Water Durable Electride Y5Si3: Electronic Structure and Catalytic Activity for Ammonia Synthesis

被引：254

作者：

Lu, Yangfan ^{[1
,2
]}

Li, Jiang ^{[1
,2
]}

Tada, Tomofumi ^{[1
]}

Toda, Yoshitake ^{[1
,2
]}

Ueda, Shigenori ^{[3
,4
]}

Yokoyama, Toshiharu ^{[1
,2
]}

Kitano, Masaaki ^{[1
]}

Hosono, Hideo ^{[1
,2
]}

机构：

[1] Tokyo Inst Technol, Mat Res Ctr Element Strategy, Midori Ku, 4259 Nagatsuta, Yokohama, Kanagawa 2268503, Japan

[2] Japan Sci & Technol Agcy, ACCEL, 4-1-8 Honcho, Kawaguchi, Saitama 3320012, Japan

[3] Natl Inst Mat Sci, Synchrotron Xray Stn SPring 8, 1-1-1 Kouto, Sayo, Hyogo 6795148, Japan

[4] NIMS, Quantum Beam Unit, 1-2-1 Sengen, Tsukuba, Ibaraki 3050047, Japan

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2016年 / 138卷 / 12期

基金：

日本科学技术振兴机构;

关键词：

3-DIMENSIONAL VISUALIZATION; WORK FUNCTION; CRYSTAL;

D O I：

10.1021/jacs.6b00124

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

We report an air and water stable electride Y5Si3 and its catalytic activity for direct ammonia synthesis. It crystallizes in the Mn5Si3-type structure and confines 0.79/f.u. anionic electrons in the quasi-one-dimensional holes. These anionic electrons strongly hybridize with yttrium 4d electrons, giving rise to improved chemical stability. The ammonia synthesis rate using Ru(7.8 wt %)-loaded Y5Si3 was as high as 1.9 mmol/g/h under 0.1 MPa and at 400 degrees C with activation energy of similar to 50 kJ/mol. Its strong electron-donating ability to Ru metal of Y5Si3 is considered to enhance nitrogen dissociation and reduce the activation energy of ammonia synthesis reaction. Catalytic activity was not suppressed even after Y5Si3, once dipped into water, was used as the catalyst promoter. These findings provide novel insights into the design of simple catalysts for ammonia synthesis.

引用

页码：3970 / 3973

页数：4

共 26 条

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