摘要
Rational design of catalytic interfaces at the atomic level is crucial for enhancing electrocatalytic CO_(2)reduction.In this study,a Zeolite imidazolate frameworks-8 derived catalyst is developed,featuring atomically dispersed Ni–Zn dual-atom sites(NiZnN_(6))coexisting with Ni_(3)ZnC_(0.7) nanoparticles on nitrogen-doped carbon nanotubes.Strong interaction between the NiZnN_(6) moieties and Ni_(3)ZnC_(0.7) nanoparticle induces charge redistribution,enhancing the electron-donating ability of Ni active sites.Simultaneously,the dual-atom configuration creates an asymmetric electronic environment,where interfacial electronic coupling facilitates partial electron transfer from Zn to Ni,leading to electron enrichment at the Ni center.Consequently,Ni sites preferentially donate electrons to active CO_(2)molecules,lowering the ^(*)COOH formation energy,while Zn sites promote ^(*)CO desorption,thus achieving high CO selectivity(99.6%@-0.7V vs.Reversible Hydrogen Electrode(RHE)).The in-depth investigation in this work provides guidance for establishing the relationship between structure and electrocatalytic activity,holding significant implications for fundamental research on the CO_(2)reduction mechanism.
基金
the financial support from the Natural Science Foundation of Shanghai(24ZR1453900)
Project for AI-Driven Reform of Research Paradigms to Empower Advancement of Disciplines(Z-2024-369-036)。
