High‐Performance Electrochemical NO Reduction into NH₃ by MoS₂ Nanosheet

Abstract

Electrochemical reduction of NO not only offers an attractive alternative to the Haber-Bosch process for ambient NH 3 production but mitigates the human-caused unbalance of nitrogen cycle. Herein, we report that MoS 2 nanosheet on graphite felt (MoS 2 /GF) acts as an efficient and robust 3D electrocatalyst for NO-to-NH 3 conversion. In acidic electrolyte, such MoS 2 /GF attains a maximal Faradaic efficiency of 76.6 % and a large NH 3 yield of up to 99.6 mmol cm À2 h À1 . Using MoS 2 nanosheet-loaded carbon paper as the cathode, a proof-ofconcept device of Zn-NO battery was assembled to deliver a discharge power density of 1.04 mW cm À2 and an NH 3 yield of 411.8 mg h À1 mg cat.À1 . Calculations reveal that the positively charged Mo-edge sites facilitate NO adsorption/activation via an acceptance-donation mechanism and disfavor the binding of protons and the coupling of NÀN bond.

Efficient nitric oxide electroreduction toward ambient ammonia synthesis catalyzed by a CoP nanoarray

“…3,9 Notably, ambient NO reduction by electrocatalysis is being investigated as a sustainable approach for NO hydrogenation to other harmless or valuable nitrogen species, using only water and electrical energy. 10–23 Among these products, NH 3 as a critical chemical for producing fertilizers and a potential carbon-free energy carrier with high energy density is a notable target molecule. 24,25 Although NH 3 can be produced by N 2 electroreduction, 26–29 it is extremely challenging from both thermodynamic and kinetic points of view since N 2 is chemically inert and poorly dissolves in water.…”

Recent advances in MoS2-based materials for electrocatalysis

“…(6) In addition to the fields of HER/NRR/CO 2 RR activity, in just the past few years, owing to its superior electronic properties and capacities, MoS 2 has also been widely employed in a wide range of applications such as the environmental applications, 222 electrochemical oxygen reduction reaction (ORR), 223 NO reduction, 224 supercapacitors, 225 sensors, 226 secondary batteries ( e.g. , Li-ion batteries (LIBs), 227 Li–S batteries, 228 Li–O 2 batteries, 229 Na–S batteries, 230 Na–O 2 batteries, 231 Mg-ion batteries, 232 Al-ion batteries, 233 and Na-ion batteries, 234 etc.…”

Coupling denitrification and ammonia synthesis via selective electrochemical reduction of nitric oxide over Fe2O3 nanorods

“…Notably, the NH 3 FE of Fe 2 O 3 /CF is higher than that of the reported NORR electrocatalysts including Nb-SA/BNC (77%), 30 Ni 2 P/CP (76.9%), 49 Ru 0.05 Cu 0.95 (64.9%), 50 MnO 2Àx (82.8%), 51 CoSe 2 @CNTs (48.41%), 52 and MoS 2 /GF (76.6%). 53 Encouragingly, at low overpotentials, the H 2 evolution on the Fe 2 O 3 /CP electrode is absolutely suppressed, as evident by the negligible FEs and yields toward H 2 production (FE H 2 ). The higher NH 3 yield than H 2 yield in the whole potential window indicates the high electrocatalytic activity of the Fe 2 O 3 nanorods toward the NORR, far exceeding the competitive HER.…”