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The electrosynthesis of multi-carbon (C 2+ ) alcohols, specifically ethanol and n-propanol through CO electroreduction (CORR) in H 2 O, presents a sustainable pathway for intermittent renewable energy storage and a low-carbon economy. However, achieving high selectivity for alcohol production at industrial current densities is kinetically hampered by side reactions such as ethylene generation and hydrogen evolution reaction, which result from competing adsorption of *CO and *H. In this study, we developed a Cu/Zn alloy catalyst to simultaneously enhance the activity and selectivity for alcohol production by increasing CO capture capacity and enriching active hydrogen on Cu sites. Our findings demonstrate that the Cu/5Zn alloy with a molar ratio of Cu to Zn of 95 : 5 exhibits a Faradaic efficiency of 50 % for the selective electrosynthesis of C 2+ alcohols during ampere-level CO electrolysis. Mechanistic investigations revealed that the Cu/Zn alloy promotes polarized Cu sites, enhancing CO adsorption while facilitating the spillover of hydrogen atoms from Zn to Cu sites, contributing to selective alcohol formation., (© 2024 Wiley-VCH GmbH.)

Solid-state electrolytes (SSEs) with high ionic conductivity, stability, and interface compatibility are indispensable for high-energy-density and long-life all-solid-state batteries (ASSBs), yet there are scarce SSEs with sufficient ionic conductivity and electrochemical stability. In this study, with a high-entropy SSE (HE-SSE, Li 2.9 In 0.75 Zr 0.1 Sc 0.05 Er 0.05 Y 0.05 Cl 6 ), we show the high configuration entropy has a thermodynamically positive relationship with the high-voltage stability. As a result, the ASSBs with HE-SSE and high-voltage cathode materials exhibit superior high-voltage and long-cycle stability, achieving 250 cycles with 81.4 % capacity retention when charged to 4.8 V (vs. Li + /Li), and even 5000 cycles if charged to 4.6 V (vs. Li + /Li). Experimental characterizations and density functional theory calculations confirm that the HE-SSE greatly suppresses the high-voltage degradation of SSE at the interface, promoting the high-voltage stability coordinately through high entropy and interface stability. The high entropy design offers a general strategy to simultaneously improve the high-voltage stability and ionic conductivity of SSEs, creating an avenue to building high-energy and long-life ASSBs., (© 2024 Wiley-VCH GmbH.)