The reducibility and oxidation states of oxide-supported rhenium: experimental and theoretical investigations
The reducibility and oxidation states of oxide-supported rhenium: experimental and theoretical investigations
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氧化物负载铼的还原性和氧化态：实验和理论研究
DOI：
10.1039/d2cp04784e
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发表时间：
2022
影响因子：
3.3
通讯作者：
Shimizu Ken-ichi
中科院分区：
文献类型：
--
作者：
Ting Kah Wei;Mine Shinya;Ait El Fakir Abdellah;Du Pengfei;Li Lingcong;Siddiki S. M. A. Hakim;Toyao Takashi;Shimizu Ken-ichi
金属与载体之间的相互作用即金属-载体相互作用（msi）对负载型金属催化剂的活性和稳定性有重要影响，具有较高的效率和活性。本文采用实验和计算方法研究了负载铼（Re）和氧化物载体（如TiO2、SiO2、Al2O3、MgO、V2O5和ZrO2）之间的msi。发现稀土的还原性强烈依赖于氧化物载体。实验研究包括H2的程序升温还原以及Re的L3-和l1边x射线吸收近边结构（XANES）分析表明，在200-400°C范围内，H2还原后Re的价态开始下降，除了MgO上的Re在500°C以上发生转变。研究了负载Re催化剂的L3-和l1边XANES光谱与Re尺寸的关系。
The activity and stability of supported metal catalysts, which exhibit high efficiency and activity, are significantly influenced by the interactions between the metal and the support, that is, metal–support interactions (MSIs). Here, we report an investigation of the MSIs between supported rhenium (Re) and oxide supports such as TiO2, SiO2, Al2O3, MgO, V2O5, and ZrO2 using experimental and computational approaches. The reducibility of the Re species was found to strongly depend on the oxide support. Experimental studies including temperature-programmed reduction by H2 as well as Re L3- and L1-edge X-ray absorption near edge structure (XANES) analysis revealed that the valency of the Re species started to decrease upon H2 reduction in the 200–400 °C range, except for Re on MgO, where the shift occurred at temperatures above 500 °C. The dependence of the Re L3- and L1-edge XANES spectra of the oxide-supported Re catalysts on the size of Re was also examined.