Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 59, Issue 50, Pages 22610-22616Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202011596
Keywords
electrocatalysis; lattice strain; nanoreactors; nitrogen fixation; TiO2 nanotubes
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Funding
- U.S. Department of Energy, Office of Science, Basic Energy Sciences [DE-SC0019019]
- Camille Dreyfus Teacher-Scholar Award
- U.S. Department of Energy (DOE) [DE-SC0019019] Funding Source: U.S. Department of Energy (DOE)
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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 N-2 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 mu g h(-1) cm(-2) (16.67 mu g h(-1) mg(cat)(-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.
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