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Dynamic tracking of exsolved PdPt alloy/perovskite catalyst for efficient lean methane oxidation

Chinese chemical Letters 2024年第4期35卷 170-175页

作者： Yanling Yang Zhenfa Ding Huimin Wang Jianhui Li Yanping Zheng Hongquan Guo Li Zhang Bing Yang Qingqing Gu Haifeng Xiong Yifei Sun College of Energy Xiamen UniversityXiamen 361005China School of Environment and Civil Engineering Dongguan University of TechnologyDongguan 523808China Department of Chemistry College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China CAS Key Laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM) Xiamen 361102China

Supported Pd based catalysts are considered as the efficient candidates for low-carbon alkane oxidation for their outstanding capability to break C-H bond. Whereas, the irreversible deactivation of Pd based catalysts was still frequently observed. Herein, we reinforced the extruded Pd nanoparticles with quantitive Pt to assemble the evenly distributed Pd Pt nanoalloy onto ferrite perovskite(Pd Pt-LCF) matrix with strengthened robustness of metal/oxide support interface. We further co-achieved the enhanced performance, anti-overoxidation as well as resistance of vapor-poisoning in durability measurement. The operando X-ray photoelectron spectroscopy(O-XPS) combined with various morphology characterizations confirms that the accumulation of surface deep-oxidation species of Pd^(4+) is the culprit for fast activity loss in exsolved Pd system, especially at high temperature of 400 ℃. Conversely, it could be completely suppressed by in-situ alloying Pd with equal amount of Pt, which helps maintain the metastable Pd^(2+)/Pd shell and metallic solid-solution core structure. The density function theory(DFT) calculations further buttress that the dissociation of C–H was facilitated on alloy/perovskite interface which is, on the contrary, resistant toward O–H bond cleavage, as compared to Pd/perovskite. Our work suggests that the modification of exsolved metal/oxide catalytic interface could further enrich the toolkit of heterogeneous catalyst design.

关键词： Exsolution PdPt alloy Operando characterization Methane conversion Deep-oxidation

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Synthesis strategies of hard carbon anodes for sodium-ion batteries

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Materials Reports(Energy) 2024年第2期4卷 1-22页

作者： Jian Yin Ye Shui Zhang Hanfeng Liang Wenli Zhang Yunpei Zhu Laboratory of Environmental Sciences and Technology Xinjiang Technical Institute of Physics&ChemistryChinese Academy of SciencesUrumqi830011China Materials Science and Engineering Physical Science and Engineering DivisionKing Abdullah University of Science and Technology(KAUST)Thuwal23955-6900Saudi Arabia School of Engineering University of AberdeenAberdeenAB243UEUK State Key Laboratory of Physical Chemistry of Solid Surfaces Tan Kah Kee Innovation Laboratory(IKKEM)College of Chemistry and Chemical EngineeringXiamen UniversityXiamen361005China Guangdong Provincial Laboratory of Chemistry and Fine Chemical Engineering Jieyang Center Jieyang515200China Guangdong Provincial Key Laboratory of Plant Resources Biorefinery School of Chemical Engineering and Light IndustryGuangdong University of Technology(GDUT)Panyu DistrictGuangzhou510006China School of Advanced Manufacturing Guangdong University of Technology(GDUT)Jieyang522000China

Sodium-ion battery(SIB)is an ideal candidate for large-scale energy storage due to high abundant sodium sources,relatively high energy density,and potentially low *** carbons,as one of the most promising anodes,could deliver high plateau capacities at low potentials,which boosts the energy densities of *** slope capacities have been demonstrated from the defect adsorption of sodium ions,while the plateau capacity depends highly on intercalation and pore ***,the specific structures of sodium ions stored in hard carbons have not been clarified,namely active sites of adsorption,intercalation,and pore-filling ***,delicate synthesis methods are required to prepare hard carbons with controllable specific structures,along with elucidating the precise active sites for enhancing the Na-ion storage *** offer databases for future designs,we summarized the synthesis strategies of hard carbon anodes for constructing active sites of plateau *** methods were highlighted with corresponding influences on the meticulous structures of hard carbons and Na-ion storage *** but not least,perspectives were proposed for developing hard carbon anodes from the points of research and practical applications.

