兼具小气载吸附、快速换样和全面温控的程序升温脱附谱装置  

Temperature-Programmed Desorption Spectrometer Combining Minimum Gas Load, Fast Substrate Replacement, and Comprehensive Temperature Control

作　　者：夏树才 董珊珊 谢慧智 李甲龙 王天骏 张未卿 车丽 任泽峰[1] 戴东旭[1] 杨学明[1] 周传耀[1,4] Shucai Xia;Shanshan Dong;Huizhi Xie;Jialong Li;Tianjun Wang;Weiqing Zhang;Li Che;Zefeng Ren;Dongxu Dai;Xueming Yang;Chuanyao Zhou(State Key Laboratory of Molecular Reaction Dynamics,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,China;Department of Chemical Physics,School of Chemistry and Materials Science,University of Science and Technologyof China,Hefei 230026,China;Department of Physics,School of Science,Dalian Maritime University,Dalian 116026,China;University of Chinese Academy of Sciences,Bejing 100049,China)

机构地区：[1]中国科学院大连化学物理研究所分子反应动力学国家重点实验室,大连116023 [2]中国科学技术大学化学与材料科学学院化学物理系,合肥230026 [3]大连海事大学理学院物理系,大连116026 [4]中国科学院大学,北京100049

出　　处：《Chinese Journal of Chemical Physics》2023年第4期373-383,I0034,共12页化学物理学报（英文）

基　　金：supported by the National Key Research and Development Program of(No.2021YFA1500601 and No.2018YFA0208703);the National Natural Science Foundation of China(No.21973010 and No.21973092);the Instrument Developing Project of the Chinese Academy of Sciences(No.YZ201504);the CAS Projects for Young Scientists in Basic Research(No.YSBR-007);the Dalian Institute of Chemical Physics Innovation Foundation(DICP I202205);LiaoNing Revitalization Talents Program(No.XLYC1907032).

摘　　要：程序升温脱附谱技术能定量识别表面物种和测量脱附动力学,因此被广泛应用于多相催化和表面科学研究.对于高效率和高质量的程序升温脱附谱实验而言,减小吸附过程中的气载并在不破坏超高真空条件下完成样品更换以及实现对样品全方位的温度控制是至关重要的.然而,现有的表面科学程序升温脱附谱装置通常无法同时满足这些条件。鉴于此,本文搭建了一台可实现小气载进样、快速换样以及全面温控的程序升温脱附谱装置。使用自动控制的基于微毛细管阵列的溢流分子束给样器,制备分子吸附的表面,让气体的进样更加精准并大幅减小了气载。借助液氮传输线并优化样品台处的热接触和热偶连接方式,使得这台程序升温脱附谱装置同时具备了快速换样、精准测温、快速降温以及稳定线性升温等功能。通过测量水从高定向热解石墨和TiO_(2)(110)表面的脱附特征以及甲氧基阴离子在TiO_(2)(110)表面的光催化氧化反应,证实了该程序升温脱附谱装置在测量脱附动力学参数、定量识别表面吸附物种和吸附位点以及分析表面光化学反应等方面的性能,本工作将为研究人员设计高效率和高质量的程序升温脱附谱装置提供宝贵的经验和思路。With the capability of quantitative identifying surface species and measuring desorption kinetics,temperatureprogrammed desorption(TPD)is widely used in heterogeneous catalysis and surface science fields.Minimum gas load during adsorption,fast substrate replacement,and comprehensive temperature control are of great significance for efficient and high quality TPD experiments.Unfortunately,these requirements usually cannot be met at the same time for the existing apparatuses in surface science.In order to increase the universality,a TPD spectrometer combining minimum gas load,fast substrate replacement,and comprehensive temperature control in our laboratory has been built.By using an automatically controlled microcapillary array-based effusive molecular beam gas doser,optimizing the thermal contact at the sample stage,using liquid nitrogen transfer line and designing thermocouple connection,controllable and reproducible molecule adsorption,minimum gas load,fast substrate replacement,rapid cooling,accurate temperature measuring and excellent linear heating are achieved simultaneously.Capabilities of the TPD spectrometer,for example,determination of desorption energy and desorption order,quantitative measurements of surface species and binding sites,and investigation of surface photochemical reactions,are demonstrated by measuring the desorption of water from highly oriented pyrolytic graphite and TiO_(2)(110)and photocatalyzed oxidation of methoxy anions on TiO_(2)(110).The apparatus described here will contribute effectively to the high throughput measurements.

关 键 词：程序升温脱附谱 气体进样 快速换样 表面化学反应 

分 类 号：O64[理学—物理化学]