<p>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 CuGa<sub>2</sub> intermetallic phases during CO<sub>2</sub> electroreduction reaction (CO<sub>2</sub>RR). As a result, the GaIn-10-Cu catalyst achieved a maximum CH<sub>4</sub> Faradaic efficiency of 73.49% at −0.8 V<sub>vs. RHE</sub>, which is significantly higher than that of Ga-Cu (61.49%). Moreover, the GaIn-10-Cu catalyst showed a significantly enhanced stability for the CH<sub>4</sub> generation over 40 h of continuous operation. <i>In-situ</i> spectroscopic studies revealed that the GaIn-10-Cu catalyst favored the formation and protonation of key *CHO and *OCH<sub>3</sub> intermediates, steering the reaction selectively toward CH<sub>4</sub>. 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.</p>

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Composition optimization of liquid Ga support for uniform Cu dispersion with sustainable electroreduction of CO2 to CH4

  • Chen Zhang,
  • Yixiao Zou,
  • Jiajun Wang,
  • Zanyu Chen,
  • Wenda Chen,
  • Peng Cui,
  • Jinfeng Zhang,
  • Jing Mao,
  • Jia Ding,
  • Xiaopeng Han,
  • Wenbin Hu

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.