Details

Autor(en) / Beteiligte

• Meng, Dong‐Li
• Zhang, Meng‐Di
• Si, Duan‐Hui
• Mao, Min‐Jie
• Hou, Ying
• Huang, Yuan‐Biao
• Cao, Rong

Titel

Highly Selective Tandem Electroreduction of CO2 to Ethylene over Atomically Isolated Nickel–Nitrogen Site/Copper Nanoparticle Catalysts

Ist Teil von

• Angewandte Chemie (International ed.), 2021-11, Vol.60 (48), p.25485-25492

Auflage

International ed. in English

Ort / Verlag

Weinheim: Wiley Subscription Services, Inc

Erscheinungsjahr

2021

Link zum Volltext

Quelle

Wiley Online Library

Beschreibungen/Notizen

• Herein, an effective tandem catalysis strategy is developed to improve the selectivity of the CO2RR towards C2H4 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 CO2RR to produce C2H4. The Faradaic efficiency of C2H4 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 CH4 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 C2H4 on the nearby Cu NP sites. The work offers an effective avenue to design electrocatalysts for the highly selective CO2RR to produce multicarbon products via a tandem route. An effective tandem catalysis strategy is developed to enhance the selectivity of the CO2 electroreduction reaction towards C2H4 with a 6‐fold increase in comparison with that of the non‐tandem catalysts. The local high concentration of CO generated by atomically isolated nickel–nitrogen sites PTF(Ni) sites can facilitate the C−C coupling to form C2H4 on the nearby Cu NP sites, thus switching from CH4 to C2H4 production with a Faradaic efficiency of 57.3 %.