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Classical strong metal–support interactions between gold nanoparticles and titanium dioxide

机译:金纳米粒子和二氧化钛之间的经典强金属-支持相互作用

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摘要

Supported metal catalysts play a central role in the modern chemical industry but often exhibit poor on-stream stability. The strong metal–support interaction (SMSI) offers a route to control the structural properties of supported metals and, hence, their reactivity and stability. Conventional wisdom holds that supported Au cannot manifest a classical SMSI, which is characterized by reversible metal encapsulation by the support upon high-temperature redox treatments. We demonstrate a classical SMSI for Au/TiO2, evidenced by suppression of CO adsorption, electron transfer from TiO2 to Au nanoparticles, and gold encapsulation by a TiOx overlayer following high-temperature reduction (reversed by subsequent oxidation), akin to that observed for titania-supported platinum group metals. In the SMSI state, Au/TiO2 exhibits markedly improved stability toward CO oxidation. The SMSI extends to Au supported over other reducible oxides (Fe3O4 and CeO2) and other group IB metals (Cu and Ag) over titania. This discovery highlights the general nature of the classical SMSI and unlocks the development of thermochemically stable IB metal catalysts.
机译:负载型金属催化剂在现代化学工业中起着核心作用,但通常表现出较差的在流稳定性。强大的金属与载体的相互作用(SMSI)提供了控制载体金属的结构特性及其活性和稳定性的途径。传统观点认为,负载的Au不能表现出经典的SMSI,其特征是在高温氧化还原处理时,载体具有可逆的金属封装。我们展示了一种用于Au / TiO 2 的经典SMSI,通过抑制CO吸附,电子从TiO 2 到Au纳米粒子的转移以及TiO 的金包封来证明高温还原后的x 覆盖层(随后的氧化作用逆转),类似于二氧化钛负载的铂族金属所观察到的。在SMSI状态下,Au / TiO 2 对CO氧化的稳定性显着提高。 SMSI延伸到其他可还原氧化物(Fe 3 O 4 和CeO 2 )和其他IB组金属(Cu和Ag)上负载的Au超过二氧化钛。这一发现突出了经典SMSI的一般性质,并开启了热化学稳定的IB金属催化剂的开发。

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