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Development of an automatic measurement system using atmospheric pressure photoionization ultrahigh-resolution mass spectrometry and application for on-line analysis of particulate matter

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Journal of Environmental Sciences 2024年第4期138卷 516-530页

作者： Yayuan Dong Ranran Liu Ling Xie Xiaole Pan Yele Sun Lin Wu ZifaWang State key laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry Institute of Atmospheric PhysicsChinese Academy of SciencesBeijing 100029China College of Earth and Planetary Sciences University of Chinese Academy of SciencesBeijing 100049China Center for Excellence in Regional Atmospheric Environment Chinese Academy of SciencesInstitute of Urban EnvironmentXiamen 361021China

On-line chemical characterization of atmospheric particulate matter(PM)with soft ionization technique and ultrahigh-resolution Mass Spectrometry(UHRMS)provides molecular information of organic constituents in real time.Here we describe the development and application of an automatic measurement system that incorporates PM_(2.5)sampling,thermal desorption,atmospheric pressure photoionization,and UHRMS analysis.Molecular formulas of detected organic compounds were deducted from the accurate(±10 ppm)molecular weights obtained at a mass resolution of 100,000,allowing the identification of small organic compounds in PM_(2.5).Detection efficiencies of 28 standard compounds were determined and we found a high sensitivity and selectivity towards organic amines with limits of detection below 10 pg.As a proof of principle,PM_(2.5)samples collected off-line in winter in the urban area of Beijing were analyzed using the Ionization Module and HRMS of the system.The automatic system was then applied to conduct on-line measurements during the summer time at a time resolution of 2 hr.The detected organic compounds comprised mainly CHON and CHN compounds below 350 m/z.Pronounced seasonal variations in elemental composition were observed with shorter carbon backbones and higher O/C ratios in summer than that in winter.This result is consistent with stronger photochemical reactions and thus a higher oxidation state of organics in summer.Diurnal variation in signal intensity of each formula provides crucial information to reveal its source and formation pathway.In summary,the automatic measurement system serves as an important tool for the on-line characterization and identification of organic species in PM_(2.5).

关键词： PM_(2.5) Chemical composition On-line measurement technique High resolution mass spectrometry

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Development and evaluation of an online monitoring single-particle optical particle counter with polarization detection

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Journal of Environmental Sciences 2024年第4期138卷 585-596页

作者： Weijie Yao Xiaole Pan Yu Tian Hang Liu Yuting Zhang Shandong Lei Junbo Zhang Yinzhou Zhang LinWu Yele Sun Zifa Wang State key laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry Institute of Atmospheric PhysicsChinese Academy of SciencesBeijing 100029China College of Earth and Planetary Sciences University of Chinese Academy of SciencesBeijing 100049China Center for Excellence in Regional Atmospheric Environment Institute of Urban EnvironmentChinese Academy of SciencesXiamen 361021China

We developed a single-particle optical particle counter with polarization detection(SOPC)for the real-time measurement of the optical size and depolarization ratio(defined as the ratio of the vertical component to the parallel component of backward scattering)of atmospheric particles,the polarization ratio(DR)value can reflect the irregularity of the particles.The SOPC can detect aerosol particles with size larger than 500 nm and the maximum particle count rate reaches~1.8×10^(5)particles per liter.The SOPC uses a modulated polarization laser to measure the optical size of particles according to forward scattering signal and the DR value of the particles by backward S and P signal components.The sampling rate of the SOPC was 106#/(sec·channel),and all the raw data were processed online.The calibration curve was obtained by polystyrene latex spheres with sizes of 0.5-10μm,and the average relative deviation of measurement was 3.96% for sub 3μm particles.T-matrix method calculations showed that the DR value of backscatter light at 120°could describe the variations in the aspect ratio of particles in the above size range.We performed insitu observations for the evaluation of the SOPC,the mass concentration constructed by the SOPC showed good agreement with the PM_(2.5)measurements in a nearby state-controlled monitoring site.This instrument could provide useful data for source appointment and regulations against air pollution.

