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Chinese Chemical Letters 2024年第3期35卷 149-152页

作者： Yujie Zhang Siyi Liu Dongdong Chen Xing Xu School of Environmental Science and Engineering Shandong UniversityQingdao 266237China

Fabrication of single atom catalysts(SACs)by a green and gentle method is important for their practical fenton-like use.In this work,a high effective iron-based catalyst was prepared from the iron-rich Enteromorpha for NPX degradation via peroxymonosulfate(PMS).Both Fe-SACs and iron-clusters was fabricated from the intrinsic iron element in Enteromorpha after the urea saturation.The Fe-SACs/clusters can achieve 100%of NPX oxidation within 20 min with the k_(obs)of 0.282 min^(-1).Quenching tests indicated that the radical pathways were not dominated in the catalytic systems,and strong electron transfer process can be induced in the Fe-SACs/clusters+PMS system by using the NPX as electron donor and FeSACs/clusters/PMS^*complexes as electron acceptor.This result was consistent with the phenomenon observed in the galvanic oxidation system.In addition,the Fe-SACs/clusters was deposited onto the ceramic membrane(CM)by the spraying-crosslinking process to form a Fe-SACs/clusters@CM,which showed an effective and continuous NPX degradation in a heterogeneous PMS system.

关键词： SACs Iron Clusters fenton-like reaction Enteromorpha

Understanding the intrinsic synergistic mechanism between Pt-O-Ti interface sites and TiO_(2) surface sites of Pt/TiO_(2) catalysts in fenton-like reaction

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Science China Chemistry 2022年第12期65卷 2596-2603页

作者： Yawen Ma Huibin Ge Siwen Yi Man Yang Dan Feng Yujing Ren Jie Gao Yong Qin Interdisciplinary Research Center of Biology&Catalysis School of Life SciencesNorthwestern Polytechnical UniversityXi’an710072China School of Materials Science and Engineering Xi’an University of TechnologyXi’an710048China Analytical&Testing Center Northwestern Polytechnical UniversityXi’an710072China State Key Laboratory of Coal Conversion Institute of Coal ChemistryChinese Academy of SciencesTaiyuan030001China

Identifying the active site of oxide-supported metal catalysts and revealing the intrinsic synergistic mechanism between metal and oxide support remain a large challenge.Herein,we report the identification and separation of the Pt-O-Ti interface and TiO_(2) surface in Pt-TiO_(2)-based catalysts by depositing different thickness of TiO_(2) shell with∼0.4-nm micropores onto the surface of Pt/TiO_(2) catalyst through atomic layer deposition(ALD).In the oxidation of 3,3′,5,5′-tetramethylbenzidine(TMB)by hydrogen peroxide(H_(2)O_(2))process,the TiO_(2) microporous shells can prevent the contact between TMB and embedded Pt clusters,but not delay the diffusion of H_(2)O_(2).The heterolysis of H_(2)O_(2) to ·OH occurs on the Pt-O-Ti interface,and the generated•OH migrates to the TiO_(2) surface to supplement the surface lattice oxygen,which sequentially oxidizes TMB to oxTMB.And the synergistic effect between Pt-O-Ti interface active sties and TiO_(2) surface active sites can significantly improve the catalytic performance.Our study provides a guide for the understanding of the intrinsic synergistic mechanism between the metal and oxide support in the metal-oxide catalysts.

