Design and Application of a High-Temperature Linear Ion Trap Reactor

Jiang, Lixue; Liu, Qingyu; Li, Xiaona; He, Sheng‐Gui

doi:10.1007/s13361-017-1828-3

Cited by 17 publications

(12 citation statements)

References 57 publications

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“…The instantaneous molecule density of He in the reactor was estimated to be 3.5 × 10 15 molecule cm –3 at a temperature of 298–559 K, which means that the Cu 2 H 2 – anions had been thermalized (by a number of collisions around 5300) to the defined temperature of LIT before they reacted with CO 2 . , The cluster ions ejected from the high-temperature LIT were detected by a reflectron time-of-flight mass spectrometer (TOF-MS). The details of running the TOF-MS, the quadrupole mass filter, and the high-temperature LIT can be found in our previous works.…”

Section: Methodsmentioning

confidence: 99%

Gas-Phase Reactions of Carbon Dioxide with Copper Hydride Anions Cu₂H₂^–: Temperature-Dependent Transformation

Liu

Jiang

et al. 2018

J. Phys. Chem. C

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The hydrogenation of carbon dioxide into value-added chemicals is of great importance for CO 2 recycling. However, the underlying mechanism of CO 2 hydrogenation remains elusive owing to the lack of experimental evidence for the formation of the C−H bond. Herein, the gas-phase reaction of copper hydride anion Cu 2 H 2 − with CO 2 at variable temperatures (∼300−560 K) was investigated. Metal hydrides are the ideal models to study the nature of C−H bond formation in CO 2 hydrogenation, while the related studies are scarcely reported, particularly for the hydrogenation reactions at temperatures above 300 K. The generation of formate (HCO 2 − ) attached on product CuH 2 CO 2 − was identified by temperature-dependent mass spectrometric experiments and density functional theory calculations. Temperature played crucial roles to fine-tune the product selectivity, from Cu 2 H 2 CO 2 − that dominates the room-temperature reaction into CuH 2 CO 2 − at elevated temperatures. The nature behind the temperature-dependent product selectivity and the mechanism of CO 2 hydrogenation has been interpreted by using theoretical calculations. The combined experimental and computational studies have provided solid evidence for the formation of formate attached in CuH 2 CO 2 − .

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Section: Methodsmentioning

confidence: 99%

Gas-Phase Reactions of Carbon Dioxide with Copper Hydride Anions Cu₂H₂^–: Temperature-Dependent Transformation

Liu

Jiang

et al. 2018

J. Phys. Chem. C

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“…The pulsed laser is a 532 nm laser with 5-8 mJ/energy pulses and 10 Hz repetition rate (140 Baytech Drive, San Jose, CA, USA). Y 2 C 4 − and Y 2 C 4 H − anion clusters were mass-selected by a quadrupole mass filter (QMF) (China Academy of Engineering Physics, Mianyang, Sichuan, China) [34] and subsequently entered into a linear ion trap (LIT) reactor (homemade) [35]. After being confined and thermalized by the pulsed gas He for about 2 ms, they interacted with N 2 for about 6 ms and 14 ms, at room temperature, respectively.…”

Section: Experimental Methodsmentioning

confidence: 99%

Experimental and Theoretical Study of N2 Adsorption on Hydrogenated Y2C4H− and Dehydrogenated Y2C4− Cluster Anions at Room Temperature

