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Reconstructed parallel sites enhance the reactive oxygen tolerance of non-noble metal catalyst for durable proton exchange membrane fuel cells

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Science China Chemistry 2024年第11期67卷 3739-3748页

作者： Wenjie Wang Hui Ding Minghao Wang Han Cheng Xiang Shi Lin Wang Chun Wang Wangsheng Chu Yi Xie Changzheng Wu National synchrotron radiation Laboratory University of Science and Technology of China School of Chemistry and Materials Science CAS Center for Excellence in Nanoscience University of Science & Technology of China Zhejiang Institute of Photoelectronics Institute of Energy Hefei Comprehensive National Science Center

The establishment of reactive oxygen species(ROS) elimination sites in iron-nitrogen-carbon(Fe-N-C) electrocatalysts to achieve durable proton-exchange membrane fuel cells(PEMFCs) performance has attracted broad interest. However, realizing ROS removal efficiency and oxygen reduction reaction(ORR) activity within a single system represents a significant challenge to date. Herein, we demonstrate uniform ROS elimination sites and ORR centers through an electrochemical reconstruction method on the parallel sites of Fe@Ce NC electrocatalyst for durable PEMFC. During the reconstruction process, the Fe sites can retain their original configuration. Meanwhile, the pristine Ce clusters will evolve into more efficient, highly dispersed ***, the reconstructed Fe and Ce sites exhibit favorable energy barriers for the ORR and ROS elimination pathways,respectively, thereby maintaining ORR activity and achieving high ROS tolerance. Consequently, the PEMFC assembled with our catalyst shows only a 2% decay in power density after the accelerated durability test. We anticipate that this parallel structure design will provide new insight into the development of more durable electrocatalysts for PEMFCs.

关键词： parallel reaction pathways sites reconstruction oxygen reduction reaction radical elimination fuel cells

Preparation of Regenerated Silk Fibroin Hybrid Fibers with Hydrogen Peroxide Sensing Properties by Wet Spinning

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Journal of Renewable Materials 2024年第6期12卷 1043-1055页

作者： Song Lu Jianjun Guo Richard Ansah Herman Xinyi Wu Lin Ma Guohua Wu College of Biotechnology Jiangsu University of Science and TechnologyZhenjiang212100China College of Agriculture Anshun UniversityAnshun561000China

Silk is widely used in the production of high-quality *** the same time,the amount of silk textiles no longer in use and discarded is increasing,resulting in significant waste and *** issue is of great concern in many countries where silk is *** peroxide as a naturally occurring compound is an important indicator of detection in both biology and the *** study aims to develop a composite fiber with hydrogen peroxide-sensing properties using discarded silk *** achieve this goal,firstly,polydopamine(PDA)was used to encapsulate the ZnFe_(2)O_(4) NPs to achieve the improvement of dispersion,and then regenerated silk fibroin(RSF)and PDA@ZnFe_(2)O_(4)/RSF hybrid fibers are prepared by wet *** has shown that PDA@ZnFe_(2)O_(4)/RSF demonstrates exceptional sensitivity,selectivity,and stability in detecting hydrogen peroxide,while maintaining high mechanical ***,the complete hybridization of PDA@ZnFe_(2)O_(4) with silk fibroin not only results in the combination of the durability of silk fibroin and PDA@ZnFe_(2)O_(4)’s rigidity,ensuring a reliable service life,but also makes PDA@ZnFe_(2)O_(4)/RSF exhibit excellent catalytic activity and ***,the composite fiber exhibits exceptional mechanical properties and reliable hydrogen peroxide sensing capabilities,making it a promising material for biological and medical applications.

