Department of Chemical and Biomolecular Engineering, Korea Advanced Institute of Science and Technology, Daejeon, 34141, South Korea.
ChemSusChem. 2018 Jan 10;11(1):104-113. doi: 10.1002/cssc.201701306. Epub 2017 Oct 10.
Single-atom catalysts (SACs), in which metal atoms are dispersed on the support without forming nanoparticles, have been used for various heterogeneous reactions and most recently for electrochemical reactions. In this Minireview, recent examples of single-atom electrocatalysts used for the oxygen reduction reaction (ORR), hydrogen oxidation reaction (HOR), hydrogen evolution reaction (HER), formic acid oxidation reaction (FAOR), and methanol oxidation reaction (MOR) are introduced. Many density functional theory (DFT) simulations have predicted that SACs may be effective for CO reduction to methane or methanol production while suppressing H evolution, and those cases are introduced here as well. Single atoms, mainly Pt single atoms, have been deposited on TiN or TiC nanoparticles, defective graphene nanosheets, N-doped covalent triazine frameworks, graphitic carbon nitride, S-doped zeolite-templated carbon, and Sb-doped SnO surfaces. Scanning transmission electron microscopy, extended X-ray absorption fine structure measurement, and in situ infrared spectroscopy have been used to detect the single-atom structure and confirm the absence of nanoparticles. SACs have shown high mass activity, minimizing the use of precious metal, and unique selectivity distinct from nanoparticle catalysts owing to the absence of ensemble sites. Additional features that SACs should possess for effective electrochemical applications were also suggested.
单原子催化剂(SACs),其中金属原子在没有形成纳米颗粒的情况下分散在载体上,已被用于各种多相反应,最近也被用于电化学反应。在这篇综述中,介绍了最近用于氧还原反应(ORR)、氢氧化反应(HOR)、析氢反应(HER)、甲酸氧化反应(FAOR)和甲醇氧化反应(MOR)的单原子电催化剂的例子。许多密度泛函理论(DFT)模拟预测,SACs 可能对 CO 还原为甲烷或甲醇的生产有效,同时抑制 H 的析出,这些情况也在此介绍。主要是 Pt 单原子已被沉积在 TiN 或 TiC 纳米颗粒、有缺陷的石墨烯纳米片、N 掺杂共价三嗪骨架、石墨相氮化碳、S 掺杂沸石模板碳和 Sb 掺杂 SnO 表面上。扫描透射电子显微镜、扩展 X 射线吸收精细结构测量和原位红外光谱已被用于检测单原子结构并证实没有纳米颗粒。由于不存在集合位点,SACs 表现出高的质量活性,最小化了贵金属的使用,并具有不同于纳米颗粒催化剂的独特选择性。还提出了 SACs 为有效电化学应用应具备的其他特征。