关键词： Instrument development Single particle detection Measurement uncertainty Optical simulation Mass concentration

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Two antibodies show broad,synergistic neutralization against SARS-CoV-2 variants by inducing conformational change within the RBD

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Protein & Cell 2024年第2期15卷 121-134页

作者： Hui Sun Tingting Deng Yali Zhang Yanling Lin Yanan Jiang Yichao Jiang Yang Huang Shuo Song Lingyan Cui Tingting Li Hualong Xiong Miaolin Lan Liqin Liu Yu Li Qianjiao Fang Kunyu Yu Wenling Jiang Lizhi Zhou Yuqiong Que Tianying Zhang Quan Yuan Tong Cheng Zheng Zhang Hai Yu Jun Zhang Wenxin Luo Shaowei Li Qingbing Zheng Ying Gu Ningshao Xia State key laboratory of Molecular Vaccinology and Molecular Diagnostics School of Public HealthSchool of Life SciencesXiamen UniversityXiamen 361102China National Institute of Diagnostics and Vaccine Development in Infectious Diseases School of Public HealthSchool of Life SciencesXiamen UniversityXiamen 361102China State key laboratory of Vaccines for Infectious Diseases School of Public HealthSchool of Life SciencesXiamen UniversityXiamen 361102China Xiang An Biomedicine laboratory Xiamen 361102China Institute for Hepatology National Clinical Research Center for Infectious DiseaseShenzhen Third People's HospitalSchool of MedicineSouthem University of Science and TechnologyShenzhen 518112China The Second Affliated Hospital School of MedicineSouthern University of Science and TechnologyShenzhen 518112China Research Unit of Frontier Technology of Structural Vaccinology Chinese Academy of Medical SciencesXiamen 361102China

Continual evolution of the severe acute respiratory syndrome coronavirus(SARS-CoV-2)virus has allowed for its gradual evasion of neutralizing antibodies(nAbs)produced in response to natural infection or vaccination.The rapid nature of these changes has incited a need for the development of superior broad nAbs(bnAbs)and/or the rational design of an antibody cocktail that can protect against the mutated virus strain.Here,we report two angiotensin-converting enzyme 2 competing nAbs—8H12 and 3E2—with synergistic neutralization but evaded by some Omicron subvariants.Cryo-electron microscopy reveals the two nAbs synergistic neutralizing virus through a rigorous pairing permitted by rearrangement of the 472-489 loop in the receptor-binding domain to avoid steric clashing.Bispecific antibodies based on these two nAbs tremendously extend the neutralizing breadth and restore neutralization against recent variants including currently dominant XBB.1.5.Together,these findings expand our understanding of the potential strategies for the neutralization of SARS-CoV-2 variants toward the design of broad-acting antibody therapeutics and vaccines.

关键词： SARS-CoV-2 broad neutralizing antibody rearrangement synergistic neutralization

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Molecular Characterization and Antibacterial Activity of a G-Type Lysozyme in Yellow Drum(Nibea albiflora)

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Journal of Ocean University of China 2024年第2期23卷 477-486页

作者： XIAO Yao LI Jiacheng TIAN Qianqian WU Baolan HAN Fang State key laboratory of Mariculture Breeding Fisheries College of Jimei UniversityXiamen 361021China

Lysozyme(EC3.***.1.17)plays an important role in the immune response;as a nonspecific immune factor,it can resist causative agents.Lysozyme can be divided into c-type and g-type in fish.In a previous study,through genome-wide association analysis,the g-type lysozyme gene,which is named NaLyg in yellow drum(Nibea albiflora),was found to be a key candidate gene for disease resistance in response to Vibrio harveyi infection.The cDNA of NaLyg was 1025 bp,including four exons and three introns,and its open reading frame(ORF)had a full-length of 582 bp,encoding 193 amino acids.NaLyg was found to be conserved during evolution through bioinformatic analyses.The NaLyg protein possessed a sugar binding domain and three catalytic sites,including Glu71,Asp84 and Asp101.Quantitative qRT-PCR results confirmed that NaLyg gene mRNA was visibly increased after V.harveyi infection.The NaLyg protein purified by prokaryotic expression killed some gram-negative bacterial pathogens by inducing cell wall destruction,including V.harveyi,Aeromonas hydrophila and Edwardsiella tarda.Moreover,the NaLyg protein killed two gram-positive bacteria,Bacillus subtilis and Staphylococcus aureus.Taken together,the experimental results suggested that the NaLyg protein of N.albiflora played an important role in fighting bacterial infections.

