Journal
ADVANCED MATERIALS
Volume 32, Issue 24, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202001267
Keywords
metal nanocrystals; nitrogen reduction reaction; rhodium; surface chalcogenation; universality
Categories
Funding
- Ministry of Science and Technology [2016YFA0204100, 2017YFA0208200]
- National Natural Science Foundation of China [21571135]
- Young Thousand Talented Program, Jiangsu Province Natural Science Fund for Distinguished Young Scholars [BK20170003]
- Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)
- Soochow University
Ask authors/readers for more resources
Electrocatalytic nitrogen reduction reaction (NRR) is a promising process relative to energy-intensive Haber-Bosch process. While conventional electrocatalysts underperform with sluggish paths, achieving dissociation of N-2 brings the key challenge for enhancing NRR. This study proposes an effective surface chalcogenation strategy to improve the NRR performance of pristine metal nanocrystals (NCs). Surprisingly, the NH3 yield and Faraday efficiency (FE) (175.6 +/- 23.6 mg h(-1) g(Rh)(-1) and 13.3 +/- 0.4%) of Rh-Se NCs is significantly enhanced by 16 and 15 times, respectively. Detailed investigations show that the superior activity and high FE are attributed to the effect of surface chalcogenation, which not only can decrease the apparent activation energy, but also inhibit the occurrence of the hydrogen evolution reaction (HER) process. Theoretical calculations reveal that the strong interface strain effect within core@shell system induces a critical redox inversion, resulting in a rather low valence state of Rh and Se surface sites. Such strong correlation indicates an efficient electron-transfer minimizing NRR barrier. Significantly, the surface chalcogenation strategy is general, which can extend to create other NRR metal electrocatalysts with enhanced performance. This strategy open a new avenue for future NH3 production for breakthrough in the bottleneck of NRR.
Authors
I am an author on this paper
Click your name to claim this paper and add it to your profile.
Reviews
Recommended
No Data Available