Hydrogenation of CO2 in Water Using a Bis(diphosphine)
Ni–H Complex
Posted on 2017-03-29 - 20:03
The water-soluble Ni bis(diphosphine)
complex [NiL2](BF4)2 (L = 1,2-[bis(dimethoxypropyl)phosphino]ethane
and the corresponding hydride, [HNiL2]BF4, were synthesized and characterized. These complexes were
specifically designed for CO2 hydrogenation. For HNiL2+, the hydricity (ΔG°H–) was determined to be 23.2(3)
kcal/mol in aqueous solution. On the basis of the hydricity of formate,
24.1 kcal/mol, the transfer of a hydride from HNiL2+ to CO2 to produce formate is favorable
by 1 kcal/mol. Starting from either NiL22+ or HNiL2+ in water, catalytic
hydrogenation of CO2 was observed with NaHCO3 (0.8 M) as the only additive. A maximum turnover frequency of [4.0(5)]
× 10–1 h–1 was observed at
80 °C and 34 atm of a 1:1 mixture of CO2 and H2. This report demonstrates the use of a homogeneous first-row
transition-metal catalyst for CO2 hydrogenation in water
using NaHCO3 as an inexpensive, readily available base.
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Burgess, Samantha
A.; Kendall, Alexander J.; Tyler, David R.; Linehan, John C.; Appel, Aaron M. (2017). Hydrogenation of CO2 in Water Using a Bis(diphosphine)
Ni–H Complex. ACS Publications. Collection. https://doi.org/10.1021/acscatal.7b00350
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AUTHORS (5)
SB
Samantha
A. Burgess
AK
Alexander J. Kendall
DT
David R. Tyler
JL
John C. Linehan
AA
Aaron M. Appel