DICP OpenIR
Subject Area物理化学
Long-Term Real-Time Monitoring Catalytic Synthesis of Ammonia in a Microreactor by VUV-Lamp-Based Charge-Transfer Ionization Time-of-Flight Mass Spectrometry
Xie, Yuanyuan1,2; Hua, Lei1; Hou, Keyong1; Chen, Ping1,2; Zhao, Wuduo1,2; Chen, Wendong1,2; Ju, Bangyu1; Li, Haiyang1; Li HY(李海洋)
Source PublicationANALYTICAL CHEMISTRY
2014-08-05
DOI10.1021/ac501576f
Volume86Issue:15Pages:7681-7687
Indexed BySCI
SubtypeArticle
WOS HeadingsScience & Technology ; Physical Sciences
WOS SubjectChemistry, Analytical
WOS Research AreaChemistry
WOS KeywordSINGLE-PHOTON IONIZATION ; ION FLOW TUBE ; VACUUM-ULTRAVIOLET LAMP ; TRACE GAS-ANALYSIS ; PHOTOELECTRON IONIZATION ; SIFT-MS ; ONLINE ; CARBON ; PRESSURE ; BREATH
AbstractWith respect to massive consumption of ammonia and rigorous industrial synthesis conditions, many studies have been devoted to investigating more environmentally benign catalysts for ammonia synthesis under moderate conditions. However, traditional methods for analysis of synthesized ammonia (e.g., off-line ion chromatography (IC) and chemical titration) suffer from poor sensitivity, low time resolution, and sample manipulations. In this work, charge-transfer ionization (CTI) with O-2(+) as the reagent ion based on a vacuum ultraviolet (VUV) lamp in a time-of-flight mass spectrometer (CTI-TOFMS) has been applied for real-time monitoring of the ammonia synthesis in a microreactor. For the necessity of long-term stable monitoring, a self-adjustment algorithm for stabilizing O-2(+) ion intensity was developed to automatically compensate the attenuation of the O-2(+) ion yield in the ion source as a result of the oxidation of the photoelectric electrode and contamination on the MgF2 window of the VUV lamp. A wide linear calibration curve in the concentration range of 0.2-1000 ppmv with a correlation coefficient (R-2) of 0.9986 was achieved, and the limit of quantification (LOQ) for NH3 was in ppbv. Microcatalytic synthesis of ammonia with three catalysts prepared by transition-metal/carbon nanotubes was tested, and the rapid changes of NH3 conversion rates with the reaction temperatures were quantitatively measured with a time resolution of 30 s. The high-time-resolution CTI-TOFMS could not only achieve the equilibrium conversion rates of NH3 rapidly but also monitor the activity variations with respect to investigated catalysts during ammonia synthesis reactions.
Language英语
WOS IDWOS:000340081100075
Citation statistics
Cited Times:19[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://cas-ir.dicp.ac.cn/handle/321008/143969
Collection中国科学院大连化学物理研究所
Corresponding AuthorLi HY(李海洋)
Affiliation1.Chinese Acad Sci, Dalian Inst Chem Phys, Key Lab Separat Sci Analyt Chem, Dalian 116023, Peoples R China
2.Chinese Acad Sci, Grad Univ, Beijing 100039, Peoples R China
Recommended Citation
GB/T 7714
Xie, Yuanyuan,Hua, Lei,Hou, Keyong,et al. Long-Term Real-Time Monitoring Catalytic Synthesis of Ammonia in a Microreactor by VUV-Lamp-Based Charge-Transfer Ionization Time-of-Flight Mass Spectrometry[J]. ANALYTICAL CHEMISTRY,2014,86(15):7681-7687.
APA Xie, Yuanyuan.,Hua, Lei.,Hou, Keyong.,Chen, Ping.,Zhao, Wuduo.,...&李海洋.(2014).Long-Term Real-Time Monitoring Catalytic Synthesis of Ammonia in a Microreactor by VUV-Lamp-Based Charge-Transfer Ionization Time-of-Flight Mass Spectrometry.ANALYTICAL CHEMISTRY,86(15),7681-7687.
MLA Xie, Yuanyuan,et al."Long-Term Real-Time Monitoring Catalytic Synthesis of Ammonia in a Microreactor by VUV-Lamp-Based Charge-Transfer Ionization Time-of-Flight Mass Spectrometry".ANALYTICAL CHEMISTRY 86.15(2014):7681-7687.
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