关键词： Regenerated silk fibroin modified zinc ferrite nanoparticles composite fiber hydrogen peroxide sensor wet spinning

Understand the Temperature Sensing Behavior of Solid-state Polymerized PEDOT Hybrid Based on X-ray Scattering Studies

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Chinese Journal of Polymer Science 2024年第1期42卷 105-112,I0010页

作者： Zhen-Hang He Guang-Feng Liu Ze-Kun Zhou Zhen Liu Yi-Shu Zeng Peng Zhang School of Materials Science and Engineering Key Laboratory for Polymeric Composite and Functional Materials of Ministry of EducationSun Yat-sen UniversityGuangzhou 510275China shanghai Advanced Research Institute(Zhangjiang Laboratory) Chinese Academy of SciencesShanghai 201204China

Poly(3,4-ethylenedioxythiophene)(PEDOT) is one of the most successful conductive polymers that recently has been used in wearable sensors for human health monitoring. In this work, we prepared a series of PEDOT hybrids consisting of PEDOT, sodium poly(styrene sulfonate)(PSSNa) and polyethylene oxide(PEO), and their preparation could be scaled-up via an adapted solid-state polymerization process. The resistance of the as-prepared PEDOT:PSS/PEO hybrid shows clear temperature response, i.e., it decreases almost linearly with the temperature increase. To understand this phenomenon, the in situ synchrotron radiation wide-and small-angle X-ray scattering(WAXS/SAXS) characterizations were undertaken to study the temperature-dependent microstructure change of the PEDOT:PSS/PEO hybrid. It demonstrated that PEDOT formed conductive paths in the hybrids, which were not destroyed by the PEO crystallization. As temperature increased, the PEO crystals' melting and the accompanying reorganization of PEDOT chains endowed the hybrid sample temperature responsiveness. Based on these fundamental knowledges, the hybrid materials were used to fabricate flexible wearable sensor that showing temperature sensing performance with an accuracy of 1 ℃. These findings shed lights on the scalable manufacturing of wearable sensors for body temperature monitoring.

关键词： Solid-state polymerization PEDOT hybrid Structure-property correlation X-ray scattering

Unveiling the pressure-driven metal–semiconductor–metal transition in the doped TiS_(2)

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Chinese Physics B 2024年第6期33卷 63-67页

作者：陈佳骏吕心邓李思敏但雅倩黄艳萍崔田 Institute of High Pressure Physics School of Physical Science and TechnologyNingbo UniversityNingbo 315211China State Key Laboratory of Superhard Materials College of PhysicsJilin UniversityChangchun 130012China

Conventional theories expect that materials under pressure exhibit expanded valence and conduction bands,leading to increased electrical ***,we report the electrical properties of the doped 1T-TiS_(2) under high pressure by electrical resistance investigations,synchrotron x-ray diffraction,Raman scattering and theoretical *** to 70 GPa,an unusual metal-semiconductor-metal transition *** first-principles calculations suggest that the observed anti-Wilson transition from metal to semiconductor at 17 GPa is due to the electron localization induced by the intercalated Ti *** electron localization is attributed to the strengthened coupling between the doped Ti atoms and S atoms,and the Anderson localization arising from the disordered *** pressures exceeding 30.5 GPa,the doped TiS_(2) undergoes a re-metallization transition initiated by a crystal structure phase *** assign the most probable space group as P2_(1)2_(1)2_(1).Our findings suggest that materials probably will eventually undergo the Wilson transition when subjected to sufficient pressure.

关键词： high pressure transition metal dichalcogenides doped TiS_(2) electronic phase transition

Stable graphene oxide-based lyotropic liquid crystals for interfacial lubrication

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Friction 2024年第5期12卷 954-967页

作者： Yumei GUO Hanglin LI Jiusheng LI Xiangqiong ZENG Laboratory for Advanced Lubricating Materials Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai201210China University of Chinese Academy of Sciences Beijing100049China