关键词： Intrinsic synergistic mechanism Pt-O-Ti interface site TiO_(2)surface site fenton-like reaction metal-oxide catalyst

Crystallinity engineering of Au nanoparticles on graphene for in situ SERS monitoring of fenton-like reaction

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Chinese Chemical Letters 2022年第3期33卷 1263-1266页

作者： Danni Guo Lixia Zhao Hui Zhang State Key Laboratory of Environmental Chemistry and Eco-toxicology Research Center for Eco-environmental SciencesChinese Academy of SciencesBeijing 100085China College of Resources and Environment University of Chinese Academy of SciencesBeijing 100049China State Key Laboratory of Water Environment Simulation School of EnvironmentBeijing Normal UniversityBeijing 100875China

Fabrication of multifunctional nanoplatform to in situ monitor fenton reaction is of vital importance to probe the underlying reaction process and design high-performance catalyst. Herein, a hybrid catalyst comprising of single-crystalline Au nanoparticles (SC Au NPs) on reduced graphene oxide (RGO) sheet was prepared, which not only exhibited an excellent ^(1)O_(2) mediated fenton-like catalytic activity in promoting rhodamine 6G (R6G) degradation by activating H_(2)O_(2), but also displayed a sensitive surface-enhanced Raman spectroscopy (SERS) detection performance to R6G with a linear response range from 1.0×10^(-8) mol/L to 1.0×10^(-5) mol/L thus providing a powerful and versatile nanoplatform for in situ SERS monitoring fenton-like catalytic reaction. The integration of catalytic and SERS activities into a single nanostructure are expected to provide great potentials for practical applications in environmental catalysis.

关键词： Au nanoparticle Crystallinity engineering fenton-like reaction SERS monitoring Environmental remediation

Comparative studies on fenton-like reactions catalyzed by Fe_(3)O_(4) loaded inside and outside halloysite nanotubes for the removal of organic pollutants

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Frontiers of Materials Science 2024年第1期18卷 15-28页

作者： Yang Li Jia-Qi Zhou Huan-Yan Xu Li-Min Dong Mao-Chang Cao Lian-Wei Shan Li-Guo Jin Xiu-Lan He Shu-Yan Qi Heilongjiang Provincial Key Laboratory of CO2 Resource Utilization and Energy Catalytic Materials School of Materials Science and Chemical EngineeringHarbin University of Science and TechnologyHarbin 150040China

In this work,Fe_(3)O_(4) nanoparticles(NPs)loaded inside and outside halloysite nanotubes(HNTs)were prepared and developed as the heterogeneous fenton-like catalysts for the removal of representative organic pollutants.Characterization results indicated that the samples with Fe_(3)O_(4) NPs loaded outside the HNTs lumen(Fe_(3)O_(4)/HNTs)and inside the HNTs lumen(Fe_(3)O_(4)@HNTs)were successfully prepared.Both samples had typical magnetic hysteresis loops,while Fe_(3)O_(4)@HNTs exhibited higher magnetization intensity.The comparative experiments showed that Fe_(3)O_(4)@HNTs had better fenton-like catalytic ability than that of Fe_(3)O_(4)/HNTs in the degradation of various organic pollutants.Taking Rhodamine B(RhB)as an example,the adsorption thermodynamics and kinetics of RhB onto Fe_(3)O_(4)/HNTs and Fe_(3)O_(4)@HNTs were also investigated.The comparative results demonstrated that the adsorption ability of Fe_(3)O_(4)/HNTs was better than that of Fe_(3)O_(4)@HNTs.Moreover,the dissolved concentration of Fe^(2+)and production amount of hydroxyl radical(·OH)in the Fe_(3)O_(4)@HNTs-H_(2)O_(2) system were significantly higher than those in the Fe_(3)O_(4)/HNTs-H_(2)O_(2) system.Based on aforementioned comparison,the nano-confinement effect in the Fe_(3)O_(4)@HNTs-H_(2)O_(2) system was verified.This work provides meaningful guidance for the cheap and convenient design of nanoreactors for fenton-like applications.

