Chen Xiao, Wang Xing-Bao, Han Shuhua, Wang Dong, Li Chuang, Guan Weixiang, Li Wen-Ying, Liang Changhai
State Key Laboratory of Fine Chemicals, Laboratory of Advanced Materials and Catalytic Engineering, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China.
Training Base of State Key Laboratory of Coal Science and Technology Jointly Constructed by Shanxi Province and Ministry of Science and Technology, Taiyuan University of Technology, Taiyuan 030024, China.
ACS Appl Mater Interfaces. 2022 Jan 12;14(1):590-602. doi: 10.1021/acsami.1c16965. Epub 2021 Dec 14.
Interactions between metals and oxide supports are crucial in determining catalytic activity, selectivity, and stability. For reducible oxide supported noble metals, a strong metal-support interaction (SMSI) has been widely recognized. Herein we report the intermediate selectivity and stability over an irreducible SiO supported Pt catalyst in the hydrogenation of anthracene that are significantly boosted due to the SMSI-induced formation of intermetallic Pt silicide and Pt-SiO interface. The limitation in the strong interaction between Pt nanoparticles and irreducible SiO has been breached by combining the strong electrostatic adsorption method and following the high temperature reduction strategy. Due to the isolated Pt active sites by Si atoms, the activated H species produced over the PtSi/SiO catalyst with an initial catalytic activity of 2.49 μmol/(m/g)/h as well as TOF of 0.95 s preferentially transfer to the outer ring of anthracene to 87% yield of symmetric octahydroanthracene (-OHA) by subsequent hydrogenation. In addition, the PtSi/SiO catalyst presents an excellent stability after five cycles, which can be attributed to the fact that intermetallic PtSi nanoparticles are anchored firmly onto the surface of the SiO support. The discovery contributes to broaden the horizons on the SMSI effect in the irreducible oxide supported metal particle catalysts and provides guidance to design the metal-SiO interface and tune the surface chemical properties in diverse application conditions.
金属与氧化物载体之间的相互作用对于决定催化活性、选择性和稳定性至关重要。对于可还原氧化物负载的贵金属,强金属-载体相互作用(SMSI)已得到广泛认可。在此,我们报道了在蒽的氢化反应中,由于SMSI诱导形成金属间化合物铂硅化物和Pt-SiO界面,负载于不可还原SiO上的Pt催化剂的中间体选择性和稳定性得到显著提高。通过结合强静电吸附法并遵循高温还原策略,突破了Pt纳米颗粒与不可还原SiO之间强相互作用的限制。由于Si原子隔离了Pt活性位点,初始催化活性为2.49 μmol/(m/g)/h、TOF为0.95 s的PtSi/SiO催化剂上产生的活化H物种优先转移到蒽的外环,通过后续氢化反应生成对称八氢蒽(-OHA)的产率达到87%。此外,PtSi/SiO催化剂在五个循环后表现出优异的稳定性,这可归因于金属间化合物PtSi纳米颗粒牢固地锚定在SiO载体表面。这一发现有助于拓宽对不可还原氧化物负载金属颗粒催化剂中SMSI效应的认识,并为设计金属-SiO界面和在不同应用条件下调节表面化学性质提供指导。