LaRuSi Electride Disrupts the Scaling Relations for Ammonia Synthesis
LaRuSi Electride Disrupts the Scaling Relations for Ammonia Synthesis
复制标题
LaRuSi 电子化合物破坏氨合成的标度关系
DOI：
10.1021/acs.chemmater.1c03821
复制
发表时间：
2022-01
影响因子：
8.6
通讯作者：
Hosono Hideo
中科院分区：
文献类型：
--
作者：
Gong Yutong;Li Hongchen;Li Can;Yang Xueqing;Wang Junjie;Hosono Hideo
在温和条件下，电子氮化物作为催化剂或载体在氨合成中显示出显著的优势。深入了解这类非常规反应动力学，将极大地促进这类新型催化剂的开发。然而，大多数基于水的催化剂是负载型的，其复杂性阻碍了机理研究。在这篇文章中，LaRuSi催化剂的催化性能背后的本质是揭示使用实验和第一性原理计算相结合。发现LaRuSi络合物能够通过两种机制破坏标度关系，这确保了NH3合成的高催化性能。首先，在Ru封端的表面上可以实现非常低的N2活化能，而不需要非常强的氮物种吸附;然后，用于NHX形成的第二有效活性位点（La位点）进一步显著降低了整体反应的势垒。通过与结构相同的未掺杂CaRuSi的对比研究，发现LaRuSi的催化作用确实来源于其阴离子电子的特性。这项研究提供了深入了解的工作机制，基于催化剂的催化剂，可以刺激设计新的催化材料，提高性能。
Electrides have shown their significant advantages in NH3synthesis as catalysts or supports under mild conditions. A better understanding of the unconventional reaction kinetics of electrides can greatly promote the development of this kind of novel catalyst. However, most electride-based catalysts are supported ones whose complexity hampers the mechanism study. In this article, the essence behind the catalytic performance of a LaRuSi electride was uncovered using a combination of experiments and first-principles calculations. The LaRuSi electride was found to be capable of disrupting the scaling relations via two mechanisms, which ensured high catalytic performance for NH3synthesis. First, a very low N2activation energy on a Ru-terminated surface can be achieved without extremely strong adsorption of nitrogen species; then, a second efficient active site (La site) for NHxformation further significantly reduces the barriers for the overall reaction. A comparative study with CaRuSi, a nonelectride but with the same structure, reveals that the catalytic effect of LaRuSi is indeed derived from the characteristics of anionic electrons. This study delivers insights into the working mechanism of electride-based catalysts and can stimulate the design of new catalytic materials with improved performance.
登录
查看更多内容
影响因子：
16.6
作者：
Liu JC;Ma XL;Li Y;Wang YG;Xiao H;Li J
通讯作者：
Li J
影响因子：
16.6
作者：
Kitano, Masaaki;Kanbara, Shinji;Inoue, Yasunori;Kuganathan, Navaratnarajah;Sushko, Peter V.;Yokoyama, Toshiharu;Hara, Michikazu;Hosono, Hideo
通讯作者：
Hosono, Hideo
影响因子：
15
作者：
Tiannan Ye;Sang-Won Park;Yangfan Lu;Jiang Li;M. Sasase;M. Kitano;H. Hosono
通讯作者：
Tiannan Ye;Sang-Won Park;Yangfan Lu;Jiang Li;M. Sasase;M. Kitano;H. Hosono
影响因子：
1.9
作者：
M.-C. Tsai;U. Seip;I. Bassignana;J. Küppers;G. Ertl
通讯作者：
M.-C. Tsai;U. Seip;I. Bassignana;J. Küppers;G. Ertl
影响因子：
21.8
作者：
Kitano, Masaaki;Inoue, Yasunori;Hosono, Hideo
通讯作者：
Hosono, Hideo