Composition optimization of liquid Ga support for uniform Cu dispersion with sustainable electroreduction of CO2 to CH4
摘要
Liquid metals (LMs) have been regarded as a promising system for designing advanced catalysts due to their unique inherent and interfacial properties. However, the migration and aggregation of active metal species during long-term operation lead to a severe performance degradation. Herein, we report a composition optimization strategy for fabricating a Ga-In eutectic LM support and reducing the surface energy. Then, a homogeneous incorporation of Cu species into the liquid GaIn support has been achieved (named GaIn-Cu) and confirmed by comprehensive high-resolution characterizations. Compared with pristine Ga LMs, the as-synthesized GaIn eutectic LMs enable a continuous and uniform dispersion of Cu active sites, thus effectively inhibiting the migration and formation of CuGa2 intermetallic phases during CO2 electroreduction reaction (CO2RR). As a result, the GaIn-10-Cu catalyst achieved a maximum CH4 Faradaic efficiency of 73.49% at −0.8 Vvs. RHE, which is significantly higher than that of Ga-Cu (61.49%). Moreover, the GaIn-10-Cu catalyst showed a significantly enhanced stability for the CH4 generation over 40 h of continuous operation. In-situ spectroscopic studies revealed that the GaIn-10-Cu catalyst favored the formation and protonation of key *CHO and *OCH3 intermediates, steering the reaction selectively toward CH4. This work demonstrates that tuning the compositional property of LMs can significantly modulate the performance of catalytic sites, and also provides a promising strategy for developing highly durable and selective LM-based materials for electrocatalysis.