Abstract
Synthesis of ethanol from non-petroleum carbon resources via syngas (a mixture of H2 and CO) is an important but challenging research target. The current conversion of syngas to ethanol suffers from low selectivity or multiple processes with high energy consumption. Here, we report a high-selective conversion of syngas into ethanol by a triple tandem catalysis. An efficient trifunctional tandem system composed of potassium-modified ZnO–ZrO2, modified zeolite mordenite and Pt–Sn/SiC working compatibly in syngas stream in one reactor can afford ethanol with a selectivity of 90%. We demonstrate that the K+–ZnO–ZrO2 catalyses syngas conversion to methanol and the mordenite with eight-membered ring channels functions for methanol carbonylation to acetic acid, which is then hydrogenated to ethanol over the Pt–Sn/SiC catalyst. The present work offers an effective methodology leading to high selective conversion by decoupling a single-catalyst-based complicated and uncontrollable reaction into well-controlled multi-steps in tandem in one reactor.
Highlights
Synthesis of ethanol from non-petroleum carbon resources via syngas is an important but challenging research target
The conversion of syngas to C2–C4 olefins or aromatics beyond traditional Fischer-Tropsch synthesis has recently been achieved by designing bifunctional catalysts that work in tandem for CO hydrogenation to CH3OH/dimethyl ether (DME) or ketene intermediate and conversion of intermediate to target product[26,27,28,29,30]
To match methanol carbonylation and acetic acid hydrogenation reactions, we first investigated catalytic behaviours of some typical metal oxides that are capable of catalysing syngas conversion to CH3OH/DME at 500–600 K
Summary
Synthesis of ethanol from non-petroleum carbon resources via syngas (a mixture of H2 and CO) is an important but challenging research target. Many studies have been devoted to the direct conversion of syngas into ethanol with a single catalyst (Fig. 1, Route A)[5,8,9,10,11] This reaction is complicated because of many elementary steps involved, which include H2 dissociation, CO dissociative and non-dissociative activation, formation of adsorbed CO, CHxO and CHx intermediates, C–C coupling between different intermediates, and formation of products[5,8,9,11]. The conversion of syngas to C2–C4 olefins or aromatics beyond traditional Fischer-Tropsch synthesis has recently been achieved by designing bifunctional catalysts that work in tandem for CO hydrogenation to CH3OH/DME or ketene intermediate and conversion of intermediate to target product[26,27,28,29,30]. The high-selective synthesis of a specific product, in particular a C2+ oxygenate, by using the concept of shape selectivity is very challenging
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