Nickel polyphthalocyanine with electronic localization at the nickel site for enhanced CO2 reduction reaction

Chen, Kejun; Cao, Maoqi; Ni, Ganghai; Chen, Shanyong; Liao, Hanxiao; Zhu, Li; Li, Hongmei; Fu, Junwei; Hu, Junhua; Cortes, Emiliano und Liu, Min (2022): Nickel polyphthalocyanine with electronic localization at the nickel site for enhanced CO2 reduction reaction. In: Applied Catalysis B: Environmental, Bd. 306, 121093

Abstract

Nickel phthalocyanine (NiPc) can be at first glance a compelling catalyst for CO2 reduction reaction (CO2RR) because of its Ni-N-4 site. Unfortunately, the pristine NiPc possesses a low catalytic activity resulting from the poor CO2 adsorption and activation capabilities of the electron-deficiency Ni site. Herein, we develop nickel polyphthalocyanine (NiPPc) with extended conjugation to tailor the electronic density at the Ni active site. The enlarged p conjugation of NiPPc evokes the d-electrons localization, increasing the electronic density at the Ni site, which enhances its CO2 adsorption and activation. Consequently, NiPPc supported on carbon nanotubes (NiPPc/CNT) in a flow cell delivers an excellent activity of 300 mA cm(-2) for CO2RR with the CO selectivity of 99.8%, which is much higher than that of NiPc dispersed on carbon nanotubes. NiPPc/CNT exhibits an outstanding stability for CO2RR of more than 30 h at a current density of 100 mA cm(-2) with an ultrahigh selectivity for CO, exceeding 99.7%. This work showcases a new way of tuning the electronic density of catalytic sites.

• Dokumententyp: Zeitschriftenartikel
• Fakultät: Physik
• Themengebiete: 500 Naturwissenschaften und Mathematik > 530 Physik
• ISSN: 0926-3373
• Sprache: Englisch
• DFG: Gefördert durch die Deutsche Forschungsgemeinschaft (DFG) - 390776260