关键词： Hard carbon anodeCarbon synthesisSodium-ion batteryStructure-function relationship

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Temperature-regulation liquid gating membrane with controllable gas/liquid separation

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Green Energy & Environment 2023年第6期8卷 1501-1508页

作者： Baiyi Chen Huimeng Wang Jiadai Xu Liting Pan Yuan Jing Xu Hou State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen361005China Department of Physics Research Institute for Biomimetics and Soft MatterFujian Provincial Key Laboratory for Soft Functional Materials ResearchJiujiang Research InstituteCollege of Physical Science and TechnologyXiamen UniversityXiamen361005China Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM) Xiamen361102China State Key Laboratory of Bio-Fibers and Eco-Textiles Qingdao UniversityQingdao266071China

Membrane separation technology with the ability to regulate gas/liquid transport and separation is critical for environmental fields, such as sewerage treatment, multiphase separation, and desalination. Although numerous membranes can dynamically control liquid-phase fluids transport via external stimuli, the transport and separation of gas-phase fluids remains a challenge. Here, we show a temperature-regulation liquid gating membrane that allows in-situ dynamically controllable gas/liquid transfer and multiphase separation by integrating a thermo-wettability responsive porous membrane with functional gating liquid. Experiments and theoretical analysis have demonstrated the temperature-regulation mechanism of this liquid gating system, which is based on thermo-responsive changes of porous membrane surface polarity, leading to changes in affinity between the porous membrane and the gating liquid. In addition, the sandwich configuration with dense Au-coated surfaces and heterogeneous internal components by a bistable interface design enables the liquid gating system to enhance response sensitivity and maintain working stability. This temperature-regulation gas/liquid transfer strategy expands the application range of liquid gating membranes,which are promising in environmental governance, water treatment and multiphase separation.

关键词： Temperature-regulation Liquid gating membrane Sandwich configuration Multiphase separation Environmental governance

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Editorial for special issue on electromagnetic wave absorbing materials

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International Journal of Minerals,Metallurgy and Materials 2023年第3期30卷 401-404页

作者： Guanglei Wu Hongjing Wu Zirui Jia Institute of Materials for Energy and Environment State Key Laboratory of Bio-fibers and Eco-textilesCollege of Materials Science and EngineeringQingdao UniversityQingdao 266071China MOE Key Laboratory of Material Physics and Chemistry under Extraordinary School of Physical Science and TechnologyNorthwestern Polytechnical UniversityXi’an 710072China College of Chemistry and Chemical Engineering Qingdao UniversityQingdao 266071China

With the rapid development of information technology and electronics industry,stealth warplanes,radar stealth,electronic countermeasures,microwave communications,and other equipment have played an increasingly important role in military ***,the design and development of new electromagnetic wave(EMW)absorbing materials with high performance and environmental applicability that can be widely used in the microwave field has become a key issue and a major strategic challenge that needs to be urgently addressed in the modernization and upgrading of major advanced military ***,how to effectively address the growing electromagnetic pollution has been an important issue that has plagued researchers in the field of EMW absorption for many years.

关键词： absorbing microwave wave

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Electrochemical conversion of methane to bridge the gap in the artificial carbon cycle

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Journal of Energy Chemistry 2025年第1期100卷 286-308页

作者： Yuhao Peng Yuefeng Song Ihar Razanau Juanxiu Xiao Wei Xiao Di Hu Guoxiong Wang College of Chemistry and Molecular Sciences Hubei Key Laboratory of Electrochemical Power SourcesWuhan UniversityWuhan 430072HubeiChina State Key Laboratory of Catalysis Dalian National Laboratory for Clean EnergyiChEM(Collaborative Innovation Center of Chemistry for Energy Materials)Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina Laboratory of Physical-Chemical Technologies SSPA Scientific and Practical Materials Research Centre of NAS of BelarusMinsk 220072Belarus State Key Laboratory of Marine Resources Utilization in South China Sea Collaborative Innovation Center of Marine Science and TechnologySchool of Marine Science and EngineeringHainan UniversityHaikou 570228HainanChina Department of Chemical and Environmental Engineering University of Nottingham Ningbo ChinaNingbo 315100ZhejiangChina

Methane, an abundant one-carbon(C_(1)) resource, is extensively used in the industrial production of vital fuels and value-added chemicals. However, current industrial methane conversion technologies are energy-and carbon-intensive, mainly due to the high activation energy required to break the inert C–H bond, low selectivity, and problematic side reactions, including CO_(2)emissions and coke deposition. Electrochemical conversion of methane(ECM) using intermittent renewable energy offers an attractive solution, due to its modular reactor design and operational flexibility across a broad spectrum of temperatures and pressures. This review emphasizes conversion pathways of methane in various reaction systems, highlighting the significance and advantages of ECM in facilitating a sustainable artificial carbon cycle. This work provides a comprehensive overview of conventional methane activation mechanisms and delineates the complete pathways of methane conversion in electrolysis contexts. Based on surface/interface chemistry, this work systematically analyzes proposed reaction pathways and corresponding strategies to enhance ECM efficiency towards various target products, including syngas, hydrocarbons, oxygenates, and advanced carbon materials. The discussion also encompasses opportunities and challenges for the ECM process, including insights into ECM pathways, rational electrocatalyst design, establishment of benchmarking protocols, electrolyte engineering, enhancement of CH4conversion rates, and minimization of CO_(2)emission.