关键词： Nibea albiflora innate immunity Vibrio harveyi g-type lysozyme antibacterial activity

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Synergistic integration of self-supported 1T/2H-WS_(2) and nitrogendoped rGO on carbon cloth for pH-universal electrocatalytic hydrogen evolution

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Nano Research 2024年第3期17卷 1267-1280页

作者： Feng Ming Yap Jian Yiing Loh Wee-Jun Ong School of Energy and Chemical Engineering Xiamen University MalaysiaSelangor Darul Ehsan 43900Malaysia Center of Excellence for NaNo Energy&Catalysis Technology(CONNECT) Xiamen University MalaysiaSelangor Darul Ehsan 43900Malaysia State key laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Gulei Innovation Institute Xiamen UniversityZhangzhou 363200China Shenzhen Research Institute of xiamen University Shenzhen 518057China

Hydrogen economy based on electrochemical water splitting exemplified one of the most promising means for overcoming the rapid consumption of fossil fuels and the serious deterioration of global climate.The development of earth-abundant,efficient,and durable electrocatalysts for hydrogen evolution reaction(HER)plays a vital role in the commercialization of water electrolysis.Regard,the self-supported electrode with unique nitrogen-doped reduced graphene oxide(N-rGO)nanoflakes and WS_(2) hierarchical nanoflower that were grown directly on carbon cloth(CC)substrate(WS_(2)/N-rGO/CC)was successfully synthesized using a facile dual-step hydrothermal approach.The as-synthesized 50%1T/2H-WS_(2)/N-rGO/CC(WGC),which possessed high metallic 1T phase of 57%not only efficiently exposed more active sites and accelerated mass/charge diffusion,but also endowed excellent structural lustiness,robust stability,and durability at a high current density.As a result,the 50%WGC exhibited lower overpotentials and Tafel slopes of 21.13 mV(29.55 mV∙dec^(-1))and 80.35 mV(137.02 mV∙dec^(-1))as compared to 20%Pt-C/CC,respectively for catalyzing acidic and alkaline hydrogen evolution reactions.Pivotally,the as-synthesized 50%WGC also depicted long-term stability for more than 8 h in the high-current-density regions(100 and 220 mA∙cm^(-2)).In brief,this work reveals a self-supported electrode as an extraordinary alternative to Pt-based catalysts for HER in a wide pH range,while paving a facile strategy to develop advanced electrocatalysts with abundant heterointerfaces for practical applications in energy-saving hydrogen production.

关键词： self-supported electrocatalyst carbon-based substrate phase engineering pH-universal water splitting

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Magnetic resonance imaging techniques for lithium-ion batteries:Principles and applications

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Magnetic Resonance Letters 2024年第2期4卷 22-39页

作者： Hongxin Lin Yanting Jin Mingming Tao Yingao Zhou Peizhao Shan Danhui Zhao Yong Yang State key laboratory for Physical Chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy Materials and Department of ChemistryCollege of Chemistry and Chemical EngineeringTan Kah Kee Innovation Laboratory(IKKEM)Xiamen UniversityXiamen361005China School of Energy Xiamen UniversityXiamen361005China

Operando monitoring of internal and local electrochemical processes within lithium-ion batteries(LIBs)is crucial,necessitating a range of non-invasive,real-time imaging characterization techniques including nuclear magnetic resonance(NMR)techniques.This review provides a comprehensive overview of the recent applications and advancements of non-invasive magnetic resonance imaging(MRI)techniques in LIBs.It initially introduces the principles and hardware of MRI,followed by a detailed summary and comparison of MRI techniques used for characterizing liquid/solid electrolytes,electrodes and commercial batteries.This encompasses the determination of electrolytes'transport properties,acquisition of ion distribution profile,and diagnosis of battery defects.By focusing on experimental parameters and optimization strategies,our goal is to explore MRI methods suitable to a variety of research subjects,aiming to enhance imaging quality across diverse scenarios and offer critical physical/chemical insights into the ongoing operation processes of LIBs.