关键词： Fe_(3)O_(4) halloysite nanotube adsorption fenton-like reaction mechanism

Synergetic PVA degradation and H2 evolution in photocatalytic fuel cells using Ag@Fe_(2)O_(3) cathode

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Frontiers of Chemical Science and Engineering 2024年第1期18卷 85-93页

作者： Likun Sun Kesi Xiong Baoning Zhang Jinghong Fang Yingchao He Min Wang Zhixing Gan Fanglin Du Qiong Sun Liyan Yu Lifeng Dong College of Materials Science and Engineering Qingdao University of Science and TechnologyQingdao 266042China Center for Future Optoelectronic Functional Materials School of Computer and Electronic InformationNanjing Normal UniversityNanjing 210023China Department of Physics Hamline UniversitySt.Paul 55104USA

In a dual-chamber photocatalytic fuel cell device,polyvinyl alcohol degradation and H2 evolution were concurrently achieved.The setup involved commercial P25 as the photoanode and Ag@Fe_(2)O_(3) nanoparticles as the cathode.Additionally,the feasibility of a fentonlike reaction in the cathode,utilizing Fe^(2+)ions and pumped O_(2),was demonstrated.Different cathode materials,polyvinyl alcohol types,and pH values’effects were assessed on device performance.Quenching tests highlighted photoinduced holes(h+)and OH·radicals as pivotal contributions to polyvinyl alcohol degradation.Long-term stability of the device was established through cycling experiments.

关键词： photocatalytic fuel cell PVA Ag@Fe_(2)O_(3) cathode materials fenton-like reaction

Weakly hydrophobic nanoconfinement by graphene aerogels greatly enhances the reactivity and ambient stability of reactivity of MIL-101-Fe in fenton-like reaction

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Nano Research 2021年第7期14卷 2383-2389页

作者： Yuwei Zhang Fei Liu Zhichao Yang Jieshu Qian Bingcai Pan Jiangsu Key Laboratory of Chemical Pollution Control and Resources Reuse School of Environmental and Biological EngineeringNanjing University of Science and TechnologyNanjing 210094China State Key Laboratory of Pollution Control and Resource Reuse School of the EnvironmentNanjing UniversityNanjing 210023China Research Center for Environmental Nanotechnology(ReCENT) Nanjing UniversityNanjing 210023China

In the pursuit of heterogeneous catalysts with high reactivity,metal organic framework(MOF)nanomaterials have received tremendous attentions.However,many MOF catalysts especially Fe-based MOFs need to be utilized immediately after synthesis or being activated using high temperature,because of the easy loss of reactivity in humid environments resulting from the occupation of active Fe sites by water molecules.Here,we describe an inspiring strategy of growing MIL-101-Fe nanoparticles inside the three-dimensional confined space of graphene aerogel(GA),generating shapeable GA/MIL-101-Fe nanocomposite convenient for practical use.Compared to MIL-101-Fe,GA/MIL-101-Fe as catalyst demonstrates much higher reactivity in fenton-like reaction,attributing to smaller MIL-101-Fe particle size,presence of active Fe(II)sites,and abundant defects in GA.Strikingly,the weakly hydrophobic nature of the composite greatly inhibits the loss of catalytic reactivity after being stored in humid air and accelerates the recovery of reactivity in mild temperature,by resisting the entrance of water molecules and helping to exclude water molecules.This work demonstrates that a delicate design of nanocomposite structure could not only improve the reactivity of the catalytic component,but also overcome its intrinsic drawback by taking advantage of the properties of host.We hope this functional nanoconfinement strategy could be extended to more scenarios in other fields.

关键词： nanoconfinement hydrophobicity MIL-101-Fe graphene aerogel fenton-like reaction

Engineering yolk-shell CuCo_(2)S_(4)@Cu_(2)O Z-scheme nanoreactors for accelerating generation of value-added chemicals and of degradation multi-organic contaminants

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Journal of Materials Science & Technology 2023年第25期156卷 54-63页

作者： Xue Feng Lei Zhang College of Chemistry Liaoning University66 Chongshan Middle RoadShenyang 110036China

