Highly Selective Tandem Electroreduction of CO<sub>2</sub> to Ethylene over Atomically Isolated Nickel–Nitrogen Site/Copper Nanoparticle Catalysts
Dongli Meng, Meng‐Di Zhang, Duan‐Hui Si, Min‐Jie Mao, Ying Hou, Yuan‐Biao Huang, Rong Cao
Abstract
Abstract Herein, an effective tandem catalysis strategy is developed to improve the selectivity of the CO 2 RR towards C 2 H 4 by multiple distinct catalytic sites in local vicinity. An earth‐abundant elements‐based tandem electrocatalyst PTF(Ni)/Cu is constructed by uniformly dispersing Cu nanoparticles (NPs) on the porphyrinic triazine framework anchored with atomically isolated nickel–nitrogen sites (PTF(Ni)) for the enhanced CO 2 RR to produce C 2 H 4 . The Faradaic efficiency of C 2 H 4 reaches 57.3 % at −1.1 V versus the reversible hydrogen electrode (RHE), which is about 6 times higher than the non‐tandem catalyst PTF/Cu, which produces CH 4 as the major carbon product. The operando infrared spectroscopy and theoretic density functional theory (DFT) calculations reveal that the local high concentration of CO generated by PTF(Ni) sites can facilitate the C−C coupling to form C 2 H 4 on the nearby Cu NP sites. The work offers an effective avenue to design electrocatalysts for the highly selective CO 2 RR to produce multicarbon products via a tandem route.