Fu Yang, Li Kangkang, Batmunkh Munkhbayar, Yu Hai, Donne Scott, Jia Baohua, Ma Tianyi
Discipline of Chemistry, School of Environmental and Life Sciences, University of Newcastle, Callaghan, New South Wales 2308, Australia.
CSIRO Energy, 10 Murray Dwyer Circuit, Mayfield West, New South Wales 2304, Australia.
ACS Appl Mater Interfaces. 2020 Oct 7;12(40):44830-44839. doi: 10.1021/acsami.0c13902. Epub 2020 Sep 23.
Electrochemical ammonia synthesis that utilizes renewable electricity in the nitrogen reduction reaction (NRR) has recently been remarkably considered. Of particular importance is to develop efficient electrocatalysts at low costs. Herein, highly selective nitrogen capture using porous aluminum-based metal-organic frameworks (MOFs) materials, MIL-100 (Al), is first designed for the electrochemical nitrogen fixation in alkaline media under ambient conditions. Owing to the unique structure, MIL-100 (Al) exhibits remarkable NRR properties (NH yield: 10.6 μg h cm mg and Faradaic efficiency: 22.6%) at a low overpotential (177 mV). Investigation indicates that the catalyst shows excellent N-selective captures due to the unsaturated metal sites binding with N. More specifically, as the Al 3p band can strongly interact with N 2p orbitals, Al as a main group metal presents a high and selective affinity to N. The utilization of multifunctional MOF catalysts delivers both high N selectivity and abundant catalytic sites, resulting in remarkable efficiency for NH production.
利用可再生电力进行氮还原反应（NRR）的电化学氨合成最近受到了显著关注。特别重要的是开发低成本的高效电催化剂。在此，首次设计了使用多孔铝基金属有机框架（MOF）材料MIL-100（Al）在环境条件下的碱性介质中进行电化学固氮的高选择性氮捕获。由于其独特的结构，MIL-100（Al）在低过电位（177 mV）下表现出显著的NRR性能（NH产率：10.6 μgh cm mg，法拉第效率：22.6%）。研究表明，由于不饱和金属位点与N结合，该催化剂表现出优异的N选择性捕获。更具体地说，由于Al 3p能带可以与N 2p轨道强烈相互作用，Al作为主族金属对N具有高选择性亲和力。多功能MOF催化剂的利用提供了高N选择性和丰富的催化位点，从而产生了显著的NH生产效率。
