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Sulfur doped iron-nitrogen-hard carbon nanosheets as efficient and robust noble metal-free catalysts for oxygen reduction reaction in PEMFC

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Journal of energy Chemistry 2024年第2期89卷 422-433,I0010页

作者： Bin Liu Jiawang Li Bowen Yan Qi Wei Xingyu Wen Huarui Xie Huan He Pei Kang Shen Zhi Qun Tian Collaborative Innovation Center of Sustainable energy materials School of Physical Science and TechnologyGuangxi UniversityGuangxi Key Laboratory of Electrochemical Energy MaterialsState Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite StructuresNanning 530004GuangxiChina

Transition metal-nitrogen-carbon(M-N-C)as a promising substitute for the conventional noble metalbased catalyst still suffers from low activity and durability for oxygen reduction reaction(ORR)in proton exchange membrane fuel cells(PEMFCs).To tackle the issue,herein,a new type of sulfur-doped ironnitrogen-hard carbon(S-Fe-N-HC)nanosheets with high activity and durability in acid media were developed by using a newly synthesized precursor of amide-based polymer with Fe ions based on copolymerizing two monomers of 2,5-thiophene dicarboxylic acid(TDA)as S source and 1,8-diaminonaphthalene(DAN)as N source via an amination *** as-synthesized S-Fe-N-HC features highly dispersed atomic Fe Nxmoieties embedded into rich thiophene-S doped hard carbon nanosheets filled with highly twisted graphite-like microcrystals,which is distinguished from the majority of M-N-C with soft or graphitic carbon *** unique characteristics endow S-Fe-N-HC with high ORR activity and outstanding durability in 0.5 M H_(2)SO_(4).Its initial half-wave potential is 0.80 V and the corresponding loss is only 21 m V after 30,000 ***,its practical PEMFC performance is a maximum power output of 628.0 mW cm^(-2)and a slight power density loss is 83.0 m W cm^(-2)after 200-cycle practical ***,theoretical calculation shows that the activity of Fe Nxmoieties on ORR can be further enhanced by sulfur doping at meta-site near FeN_(4)*** results evidently demonstrate that the dual effect of hard carbon substrate and S doping derived from the precursor platform of amid-polymers can effectively enhance the activity and durability of Fe-N-C catalysts,providing a new guidance for developing advanced M-N-C catalysts for ORR.

关键词： Transition metal-nitrogen-carbon Oxygen reduction reaction Hard carbon Amide based polymer reaction Proton exchange membrane cells

Reversibly Cross-Linking Polyimide and Cyclophosphazene Toward Closed-Loop Recyclable Plastics with High Mechanical Strength,Excellent Flame Retardancy,and Chemical Resistance

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CCS Chemistry 2024年第4期6卷 976-987页

作者： Tingting Guan Xiaohan Wang Xi Zhao Xingyuan Lu Xiu-Li Wang Yu-Zhong Wang Junqi Sun state key laboratory of Supramolecular Structure and materials College of ChemistryJilin UniversityChangchun 130012 The Collaborative Innovation Center for Eco-friendly and Fire-Safety Polymeric materials(MoE) National Engineering Laboratory of Eco-Friendly Polymeric Materials(Sichuan)State Key Laboratory of Polymer Materials EngineeringCollege of ChemistrySichuan UniversityChengdu 610064

Traditional flame-retardant plastics are technically difficult to chemically *** development of newtypes of flame-retardant plastics that are intrinsically capable of being closed-loop recycled and are sufficiently robust and stable to satisfy their practical application is urgently *** this study,closed-loop recyclable flame-retardant plastics with high mechanical strength and excellent chemical resistance are fabricated by cross-linking amino-terminated polyimide(PI-NH_(2))and aldehyde-terminated cyclophosphazene(CP-CHO)with imine *** resultant flame-retardant plastic,which is denoted as PI-CP,exhibits a tensile strength of∼115.6 MPa,Young’s modulus of∼2.5 GPa,and glass transition temperature of 316°*** the PI-CP plastic,the imine bonds are isolated within hydrophobic microenvironments generated by the rigid and hydrophobic polyimide chains and the benzene ring of *** a result,the PI-CP plastics are highly stable in highly acidic and basic aqueous solutions and other commonly used organic *** PI-CP plastic shows outstanding flame retardancy with a limiting oxygen index value of 48.8%.More importantly,the PI-CP plastic can be depolymerized to generate the original PI-NH_(2)and CPCHO monomers in high yields(∼97%)and *** recovered monomers can be used to refabricate the original plastics,establishing highly efficient polymer-monomer-polymer circulation and a sustainable plastics economy.