Lyotropic liquid crystals have lubricating properties due to their ordered assembly and fluidity,whose mesogens are often characterized by amphiphilic *** the attention that graphene oxide(GO)has been studied as a novel amphiphilic lyotropic mesogen this decade,and GO applied as a lubrication additive has been demonstrated in both oil and water-based systems,little research reveals the interfacial lubrication of GO liquid crystals *** work reports that GO aqueous dispersion can form lyotropic liquid crystals above a specific critical concentration of 5.00 mg/mL,providing a form of stable water-based lubricant,which can keep stable for several months and can reduce friction by 37.3%and wear by 25.24%.The liquid crystal phase was verified by polarizing microscope and synchrotron radiation small-angle X-ray scattering,and its rheological properties and viscoelasticity were studied by interfacial *** formation of lyotropic liquid crystals can enhance the stability of GO aqueous dispersions at high density,simultaneously ensuring friction decrease and anti-wear *** is attributed to the stable nematic network by the ordered GO *** ordered assembly structure bears vertical shear force,therefore,reducing the *** is also assumed that the wide lateral size of graphene oxide promotes the nematic phase thus smoothes the graphene oxide film composed spontaneously under the coincidence of lamellar liquid crystal and 2D layered *** this work,the interlayer lubrication of GO was optimized,and the problem of GO dispersion sedimentation was solved by *** range of interfacial lubrication of GO aqueous dispersion has been expanded and the synergistic effect is conducive to the environmentally friendly lubricants.

关键词： lyotropic liquid crystal graphene oxide aqueous lubrication tribological behavior

Exciting lattice oxygen of nickel–iron bi-metal alkoxide for efficient electrochemical oxygen evolution reaction

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Journal of Energy Chemistry 2024年第1期88卷 194-201,I0005页

作者： Saihang Zhang Senchuan Huang Fengzhan Sun Yinghui Li Li Ren Hao Xu Zhao Li Yifei Liu Wei Li Lina Chong Jianxin Zou National Engineering Research Center of Light Alloy Net Forming&State Key Laboratory of Metal Matrix Composites Center of Hydrogen ScienceSchool of Materials Science and EngineeringShanghai Jiao Tong UniversityShanghai 200240China Department of Chemistry Laboratory of Advanced MaterialsShanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsiChEM and State Key Laboratory of Molecular Engineering of PolymersCollege of Chemistry and MaterialsFudan UniversityShanghai 200433China

High efficiency,cost-effective and durable electrocatalysts are of pivotal importance in energy conversion and storage *** electro-oxidation of water to oxygen plays a crucial role in such energy conversion ***,we report a robust method for the synthesis of a bimetallic alkoxide for efficient oxygen evolution reaction(OER)for alkaline electrolysis,which yields current density of 10 mA cm^(-2)at an overpotential of 215 mV in 0.1 M KOH *** catalyst demonstrates an excellent durability for more than 540 h operation with negligible degradation in *** spectra revealed that the catalyst underwent structure reconstruction during OER,evolving into oxyhydroxide,which was the active site proceeding OER in alkaline ***-situ synchrotron X-ray absorption experiment combined with density functional theory calculation suggests a lattice oxygen involved electrocatalytic reaction mechanism for the in-situ generated nickel–iron bimetal-oxyhydroxide *** mechanism together with the synergy between nickel and iron are responsible for the enhanced catalytic activity and *** findings provide promising strategies for the rational design of nonnoble metal OER catalysts.

关键词： Oxygen evolution reaction Nickel-iron bi-metal alkoxide Lattice oxygen-mediated reaction mechanism Alkaline electrolysis Electrocatalysts

Boosting rate performance of layered lithium-rich cathode materials by oxygen vacancy induced surface multicomponent integration

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Journal of Energy Chemistry 2024年第5期92卷 250-262页

作者： Youyou Fang Yuefeng Su Jinyang Dong Jiayu Zhao Haoyu Wang Yun Lu Bin Zhang Hua Yan Feng Wu Lai Chen Beijing Key Laboratory of Environmental Science and Engineering School of Material Science and EngineeringBeijing Institute of TechnologyBeijing 100081China Chongqing Innovation Center Beijing Institute of TechnologyChongqing 401120China Yibin Libode New Materials Co. Ltd.Yibin 64400SichuanChina School of Metallurgy and Environment Central South UniversityChangsha 410083HunanChina Engineering Research Center of the Ministry of Education for Advanced Battery Materials Central South UniversityChangsha 410083HunanChina

