Ambient electrosynthesis of ammonia with efficient denitration

Abstract

The NH 3 electrosynthesis under ambient conditions represents an attractive alternative to the traditional Haber−Bosch industrial process, and NO is one of the major air pollutants. Here, with single-atom-site Nb catalyst, the ambient electrochemical denitration of NO exhibited a record high NH 3 yield rate of 8.2 × 10 −8 mol cm −2 s −1 , which is two orders of magnitude larger than those achieved by the best-reported catalysts for the ambient NH 3 electrosynthesis and approaches the US Department of Energy target. Theoretical calculations reveal that the single-atomic Nb sites not only facilitate the NO adsorption but also lower the energy barrier of the potential-determining step. High-efficiency electrocatalytic NO-to-NH 3 conversion was realized by Nb single-atom-site catalysis under ambient conditions. The Nb single-site catalyst achieved a record high NH 3 yield rate of 8.2 × 10 −8 mol cm −2 s −1 , approaching the DOE target. • A series of single metal atoms supported on B,N co-doped carbon nanotubes have been synthesized for NH 3 electrosynthesis. • The Nb catalyst achieves a record high NH 3 yield rate of 8.2 × 10 −8 mol cm −2 s −1 , which is approacheing the US DOE target. • This electrochemical NO reaction strategy well integrates the NH 3 production as well as environmental protection.