Highly Efficient Electrochemical Reduction of Nitrogen to Ammonia on Surface Termination Modified Ti₃C₂T_x MXene Nanosheets

Abstract

MXene-based catalysts exhibit extraordinary advantages for many catalysis reactions, such as the hydrogen evolution and oxygen reduction reactions. However, MXenes exhibit inadequate catalytic activity for the electrochemical nitrogen reduction reaction (NRR) because they are typically terminated with inactive functional groups, F* and OH*, which mask the active metal sites for N 2 binding. Here we modified the surface termination of MXene (Ti 3 C 2 T x ) nanosheets to achieve high surface catalytic reactivity for the NRR by ironing out inactive F*/OH* terminals to expose more active sites and by introducing Fe to greatly reduce the surface work function. The optimally performing catalyst (MXene/TiFeO x -700) achieved excellent Faradaic efficiency of 25.44% and an NH 3 yield rate of 2.19 μg/cm 2 •h (21.9 μg/mg cat •h), outperforming all reported MXene-based NRR catalysts. Our work provides a feasible strategy for rationally improving the surface reactivity of MXene-based catalysts for efficient electrochemical conversion of N 2 to NH 3 .

Enhancing N2 Fixation Activity by Converting Ti3C2 MXenes Nanosheets to Nanoribbons

“…Xia et al., [11] on the contrary, indicated that exposed Ti sites in Ti 3 C 2 OH facilitate the electron transfer and promote the adsorption and activation of dinitrogen. Guo et al [12] . suggested that OH terminal groups of MXene are inactive, indicating thus that a modification of the surface chemical states by introducing Fe heteroatoms is necessary to increase the activity.…”

Highly Sensitive and Selective Gas Sensor Using Heteroatom Doping Graphdiyne: A DFT Study

“…In particular, 2D materials have attracted great attention due to their own superiority of abundant adsorption sites, large specific surface area, and tunable surface chemistry. [ 4,5 ] Recently, g‐C 3 N 4 through Ag doping have been proved to exhibit selectivity toward NO 2 , [ 6 ] but the whole process consumed expensive noble‐metal. Zhu et.…”

Folic Acid Self-Assembly Enabling Manganese Single-Atom Electrocatalyst for Selective Nitrogen Reduction to Ammonia

“…To analyze the yield rate and Faradaic efficiency of ammonia, the produced NH 3 in the electrolyte was detected by the typical indophenol blue method [33,34]. All the yield rate and Faradaic efficiency are calculated from the average values of three repetitive measurements.…”