Andreas Weilhard1, Stephen P Argent2, Victor Sans3,4. 1. Faculty of Engineering, University of Nottingham, Nottingham, NG7 2RD, UK. 2. School of Chemistry, University of Nottingham, Nottingham, NG7 2RD, UK. 3. Faculty of Engineering, University of Nottingham, Nottingham, NG7 2RD, UK. sans@uji.es. 4. Institute of Advanced Materials (INAM), Universitat Jaume I, 12071, Castellon, Spain. sans@uji.es.
Abstract
The efficient transformation of CO2 into chemicals and fuels is a key challenge for the decarbonisation of the synthetic production chain. Formic acid (FA) represents the first product of CO2 hydrogenation and can be a precursor of higher added value products or employed as a hydrogen storage vector. Bases are typically required to overcome thermodynamic barriers in the synthesis of FA, generating waste and requiring post-processing of the formate salts. The employment of buffers can overcome these limitations, but their catalytic performance has so far been modest. Here, we present a methodology utilising IL as buffers to catalytically transform CO2 into FA with very high efficiency and comparable performance to the base-assisted systems. The combination of multifunctional basic ionic liquids and catalyst design enables the synthesis of FA with very high catalytic efficiency in TONs of >8*105 and TOFs > 2.1*104 h-1.
The efficient transformation of class="Chemical">CO2 into chemicals and fuels is a key challenge for the den class="Chemical">carbonisation of the synthetic production chain. Formic acid (FA) represents the first product of CO2hydrogenation and can be a precursor of higher added value products or employed as a hydrogen storage vector. Bases are typically required to overcome thermodynamic barriers in the synthesis of FA, generating waste and requiring post-processing of the formate salts. The employment of buffers can overcome these limitations, but their catalytic performance has so far been modest. Here, we present a methodology utilising IL as buffers to catalytically transform CO2 into FA with very high efficiency and comparable performance to the base-assisted systems. The combination of multifunctional basic ionic liquids and catalyst design enables the synthesis of FA with very high catalytic efficiency in TONs of >8*105 and TOFs > 2.1*104 h-1.
Authors: Yuanyuan Zhang; Alex D MacIntosh; Janice L Wong; Elizabeth A Bielinski; Paul G Williard; Brandon Q Mercado; Nilay Hazari; Wesley H Bernskoetter Journal: Chem Sci Date: 2015-05-28 Impact factor: 9.825