DFT研究三单原子催化剂用于一步N–C–N偶联合成 尿素

Electrocatalytic synthesis of urea from carbon dioxide (CO2) and nitrous oxides (NOx) provides promising approaches to alleviate the greenhouse effect. However, this approach still lacks efficient electrocatalysts, which is a key challenge. Here we design group electrocatalysts that are triple-single-atom supported on C9N4 monolayer for production. Our extensive density functional theory calculations, including reaction barrier obtained through transition state theory, suggest as-designed triple-atom catalyst (TAC) Ni2Zn/C9N4 enables electrocatalytic production chemicals require multiple coupling, such as urea. can catalyse conversion CO2 NOx coupling precursors, also facilitate between precursors via concurrent N—C—N mechanism. Within mechanism, *CO inserts into *NO-dimerization derived H2N*—*NH2 binds concurrently with two N atoms. The mechanism promotes direct selective NO, whilst competing CO NH3 formations inhibited due unfavorable thermodynamics sluggish kinetics. findings show TAC in electrosynthesis one-step bond synthesis, potential expand sustainable other organonitrogens needs synergistic catalysis.