Issue 4, 2024

Solvent- and catalyst-free reduction of CO2 with ammonia borane

Abstract

Ammonia borane (AB) has been extensively studied as a solid-state hydrogen storage material. On the other hand, its reactivity with CO2 is still unclear, especially in the solid state. By carefully controlling the CO2 pressure and temperature, AB efficiently reduces a large amount of CO2 without solvent or catalyst. 40 mmol of CO2 reacts with one mole of AB at 0.5 MPa and 60 °C. The mechanism was investigated by NMR and DFT calculation. The reaction proceeds through the formation of diammoniate of diborane (DADB) as an intermediate, followed by the reduction and fixation of CO2 with BH4 to give triformatoborohydride ([HB(OCHO)3]). Aldehyde is then transferred from B to N, yielding formamide as the main final product. The N-formylation of secondary amine can also be achieved without solvent. Finally, the pyrolysis of the product between AB and CO2 produces N-doped amorphous carbon, opening the door to new clean CO2 valorisation pathways.

Graphical abstract: Solvent- and catalyst-free reduction of CO2 with ammonia borane

Supplementary files

Article information

Article type
Paper
Submitted
14 Nov 2023
Accepted
05 Jan 2024
First published
05 Jan 2024

Green Chem., 2024,26, 2183-2189

Solvent- and catalyst-free reduction of CO2 with ammonia borane

L. Lombardo, T. Nishiguchi, Y. Ko, L. Zhong, N. Horike, A. Züttel and S. Horike, Green Chem., 2024, 26, 2183 DOI: 10.1039/D3GC04399A

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