关键词： Methane Electrochemical conversion Reaction mechanism Catalyst design Electrode Electrocatalysis

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Thermal energy dependent transient permittivity of epsilon-near-zero material

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science China(physics,Mechanics & Astronomy) 2022年第8期65卷 96-101页

作者： Heng Wang Lixun Sun Kang Du Wending Zhang SooJin Chua Guixin Li Ting Mei MOE Key Laboratory of Material Physics and Chemistry under Extraordinary Conditions and Shaanxi Key Laboratory of Optical Information TechnologySchool of Physical Science and TechnologyNorthwestern Polytechnical UniversityXi’an710129China Department of Materials Science and Engineering Southern University of Science and TechnologyShenzhen518055China Shenzhen Institute for Quantum Science and Engineering Southern University of Science and TechnologyShenzhen518055China Department of Electrical and Computer Engineering National University of SingaporeSingapore117583Singapore LEES Program Singapore-MIT Alliance for Research&Technology(SMART)Singapore138602Singapore

Transparent conductive oxides exhibit attractive optical nonlinearity with ultrafast response and giant refractive index change near the epsilon-near-zero(ENZ) wavelength, originating from the intraband dynamics of conduction electrons. The optical nonlinearity of ENZ materials has been explained by using the overall-effective-mass and the overall-scattering-time of electrons in the extended Drude model. However, their response to optical excitation is yet the last building block to complete the theory. In this paper, the concept of thermal energy is theoretically proposed to account for the total energy of conduction electrons exceeding their thermal equilibrium value. The time-varying thermal energy is adopted to describe the transient optical response of indium-tin-oxide(ITO), a typical ENZ material. A spectrally-resolved femtosecond pump-probe experiment was conducted to verify our theory. By correlating the thermal energy with the pumping density, both the giant change and the transient response of the permittivity of ITO can be predicted. The results in this work provide a new methodology to describe the transient permittivities of ENZ materials, which will benefit the design of ENZ-based nonlinear photonic devices.

关键词： epsilon-near-zero optical nonlinearity transient response thermal energy hot electron indium tin oxide

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Fe^(3+) ion quantification with reusable bioinspired nanopores

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Chinese chemical Letters 2025年第2期36卷 179-184页

作者： Yanqiong Wang Yaqi Hou Fengwei Huo Xu Hou Institute of Flexible Electronics(IFE Future Technologies)Xiang'an CampusXiamen UniversityXiamen 361102China State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Institute of Artificial Intelligence Xiamen UniversityXiamen 361005China Department of Physics Research Institute for Biomimetics and Soft MatterFujian Provincial Key Laboratory for Soft Materials ResearchJiujiang Research InstituteCollege of Physical Science and TechnologyXiamen UniversityXiamen 361005China Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM) Xiamen 361102China Engineering Research Center of Electrochemical Technologies of Ministry of Education Xiamen UniversityXiamen 361005China

Excessive Fe^(3+) ion concentrations in wastewater pose a long-standing threat to human *** low-cost,high-efficiency quantification of Fe^(3+) ion concentration in unknown solutions can guide environmental management decisions and optimize water treatment *** this study,by leveraging the rapid,real-time detection capabilities of nanopores and the specific chemical binding affinity of tannic acid to Fe^(3+),a linear relationship between the ion current and Fe^(3+) ion concentration was *** this linear relationship,quantification of Fe^(3+) ion concentration in unknown solutions was ***,ethylenediaminetetraacetic acid disodium salt was employed to displace Fe^(3+) from the nanopores,allowing them to be restored to their initial conditions and reused for Fe^(3+) ion *** reusable bioinspired nanopores remain functional over 330 days of *** recycling capability and the long-term stability of the nanopores contribute to a significant reduction in *** study provides a strategy for the quantification of unknown Fe^(3+) concentration using nanopores,with potential applications in environmental assessment,health monitoring,and so forth.

关键词： Bioinspired nanopores Fe^(3+)ion quantification chemical binding affinity Tannic acid Reusability

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Highly insulating alkane rings with destructive σ-interference

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science China Chemistry 2022年第9期65卷 1822-1828页

作者： Jingyao Ye Alaa Al-Jobory Qian-Chong Zhang Wenqiang Cao Abdullah Alshehab Kai Qu Turki Alotaibi Hang Chen Junyang Liu Ali K.Ismael Zhong-Ning Chen Colin J.Lambert Wenjing Hong State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Department of Physics Lancaster UniversityLancaster LA14YBUK State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China Department of Physics College of Education for Pure ScienceTikrit UniversityTikritIraq Department of Physics College of ScienceUniversity of AnbarAnbarIraq School of Physical Science and Technology Shanghai Tech UniversityShanghai 201210China Department of Physics College of ScienceKing Faisal UniversityAlAhsaSaudi Arabia Department of Physics College of ScienceJouf UniversitySkakaSaudi Arabia

