Hydrogenation of CO2 in Water Using a Bis(diphosphine) Ni-H Complex

Samantha A. Burgess, Alexander J. Kendall, David R. Tyler, John Linehan, Aaron Appel

Research output: Contribution to journalArticle

40 Citations (Scopus)

Abstract

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 NiL2 2+ 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.

Original languageEnglish
Pages (from-to)3089-3096
Number of pages8
JournalACS Catalysis
Volume7
Issue number4
DOIs
Publication statusPublished - Apr 7 2017

Keywords

  • aqueous bicarbonate
  • CO hydrogenation
  • homogeneous catalysis
  • hydricity
  • nickel

ASJC Scopus subject areas

  • Catalysis

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