A Surface‐Strained and Geometry‐Tailored Nanoreactor that Promotes Ammonia Electrosynthesis

• Published in: Angewandte Chemie (International ed.) 2020-12, Vol.59 (50), p.22610-22616
• Main Authors: Li, Panpan, Jin, Zhaoyu, Fang, Zhiwei, Yu, Guihua
• Format: Article
• Language: English
• Subjects: Ammonia; Catalysis; electrocatalysis; Geometry; INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Lattice strain; Mass transport; nanoreactors; Nitrogen fixation; Nitrogenation; Renewable energy; Selectivity; TiO2 nanotubes; Titanium dioxide
• ISSN: 1433-7851; 1521-3773
• DOI: 10.1002/anie.202011596

A surface‐strained and geometry‐optimized TiO2 nanoreactor enhances the performance of electrocatalytic nitrogen fixation. The nanotubular confinement allows spatial regulation of the mass transport of nitrogen during the NRR process and offers an enlarged surface area, thus boosting the ammonia production with high selectivity. Both experimental and theoretical evidence support strained Ti3+ sites, demonstrating a more favorable pathway for the N2 activation and selective NH3 production with a faster kinetic rate than the pristine TiO2. The TiO2‐based nanoreactor with surface and bulk structure tailoring delivered an NH3 yield rate up to 5.50 μg h−1 cm−2 (16.67 μg h−1 mgcat−1) and high faradaic efficiency of 26 % under ambient aqueous conditions. Our findings highlight the concept of lattice strain and geometry modified nanoreactors, which will have broad implications in the renewable energy catalysis and electrosynthesis of valuable products. A surface‐strained and geometry‐optimized TiO2 nanoreactor was designed to enhance the electrocatalytic nitrogen reduction reaction. The nanotubular structure enables spatial confinement to regulate mass transfer during NRR process, thus boosting ammonia production with high selectivity. The tensile strain induced by Li+ intercalation/deintercalation favors N2 adsorption, thereby achieving a faster kinetic rate.