关键词： Lithium-ion batteries Magnetic resonance imaging(MRI) Electrolytes Electrodes Commercial batteries

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A short overview of the lead iodide residue impact and regulation strategies in perovskite solar cells

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Journal of Energy Chemistry 2024年第3期90卷 504-510,I0012页

作者： Eng Liang Lim Zhanhua Wei xiamen key laboratory of Optoelectronic Materials and Advanced Manufacturing Institute of Luminescent Materials and Information DisplaysCollege of Materials Science and EngineeringHuaqiao UniversityXiamen 361021FujianChina

Lead iodide(PbI2) is a vital raw material for preparing perovskite solar cells(PSCs),and it not only takes part in forming the light absorption layer but also remains in the grain boundary as a passivator.In other words,the PbI2 content in the precursor and as formed film will affect the efficiency and stability of the PSCs.With moderate residual PbI2,it passivates the bulk/surface defects of perovskite,reduces the interfacial recombination,promotes the perovskite stability,minimizes the device hysteresis,and so on.Deficient PbI2 residue will reduce the interfacial passivation effect and device performance.In addition to facilitating the non-radiative recombination,over PbI2 residue can also lead to electronic insulation in the grain boundary and deteriorate the device performance.However,the impact and regulation of PbI2 residue on the device performance and stability is still not fully understood.Herein,a comprehensive and detailed review is presented by discussing the PbI2 residue impact and its regulation strategies(i.e., elimination,facilitation and conversion of the residue PbI2) to manipulate the PbI2 content,distribution and forms.Finally,we also show future outlooks in this field,with an aim to help further the progression of high-efficiency and stable PSCs.

关键词： Lead iodide Residue Regulation Perovskite solar cells Efficiency Stability

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Composite laminar membranes for electricity generation from water evaporation

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Nano Research 2024年第1期17卷 307-311页

作者： Xiao Wang Gang Yuan Han Zhou Yu Jiang Shuo Wang Jiaojiao Ma Chongyang Yang Sheng Hu State key laboratory of Physical Chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy Materials(iChEM)College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Innovation laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM) Xiamen 361005China Pen-Tung Sah Institute of Micro-Nano Science and Technology Xiamen UniversityXiamen 361005China

Harvesting clean energy from water evaporation has been extensively investigated due to its sustainability.To achieve high efficiency,energy conversion materials should contain multiple features which are difficult to be simultaneously obtained from single-component materials.Here we use composite laminar membranes assembled by nanosheets of graphene oxide and mica,and find a sustained power density induced by water evaporation that is two orders of magnitude larger than that from membranes made by either of the components.The power output is attributed to selective proton transport driven by water evaporation through the interlayer nanochannels in the membranes.This process relies on the synergistic effects from negatively charged and hydrophilic mica surfaces that are important for proton selectivity and water transport,and the tunable electrical conductivity of graphene oxide that provides optimized internal resistance.The demonstrated composite membranes offer a strategy of enhancing power generation by combining the advantages from each of their components.

关键词： graphene oxide mica water evaporation electrical double layer surface charge ion selectivity

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

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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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Assembly of peptide nanostructures with controllable sizes

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Nano Research 2024年第1期17卷 151-161页

作者： Dan Cheng Fan Jia Yun-Bao Jiang Vincent P.Conticello Tao Jiang The MOE key laboratory of Spectrochemical Analysis and Instrumentation Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Innovation laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM) Xiamen 361005China Department of Chemistry Emory UniversityAtlanta 30033USA

Controlled peptide assembly offers significant promise to develop synthetic supramolecular nanostructures to display material and biological properties that mimic protein assemblies in nature.Despite the progress in forming peptide nanostructures of various morphology,there exists a distinct gap between natural and synthetic assembly systems in terms of size control.Constructing nanostructures with a narrow size distribution that can be tuned over a wide range of length-scales is essential for applications that require precise spacing between objects.This approach provides the opportunity to correlate materials and biological properties of interest with assembly size.In this review,we discuss representative endeavors over the past two decades for design of size-controllable peptide nanostructures using tunable building blocks.Other mechanisms for size control,e.g.,molecular frustration,template-directed peptide assembly,and multi-component peptide co-assembly,will also be discussed.We also demonstrate the applicable scopes of these strategies and suggest potential future avenues for scientific advances in this field.

关键词： peptide assembly controllable size template multi-component

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