Hydrogen spillover-driven synthesis of high-entropy alloy nanoparticles as a robust catalyst for CO2 hydrogenation

被引:221
作者
Mori, Kohsuke [1 ,2 ,3 ]
Hashimoto, Naoki [1 ]
Kamiuchi, Naoto [4 ]
Yoshida, Hideto [4 ]
Kobayashi, Hisayoshi [5 ]
Yamashita, Hiromi [1 ,2 ,3 ]
机构
[1] Osaka Univ, Grad Sch Engn, Div Mat & Mfg Sci, Osaka, Japan
[2] Kyoto Univ, Elements Strategy Initiat Catalysts Batteries ESI, Kyoto, Japan
[3] Osaka Univ, Innovat Catalysis Sci Div, Inst Open & Transdisciplinary Res Initiat ICS OTR, Osaka, Japan
[4] Osaka Univ, Inst Sci & Ind Res, Osaka, Japan
[5] Kyoto Inst Technol, Kyoto, Japan
关键词
ELECTRONIC-STRUCTURE; RADIATION-DAMAGE; PHASE-STABILITY; RECENT PROGRESS; MECHANISMS; SURFACE; DFT; METHANATION; DIFFUSION; ENERGY;
D O I
10.1038/s41467-021-24228-z
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
High-entropy alloys (HEAs) have been intensively pursued as potentially advanced materials because of their exceptional properties. However, the facile fabrication of nanometer-sized HEAs over conventional catalyst supports remains challenging, and the design of rational synthetic protocols would permit the development of innovative catalysts with a wide range of potential compositions. Herein, we demonstrate that titanium dioxide (TiO2) is a promising platform for the low-temperature synthesis of supported CoNiCuRuPd HEA nanoparticles (NPs) at 400 degrees C. This process is driven by the pronounced hydrogen spillover effect on TiO2 in conjunction with coupled proton/electron transfer. The CoNiCuRuPd HEA NPs on TiO2 produced in this work were found to be both active and extremely durable during the CO2 hydrogenation reaction. Characterization by means of various in situ techniques and theoretical calculations elucidated that cocktail effect and sluggish diffusion originating from the synergistic effect obtained by this combination of elements. Facile fabrication of high-entropy alloys (HEAs) nanoparticles (NPs) on conventional catalyst supports remains challenging. Here the authors show TiO2 is a promising platform for the low-temperature synthesis of supported CoNiCuRuPd HEA NPs with excellent activity and durability in CO2 hydrogenation.
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页数:11
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