Indexed by:
Abstract:
Ammonia (NH3) plays an important role in the development and evolution of Earth's life system. The extremely high bond energy (941 kJ mol(-1)) of N-2 hinder the conversion of N-2 to NH3 under mild conditions. Meanwhile, clearly identifying the distribution of intermediates for NH3 synthesis remains a huge challenge in the experiment. Herein, we anchored carbon clusters (C-60 or C-70) onto Ru catalysts supported on rare earth oxides, forming a class of Ru-carbon cluster co-catalysts that exhibit strong electronic metal-carbon cluster interaction (EMCI). Carbon clusters function as an electron buffer that induced electron uptake from metallic Ru sites and concurrently provides electron feedback to Ru delta+ in a reversible manner, achieving a flexible balance of electron density at the Ru active sites. Moreover, H-affinitive carbon clusters serve as the site for the adsorption, activation and migration of hydrogen. With Ru and carbon clusters synergistically bridged by hydrogen spillover, the Ru-C-60 co-catalyst exhibits an exceptionally high NH3 synthesis rate and remarkable stability. Experimental provides direct evidence of the distribution and evolution of *N2Hx (x = 1 similar to 3) intermediates, with the hydrogenation of *NH2 to form *NH3 identified as the rate-determining step. This work paves the way for utilizing carbon clusters in important chemical reactions.
Keyword:
Reprint 's Address:
Email:
Version:
Source :
ADVANCED FUNCTIONAL MATERIALS
ISSN: 1616-301X
Year: 2024
Issue: 8
Volume: 35
1 8 . 5 0 0
JCR@2023
Cited Count:
SCOPUS Cited Count:
ESI Highly Cited Papers on the List: 0 Unfold All
WanFang Cited Count:
Chinese Cited Count:
30 Days PV: 1