Ethanol Upgrading Catalysis for Advanced Biofuels - A Combined Computational Experimental Study

点击翻译按钮获取中文摘要

The Wass group have developed several catalysts that are highly effective in upgrading (bio)ethanol or methanol/ethanol mixtures to butanols, which are valuable advanced biofuels (see references 1 and 2). Despite significant advances in this field, there are still several critical unanswered questions: (1) What is the origin of the high selectivity of our catalysts? (2) Why do structurally very similar catalysts sometimes make ethyl acetate instead of butanols? (3) Why do some catalysts make 2-butanol rather than 1- butanol? (4) Why is Ru the best metal for this? Can we develop catalysts on cheaper first row metals? Answering these questions is of fundamental scientific interest as well as being crucial for the development of this technology. Increasingly, computational methods are used hand-in-hand with experiment to determine mechanism and design catalysts, and this project will use this powerful combination to address these questions. Taking the question of first row catalysts as an example; we have screened many iron catalysts with various bidentate ligands similar to those successful on ruthenium - all have failed. Clearly a more sophisticated approach is needed and the ability to understand the key mechanistic steps in the ruthenium-catalysed reaction by computation (backed up with experimental verification) will instruct us in catalysts design.