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Achieving asymmetric redox chemistry for oxygen evolution reaction through strong metal-support interactions

Journal of Energy Chemistry 2024年第9期96卷 526-535页

作者： Shihao wang Meiling fan Hongfei Pan Jiahui Lyu Jinsong wu Haolin Tang Haining Zhang State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070HubeiChina National Energy Key Laboratory for New Hydrogen-Ammonia Energy Technologies Foshan Xianhu LaboratoryFoshan 528200GuangdongChina International School of Materials Science and Engineering(School of Materials and Microelectronics) Wuhan University of TechnologyWuhan 430070HubeiChina Nanostructure Research Centre Wuhan University of TechnologyWuhan 430070HubeiChina Hubei Key Laboratory of Fuel Cell Wuhan University of TechnologyWuhan 430070HubeiChina

water electrolysis poses a significant challenge for balancing catalytic activity and stability of oxygen evolution reaction(OER)*** this study,we address this challenge by constructing asymmetric redox chemistry through elaborate surface OO–Ru–OH and bulk Ru–O–Ni/Fe coordination moieties within single-atom Ru-decorated defective NiFe LdH nanosheets(Ru@d-NiFe LdH)in conjunction with strong metal-support interactions(SMSI).Rigorous spectroscopic characterization and theoretical calculations indicate that single-atom Ru can delocalize the O 2p electrons on the surface and optimize d-electron configurations of metal atoms in bulk through ***^(18)O isotope labeling experiment based on operando differential electrochemical mass spectrometry(dEMS),chemical probe experiments,and theoretical calculations confirm the encouraged surface lattice oxygen,stabilized bulk lattice oxygen,and enhanced adsorption of oxygen-containing intermediates for bulk metals in Ru@d-NiFe LdH,leading to asymmetric redox chemistry for *** Ru@d-NiFe LdH electrocatalyst exhibits exceptional performance with an overpotential of 230 mV to achieve 10 mA cm^(−2)and maintains high robustness under industrial current *** approach for achieving asymmetric redox chemistry through SMSI presents a new avenue for developing high-performance electrocatalysts and instills confidence in its industrial applicability.

关键词： Reaction redox chemistry Strong metal-support interactions Layered double hydroxides Electrocatalysts water electrolysis

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Co-aromatization of methane and hexane over Pt encapsulated in ZSM-5 zeolite and the electronic effect of K promoters

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Science China Chemistry 2024年第3期67卷 1017-1027页

作者： Bei Liu fan wang Xiaomeng dou Pengfei Li Hongwei Xiang Yong Yang Peng He State Key Laboratory of Coal Conversion Institute of Coal ChemistryChinese Academy of SciencesTaiyuan 030001China department of Chemistry Tsinghua UniversityBeijing 100084China National Energy R&d Center for Coal to Liquid Fuels Synfuels China Technology Co.Ltd.Beijing 101407China University of Chinese Academy of Sciences Beijing 101408China Leibniz-Institut für Katalyse e.V.an der Universitat Rostock Rostock 18059Germany

The co-aromatization of methane with higher hydrocarbons represents a promising route to valorize methane, an abundant but underexploited carbon resource. In this study, we elucidate a novel approach to enhance the catalytic co-aromatization of hexane and methane by confining Pt within zeolite catalysts and modulating its electron density. Our findings show that encapsulating Pt within MFI structure is pivotal for activating the feedstock and fostering the formation of aromatic products. Interaction between K atoms and the silanol nest forms siloxy groups which are critical for the stabilization of Pt species. Tuning the K content in PtSn@MFI catalysts adeptly alters the electronic configuration of Pt clusters. This modification is corroborated by infrared and X-ray photoelectron spectroscopy analysis, and density functional theory calculations. Remarkably, the catalyst with 0.8 wt% K exhibits an optimal Pt electron density, driving its superior efficacy in the co-aromatization reaction, converting 0.78 mol of methane for each mole of hexane processed. By employing ~(13)C isotopic labeling and solid-state NMR studies, we demonstrate the participation of methane in the adsorbed species inside the zeolite channel and its incorporation to the benzyl site of the substitute group and phenyl rings in aromatic compounds, underscoring the importance of Pt encapsulation.

