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金纳米颗粒与二氧化钛之间的经典强金属-载体相互作用。

Classical strong metal-support interactions between gold nanoparticles and titanium dioxide.

作者信息

Tang Hailian, Su Yang, Zhang Bingsen, Lee Adam F, Isaacs Mark A, Wilson Karen, Li Lin, Ren Yuegong, Huang Jiahui, Haruta Masatake, Qiao Botao, Liu Xin, Jin Changzi, Su Dangsheng, Wang Junhu, Zhang Tao

机构信息

State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China.

Mössbauer Effect Data Center, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China.

出版信息

Sci Adv. 2017 Oct 13;3(10):e1700231. doi: 10.1126/sciadv.1700231. eCollection 2017 Oct.

Abstract

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/TiO, evidenced by suppression of CO adsorption, electron transfer from TiO to Au nanoparticles, and gold encapsulation by a TiO overlayer following high-temperature reduction (reversed by subsequent oxidation), akin to that observed for titania-supported platinum group metals. In the SMSI state, Au/TiO exhibits markedly improved stability toward CO oxidation. The SMSI extends to Au supported over other reducible oxides (FeO and CeO) 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.

摘要

负载型金属催化剂在现代化学工业中起着核心作用,但往往表现出较差的在线稳定性。强金属-载体相互作用(SMSI)为控制负载型金属的结构性质提供了一条途径,从而控制其反应活性和稳定性。传统观点认为,负载型金不能表现出典型的SMSI,其特征是在高温氧化还原处理时载体对金属进行可逆封装。我们证明了Au/TiO存在典型的SMSI,这表现为CO吸附受到抑制、电子从TiO转移到金纳米颗粒以及在高温还原后金被TiO覆盖层封装(随后的氧化可使其逆转),这与二氧化钛负载的铂族金属的情况类似。在SMSI状态下,Au/TiO对CO氧化表现出显著提高的稳定性。这种SMSI扩展到负载在其他可还原氧化物(FeO和CeO)上的金以及负载在二氧化钛上的其他IB族金属(Cu和Ag)。这一发现突出了典型SMSI的普遍性,并为热化学稳定的IB族金属催化剂的开发开辟了道路。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/99f1/5640381/9ed2616c56f0/1700231-F1.jpg

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