Destructive quantum interference(DQI)provides a unique approach to controlling the leakage current in the OFF state of molecular ***,the DQI in π-conjugated molecular building blocks cannot exhibit ultralow conductance due to the existence of covalently bonded σ-transport ***,suppressing the σ-contribution via σ-DQI is essential for the fabrication of molecular junctions with high insulation and effective modulation of conductance in single-molecule ***,we demonstrate the existence of σ-DQI even in a simple series of C_(m)C_(n) ring molecules,with parallel chains of m and n alkyl units(where m,n=6,8 or 10),by measuring their electrical conductance and Seebeck ***,the conductance of the symmetric C_(n)C_(n) rings is lower than that of the corresponding single chains(C_(n)),which is in contrast to the conductance superposition law in multi-channeled *** theoretical calculations reveal that the gauche conformation in a shorter chain fixed by another chain leads to the decreased conductance in alkyl rings,which originates from the phase-coherent tunneling and DQI in σ-conjugated *** finding suggests that through appropriate conformation locking by cyclization,the covalent alkane system can exhibit DQI,which offers strategies for future designs of molecular electronic devices and materials.

关键词： destructiveσ-interference charge transport single-molecule electronics insulating material alkane ring

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Size-dependent cellular uptake and sustained drug release of PLGA particles

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Particuology 2023年第2期73卷 1-7页

作者： Rui Sun Xia Liu Yu Zhang Qian Li Ying Zhu Chunhai Fan Division of Physical Biology CAS Key Laboratory of Interfacial Physics and TechnologyShanghai Institute of Applied PhysicsChinese Academy of SciencesShanghai 201800China The Interdisciplinary Research Center Shanghai Synchrotron Radiation FacilityZhangjiang LaboratoryShanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201210China University of Chinese Academy of Sciences Beijing 100049China School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative Molecules and National Center for Translational MedicineShanghai Jiao Tong UniversityShanghai 200240China

Poly(lactic-co-glycolic)acid(PLGA)particles have become a commonly used drug delivery strategy in the pharmaceutical *** this work,we aim to investigate the size-dependent cellular internalization of PLGA particles and its effects on sustained drug *** prepared three different-sized particles using PLGA(200,500 and 2000 nm)ranging from submicrometer to ***(DEX)with excellent anti-inflammatory properties was used as a model drug to prepare DEX-loaded PLGA particles(DPs).We comprehensively investigated the encapsulation efficiency,cellular uptake and in vitro drug release *** assessment revealed that,in the lipopolysaccharide(LPS)-induced RAW 264.7 cells model,500 nm DPs showed sustained anti-inflammatory *** work provides important information for designing PLGA-based drug delivery systems for biomedical applications.

关键词： DEX-loaded PLGA particles(DPs) Sustained release Anti-inflammatory efficacy

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Fused-ring induced end-on orientation in conjugated molecular dyads toward efficient single-component organic solar cells

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Aggregate 2023年第2期4卷 291-299页

作者： Dongdong Xia Shengxi Zhou Wen Liang Tan Safakath Karuthedath Chengyi Xiao Chaowei Zhao Frédéric Laquai Christopher R.McNeill Weiwei Li Institute of Applied Chemistry Jiangxi Academy of SciencesNanchangChina Beijing Advanced Innovation Center for Soft Matter Science and Engineering&State Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical TechnologyBeijingChina Department of Materials Science and Engineering Monash UniversityClaytonAustralia KAUST Solar Center(KSC) Physical Sciences and Engineering Division(PSE)Material Science and Engineering Program(MSE)King Abdullah University of Science and Technology(KAUST)ThuwalSaudi Arabia

The molecular orientations of conjugated materials on the substrate mainly include edge-on,face-on,and ***-on and face-on orientations have been widely observed,while end-on orientation has been rarely *** in organic solar cells(OSCs)charge transport is along the vertical direction,end-on orientation with conjugated backbones perpendicular to the substrate is recognized as the ideal microstructure for *** this work,we for the first time obtained the preferential end-on orientation in a conjugated molecular dyad that contains a conjugated backbone as donor and perylene bisimide side units as *** was realized by introducing a fused-ring structure to replace linear terthiophenes with conjugated backbones,yielding F-MDPBI and L-MDPBI ***,a shifting trend of the molecular orientation from dominating edge-on in L-MDPBI to preferential end-on in F-MDPBI was *** a consequence,vertical charge carrier mobilities in F-MDPBI are one order of magnitude higher than those with preferential edge-on orientation,so single-component OSCs based on this molecular dyad as a single photoactive layer provided a power conversion efficiency of 4.89% compared to 1.70% based on L-MDPBI with preferential edge-on orientation.

关键词： conjugated molecular dyads crystallinity edge-on end-on single-component organic solar cells

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