Homogeneous Catalysis for Sustainable Hydrogen Storage in Formic Acid and Alcohols.
Homogeneous Catalysis for Sustainable Hydrogen Storage in Formic Acid and Alcohols.
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DOI：
10.1021/acs.chemrev.7b00182
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发表时间：
2017-10
期刊：
影响因子：
62.1
通讯作者：
Katerina Sordakis;Conghui Tang;Lydia K. Vogt;H. Junge;P. Dyson;M. Beller;G. Laurenczy
中科院分区：
文献类型：
--
作者：
Katerina Sordakis;Conghui Tang;Lydia K. Vogt;H. Junge;P. Dyson;M. Beller;G. Laurenczy
氢气是一种可储存的化学能，可以补充间歇性的可再生能源转换。氢气的主要缺点之一是密度低，因此，有效的处理和储存方法是实现氢基经济需要解决的关键因素。基于液体的储存系统，特别是甲酸和酒精，是非常有吸引力的氢载体，因为它们可以由二氧化碳或其他可再生材料制成，它们可以用于固定的储能装置，如加氢站，它们可以直接用作运输燃料。然而，为了改变我们的能源基础设施，需要从这些分子中释放氢气的高效催化过程，以及从二氧化碳和氢气中再生这些分子的催化剂。本文综述了均相催化技术在二氧化碳加氢合成甲酸和甲醇以及反脱氢反应等关键反应中的研究进展。还介绍了可再生原料中高级醇的脱氢反应。分析了催化剂的关键结构特征以及添加剂的作用，这些添加剂在许多系统中都是必需的。特别关注可持续催化工艺的进展，特别是基于地球上丰富的金属离子的无添加剂工艺和催化剂。此外，还介绍了机理信息，希望这篇综述不仅提供了该领域的最新进展，也为未来如何获得更好的催化系统提供了洞察力。
Hydrogen gas is a storable form of chemical energy that could complement intermittent renewable energy conversion. One of the main disadvantages of hydrogen gas arises from its low density, and therefore, efficient handling and storage methods are key factors that need to be addressed to realize a hydrogen-based economy. Storage systems based on liquids, in particular, formic acid and alcohols, are highly attractive hydrogen carriers as they can be made from CO2 or other renewable materials, they can be used in stationary power storage units such as hydrogen filling stations, and they can be used directly as transportation fuels. However, to bring about a paradigm change in our energy infrastructure, efficient catalytic processes that release the hydrogen from these molecules, as well as catalysts that regenerate these molecules from CO2 and hydrogen, are required. In this review, we describe the considerable progress that has been made in homogeneous catalysis for these critical reactions, namely, the hydrogenation of CO2 to formic acid and methanol and the reverse dehydrogenation reactions. The dehydrogenation of higher alcohols available from renewable feedstocks is also described. Key structural features of the catalysts are analyzed, as is the role of additives, which are required in many systems. Particular attention is paid to advances in sustainable catalytic processes, especially to additive-free processes and catalysts based on Earth-abundant metal ions. Mechanistic information is also presented, and it is hoped that this review not only provides an account of the state of the art in the field but also offers insights into how superior catalytic systems can be obtained in the future.