The synthesis of solar-driven chemical value-added products and the degradation of pollutants is a promising approach for sustainable development. However, achieving these works via photocatalysts with efficient charge-separation, photo-absorption is challenging. A yolk-shell CuCo_(2)S_(4)@Cu_(2)O Z-scheme nanoreactor (YS-CuCo_(2)S_(4)@Cu_(2) O-NR) with octahedron Cu_(2)O as the core and tubular CuCo2 S4 as the shell, has been synthesized by regulating composition and morphology. YS-CuCo_(2)S_(4)@Cu_(2)O-NR shows superior photocatalytic activities for producing H_(2) O_(2) collaborates by selective oxidation of benzyl alcohol (BA) to high value-added benzaldehyde (BAD)/utilized fenton-like reaction to degrade multi-pollutants through space-confinement effect, reaching 80% conversion and 99% selectivity of BA, a yield of 12 mM g^(−1) for H_(2)O_(2) and above 90% degradation efficiency for multi-pollutants. A photocatalysis nanoconfinement reactor system is proposed and demonstrated by using yolk-shell to enhance the performance of the chemical reaction. Mechanism studies show that the yolk-shell provides confined space to accelerate redox reaction kinetics;while the inner void promotes light harvesting and keeps yolk Cu_(2) O from deactivation;combined with the Z-scheme charge transfer, engineering Cu^(+) /Cu^(2+) active composition, they are favorable for enhancing the H_(2) O_(2) generation and fenton-like activity. These findings provide new opportunities for application of yolk-shell Z-scheme metal-oxide-based photocatalysts.

关键词： Octahedron yolk-shell structure catalyzer Z-scheme charge transfer H2O_(2)generation Selective oxidation of BA fenton-like reaction

Sustainable micro-activation of dissolved oxygen driving pollutant conversion on Mo-enhanced zinc sulfide surface in natural conditions

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Fundamental Research 2023年第3期3卷 422-429页

作者： Chao Lu Qian Fang Chun Hu Lai Lyu Key Laboratory for Water Quality and Conservation of the Pearl River Delta Ministry of EducationInstitute of Environmental Research at Greater BayGuangzhou UniversityGuangzhou 510006China Institute of Rural Revitalization Guangzhou UniversityGuangzhou 510006China

The activation of inert oxygen(O_(2))often consumes enormous amounts of energy and resources,which is a global challenge in the field of environmental remediation and fuel cells.Organic pollutants are abundant in electrons and are promising alternative electron donors.Herein,we implement sustainable microactivation of dissolved oxygen(DO)by using the electrons and adsorption energy of pollutants by creating a nonequilibrium microsurface on nanoparticle-integrated molybdenum(Mo)lattice-doped zinc sulfide(ZnS)composites(MZS-1).Organic pollutants were quickly removed by DO microactivation in the MZS-1 system under natural conditions without any additional energy or electron donor.The turnover frequency(TOF,per Mo atom basis)is 5 orders of magnitude higher than those of homogeneous systems.Structural and electronic characterization technologies reveal the change in the crystalline phase(Zn-S-Mo)and the activation of π-electrons on six-membered rings of ZnS after Mo doping,which results in the formation of a nonequilibrium microsurface on MZS-1.This is the key for the strong interfacial interaction and directional electron transfer from pollutants to MZS-1 through the delocalized π-π conjugation effect and from MZS-1 to DO via Zn-S-Mo,as demonstrated by electron paramagnetic resonance(EPR)techniques and density functional theory(DFT)calculations.This process achieves the efficient use of pollutants and the low-energy activation of O_(2) through the construction of a nonequilibrium microsurface,which shows new significance for water treatment.

