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Title: Reduction of CO 2 to methanol using aluminum ester FLPs

Herein we report the synthesis of Al-based esters containing halogenated benzene rings. These Lewis acids were paired with phosphines to form frustrated Lewis pairs (FLPs) which could subsequently bind CO 2. While these FLPs were not sufficiently water-stable to catalyze the reduction of CO 2 to MeOH using NH 3BH 3 as the reductant, we examine the effect of varying Lewis acid strength. Frustrated Lewis pairs (FLPs) are combinations of Lewis acids and Lewis bases where the acid and base are either sterically or geometrically restricted from interacting as strongly as their electronic structures would allow. This effect leads to enhanced reactivity towards small molecules and, consequently, interest in their potential as metal-free catalysts [1], [2], [3], [4] and [5]. Furthermore, to-date, the biggest success has been based around the ability of a myriad of systems to heterolytically cleave H 2 and perform catalytic hydrogenations [2] and [3].
Authors:
 [1] ;  [2] ;  [2] ;  [2] ;  [2] ;  [1] ;  [1] ; ORCiD logo [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. The Univ. of Alabama, Tuscaloosa, AL (United States)
Publication Date:
Report Number(s):
LA-UR-15-26338
Journal ID: ISSN 1387-7003
Grant/Contract Number:
AC52-06NA25396
Type:
Accepted Manuscript
Journal Name:
Inorganic Chemistry Communications
Additional Journal Information:
Journal Volume: 61; Journal Issue: C; Journal ID: ISSN 1387-7003
Publisher:
Elsevier
Research Org:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org:
USDOE Laboratory Directed Research and Development (LDRD) Program
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; inorganic and physical chemistry; frustrated Lewis pair; CO2; MeOH; ammonia borane
OSTI Identifier:
1329898