Formation of Gas-Phase Formate in Thermal Reactions of Carbon Dioxide with Diatomic Iron Hydride Anions

Li Xue Jiang; Chongyang Zhao; Xiao Na Li; Hui Chen; Sheng Gui He

doi:10.1002/anie.201611483

Formation of Gas-Phase Formate in Thermal Reactions of Carbon Dioxide with Diatomic Iron Hydride Anions

Li Xue Jiang, Chongyang Zhao, Xiao Na Li^*, Hui Chen, Sheng Gui He

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

52 Citations (Scopus)

Abstract

The hydrogenation of carbon dioxide involves the activation of the thermodynamically very stable molecule CO₂ and formation of a C−H bond. Herein, we report that HCO₂⁻ and CO can be formed in the thermal reaction of CO₂ with a diatomic metal hydride species, FeH⁻. The FeH⁻ anions were produced by laser ablation, and the reaction with CO₂ was analyzed by mass spectrometry and quantum-chemical calculations. Gas-phase HCO₂⁻ was observed directly as a product, and its formation was predicted to proceed by facile hydride transfer. The mechanism of CO₂ hydrogenation in this gas-phase study parallels similar behavior of a condensed-phase iron catalyst.

Original language	English
Pages (from-to)	4187-4191
Number of pages	5
Journal	Angewandte Chemie - International Edition
Volume	56
Issue number	15
DOIs	https://doi.org/10.1002/anie.201611483
Publication status	Published - 3 Apr 2017
Externally published	Yes

Keywords

carbon dioxide
hydrogenation
iron hydride
mass spectrometry
quantum-chemical calculations

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10.1002/anie.201611483

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title = "Formation of Gas-Phase Formate in Thermal Reactions of Carbon Dioxide with Diatomic Iron Hydride Anions",

abstract = "The hydrogenation of carbon dioxide involves the activation of the thermodynamically very stable molecule CO2 and formation of a C−H bond. Herein, we report that HCO2− and CO can be formed in the thermal reaction of CO2 with a diatomic metal hydride species, FeH−. The FeH− anions were produced by laser ablation, and the reaction with CO2 was analyzed by mass spectrometry and quantum-chemical calculations. Gas-phase HCO2− was observed directly as a product, and its formation was predicted to proceed by facile hydride transfer. The mechanism of CO2 hydrogenation in this gas-phase study parallels similar behavior of a condensed-phase iron catalyst.",

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T1 - Formation of Gas-Phase Formate in Thermal Reactions of Carbon Dioxide with Diatomic Iron Hydride Anions

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AU - Zhao, Chongyang

AU - Li, Xiao Na

AU - Chen, Hui

AU - He, Sheng Gui

PY - 2017/4/3

Y1 - 2017/4/3

N2 - The hydrogenation of carbon dioxide involves the activation of the thermodynamically very stable molecule CO2 and formation of a C−H bond. Herein, we report that HCO2− and CO can be formed in the thermal reaction of CO2 with a diatomic metal hydride species, FeH−. The FeH− anions were produced by laser ablation, and the reaction with CO2 was analyzed by mass spectrometry and quantum-chemical calculations. Gas-phase HCO2− was observed directly as a product, and its formation was predicted to proceed by facile hydride transfer. The mechanism of CO2 hydrogenation in this gas-phase study parallels similar behavior of a condensed-phase iron catalyst.

AB - The hydrogenation of carbon dioxide involves the activation of the thermodynamically very stable molecule CO2 and formation of a C−H bond. Herein, we report that HCO2− and CO can be formed in the thermal reaction of CO2 with a diatomic metal hydride species, FeH−. The FeH− anions were produced by laser ablation, and the reaction with CO2 was analyzed by mass spectrometry and quantum-chemical calculations. Gas-phase HCO2− was observed directly as a product, and its formation was predicted to proceed by facile hydride transfer. The mechanism of CO2 hydrogenation in this gas-phase study parallels similar behavior of a condensed-phase iron catalyst.

KW - carbon dioxide

KW - hydrogenation

KW - iron hydride

KW - mass spectrometry

KW - quantum-chemical calculations

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SN - 1433-7851

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JF - Angewandte Chemie - International Edition

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Formation of Gas-Phase Formate in Thermal Reactions of Carbon Dioxide with Diatomic Iron Hydride Anions

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