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三元催化反应过程中镍铜合金催化剂的自再生过程——一项研究

Self-Regeneration Process of Ni-Cu Alloy Catalysts during a Three-Way Catalytic Reaction-An Study.

作者信息

Asakura Hiroyuki, Onuki Tetsuo, Hosokawa Saburo, Teramura Kentaro, Tanaka Tsunehiro

机构信息

Department of Molecular Engineering, Graduate School of Engineering, Kyoto University, Kyotodaigaku Katsura, Nishikyo-ku, Kyoto 615-8510, Japan.

Elements Strategy Initiative for Catalysts & Batteries (ESICB), Kyoto University, 1-30 Goryo-Ohara, Nishikyo-ku, Kyoto 615-8245, Japan.

出版信息

ACS Appl Mater Interfaces. 2020 Dec 16;12(50):55994-56003. doi: 10.1021/acsami.0c17256. Epub 2020 Dec 7.

Abstract

It is important to understand the reduction processes of mixed metal oxides or metal oxide interfaces in three-way catalytic reactions toward replacing the currently used high-cost Pt group metal catalysts. The redox behavior of simple Ni-Cu alloy catalysts, which exhibit high catalytic activity and durability during a three-way catalytic reaction, was studied by X-ray absorption spectroscopy (XAS). The XAS analyses revealed that Ni-Cu species changed from the NiO-CuO to Ni-Cu alloy and vice versa under reductive and oxidative conditions, respectively. The real-time monitoring of the oxidation states of Ni and Cu species indicated that the Cu species assisted the reduction of Ni species, in agreement with the density functional theory-based study of NiO reduction by carbon monoxide in the presence of metallic Cu nanoparticles.

摘要

对于三元催化反应中混合金属氧化物或金属氧化物界面的还原过程,为了替代目前使用的高成本铂族金属催化剂,了解这些过程非常重要。通过X射线吸收光谱(XAS)研究了在三元催化反应中表现出高催化活性和耐久性的简单Ni-Cu合金催化剂的氧化还原行为。XAS分析表明,在还原和氧化条件下,Ni-Cu物种分别从NiO-CuO转变为Ni-Cu合金,反之亦然。对Ni和Cu物种氧化态的实时监测表明,Cu物种有助于Ni物种的还原,这与基于密度泛函理论的在金属Cu纳米颗粒存在下一氧化碳还原NiO的研究结果一致。

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