Theoretical Screening, Regulation, and Prediction of Transition Metal Phthalocyanine Electrocatalysts for NO Reduction into NH<sub>3</sub>
Yu Zhang, Jie Lin, Zhan Cheng, Jiajia Li, Jia Zhu, Quan‐Quan Zhou, Wei Li, Guobing Zhou, Zhen Yang
Abstract
The emerging electrochemical nitric oxide reaction reduction (NORR) has received great attention due to its 2-fold functions in producing NH 3 and eliminating toxic NO molecule. However, developing applicable NORR electrocatalysts with good stability and low-cost features remains challenging. Herein, we combine density functional theory (DFT) and a descriptor-based method to study the catalytic performance of 3d and 4d transition metal phthalocyanine (MPc) and its derivative with axial chlorine ligand (MPc-Cl) electrocatalysts toward NORR. First, we perform DFT calculations to sample MPc/MPc-Cl candidates via a “Three-step” strategy encompassing NO adsorbability, the first hydrogenation step, and NH 3 selectivity. The screened MPc-Cl is found to display remarkably lower limiting potential than MPc. Moreover, we develop a novel descriptor to correlate NORR activity, and the descriptor-predicted NORR limiting potentials are consistent with the DFT-calculated results with a correlation coefficient of 0.98. Our work not only builds a protocol to screen suitable MPc for NO-to-NH 3 conversion but also provides guidance to design high-performance MPc-based electrocatalysts.