Gao

Ding

2022

IJMS

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The adsorption of atmospheric dinitrogen (N2) on transition metal sites is an important topic in chemistry, which is regarded as the prerequisite for the activation of robust N≡N bonds in biological and industrial fields. Metal hydride bonds play an important part in the adsorption of N2, while the role of hydrogen has not been comprehensively studied. Herein, we report the N2 adsorption on the well-defined Y2C4H0,1− cluster anions under mild conditions by using mass spectrometry and density functional theory calculations. The mass spectrometry results reveal that the reactivity of N2 adsorption on Y2C4H− is 50 times higher than that on Y2C4− clusters. Further analysis reveals the important role of the H atom: (1) the presence of the H atom modifies the charge distribution of the Y2C4H− anion; (2) the approach of N2 to Y2C4H− is more favorable kinetically compared to that to Y2C4−; and (3) a natural charge analysis shows that two Y atoms and one Y atom are the major electron donors in the Y2C4− and Y2C4H− anion clusters, respectively. This work provides new clues to the rational design of TM-based catalysts by efficiently doping hydrogen atoms to modulate the reactivity towards N2.

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“…[59][60][61][62][63][64] The reactivity of ESI isolated TM complexes has also been characterized in RF or ICR ion traps in conjunction with some spectroscopic elucidation and partly under cryogenic conditions. [65][66][67][68][69][70][71][72] A high temperature linear ion trap reactor design [73] proved useful for characterizing the reactivity and catalytic activity of oligomeric TM compounds, [74,75] and it helped to survey Rhodium cluster chemistry [76] and N 2 activation by some of these oligomeric TM compounds. [77][78][79][80] Independently, the room temperature size-dependence of the reactivity of tantalum cluster cations with small alcohols has received some attention.…”

Section: Manfred Kappes Studied Chemistry In Montreal and Cambridge (Massachusetts) His Phd Work With Ralph Staley At Mit (1981) Was On Imentioning

confidence: 99%

Advancing Inorganic Coordination Chemistry by Spectroscopy of Isolated Molecules: Methods and Applications

Niedner‐Schatteburg

Kappes

2021

Chemistry A European J

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A unique feature of the work carried out in the Collaborative Research Center 3MET continues to be its emphasis on innovative, advanced experimental methods which hyphenate mass-selection with further analytical tools such as laser spectroscopy for the study of isolated molecular ions. This allows to probe the intrinsic properties of the species of interest free of perturbing solvent or matrix effects. This review explains these methods and uses examples from past and ongoing 3MET studies of specific classes of multicenter metal complexes to illustrate how coordination chemistry can be advanced by applying them. As a corollary, we will show how the challenges involved in providing welldefined, for example monoisomeric, samples of the molecular ions have helped to further improve the methods themselves thus also making them applicable to many other areas of chemistry.

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Design and Application of a High-Temperature Linear Ion Trap Reactor

Cited by 17 publications

References 57 publications

Gas-Phase Reactions of Carbon Dioxide with Copper Hydride Anions Cu₂H₂^–: Temperature-Dependent Transformation

Gas-Phase Reactions of Carbon Dioxide with Copper Hydride Anions Cu₂H₂^–: Temperature-Dependent Transformation

Experimental and Theoretical Study of N2 Adsorption on Hydrogenated Y2C4H− and Dehydrogenated Y2C4− Cluster Anions at Room Temperature

Advancing Inorganic Coordination Chemistry by Spectroscopy of Isolated Molecules: Methods and Applications

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Design and Application of a High-Temperature Linear Ion Trap Reactor

Cited by 17 publications

References 57 publications

Gas-Phase Reactions of Carbon Dioxide with Copper Hydride Anions Cu2H2–: Temperature-Dependent Transformation

Gas-Phase Reactions of Carbon Dioxide with Copper Hydride Anions Cu2H2–: Temperature-Dependent Transformation

Experimental and Theoretical Study of N2 Adsorption on Hydrogenated Y2C4H− and Dehydrogenated Y2C4− Cluster Anions at Room Temperature

Advancing Inorganic Coordination Chemistry by Spectroscopy of Isolated Molecules: Methods and Applications

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Gas-Phase Reactions of Carbon Dioxide with Copper Hydride Anions Cu₂H₂^–: Temperature-Dependent Transformation

Gas-Phase Reactions of Carbon Dioxide with Copper Hydride Anions Cu₂H₂^–: Temperature-Dependent Transformation