Zhang Nan, Li Leigang, Wang Juan, Hu Zhiwei, Shao Qi, Xiao Xiangheng, Huang Xiaoqing
College of Chemistry, Chemical Engineering and Materials Science Soochow University, Suzhou, 215123, Jiangsu, China.
Department of Physics and Key Laboratory of Artificial Micro- and Nano-Structures of Ministry of Education, Hubei Nuclear Solid Physics Key Laboratory, Wuhan University, Wuhan, 430072, Hubei, China.
Angew Chem Int Ed Engl. 2020 May 18;59(21):8066-8071. doi: 10.1002/anie.201915747. Epub 2020 Mar 18.
Surface regulation is an effective strategy to improve the performance of catalysts, but it has been rarely demonstrated for nitrogen reduction reaction (NRR) to date. Now, surface-rough Rh Sb nanorod (RNR) and surface-smooth Rh Sb NR (SNR) were selectively created, and their performance for NRR was investigated. The high-index-facet bounded Rh Sb RNRs/C exhibit a high NH yield rate of 228.85±12.96 μg h mg at -0.45 V versus reversible hydrogen electrode (RHE), outperforming the Rh Sb SNRs/C (63.07±4.45 μg h mg ) and Rh nanoparticles/C (22.82±1.49 μg h mg ), owing to the enhanced adsorption and activation of N on high-index facets. Rh Sb RNRs/C also show durable stability with negligible activity decay after 10 h of successive electrolysis. The present work demonstrates that surface regulation plays an important role in promoting NRR activity and provides a new strategy for creating efficient NRR electrocatalysts.
表面调控是提高催化剂性能的有效策略,但迄今为止在氮还原反应(NRR)中鲜有例证。现在,选择性地制备了表面粗糙的RhSb纳米棒(RNR)和表面光滑的RhSb纳米棒(SNR),并研究了它们的NRR性能。与可逆氢电极(RHE)相比,在-0.45 V时,高指数面边界的RhSb RNRs/C表现出228.85±12.96 μg h mg的高NH产率,优于RhSb SNRs/C(63.07±4.45 μg h mg)和Rh纳米颗粒/C(22.82±1.49 μg h mg),这归因于高指数面上N的吸附和活化增强。RhSb RNRs/C在连续电解10小时后也表现出持久的稳定性,活性衰减可忽略不计。目前的工作表明,表面调控在促进NRR活性方面起着重要作用,并为制备高效的NRR电催化剂提供了一种新策略。