photocatalytic activity and good recyclability, suggesting the great prospects of the practical application of N-HMCs@MnO.

关键词： N-HMCs@MnO2 N-doped hollow carbon microspheres tetracycline degradation Photocatalysis

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Decoration of CdMoO_(4) micron polyhedron with Pt nanoparticle and their enhanced photocatalytic performance in N_(2) fixation and water purification

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Frontiers of Chemical Science and Engineering 2023年第12期17卷 1949-1961页

作者： Xujie Ren Junfeng Wang Shude Yuan Chunran Zhao Lin Yue Zhihao Zeng Yiming He Department of Materials Science and Engineering Zhejiang Normal UniversityJinhua 321004China Key Laboratory of Solid State Optoelectronic Devices of Zhejiang Province Zhejiang Normal UniversityJinhua 321004China Key Laboratory of the Ministry of Education for Advanced Catalysis Materials College of Chemistry and Materials ScienceZhejiang Normal UniversityJinhua 321004China

This study aimed to prepare and apply a novel Pt/CdMoO_(4) composite photocatalyst for photocatalytic N2 fixation and tetracycline degradation. The Pt/CdMoO_(4) composite was subjected to comprehensive investigation on the morphology, structure, optical properties, and photoelectric chemical properties. The results demonstrate the dispersion of Pt nanoparticles on the CdMoO_(4) surface. Close contact between CdMoO_(4) and Pt was observed, resulting in the formation of a heterojunction structure at their contact region. Density functional theory calculation and Mott-Schottky analysis revealed that Pt possesses a higher work function value than CdMoO_(4), resulting in electron drift from CdMoO_(4) to Pt and the formation of a Schottky barrier. The presence of this barrier increases the separation efficiency of electron-hole pairs, thereby improving the performance of the Pt/CdMoO_(4) composite in photocatalysis. When exposed to simulated sunlight, the optimal Pt/CdMoO_(4) catalyst displayed a photocatalytic nitrogen fixation rate of 443.7 μmol·L‒^(1)·g‒^(1)·h‒^(1), which is 3.2 times higher than that of pure CdMoO_(4). In addition, the composite also exhibited excellent performance in tetracycline degradation, with hole and superoxide species identified as the primary reactive species. These findings offer practical insights into designing and synthesizing efficient photocatalysts for photocatalytic nitrogen fixation and antibiotics removal.

关键词： photocatalytic N2 fixation Pt CdMoO4 tetracycline degradation Schottky barrier

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In situ meso-tetra(4-carboxyphenyl)porphyrin ligand substitution in Hf-MOF for enhanced catalytic activity and stability in photoredox reactions

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Rare Metals 2024年第6期43卷 2682-2694页

作者： Jie Hu Hong-Xin Lao Xiu-Wu Xu Wei-Kang Wang Le-Le Wang Qin-Qin Liu School of Materials Science and Engineering Jiangsu UniversityZhenjiang 212013China College of Chemistry and Materials Engineering Research Center of Carbon NeutralityAnhui Normal UniversityWuhu 241002China Fujian Provincial Key Laboratory of Ecology-Toxicological Effects and Control for Emerging Contaminants Putian UniversityPutian 351100China

Though there are numerous intrinsic merits of metal-organic frameworks(MOFs),low charge separation efficiency has imposed heavy restrictions on their photocatalytic ***,in situ porphyrin ligand substitution,as a strategy for improving the charge separation efficiency and increasing the amounts of active sites,has been designed and realized in a Hf-biphenyl dicarboxylic acid(BPDC)***,a size and geometry matched meso-tetra(4-carboxyphenyl)porphyrin(TCPP)ligand was selected and doped into Hf-BPDC MOF by forming coordinating bonds with Hf centers,forming dualligand Hf-BPDC-TCPP *** resultant Hf-BPDC-TCPP MOF showed significantly improved activity and chemical stability in the photocatalytic H_(2)generation(261μmol·g^(-1)·h^(-1))and tetracycline(TC)degradation reactions(95.8%),which was 48 and 1.47 folds higher than that of the Hf-BPDC *** and electrochemical studies revealed that the introduction of porphyrin ligand could generate a stronger internal electric field for boosting the charge separation and transfer,increase the specific surface area for providing more active sites,and narrow the band gap to enhance the visible light *** in situ ligand substitution method provides a promising approach to build a tunable platform for constructing high-performance MOF photocatalysts.

关键词： Ligand substitution Metal organic frameworks Meso-tetra(4-carboxyphenyl)porphyrin Hydrogen evolution reaction tetracycline degradation

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