Exposed facet-controlled N2 electroreduction on distinct Pt3Fe nanostructures of nanocubes, nanorods and nanowires

作     者：Wu Tong Bolong Huang Pengtang Wang Qi Shao Xiaoqing Huang Wu Tong;Bolong Huang;Pengtang Wang;Qi Shao;Xiaoqing Huang

作者机构：College of ChemistryChemical Engineering and Materials Science Soochow University Department of Applied Biology and Chemical TechnologyHong Kong Polytechnic University 

出 版 物：《National Science Review》 (国家科学评论(英文版))

年 卷 期：2021年第8卷第1期

页      面：117-126页

核心收录：

学科分类：081702[工学-化学工艺] 081705[工学-工业催化] 07[理学] 070205[理学-凝聚态物理] 08[工学] 0817[工学-化学工程与技术] 080501[工学-材料物理与化学] 080502[工学-材料学] 0805[工学-材料科学与工程（可授工学、理学学位）] 0702[理学-物理学] 

基　　金：supported by the Ministry of Science and Technology (2016YFA0204100 and 2017YFA0208200) the National Natural Science Foundation of China (21571135) Young Thousand Talented Program Jiangsu Province Natural Science Fund for Distinguished Young Scholars (BK20170003) the Priority Academic Program Development of Jiangsu Higher Education Institutions the start-up funding from Soochow University 

主　　题：Pt_3Fe nanowire high-index facet-controlled N2 reduction 

摘      要：Understanding the correlation between exposed surfaces and performances of controlled nanocatalysts can aid effective strategies to enhance electrocatalysis, but this is as yet unexplored for the nitrogen reduction reaction （NRR）. Here, we first report controlled synthesis of well-defined Pt3Fe nanocrystals with tunable morphologies （nanocube, nanorod and nanowire） as ideal model electrocatalysts for investigating the NRR on different exposed facets. The detailed electrocatalytic studies reveal that the Pt3Fe nanocrystals exhibit shape-dependent NRR electrocatalysis. The optimized Pt3Fe nanowires bounded with high-index facets exhibit excellent selectivity （no N2H4 is detected）, high activity with NH3yield of 18.3μg h-1mg-1cat(0.52μg h-1cm-2ECSA; ECSA:electrochemical active surface area) and Faraday efficiency of 7.3%at-0.05 V versus reversible hydrogen electrode, outperforming the{200}facet-enclosed Pt3Fe nanocubes and{111}facet-enclosed Pt3Fe nanorods. They also show good stability with negligible activity change after five cycles. Density functional theory calculations reveal that, with high-indexed facet engineering, the Fe-3d band is an efficient d-d coupling correlation center for boosting the Pt 5d-electronic exchange and transfer activities towards the NRR.