Han Jianyu, Yang Jingyi, Zhang Zhixin, Jiang Xunzhu, Liu Wei, Qiao Botao, Mu Junju, Wang Feng
State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116000, P. R. China.
University of Chinese Academy of Sciences, Beijing 100049, P. R. China.
J Am Chem Soc. 2023 Oct 18;145(41):22671-22684. doi: 10.1021/jacs.3c07915. Epub 2023 Oct 9.
Multicomponent alloy (MA) contains a nearly infinite number of unprecedented active sites through entropy stabilization, which is a desired platform for exploring high-performance catalysts. However, MA catalysts are usually synthesized under severe conditions, which induce support structure collapse and further deteriorate the synergy between MA and support. We propose that a strong metal-support interaction (SMSI) could facilitate the formation of MA by establishing a tunnel of oxygen vacancy for metal atom transport under low reduction temperature (400-600 °C), which exemplifies the holistic design of MA catalysts without deactivating supports. PtPdCoFe MA is readily synthesized on anatase TiO with the help of SMSI, which exhibits good catalytic activity and stability for methane combustion. This strategy demonstrates excellent universality on various supports and multicomponent alloy compositions. Our work not only reports a holistic synthesis strategy for MA synthesis by synergizing unique properties of reducible oxides and the mixing entropy of alloy but also offers a new insight that SMSI plays a vigorous role in the formation of alloy NPs on reducible oxides.
多组分合金（MA）通过熵稳定作用含有近乎无限数量的前所未有的活性位点，这是探索高性能催化剂的理想平台。然而，MA催化剂通常在苛刻条件下合成，这会导致载体结构坍塌，并进一步恶化MA与载体之间的协同作用。我们提出，强金属-载体相互作用（SMSI）可以通过在低温还原（400-600°C）下建立氧空位隧道以促进金属原子传输，从而促进MA的形成，这体现了MA催化剂的整体设计且不会使载体失活。借助SMSI，PtPdCoFe MA易于在锐钛矿TiO上合成，其对甲烷燃烧表现出良好的催化活性和稳定性。该策略在各种载体和多组分合金组成上表现出优异的通用性。我们的工作不仅报道了一种通过协同还原氧化物的独特性质和合金的混合熵来合成MA的整体合成策略，还提供了一个新的见解，即SMSI在可还原氧化物上合金纳米颗粒的形成中起着重要作用。
