The Electrochemical Energy, Catalysis and Material Science Laboratory, Department of Chemistry, Chemical Engineering Division, Technical University Berlin, 10623 Berlin, Germany.
Chem Soc Rev. 2018 Feb 5;47(3):715-735. doi: 10.1039/c7cs00759k.
This 2007 Chemistry Nobel prize update covers scientific advances of the past decade in our understanding of electrocatalytic processes on surfaces of nanoscale shape-controlled polyhedral solids. It is argued that the field of chemical reaction processes on solid surfaces has recently been paying increasing attention to the fundamental understanding of electrified solid-liquid interfaces and toward the operando study of the minute fraction of catalytically active, structurally dynamic non-equilibrium Taylor-type surface sites. Meanwhile, despite mounting evidence of acting as structural proxies in some cases, the concept of catalytic structure sensitivity of well-defined nanoscale solid surfaces continues to be a key organizing principle for the science of shape-controlled nanocrystals and, hence, constitutes a central recurring theme in this review. After addressing key aspects and recent progress in the wet-chemical synthesis of shaped nanocatalysts, three areas of electrocatalytic processes on solid shape-controlled nanocrystals of current scientific priority are discussed in more detail: the oxygen electroreduction on shape-controlled Pt-Ni polyhedra with its technological relevance for low temperature fuel cells, the CO electroreduction to hydrocarbons on Cu polyhedra and the puzzling interplay between chemical and structural effects, and the electrocatalytic oxygen evolution reaction from water on shaped transition metal oxides. The review closes with the conclusion that Surface Science and thermal catalysis, honored by Ertl's Nobel prize a decade ago, continue to show major repercussions on the emerging field of Interface Science.
这篇 2007 年诺贝尔化学奖更新涵盖了过去十年中我们对纳米级形状控制多面体固体表面电催化过程理解的科学进展。有人认为,近年来,固体表面化学反应过程领域越来越关注对带电固液界面的基本理解,并朝着对催化活性微小部分的操作研究和结构动态非平衡泰勒型表面位点的研究方向发展。与此同时,尽管越来越多的证据表明在某些情况下可以作为结构代理,但具有明确纳米结构的催化结构敏感性的概念继续是形状控制纳米晶体科学的关键组织原则,因此构成了这篇综述的核心主题。在讨论了形状控制纳米催化剂的湿化学合成的关键方面和最新进展之后,本文更详细地讨论了当前科学优先领域的三个固体形状控制纳米晶体电催化过程领域:形状控制 Pt-Ni 多面体上的氧还原反应及其对低温燃料电池的技术相关性、Cu 多面体上的 CO 还原为烃以及化学和结构效应之间令人费解的相互作用,以及在过渡金属氧化物上的水的电催化氧气析出反应。这篇综述的结论是,表面科学和热催化,十年前由 Ertl 获得诺贝尔化学奖,继续对新兴的界面科学领域产生重大影响。