关键词： closed-loop recyclable plastics recyclable polymers reversibly cross-linked polymers flame retardancy supramolecular polymers

Unique electromagnetic wave absorber for three-dimensional framework engineering with copious heterostructures

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Journal of materials Science & Technology 2024年第3期170卷 129-139页

作者： Liyuan Yu Qianqian Zhu Zhiqiang Guo Yuhang Cheng Zirui Jia Guanglei Wu Institute of materials for energy and environment State Key Laboratory of Bio-fibers and Eco-textilesCollege of Materials Science and EngineeringQingdao UniversityQingdao 266071China College of Chemistry and Chemical Engineering Qingdao UniversityQingdao 266071China

In order to obtain high-performance electromagnetic wave absorbers,the adjustment of structure and components is *** on the above requirements,this system forms a three-dimensional frame structure consisting of MXene and transition metal oxides(TMOs)through efficient electrostatic *** three-dimensional network structure has rich heterojunction structures,which can cause a large amount of interface polarization and conduction losses in incident electromagnetic *** structures cause multiple reflections and scattering of electromagnetic waves,which is also an important reason for further increasing electromagnetic wave *** the doping ratio is 1:1,the system has the best impedance matching,the maximum effective absorption bandwidth(EAB max)can reach 5.12 GHz at 1.7 mm,and the minimum reflection loss(RL_(min))is-50.30 dB at 1.8 *** provides a reference for the subsequent formation of 2D-MXene materials into 3D materials.

关键词： MXene Three-dimensional frame Heterojunction structure Conduction loss Electromagnetic wave absorption

Iron–doped bismuth oxybromides as visible-light-responsive Fenton catalysts for the degradation of atrazine in aqueous phases

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Journal of environmental Sciences 2024年第3期137卷 321-332页

作者： Yong-Li Cai Yu-Hang Xu Ji-Zun Xiang Zhi-Qiang Zhang Qiu-Xiang He Ya-Feng Li Jian Lü Fujian Provincial key laboratory of Soil environmental Health and Regulation College of Resources and EnvironmentFujian Agriculture and Forestry UniversityFuzhou 350002China state key laboratory of Photocatalysis on energy and environment Fuzhou UniversityFuzhou 350116China

Pesticides and its degradation products,being well–known residues in soil,have recently been detected in many water bodies as pollutants of emerging concerns,and thus there is a contemporary demand to develop viable and cost–effective techniques for the removal of related organic pollutants in aqueous ***,a visible-light-responsive Fenton system was constructed with iron–doped bismuth oxybromides(Fe–BiOBr)as the *** the advantage of sustainable Fe(Ⅲ)/Fe(Ⅱ)conversion and optimized H_(2)O_(2)utilization,the optimal Fe–BiOBr–2 catalyst showed an excellent atrazine removal efficiency of 97.61%in 120 min,which is superior than the traditional homogeneous Fenton and the majority of heterogeneous processes documented in the *** this photo–Fenton system,hydroxyl(·OH)and superoxide(·O_(2)^(-))radicals were dominant active species contributed to the oxidative degradation of *** to the production of various active radicals,five degradation pathways were proposed based on the identification of intermediates and degradation ***,this work not only demonstrates a fundamental insight into creating highly efficient and atom economic photo-Fenton systems,but also provides a complementary strategy for the treatment of organic pollutants in water.

关键词： Bismuth oxybromide Photo–Fenton Atrazine Catalytic degradation

Nitrogen-doped titanium dioxide/schwertmannite nanocomposites as heterogeneous photo-Fenton catalysts with enhanced efficiency for the degradation of bisphenol A

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Journal of environmental Sciences 2024年第9期143卷 1-11页

作者： Xing-Xing Qiao Yu-Hang Xu Xiang-Ji Liu Sai-Le Chen Zhou Zhong Ya-Feng Li Jian Lü Fujian Provincial key laboratory of Soil environmental Health and Regulation College of Resources and EnvironmentFujian Agriculture and Forestry UniversityFuzhou 350002China state key laboratory of Photocatalysis on energy and environment Fuzhou UniversityFuzhou 350116China