关键词： Pt encapsulation MFI zeolite methane activation co-aromatization ^(13)C solid-state NMR

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The enhanced mechanical properties of SiC nanowires/Ba0.75Sr0.25Al2Si2O8 ceramics with embedded SiO2 interface

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Journal of Advanced Ceramics 2024年第7期13卷 933-941页

作者： Xin Li Xiaomeng fan Haojie Luo Xiaoke Lu Jimei Xue fang Ye Yongsheng Liu Science and Technology on Thermostructural Composite Materials Laboratory Northwestern Polytechnical UniversityXi’an 710072China Frontier Institute of Science and Technology Xi’an Jiaotong UniversityXi’an 710049China

In this work,low-softening-temperature and low-modulus SiO2 was introduced as an embedded interface between SiC nanowires(SiCnws)and a BaxSr1−xAl2Si2O8 ceramic matrix to enhance strength and toughness of the *** the sintering process,molten SiO2 enhances the flowability of the ceramic powders and modifies the dispersion of *** strengthening effect of SiCnws was fully realized,and the flexural strength of the optimized ceramics reached 193±16 MPa,which represents an increase of 52.6%.After the formation of the embedded SiO2 interface with a low modulus,cracks can deflect along the SiCnws surface,which is consistent with the criterion of He and *** can effectively extend the crack propagation path,and the fracture toughness(K_(IC))is thus improved by 94.0%,reaching 3.1±0.5 MPa·m^(1/2).

关键词： multiphase ceramics SiO2 interface densification mechanical properties

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Exploring precursor effect in in-situ reconstruction of Bi metal organic-frameworks during CO_(2)electroreduction reaction to tailor formate selectivity towards 100%

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Science China Chemistry 2024年第7期67卷 2190-2198页

作者： Zhida Liu Qikui fan Hang Huo fanglei Yao Xiaoping Gao Jin wang College of Materials Science and Engineering Shenzhen UniversityShenzhen 518071China College of Physics and Optoelectronic Engineering Shenzhen UniversityShenzhen 518060China Key Laboratory of Functional Molecular Solids Ministry of EducationCollege of Chemistry and Materials ScienceAnhui Normal UniversityWuhu 241002China Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of ChinaHefei 230026China

Bi-based metal-organic frameworks(Bi-MOFs)as efficient catalysts for the CO_(2)electroreduction reaction(CRR)have been extensively *** has been established that Bi-MOFs usually undergo in-situ transformation during the CRR,ultimately converting into Bi ***,the effect of the MOF precursors on the structure of the derived Bi catalysts and consequently on their electrocatalytic properties has not been clearly *** this work,we prepared four variants of a novel Bi-MOF with different morphologies and dimensions,and explored the effects of the precursors on the resulting Bi catalysts and their CRR performance.A precursor-dependent in-situ transformation and its profound impact on tuning the CO_(2)-formate FE towards~100%have been *** the four examined variants,Bi-MOF with nanocube-like morphology(BiMOF-NC)is transformed into thin and flat Bi nanosheets capable of successfully enveloping the fibers of carbon paper(working electrode),while the other three variants with increased size and dodecahedral/octahedral geometry have been transformed into Bi nanoflowers,exposing a fair portion of the carbon fibers in the working ***,the transformation rate was found to be dependent on the precursors and BiMOF-NC exhibited the highest rate of reconstruction compared with other ***,the Bi catalyst derived from BiMOF-NC delivered a selectivity for the formate product of nearly 100%at-1.2 V(*** hydrogen electrode(RHE))and of over 95%in a wide potential range due to efficient suppression of the competing hydrogen evolution reaction(HER)over carbon *** in-situ transformed BiMOFNC also demonstrated equivalently high formate selectivity at large current densities(≥100 mA cm^(-2))in flow cell reactors as that in H-type reactors,underscoring its potential for industrial *** work highlights the necessity of finely tuning the structural features of MOF precursors to achieve optim

关键词： Bi-MOFs precursor effect in-situ transformation Bi nanosheets CO_(2)-to-formate

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Flexible and Stretchable Electrodes for In Vivo Electrophysiological and Electrochemical Monitoring

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Chinese Journal of Chemistry 2024年第13期42卷 1523-1545页

作者： Kai-Kai Sheng Yi-Fei Lu wen-Ting fan Yan-Ling Liu College of Chemistry and Molecular Sciences Wuhan University WuhanHubei 430072China Core Facilty of wuhan University WuhanHubei 430072China

In vivo monitoring of bioelectrical and biochemical signals with implanted electrodes has received great interest over the past ***,this faces huge challenges because of the severe mechanical mismatch between conventional rigid electrodes and soft biological *** recent years,the emergence of flexible and stretchable electrodes offers seamless and conformable biological-electronic interfaces and has demonstrated significant advantages for in vivo electrochemical and electrophysiological *** review first summarizes the strategies for electrode fabrication from the point of substrate and conductive ***,recent progress in electrode functionalization for improved performance is ***,the advances of flexible and stretchable electrodes in exploring bioelectrical and biochemical signals are ***,we present some challenges and perspectives ranging from electrode fabrication to application.

