Nature2014-06-18 6:20 PM

一种具有节能潜力的新型催化剂 Electroreduction of carbon monoxide to liquid fuel on oxide-derived nano crystalline copper

论文摘要 

可再生电力经常是在不需要的时候被生产出来的。如果多余的电力能够被利用来驱动CO2和水向液体燃料的转化,那么能源就不会被浪费,通过碳捕获所产生的CO2也将会派上用场。所有这些都需要能将CO2不仅还原成CO、而且还能进一步还原成燃料化学物质的高效电催化剂。铜能做到这一点,但效率低、选择性差。现在,Christina Li等人发现,铜的内在催化性能可以通过从其氧化物中作为相互连接的纳米晶体来生成它而得到提高。他们所获得的性能得到增强的催化剂主要产生乙醇,它表明以可再生电力为动力通过两步将CO2转化成液体燃料也许是可能的。

Abstract 

The electrochemical conversion of CO2 and H2O into liquid fuel is ideal for high-density renewable energy storage and could provide an incentive for CO2 capture. However, efficient electrocatalysts for reducing CO2 and its derivatives into a desirable fuel are not available at present. Although many catalysts can reduce CO2 to carbon monoxide (CO), liquid fuel synthesis requires that CO is reduced further, using H2O as a H+ source. Copper (Cu) is the only known material with an appreciable CO electroreduction activity, but in bulk form its efficiency and selectivity for liquid fuel are far too low for practical use. In particular, H2O reduction to H2 outcompetes CO reduction on Cu electrodes unless extreme overpotentials are applied, at which point gaseous hydrocarbons are the major CO reduction products. Here we show that nanocrystalline Cu prepared from Cu2O (‘oxide-derived Cu’) produces multi-carbon oxygenates (ethanol, acetate and n-propanol) with up to 57% Faraday efficiency at modest potentials (–0.25 volts to –0.5 volts versus the reversible hydrogen electrode) in CO-saturated alkaline H2O. By comparison, when prepared by traditional vapour condensation, Cu nanoparticles with an average crystallite size similar to that of oxide-derived copper produce nearly exclusive H2 (96% Faraday efficiency) under identical conditions. Our results demonstrate the ability to change the intrinsic catalytic properties of Cu for this notoriously difficult reaction by growing interconnected nanocrystallites from the constrained environment of an oxide lattice. The selectivity for oxygenates, with ethanol as the major product, demonstrates the feasibility of a two-step conversion of CO2 to liquid fuel that could be powered by renewable electricity.

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