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用于低温CO分解的钯掺杂氧化铟氧载体的独特氧化还原活性

Unmatched Redox Activity of the Palladium-Doped Indium Oxide Oxygen Carrier for Low-Temperature CO Splitting.

作者信息

Park Seyeon, Oh DongHwan, Jang Myeong Gon, Seo Hwakyoung, Kim Uisik, Ahn Jaewan, Choi Yoonseok, Shin Dongjae, Han Jeong Woo, Jung WooChul, Kim Il-Doo

机构信息

Department of Materials Science and Engineering, Korea Advanced Institute of Science and Technology (KAIST), Daejeon 34141, Republic of Korea.

Department of Materials Science and Engineering, Research Institute of Advanced Materials, Seoul National University, Seoul 08826, Republic of Korea.

出版信息

ACS Nano. 2024 Sep 17;18(37):25577-25590. doi: 10.1021/acsnano.4c06244. Epub 2024 Aug 27.

Abstract

The chemical conversion of CO into value-added products is the key technology to realize a carbon-neutral society. One representative example of such conversion is the reverse water-gas shift reaction, which produces CO from CO. However, the activity is insufficient at ambient pressure and lower temperatures (<600 °C), making it a highly energy-intensive and impractical process. Herein, we report indium oxide nanofibers modified with palladium catalysts that exhibit significantly potent redox activities toward the reduction of CO splitting via chemical looping. In particular, we uncover that the doped palladium cations are selectively reduced and precipitated onto the host oxide surface as metallic nanoparticles. These catalytic gems formed operando make InO lattice oxygen more redox-active in H and CO environments. As a result, the composite nanofiber catalysts demonstrate the reverse water-gas shift reaction via chemical looping at record-low temperatures (≤350 °C), while also imparting high activities (CO conversion: 45%). Altogether, our findings expand the viability of CO splitting at lower temperatures and provide design principles for indium oxide-based catalysts for CO conversion.

摘要

将一氧化碳化学转化为增值产品是实现碳中和社会的关键技术。这种转化的一个典型例子是逆水煤气变换反应,该反应由二氧化碳生成一氧化碳。然而,在常压和较低温度(<600°C)下,其活性不足,这使得该过程能源密集度高且不切实际。在此,我们报道了用钯催化剂改性的氧化铟纳米纤维,其对通过化学链实现的一氧化碳裂解还原表现出显著的氧化还原活性。特别是,我们发现掺杂的钯阳离子被选择性还原并以金属纳米颗粒的形式沉淀在主体氧化物表面。原位形成的这些催化活性位点使氧化铟晶格氧在氢气和一氧化碳环境中更具氧化还原活性。结果,复合纳米纤维催化剂在创纪录的低温(≤350°C)下通过化学链实现了逆水煤气变换反应,同时还具有高活性(一氧化碳转化率:45%)。总之,我们的研究结果扩展了低温下一氧化碳裂解的可行性,并为用于一氧化碳转化的氧化铟基催化剂提供了设计原则。

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