关键词： Flexible electrodes Conductive materials Stretchable structures Electrode functionalization In vivo monitoring Biochemical signals Bioelectrical signals

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Low-complexity model predictive control of a four-level active neutral point clamped inverter without weighting factors

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Transportation Safety and Environment 2024年第2期6卷 96-103页

作者： Chaoqun Xiang Ziyin fan Songyang Jiang Xinan Zhang Shu Cheng School of Traffic and Transportation Engineering Central South UniversityChangsha 410075HunanChina CRRC dalian Electric Traction R&d Center Co. LtdDalian 116200LiaoningChina School of Engineering The University of Western AustraliaPerthWA 6009Australia

The four-level active neutral point clamped(ANPC)inverter has become increasingly widely used in the renewable energy indus-try since it offers one more voltage level without increasing the total number of active switches compared to the three-level ANPC *** model predictive current control(MPCC)is a promising control method for multi-level ***,the conven-tional MPCC suffers from high computational complexity and tedious weighting factor tuning in multi-level inverter applications.A low-complexity MPCC without weighting factors for a four-level ANPC inverter is proposed in this *** computational burden and voltage vector candidate set are reduced according to the relationship between voltage vector and neutral point voltage *** proposed MPCC shows excellent steady-state and dynamics performances while ensuring the neutral point voltage *** efficacy of the proposed MPCC is verified by simulation and experimental results.

关键词： four-level active neutral point clamped(ANPC)inverter model predictive current control(MPCC) low complexity without weighting factors

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The efficacy of vitamin E in preventing arthrofibrosis after joint replacement

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Animal Models and Experimental Medicine 2024年第2期7卷 145-155页

作者： Yingfang fan Jean Yuh Sashank Lekkala Mehmet d.Asik Andrew Thomson Madeline McCanne Mark A.Randolph Antonia F.Chen Ebru Oral Harris Orthopaedic Laboratory Department of Orthopaedic SurgeryMassachusetts General HospitalBostonMassachusettsUSA department of Orthopaedic Surgery Harvard Medical SchoolBostonMassachusettsUSA department of Surgery Harvard Medical SchoolBostonMassachusettsUSA department of Orthopaedic Surgery Brigham and Women's HospitalBostonMassachusettsUSA

Background:Arthrofibrosis is a joint disorder characterized by excessive scar formation in the joint *** E is an antioxidant with potential anti-fibroblastic *** aim of this study was to establish an arthrofibrosis rat model after joint replacement and assess the effects of vitamin E supplementation on joint ***:we simulated knee replacement in 16 male Sprague–dawley *** immobilized the surgical leg with a suture in full *** control groups were killed at 2 and 12 weeks(n=5 per group),and the test group was supplemented daily with vitamin E(0.2 mg/mL)in their drinking water for 12 weeks(n=6).we performed histological staining to investigate the presence and severity of *** staining andα2-macroglobulin(α2M)enzyme-linked immunosorbent assay(ELISA)were used to assess local and systemic *** weight bearing(total internal reflection)and range of motion(ROM)were collected for functional ***:The ROM and weight-bearing symmetry decreased after the procedure and recovered slowly with still significant deficit at the end of the study for both *** analysis confirmed fibrosis in both lateral and posterior periarticular *** E supplementation showed a moderate anti-inflammatory effect on the local and systemic *** vitamin E group exhibited significant improvement in ROM and weight-bearing symmetry at day 84 compared to the control ***:This model is viable for simulating arthrofibrosis after joint *** E may benefit postsurgical arthrofibrosis,and further studies are needed for dosing requirements.

关键词： arthrofibrosis range of motion total knee arthroplasty vitamin E

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Effect of Rare-Earth Element Substitution in Superconducting R_(3)Ni_(2)O_(7) under Pressure

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Chinese Physics Letters 2024年第8期41卷 77-81页

作者： Zhiming Pan Chen Lu fan Yang Congjun wu Institute for Theoretical Sciences Westlake UniversityHangzhou 310024China New Cornerstone Science Laboratory Department of PhysicsSchool of ScienceWestlake UniversityHangzhou 310024China School of Physics Beijing Institute of TechnologyBeijing 100081China Key Laboratory for Quantum Materials of Zhejiang Province School of ScienceWestlake UniversityHangzhou 310024China Institute of Natural Sciences Westlake Institute for Advanced StudyHangzhou 310024China

Recently,high temperature(T_(c)≈80 K)superconductivity(SC)has been discovered in La_(3)Ni_(2)O_(7)(LNO)under *** raises the question of whether the superconducting transition temperature T_(c) could be further enhanced under suitable *** possible route for achieving higher T_(c) is element *** SC could appear in the Fmmm phase of rare-earth(RE)R_(3)Ni_(2)O_(7)(RNO,R=RE element)material series under suitable *** electronic properties in the RNO materials are dominated by the Ni 3d orbitals in the bilayer NiO_(2) *** the strong coupling limit,the SC could be fully characterized by a bilayer single 3d_(x^(2)−y^(2))-orbital t–J‖–J⊥ *** RE element substitution from La to other RE element,the lattice constant of the Fmmm RNO material decreases,and the resultant electronic hopping integral increases,leading to stronger superexchanges between the 3d_(x^(2)−y^(2)) *** on the slave-boson mean-field theory,we explore the pairing nature and the evolution of T_(c) in RNO materials under ***,it is found that the element substitution does not alter the pairing nature,i.e.,the inter-layer s-wave pairing is always favored in the superconducting RNO under ***,the T_(c) increases from La to Sm,and a nearly doubled T_(c) could be realized in SmNO under *** work provides evidence for possible higher T_(c) R_(3)Ni_(2)O_(7) materials,which may be realized in further experiments.

