Interplay of [C <sub>60</sub> ]Fullerene and Cu <sub>2</sub> O Nanocrystals for Stable CO <sub>2</sub> Electroreduction to C <sub>2+</sub> Products
Na Chen, Xuantao Deng, Zuo‐Chang Chen, Peng Du, Xu‐Feng Liu, Jia Liu, Bilyu Hong, Ruixuan Qin, Jianwei Zheng, Jun Li, Su‐Yuan Xie, Youzhu Yuan
Abstract
High Resolution Image Download MS PowerPoint Slide Copper oxides such as Cu 2 O are promising catalysts for the electrochemical CO 2 reduction reaction (CO 2 RR) to C 2+ products, yet their intrinsic susceptibility to Cu + reduction and morphology degradation severely limits their long-term performance. Herein, we report a facile two-step wet-chemical route to interface [C 60 ]fullerene with cubic Cu 2 O ( c -Cu 2 O), octahedral ( o -Cu 2 O), and dodecahedral ( d -Cu 2 O) crystals. The resulting composite optimal c -Cu 2 O–C 60 achieves substantial Faradaic efficiencies of 60.4% in an H-cell and 65.6% in a flow-cell for C 2+ products, which is 3-fold higher than pristine c -Cu 2 O, while maintaining stable operation for 100 h at –1.2 V versus RHE without detectable activity loss. Our experimental results and theoretical study demonstrate that the strategic incorporation of C 60 during the synthesis of Cu 2 O directly endows the surfaces of the resultant Cu 2 O crystals with abundant Cu + /Cu 0 grain boundaries. Additionally, the presence of C 60 induces the formation of more Cu + /Cu 0 boundaries during the CO 2 RR process, which synergistically facilitate the generation of C 2+ products. Moreover, C 60 acts as an electron buffer, preventing Cu + from being over-reduced during the reduction process, thereby sustaining active Cu + /Cu 0 interfaces and maintaining the catalytic activity for C 2+ products. Extension to hydroxylated and fluorinated fullerene derivatives delivers comparable C 2+ selectivity, underscoring the generality of this fullerene-mediated stabilization strategy for designing robust Cu-based CO 2 RR catalysts.