Transition Metals Embedded Two-Dimensional Square Tetrafluorotetracyanoquinodimethane Monolayers as a Class of Novel Electrocatalysts for Nitrogen Reduction Reaction
Shengyao Lv, Guoliang Li, Li‐Ming Yang
Abstract
The combination of transition metal (TM) atoms and high electron affinity organic framework tetrafluorotetracyanoquinodimethanes (F4TCNQs) makes the TM-embedded two-dimensional (2D) square F4TCNQ monolayers (TM-sF4TCNQ) possible to have excellent characteristics of single-atom catalysts and 2D materials. For the first time, the TM-sF4TCNQ monolayers have been considered for application in the electrocatalytic nitrogen reduction reaction (eNRR) field. Through high-throughput screening, the catalytic performance of 30 TM-sF4TCNQ (TM = 3d∼5d TMs) monolayers for eNRR was comprehensively evaluated. The Mo-, Nb-, and Tc-sF4TCNQ catalysts stand out with the onset potentials of −0.18, −0.44, and −0.54 V, respectively, through the optimal reaction paths. Our work will provide guidance for the green and sustainable development of electrocatalytic nitrogen fixation.