Tu Yi, Huang Luchao, Cheng Xingwang, Tian Bingchu, Zhang Dongling, Hu Jun, Ding Honghe, Xu Qian, Ye Yifan, Zhu Junfa
National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230029, People's Republic of China.
Department of Chemical Physics and Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, University of Science and Technology of China, Hefei 230026, People's Republic of China.
J Phys Chem Lett. 2024 Apr 18;15(15):4096-4104. doi: 10.1021/acs.jpclett.4c00810. Epub 2024 Apr 8.
Structure-optimized bimetallic and multicomponent catalysts often outperform single-component catalysts, inspiring a detailed investigation of metal-metal and metal-support interactions in the system. We investigated the geometric and electronic structures of ceria-supported Ni-Cu particles prepared using different metal deposition sequences employing a combination of X-ray photoelectron spectroscopy, resonant photoemission spectroscopy, and infrared reflection absorption spectroscopy. The bimetallic model catalyst structure was altered by a distinct surface evolution process determined by the metal deposition sequence. The postdeposited Cu stays on the surface of Ni predeposited CeO and forms only a limited Ni-Cu alloy in the Cu-contacted Ni region. However, when Ni is deposited on the Cu predeposited CeO surface, Ni can migrate through the Cu layer to the Cu-ceria interface and form an extended Ni-Cu alloy to the whole deposited metal layer on the ceria surface. The dynamic metal diffusion in the CeO-supported Ni-Cu system indicates that metal-support interactions can be used to achieve the rational design of a bimetallic composition distribution during catalyst preparation.
结构优化的双金属和多组分催化剂通常优于单组分催化剂,这激发了对体系中金属-金属和金属-载体相互作用的详细研究。我们结合X射线光电子能谱、共振光发射光谱和红外反射吸收光谱,研究了采用不同金属沉积顺序制备的二氧化铈负载的Ni-Cu颗粒的几何结构和电子结构。双金属模型催化剂结构通过由金属沉积顺序决定的独特表面演化过程而改变。后沉积的Cu停留在预沉积Ni的CeO表面,仅在与Cu接触的Ni区域形成有限的Ni-Cu合金。然而,当Ni沉积在预沉积Cu的CeO表面时,Ni可以穿过Cu层迁移到Cu-二氧化铈界面,并在二氧化铈表面形成延伸至整个沉积金属层的Ni-Cu合金。CeO负载的Ni-Cu体系中的动态金属扩散表明,在催化剂制备过程中,金属-载体相互作用可用于实现双金属组成分布的合理设计。