Electrochemical Ammonia Synthesis via NO Reduction on 2D-MOF

Chemphyschem. 2021 Nov 29. doi: 10.1002/cphc.202100785. Online ahead of print.ABSTRACTDeveloping new catalysts, which effectively promote electrocatalytic NO reduction (ENOR), is very important for the industrial field. A two-dimensional (2D) metal-organic framework (MOF) with hexaaminobenzene (HAB) ligands (TM-HAB MOF, TM = Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Mo, Ru, Rh and Pd) as an electrocatalyst of ENOR has been systematically explored in this work by means of well-defined density functional theory (DFT) calculations. We predicted the impacts of the coordination structure of different MOFs on its catalytic performance, and found that the suitable candidates are the Co- and Rh-HAB MOFs due to moderate binding strength between NO and substrates. The further calculation indicated that Co-HAB MOF has the best ENOR catalytic activity with a limiting potential of -0.26 V toward NH 3 product at low NO coverage, yet NO reduction to N 2 O at high NO coverage has been limited due to high limiting potential. The scaling relationship with a good correlation coefficient between several electronic properties and the adsorption Gibbs free energy change of *NO (ΔG *NO ) were found, which implied that ΔG *NO can be used as a simple descriptor for screening out suitable electrocatalysts. This work offers a new paradigm for ENOR toward NH 3 under ambient conditions.PMID:34845837 | DOI:10.1002/cphc.202100785

Source: Chemphyschem - November 30, 2021 Category: Chemistry Authors: Bin Huang Bibo Chen Guoping Zhu Jiahe Peng Peng Zhang Yong Qian Neng Li Source Type: research