关键词： Wastewater treatment Microelectric field surface construction fenton-like reaction Oxygen activation Pollutant electron donation

Peroxymonosulfate decomposition by homogeneous and heterogeneous Co: Kinetics and application for the degradation of acetaminophen

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Journal of Environmental Sciences 2020年第7期32卷 30-40页

作者： Oscar M.Rodríguez-Narvaez Ruwini D.Rajapaksha Mahinda I.Ranasinghe Xuelian Bai Juan Manuel Peralta-Hernández Erick R.Bandala Departamento de Química DCNEUniversidad de GuanajuatoGuanajuato C.P.3C6040Mexico Department of Chemistry New Mexico Institute of Mining and TechnologySocorroNM 87801USA Division of Hydrologic Sciences Desert Research InstituteLas VegasNV 89119-7363USA

Peroxymonosulfate(PMS)decomposition,hydroxyl radical(·OH)generation,and acetaminophen(ACT)degradation by the Co/PMS system using homogeneous(dissolved cobalt)and heterogeneous(suspended Co3O4)cobalt were assessed.For the homogeneous process,>99%PMS decomposition was observed and 10 mmol/L of·OH generation was produced using 5 mmol/L of PMS and different dissolved cobalt concentrations after 30 min.A dissolved cobalt concentration of 0.2 mmol/L was used to achieve>99%ACT degradation using the homogeneous process.For the heterogeneous process,60%PMS decomposition and negligible·OH generation were observed for 5 mmol/L of the initial PMS concentration using 0.1 and 0.2 g/L of Co3O4.Degradation of ACT greater than 80%was achieved for all experimental runs using 5 mmol/L of the initial PMS concentration independently of the initial Co3O4 load used.For the heterogeneous process,the best experimental conditions for ACT degradation were found to be 3 mmol/L of PMS and 0.2 g/L of Co3O4,for which>99%ACT degradation was achieved after 10 min.Because negligible·OH was produced by the Co3O4/PMS process,a second-order kinetic model was proposed for sulfur-based free radical production to allow fair comparison between homogeneous and heterogeneous processes.Using the kinetic data and the reaction by-products identified,a mechanistic pathway for ACT degradation is suggested.

关键词： Co3O4 PMS decomposition fenton-like reaction Acetaminophen ·OH production

Tailored core-shell dual metal-eorganic frameworks as a versatile nanomotor for effective synergistic antitumor therapy

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Acta Pharmaceutica Sinica B 2020年第11期10卷 2198-2211页

作者： Biyuan Wu Jintao Fu Yixian Zhou Sulan Luo Yiting Zhao Guilan Quan Xin Pan Chuanbin Wu School of Pharmaceutical Sciences Sun Yat-sen UniversityGuangzhou 510006China College of Pharmacy Jinan UniversityGuangzhou 510632China

Malignant tumor has become an urgent threat to global public healthcare.Because of the heterogeneity of tumor,single therapy presents great limitations while synergistic therapy is arousing much attention,which shows desperate need of intelligent carrier for co-delivery.A core-shell dual metaleorganic frameworks(MOFs)system was delicately designed in this study,which not only possessed the unique properties of both materials,but also provided two individual specific functional zones for co-drug delivery.Photosensitizer indocyanine green(ICG)and chemotherapeutic agent doxorubicin(DOX)were stepwisely encapsulated into the nanopores of MIL-88 core and ZIF-8 shell to construct a synergistic photothermal/photodynamic/chemotherapy nanoplatform.Except for efficient drug delivery,the MIL-88 could be functioned as a nanomotor to convert the excessive hydrogen peroxide at tumor microenvironment into adequate oxygen for photodynamic therapy.The DOX release from MIL-88-ICG@ZIF-8-DOX nanoparticles was triggered at tumor acidic microenvironment and further accelerated by near-infrared(NIR)light irradiation.The in vivo antitumor study showed superior synergistic antitumor effect by concentrating the nanoparticles into dissolving microneedles as compared to intravenous and intratumoral injection of nanoparticles,with a significantly higher inhibition rate.It is anticipated that the multi-model synergistic system based on dual-MOFs was promising for further biomedical application.

关键词： Metaleorganic frameworks Core-shell structure Synergistic therapy Photothermal therapy Photodynamic therapy fenton-like reaction