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Building Feedback-Regulation System Through Atomic Design for Highly Active SO_(2)Sensing

Nano-Micro Letters 2024年第7期16卷 343-357页

作者： Xin Jia Panzhe Qiao Xiaowu Wang Muyu Yan Yang Chen Bao-Li An Pengfei Hu Bo Lu Jing xu Zhenggang xue jiaqiang xu NEST Lab Department of ChemistryCollege of SciencesShanghai UniversityShanghai 200444People’s Republic of China Shanghai Synchrotron Radiation Facility Zhangjiang LabShanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201204People’s Republic of China School of Chemistry and Materials Science University of Science and Technology of ChinaHefei 230026People’s Republic of China Key Laboratory of Organic Compound Pollution Control Engineering(MOE) School of Environmental and Chemical EngineeringShanghai UniversityShanghai 200444People’s Republic of China Shanghai University Instrumental Analysis&Research Center of Shanghai UniversityShanghai 200444People’s Republic of China

Reasonably constructing an atomic interface is pronouncedly essential for surface-related gas-sensing reaction.Herein,we present an ingen-ious feedback-regulation system by changing the interactional mode between single Pt atoms and adjacent S species for high-efficiency SO_(2)sensing.We found that the single Pt sites on the MoS_(2)surface can induce easier volatiliza-tion of adjacent S species to activate the whole inert S plane.Reversely,the activated S species can provide a feedback role in tailoring the antibonding-orbital electronic occupancy state of Pt atoms,thus creating a combined system involving S vacancy-assisted single Pt sites(Pt-Vs)to synergistically improve the adsorption ability of SO_(2)gas molecules.Further-more,in situ Raman,ex situ X-ray photoelectron spectroscopy testing and density functional theory analysis demonstrate the intact feedback-regulation system can expand the electron transfer path from single Pt sites to whole Pt-MoS_(2)supports in SO_(2)gas atmosphere.Equipped with wireless-sensing modules,the final Pt1-MoS_(2)-def sensors array can further realize real-time monitoring of SO_(2)levels and cloud-data storage for plant growth.Such a fundamental understanding of the intrinsic link between atomic interface and sensing mechanism is thus expected to broaden the rational design of highly effective gas sensors.

关键词： Feedback-regulation system Atomic interface SO_(2)sensor Single-atom sensing mechanism Intelligent-sensing array

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Fabrication of high sensitivity 2-PEA sensor based on Aldehyde-functionalized mesoporous carbon

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Chinese Chemical Letters 2023年第1期34卷 499-502页

作者： Ye Zhu Yongheng Zhu jiaqiang xu Department of Stomatology Huashan Hospital Affiliated to Fudan UniversityShanghai 200040China Department of Physics&Department of Chemistry College of ScienceShanghai UniversityShanghai 200444China College of Food Science&Technology Shanghai Ocean UniversityShanghai 213064China

2-Phenylethylamine(2-PEA)is one of the main ingredients for stimulants.Therefore,it is necessary to limit its use and illegal trade by conveniently detecting 2-PEA vapour.Here,a QCM based 2-PEA gas sensor was constructed by using aldehyde functionalized mesoporous carbon(FDU-15-CHO)as sensing materials designed according to Schiff base adsorption role.The 2D hexagonal mesoporous structures of the sensing material have been confirmed by small-angle X-ray diffraction(SXRD),transmission electron microscopy(TEM),and N2adsorption-desorption isotherms.The covalent grafting of aldehyde group onto the FDU-15 was confirmed by Fourier transform infrared spectroscopy(FT-IR).FDU-15-CHO based Quartz Crystal Microbalance(QCM)sensor shows better sensitivity to 2-PEA than its parent FDU-15.Besides,the detection limit of FDU-15-CHO based sensor can reach down to 1 ppm,and its selectivity and reproducibility are satisfactory.The high concentrations of active sites in the mesopores of FDU-15 are believed to facilitate 2-PEA adsorption,and thus the presence of the-CHO group leading to sensitive and selective response,which is verified by Gaussian simulation.

关键词： Quartz crystal microbalance(QCM) 2-Phenylethylamine FDU-15-CHO Gas sensor Gaussian software

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Preparation of functional ordered mesoporous carbons and their application as the QCM sensor with ultra-low humidity

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Chinese Chemical Letters 2020年第8期31卷 2150-2154页

作者： Ye Zhu Weijia Zhang jiaqiang xu The State Key Laboratory of Molecular Engineering of Polymers Department of ChemistryFudan UniversityShanghai 200433China Department of Physics&Department of Chemistry College of ScienceShanghai UniversityShanghai 200444China

Ordered mesoporous carbon(OMCs)FDU-15 was synthesized through an EISA(Evaporation-Induced Self-Assembly)method,and the oxidized OMCs(FDU-15-COOH)were obtained by subsequent oxidation treatments in liquid phase to introduce functional groups,The samples were characterized by XRD,TEM,FT-IR and nitrogen adsorption-desorption test,The low humidity sensing performances of FDU-15 and FDU-15-COOH thin films were investigated by using a quartz crystal microbalance(QCM)transducer.The responses of FDU-15-COOH is higher than that of the pristine FDU-15 at very low humidity(<729 ppmv)with high long-term stability,implying that FDU-15-COOH is a good candidate for low humidity QCM sensor.