The rapid development of electric vehicles and portable energy storage systems demands improvements in the energy density and cost-effectiveness of lithium-ion batteries,a domain in which Lithium-rich layered cathode(LLO)materials inherently ***,these materials face practical challenges,such as low initial Coulombic efficiency,inferior cycle/rate performance,and voltage decline during cycling,which limit practical *** study introduces a surface multi-component integration strategy that incorporates oxygen vacancies into the pristine LLO material Li1.2Mn_(0.6)Ni_(0.2)O_(2).This process involves a brief citric acid treatment followed by calcination,aiming to explore rate-dependent degradation *** induced surface oxygen vacancies can reduce surface oxygen partial pressure and diminish the generation of O_(2)and other highly reactive oxygen species on the surface,thereby facilitating the activation of Li ions trapped in tetrahedral sites while overcoming transport ***,the formation of a spinel-like phase with 3D Li+diffusion channels significantly improves Li^(+)diffusion kinetics and stabilizes the surface *** optimally modified sample boasts a discharge capacity of 299.5 mA h g^(-1)at a 0.1 C and 251.6 mA h g^(-1)at a 1 C during the initial activation cycle,with an impressive capacity of 222.1 mA h g^(-1)at a 5 *** notably,it retained nearly 70%of its capacity after 300 cycles at this elevated *** straightforward,effective,and highly viable modification strategy provides a crucial resolution for overcoming challenges associated with LLO materials,making them more suitable for practical application.

关键词： Lithium-ion battery Layered lithium rich cathode Surface multicomponent integration Rate-dependent degradation and Li^(+) diffusion kinetics

Surface-sensitive electronic structure of kagome superconductor CsV_(3)Sb_(5)

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Chinese Physics B 2024年第10期33卷 35-40页

作者： Zhisheng Zhao Jianghao Yao Rui Xu Yuzhe Wang Sen Liao Zhengtai Liu Dawei Shen Shengtao Cui Zhe Sun Yilin Wang Donglai Feng Juan Jiang School of Emerging Technology and Department of Physics University of Science and Technology of ChinaHefei 230026China shanghai synchrotron radiation facility Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201210China National synchrotron radiation Laboratory School of Nuclear Science and Technology and New Cornerstone Science LaboratoryUniversity of Science and Technology of ChinaHefei 230026China

We systematically study the electronic structure of a kagome superconductor CsV_(3)Sb_(5)at different temperatures coveringboth its charge density wave state and normal state with angle-resolved photoemission *** observe thatthe V-shaped band aroundГshows three different behaviors,referred to as a/a',βandγ,mainly at different *** investigations confirm that these bands are all from the same bulk Sb-p_(z)origin,but they are quite sensitiveto the sample surface conditions mainly modulated by ***,the intriguing temperature dependent electronicbehavior of the band nearГis affected by the sample surface condition,rather than intrinsic electronic behavior originatingfrom the phase *** result systematically reveals the confusing electronic structure behavior of the energy bandsaroundГ,facilitating further exploration of the novel properties in this material.

关键词： kagome ARPES charge density wave surface sensitive

Towards full-stack deep learning-empowered data processing pipeline for synchrotron tomography experiments

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The Innovation 2024年第1期5卷 127-138页

作者： Zhen Zhang Chun Li Wenhui Wang Zheng Dong Gongfa Liu Yuhui Dong Yi Zhang National synchrotron radiation Laboratory University of Science and Technology of ChinaHefei 230029China Beijing synchrotron radiation facility Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China

synchrotron tomography experiments are transitioning into multifunctional,cross-scale,and dynamic characterizations,enabled by new-generation synchrotron light sources and fast developments in beamline ***,with the spatial and temporal resolving power entering a new era,this transition generates vast amounts of data,which imposes a significant burden on the data processing ***,as a highly accurate and efficient data processing method,deep learning shows great potential to address the big data challenge being encountered at future synchrotron *** this review,we discuss recent advances employing deep learning at different stages of the synchrotron tomography data processing *** also highlight how applications in other data-intensive fields,such as medical imaging and electron tomography,can be migrated to synchrotron ***,we provide our thoughts on possible challenges and opportunities as well as the outlook,envisioning selected deep learning methods,curated big models,and customized learning strategies,all through an intelligent scheduling solution.

关键词： processing pipeline outlook