Potential health risks related to environmental endocrine disruptors(EEDs)have aroused research hotspots at the forefront of water treatment ***,nitrogen-doped titanium dioxide/schwertmannite nanocomposites(N-TiO_(2)/SCH)have been successfully developed as heterogeneous catalysts for the degradation of typical EEDs via photo-Fenton *** to the sustainable Fe(Ⅲ)/Fe(Ⅱ)conversion induced by photoelectrons,as-prepared N-TiO_(2)/SCH nanocomposites exhibit much enhanced efficiency for the degradation of bisphenol A(BPA;ca.100% within 60 min under visible irradiation)in a wide pH range of 3.0-7.8,which is significantly higher than that of the pristine schwertmannite(ca.74.5%)or N-TiO_(2)(ca.10.8%).In this photo-Fenton system,the efficient degradation of BPA is mainly attributed to the oxidation by hydroxyl radical(·OH)and singlet oxygen(^(1)O_(2)).Moreover,the possible catalytic mechanisms and reaction pathway of BPA degradation are systematically investigated based on analytical and photoelectrochemical *** work not only provides a feasible means for the development of novel heterogeneous photo-Fenton catalysts,but also lays a theoretical foundation for the potential application of mineral-based materials in wastewater treatment.

关键词： Titanium dioxide Schwertmannite Fenton reaction environmental endocrine disruptors Photocatalysis

Insights into the role of oxygen-containing functional groups on carbon surface in water–electricity generation

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Nano Research 2024年第7期17卷 6645-6653页

作者： Wan Xue Zongbin Zhao Honghui Bi Bolun Zhang Xuzhen Wang Jieshan Qiu state key laboratory of Fine Chemicals Liaoning Key Laboratory for Energy Materials and Chemical EngineeringSchool of Chemical EngineeringDalian University of TechnologyDalian 116024China state key laboratory of Fine Chemicals Liaoning Key Laboratory for Energy Materials and Chemical EngineeringSchool of ChemistryDalian University of TechnologyDalian 116024China state key laboratory of Chemical Resource Engineering College of Chemical EngineeringBeijing University of Chemical TechnologyBeijing 100029China

A deep understanding of the electricity generation mechanism from the interaction between water molecules and carbon material surfaces is attractive for next-generation water-based energy conversion and storage ***,an asymmetric generator was assembled based on functionalized carbon nanotubes films to investigate the relative contribution from various oxygen functional groups on carbon surface to the water-electrical *** and calculations demonstrate that the electricity mainly originates from the water molecule adsorption by carboxyl groups and dissociation of functional groups on carbon surface,which leads to the formation of electrical double layers at *** device allows the electricity generation with a variety of water sources,such as deionized water,tap water,as well as *** particular,the generator based on carboxyl carbon nanotubes can induce a voltage of over 200 mV spontaneously in natural seawater with the power density of about 0.11 mW·g^(−1).High voltages can be achieved easily through the series-connection strategy to power electronic products such as a liquid crystal *** work reveals the dominant role of carboxyl groups in carbon-based water–electricity conversion and is expected to offer inspiration for the preparation of carbon materials with high electrical performance.

关键词： electricity generation water adsorption dissociation carboxyl groups carbon nanotubes

Hybrid assembly of conducting nanofiber network for ultra-stretchable and highly sensitive conductive hydrogels

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Journal of materials Science & Technology 2024年第2期169卷 1-10页

作者： Yalei Wang Shulong Zeng Shaohong Shi Yuheng Jiang Zhiwei Du Bingzhen Wang Xiurong Li state key laboratory of Featured Metal materials and Life-cycle Safety for Composite Structures School of ResourcesEnvironment and MaterialsGuangxi UniversityNanning 530004China state key laboratory of Polymer materials Engineering Polymer Research Institute of Sichuan UniversitySichuan UniversityChengdu 610065China