关键词： Low humidity Sensor Mesoporous carbon Functional QCM

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Hydrogen Sensing Characteristics of ZnSnO_3 Micro-Particles Doped with Noble Metal Pd

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稀有金属材料与工程 2006年第A3期35卷 167-169页

作者： jiaqiang xu Xiaohua Jia Xiangdong Lou College of Material and Chemical Engineering Zhengzhou University of Light Industry Zhengzhou 450002 China College of Chemistry and Environmental Science Henan Normal University Xinxiang 453007 China

Perovskite-type oxide ZnSnO_3 doped with 0.5 wt% Pd was prepared directly by a hydrothermal process,its crystal structure and ceramic microstructure were characterized by XRD and TEM,and the gas sensing properties were tested in static state.It is found that the sensors based on ZnSnO_3 micro-particles have good sensitivity and selectivity to H_2.Its sensitivity can be changed with working temperature;the sensitivity of the sensors to H_2 could arrive 21 times when the working temperature is 332℃.

关键词： hydrothermal method perovskite-type oxide gas sensor ZnSnO3

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Noble Metal-Doped In_2O_3 for Enhancing Response to H_2

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稀有金属材料与工程 2006年第A3期35卷 136-139页

作者： jiaqiang xu Xiaohua Wang Jianian Shen College of Materials and Chemical Engineering Zhengzhou University of Light Industry Zhengzhou 450002 China Institute of Materials Shanghai University Shanghai 200072 China

Nanocrystalline In_2O_3 was synthesized through a controllable solvothermal process in one-step at 210℃for 24 h. Gas sensing properties were tested by mixing gas in air in static state.At 268.5℃,the nanocrystal showed high sensitivity to LPG but lower sensitivity to H_2 and CO.In order to enhance the sensitivities to H_2 and CO,0.5 mass % Au and Pd were doped by an impregnation process.The sensitivities to H_2 and CO were increased under different working temperature.Au-doped In_2O_3 was superior to Pd-doped In_2O_3 whatever to H_2 or CO;the sensitivity was increased with the increase of working temperature;gas sensing properties to H_2 overmatched to CO.

关键词： solvothermal process indium oxide noble metal H2 sensor

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Synthesis of iron oxide cubes/reduced graphene oxide composite and its enhanced lithium storage performance

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Chinese Chemical Letters 2021年第1期32卷 113-118页

作者： Chenran Hao Tiange Gao Anbao Yuan jiaqiang xu NEST Lab Department of ChemistryCollege of SciencesShanghai UniversityShanghai 200444 China

Fe_(3)O_(4) is considered as a promising electrode material for lithium-ion batteries(LIBs) due to its low cost and high theoretical capacity(928 mAh/g).Nevertheless,the huge volume expansion and poor conductivity seriously hamper its practical applications.In this study,we use a facile hydrothermal reaction together with a post heat treatment to construct the three-dimensional heterostructured composite(Fe_(3)O_(4)/rGO) inwhich reduced graphene oxide sheets wraped the Fe_(3)O_(4) submicron cubes as the conductive network.The electric conduction and electrode kinetics of lithium ion insertion/extraction reaction of the composite is enhanced due to the assist of conductive rGO,and thus the Listorage performance is obviously improved.The composite exhibits a reversible charge capacity of772.1 mAh/g at the current density of 0.1 A/g,and the capacity retention reaches 70.3% after400 cycles at0.5 A/g,demonstrating obviously higher specific capacity and rate capability over the Fe_(3)O_(4) submicron cubes without rGO,and much superior cycling stability to the parent Fe_2 O_3 submicron cubes without rGO.On the other hand,as a synergic conductive carbon support,the flexible rGO plays an important role in buffering the large volume change during the repeated discharge/charge cycling.

