Liu Ya-Ping, Li Yu-Biao, Zhang Hu, Chu Ke
School of Materials Science and Engineering , Lanzhou Jiaotong University , Lanzhou 730070 , China.
School of Materials Science and Engineering , University of Science and Technology Beijing , Beijing 100083 , China.
Inorg Chem. 2019 Aug 5;58(15):10424-10431. doi: 10.1021/acs.inorgchem.9b01823. Epub 2019 Jul 26.
The development of highly active and durable electrocatalysts toward the N reduction reaction (NRR) holds a key to ambient electrocatalytic NH synthesis. Herein, fluorine (F)-doped SnO mesoporous nanosheets on carbon cloth (F-SnO/CC) were developed as an efficient NRR electrocatalyst. Benefiting from the combined structural advantages of mesoporous nanosheet structure and F-doping, the F-SnO/CC exhibited high NRR activity with an NH yield of 19.3 μg h mg and a Faradaic efficiency of 8.6% at -0.45 V (vs RHE) in 0.1 M NaSO, comparable or even superior to those of most reported NRR electrocatalysts. Density functional theory calculations revealed that the F-doping could readily tailor the electronic structure of SnO to render it with improved conductivity and increased positive charge on active Sn sites, leading to the lowered reaction energy barriers and boosted NRR activity.
开发用于氮还原反应（NRR）的高活性和耐用的电催化剂是实现环境电催化合成氨的关键。在此，碳布上的氟（F）掺杂SnO介孔纳米片（F-SnO/CC）被开发为一种高效的NRR电催化剂。受益于介孔纳米片结构和F掺杂的综合结构优势，F-SnO/CC在0.1 M NaSO中于-0.45 V（相对于可逆氢电极）时表现出高NRR活性，氨产率为19.3 μg h mg，法拉第效率为8.6%，与大多数已报道的NRR电催化剂相当甚至更优。密度泛函理论计算表明，F掺杂能够轻松调整SnO的电子结构，使其具有更高的导电性以及活性Sn位点上增加的正电荷，从而降低反应能垒并提高NRR活性。