关键词： element substitution Rare

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Classification of high-ordered topological nodes towards Moiré flat bands in twisted bilayers

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Science China(Physics,Mechanics & Astronomy) 2024年第9期Mechanics & Astronomy) .卷 137-151页

作者： fan Cui Congcong Le Qiang Zhang Xianxin wu Jiangping Hu Ching-Kai Chiu Beijing National Laboratory for Condensed Matter Physics Institute of PhysicsChinese Academy of Sciences School of Physical Sciences University of Chinese Academy of Sciences RIKEN Interdisciplinary Theoretical and Mathematical Sciences(iTHEMS) CAS Key Laboratory of Theoretical Physics Institute of Theoretical PhysicsChinese Academy of Sciences Kavli Institute of Theoretical Sciences University of Chinese Academy of Sciences New Cornerstone Science Laboratory

At magic twisted angles, dirac cones in twisted bilayer graphene(TBG) can evolve into flat bands, serving as a critical playground for the study of strongly correlated physics. when chiral symmetry is introduced, rigorous mathematical proof confirms that the flat bands are locked at zero energy in the entire Moiré Brillouin zone(BZ). Yet, TBG is not the sole platform that exhibits this absolute band flatness. Central to this flatness phenomenon are topological nodes and their specific locations in the BZ. In this study, considering twisted bilayer systems that preserve chiral symmetry, we classify various ordered topological nodes in base layers and all possible node locations across different BZs. Specifically, we constrain the node locations to rotational centers,such as Γ and M points, to ensure the interlayer coupling retains equal strength in all directions. Using this classification as a foundation, we systematically identify the conditions under which Moiré flat bands emerge. Additionally, through the extension of holomorphic functions, we provide proof that flat bands are locked at zero energy, shedding light on the origin of the band flatness. Remarkably, beyond dirac cones, numerous twisted bilayer nodal platforms can host flat bands with a degeneracy number of more than two, such as four-fold, six-fold, and eight-fold. This multiplicity of degeneracy in flat bands might unveil more complex and enriched correlation physics.

关键词： twisted bilayer systems high-ordered topological nodes Morié flat bands high degeneracy

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when quantum dots meet blue phase liquid crystal elastomers:visualized full-color and mechanically-switchable circularly polarized luminescence

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Light(Science & Applications) 2024年第6期13卷 1210-1220页

作者： Shan Li Yuqi Tang Qingyan fan Ziyuan Li Xinfang Zhang Jingxia wang Jinbao Guo Quan Li Key Laboratory of Carbon Fibers and Functional Polymers Ministry of Educationand College of Materials Science and EngineeringBeijing University of Chemical Technology100029BeijingChina Institute of Advanced Materials and School of Chemistry and Chemical Engineering Southeast UniversityNanjing211189China Materials Science Graduate Program Kent State UniversityKentOH44242USA CAS Key Laboratory of Bio-Inspired Materials and Interfacial Sciences Technical Institute of Physics and ChemistryChinese Academy of Sciences100190BeijingChina

Polymer-based circularly polarized luminescence(CPL)materials with the advantage of diversified structure,easy fabrication,high thermal stability,and tunable properties have garnered considerable ***,adequate and precise tuning over CPL in polymer-based materials remains challenging due to the difficulty in regulating chiral ***,visualized full-color CPL is achieved by doping red,green,and blue quantum dots(Qds)into reconfigurable blue phase liquid crystal elastomers(BPLCEs).In contrast to the CPL signal observed in cholesteric liquid crystal elastomers(CLCEs),the chiral 3d cubic superstructure of BPLCEs induces an opposite CPL ***,this effect is entirely independent of photonic bandgaps(PBGs)and results in a high glum value,even without matching between PBGs and the emission bands of ***,the lattice structure of the BPLCEs can be reversibly switched via mechanical stretching force,inducing on-off switching of the CPL signals,and these variations can be further fixed using dynamic disulfide bonds in the ***,the smart polymer-based CPL systems using the BPLCEs for anti-counterfeiting and information encryption have been demonstrated,suggesting the great potential of the BPLCEs-based CPL active materials.

关键词： circular quantum crystal

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