关键词： Iron oxide Reduced graphene oxide Composite Lithium ion battery Anod

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Enhanced CO sensing properties of Pd modified ZnO porous nanosheets

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Chinese Chemical Letters 2020年第8期31卷 2033-2036页

作者： Na Luo Bo Zhang Dan Zhang jiaqiang xu NEST Lab Department of ChemistryDepartment of PhysicsCollege of ScienceShanghai UniversityShanghai 200444China School of Materials Science and Engineering Cultivating Base for Key Laboratory of Environment-friendly Inorganic Materials in University of Henan ProvinceHenan Polytechnic UniversityJiaozuo 454000China

Noble metal is usually used to improve the gas sensing performance of metal oxide semiconductor(MOS)due to its better catalytic properties.In this work,we reported a synthesis of Pd/ZnO nanocomposite by an in situ reduction with ascorbic acid(AA).It was found that Pd/ZnO sensor has excellent selectivity to CO and the response of the Pd/ZnO sensor towards 100 ppm CO was as high as 15(Ra/Rg),obviously higher than that of the pristine ZnO sensor(1.4)when the working temperature is 220℃.Moreover,the pure ZnO sensor almost has no selectivity to CO,but the Pd/ZnO sensor has excellent selectivity to CO,which may be ascribed to the electronic sensitization of Pd.Our present results demonstrate that the Pd can significantly improve the gas-sensing performance of metal oxide semiconductor and the obtained sensor has great potential in monitoring coal mine gas.

关键词： CO sensor ZnO nanosheet Pd modifying Low concentration Nanocomposite

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Preparation and NO_2 Sensing Characteristics of LaFeO_3 Nanoparticles

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稀有金属材料与工程 2006年第A3期35卷 165-166页

作者： Xiangdong Lou Xiaohua Jia jiaqiang xu College of Chemistry and Environmental Science Henan Normal University Xinxiang 453007 China College of Materials and Chemical Engineering Zhengzhou University of Light Industry Zhengzhou 450002 China

LaFeO_3 nanoparticles were prepared by decomposing a precursor La[Fe(CN)_6]·4H_2O at 800℃,the precursor was synthesized by a coordination precipitation process at room temperature.The decomposing mechanism of the precursor was investigated by analyzing TG-DSC curves.Its crystal structure,particle size and ceramic microstructure were characterized by X-ray diffraction (XRD) and transmission electron microscopy (TEM).Furthermore,the gas sensing properties were tested at static state.It can be shown that LaFeO_3 nanoparticles are highly crystallized after sintering at 800℃,the particle size is about 50 nm.The sensor based on LaFeO_3 nanoparticles shows remarkable sensitivity to NO_2.

关键词： thermal decomposition gas sensor LaFeO3

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Gas Sensing Properties of ZnO Tetrapod-Like Whiskers Prepared by Hydrothermal Process

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稀有金属材料与工程 2006年第A3期35卷 185-187页

作者： jiaqiang xu Yuping Chen Huanxin Wang Jianian Shen College of Materials and Chemical Engineering Zhengzhou University of Light Industry Zhengzhou 450002 China Institute of Materials Shanghai University Shanghai 200072 China

ZnO tetrapod-like whiskers were prepared through a hydrothermal process using zinc powder as raw material.Its microstructure and morphology were characterized by X-ray diffraction (XRD) and transmission electron microscopy (TEM). The XRD results showed that the crystal structure of as-obtained sample can be indexed to hexagonal wurtzite ZnO.TEM results revealed that the ZnO sample took on tetrapod-like whisker shape.The gas sensors were prepared with the traditional sintering process and their gas sensitivities were detected.The test results of gas sensitivity showed that the sensors based on ZnO tetrapod-like whiskers are very sensitive to dilute ethanol vapor and H_2S.The relatively high sensitivity and selectivity of these sensors made from ZnO tetrapod-like whiskers demonstrated the potential for developing a new class of selective ethanol sensors.

关键词： hydrothermal process gas sensor zinc oxide whisker

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Materials design and sensing mechanism of novel calix[6]arene composite for sensitively detecting amine drugs

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Chinese Chemical Letters 2020年第8期31卷 2129-2132页

作者： Nana Liu Yu Fan Zhiheng Ma Haixia Lin jiaqiang xu NEST Lab Department of ChemistryCollege of Sciences.Shanghai UniversityShanghai 200444China Department of Physics College of ScienceShanghai UniversityShanghai 200444China

In order to improve the co nvenie nce and sensitivity of amphetamines drug testing and reduce the threat of drugs to humans,we have designed a QCM gas sensor to detect amine-containing drugs.The sensing material is designed based on the chemical nature of amine drugs.The sensing mechanism is derived from a reve rsible Schiff base interaction between the amino group of the drug and the carbonyl group of the novel calix[6]arene derivatives as well as the hydrogen bond interaction between amino group and hydroxyl.The new composite material was well characterized by different analytical techniques including 1 H nuclear magnetic resonance(1 H-NMR),fourier transform infrared spectroscopy(FT-IR),scanning electro nic microscopy(SEM),transmission electron microscope(TEM),Raman spectra,powder X-ray diffraction,etc.The sensing experiments were conducted by coating the composite onto quartz crystal microbalance(QCM)transducers.The experimental results indicated that the novel calixarene derivatives and their GO complexes based on the design have excellent selectivity,high sensitivity and repeatability toβ-phenylethylamine.

关键词： Drug detection Calixarene derivative GO complexes Quartz crystal microbalance sensor Schiff base interaction

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