文献类型：期刊文献

英文题名：A General Strategy to Boost Electrocatalytic Nitrogen Reduction on Perovskite Oxides via the Oxygen Vacancies Derived from A-Site Deficiency

作者：Chu, Kaibin[1];Liu, Fuzhu[2];Zhu, Jiawei[1];Fu, Hui[1];Zhu, Haiyan[1];Zhu, Yinlong[3];Zhang, Yu[4];Lai, Feili[5];Liu, Tianxi[1]

机构：[1]Jiangnan Univ, Key Lab Synthet & Biol Colloids, Minist Educ, Sch Chem & Mat Engn, Wuxi 214122, Jiangsu, Peoples R China;[2]Xi An Jiao Tong Univ, State Key Lab Mech Behav Mat, Xian 710049, Shanxi, Peoples R China;[3]Monash Univ, Dept Chem Engn, Clayton, Vic 3800, Australia;[4]East China Univ Sci & Technol, Sch Mech & Power Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China;[5]Katholieke Univ Leuven, Dept Chem, Celestijnenlaan 200F, B-3001 Leuven, Belgium

年份：2021

卷号：11

期号：11

外文期刊名：ADVANCED ENERGY MATERIALS

收录：;EI(收录号：20210509839754);WOS:【SCI-EXPANDED(收录号:WOS:000612637500001)】；

基金：K.C. and F.L. contributed equally to this work. The authors are grateful for the financial support from the National Natural Science Foundation of China (51433001), the Shanghai Scientific and Technological Innovation Project (18JC1410600), and the Program of Shanghai Academic Research Leader (17XD1400100). DFT calculations were performed using the HPC Platform of Xi'an Jiaotong University.

语种：英文

外文关键词：cation deficiency; electrocatalytic N-2 reduction; oxygen vacancy; perovskite oxide

摘要：The electrocatalytic N-2 reduction reaction (NRR) under ambient conditions is an attractive strategy for green synthesis of NH3. Due to the ultra-stable N(sic)N covalent triple bond, it is very challenging to develop highly selective and efficient electrocatalysts toward NRR. Here a general strategy to enhance the NRR activity through modulating A-site-deficiency-induced oxygen vacancies of perovskite oxides is reported. One successful example is LaxFeO3-delta (LxF, x = 1, 0.95, and 0.9) perovskite oxides with tunable oxygen vacancies that are directly proportional to the La-site deficiencies. As compared to the pristine LF, the L0.95F and L0.9F exhibit significantly improved NRR activities, which are positively correlated with the La-site deficiency and the amount of oxygen vacancies. Among them, the L0.9F delivers the best activity, with an NH3 yield rate of 22.1 mu g center dot h(-1)center dot mg(cat.)(-1) at -0.5 V and a Faradaic efficiency of 25.6% at -0.3 V, which are 2.2 and 1.6 times those of the pristine LF, respectively. Both experimental characterizations and theoretical calculations suggest that the enhanced NRR activity can be mainly attributed to the favorable merits produced by the oxygen vacancies: the promoted adsorption/activation of reaction species, and thus optimized reaction pathways. Previous studies on other perovskite oxides have generated similarly successful results.