Plasmon-induced photocatalytic nitrogen fixation on medium-spin Au3Fe1/Mo single-atom alloy antenna reactor

被引：7

作者：

Wang, Bing-Hao ^{[1
]}

Hu, Biao ^{[1
]}

Chen, Guang-Hui ^{[1
]}

Wang, Xiong ^{[1
]}

Tian, Sheng ^{[1
]}

Li, Yang ^{[1
]}

Hu, Xing-Sheng ^{[1
]}

Wang, Huijuan ^{[1
]}

Au, Chak-Tong ^{[3
]}

Jiang, Li-Long ^{[3
]}

Chen, Lang ^{[1
]}

Yin, Shuang-Feng ^{[1
,2
]}

机构：

[1] Hunan Univ, Coll Chem & Chem Engn, Adv Catalyt Engn Res Ctr,Minist Educ, State Key Lab Chemo Biosensing & Chemometr, Changsha 410082, Peoples R China

[2] Cent South Univ Forestry & Technol, Coll Chem & Chem Engn, Changsha 410004, Peoples R China

[3] Fuzhou Univ, Coll Chem Engn, Fuzhou 350002, Peoples R China

来源：

CHEM CATALYSIS | 2024年 / 4卷 / 09期

关键词：

RATIONAL DESIGN; HOT-CARRIER; CATALYSTS; AMMONIA; GOLD;

D O I：

10.1016/j.checat.2024.101083

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Developing photocatalysts with active sites that have appropriate interactions with both N-2 and reactive intermediates has proved to be feasible for direct nitrogen reduction but is still a formidable challenge. Herein, a medium-spin Au3Fe1/Mo single-atom alloy photocatalyst with optical antenna structure is fabricated through an alloying strategy. Fe atoms of a medium-spin state anchored on Au nanoparticles at the single-atom level via Au-Fe bonding is confirmed by combined characterizations of aberration-corrected high-angle annular dark field scanning transmission electron microscopy (AC-HAADF-STEM), X-ray absorption fine structure (XAFS), and M & ouml;ssbauer spectroscopic techniques. With strong Mo-Fe-Au electronic interactions, the Fe sites act as intrinsic centers apt for nitrogen adsorption and activation, which is conducive to the preferential cleavage of the N equivalent to N bond and modulate adsorption of reactive intermediates. Due to synergistic effect of Au nanoparticles acting as optical antennae, the Au3Fe1/Mo photocatalyst showed excellent photocatalytic nitrogen reduction reaction (pNRR) performance, giving an ammonia formation rate of 484.2 mu mol h(-1) g(-1) and solar-to-ammonia (STA) conversion efficiency up to 0.12%.

引用

页数：16