Conductive hydrogels have attracted extensive attention owing to their promising application prospects in flexible and wearable ***,achieving both high sensitivity and mechanical robustness remains ***,a novel and versatile conductive hydrogel based on the hybrid assem-bly of conductive cellulose nanofiber(CNF)networks has been designed and *** by the templating effect of CNFs and stabilizing effect of negatively charged poly(styrene sulfonate)(PSS),conducting polymer poly(3,4-ethylenedioxythiophene)(PEDOT)was self-organized into three-dimensional nanostructures which constructed a robust conductive network after in-situ oxidative *** unique structure derived from CNF bio-template endowed polyacrylamide(PAM)hydrogels with improved electrical conductivity and excellent mechanical *** a result,the as-fabricated CNF/PEDOT:PSS/PAM hydrogel exhibited an ultimate tensile strain of 1881%and toughness of 3.72 MJ/m^(3),which were 4.07 and 8.27 times higher than the CNF-free hydrogel,*** significantly,the resultant hydrogel sensor showed highly desirable sensing properties,including remarkable sensing range(1100%),high gauge factor(GF=5.16),fast response time(185 ms),and commendable durability,as well as good ***,the hydrogel sensor was able to distinguish subtle physiological activities including phonation and facial expression,and monitor large human body motions such as finger flexion and elbow ***,it was feasible to integrate the strain sensor on the joints of robots to recognize complicated machine motion signals,showing potential in advanced human-machine interactions.

关键词： Strain sensor Cellulose nanofibers PEDOT:PSS Conductive hydrogel Templating method

Metal-organic frameworks on 3D interconnected macroporous sponge foams for large-scale water decontamination:A mini review

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Chinese Chemical Letters 2024年第5期35卷 77-84页

作者： Xiao-Hong Yi Chong-Chen Wang Beijing key laboratory of Functional materials for Building Structure and environment Remediation School of Environment and Energy EngineeringBeijing University of Civil Engineering and ArchitectureBeijing 100044China

Water pollution caused by global population growth,urban expansion and industrialization development is one of the urgent issues that need to be addressed in the 21st *** to now,it was challenging for metal-organic frameworks(MOFs)to be used in the actual water treatment due to that the powder MOFs suffered from difficult reuse,poor water stability and easy *** is an effective strategy to immobilize MOFs powder onto porous sponge foam carriers for accomplishing large flux,facile recycling,easy processing water treatment *** this review article,the fabrication approaches and applications of different MOFs/sponge composites were highlighted,in which the fluorescence detection of pollutants,adsorption and separation of pollutants,catalytic reduction and oxidation of pollutants were ***,the future challenges and opportunities of MOF/sponge for water treatment are proposed,aiming to provide in-depth guidance for the future design and manufacture of the immobilized MOFs onto sponge foams.

关键词： Metal-organic frameworks Sponge foam Water decontamination Adsorption Catalysis

Facile construction of Mxene-supported niobium hydride nanoparticles toward reversible hydrogen storage in magnesium borohydride

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Rare Metals 2024年第9期43卷 4387-4400页

作者： Ao Xia Jia-Guang Zheng Qing-Bo Zhang Yu-Gang Shu Cheng-Guo Yan Liu-Ting Zhang Zhan-Liang Tao Li-Xin Chen School of energy and Power Jiangsu University of Science and Technology key laboratory of Advanced energy materials Chemistry(Ministry of Education) Nankai University state key laboratory of Silicon and Advanced Semiconductor materials School of Materials Science and EngineeringZhejiang University

The facile construction of nanoscale NbHxsupported by Ti3C2（NbHx@Ti3C2） was achieved using facile ball milling strategy to improve the hydrogen desorption kinetics and reversibility of magnesium borohydride (Mg（BH4）2).The doping of 30 wt%NbHx@Ti3C2catalyst reduced the onset dehydrogenation temperature of Mg（BH4）2to 71.2℃.Additionally,the Mg（BH4）2+30NbHx@Ti3C2composite achieved remarkable hydrogen release of over 9.2 wt% at a temperature as low as 230℃,indicating unexpected dehydrogenation ***,the reversibility of NbHx@Ti3C2doped Mg（BH4）2was retained to more than 4.2 wt%after four cycles,which was increased by 68% compared to that of undoped Mg（BH4）*** strong catalysis of NbHx@Ti3C2catalyst could be attributed to the synergistic effect of NbHxand Ti3C2in hydrogen spillover and *** as a??hydrogen pump??for effective hydrogen spillover,while Ti3C2created numerous diffusion channels for hydrogen dissolution and provided the active catalytic site to facilitate the re/dehydrogenation of Mg（BH4）2.

关键词： Catalysts Hydrogen storage Magnesium borohydride Mxene