Developing efficient systems for the conversion of carbon dioxide to valuable chemicals using solar power is critical for mitigating climate change and ascertaining the world’s future supply of clean fuels. Here, we introduce a mesoscopic cathode consisting of Cu nanowires decorated with Ag islands, by the reduction of Ag-covered Cu2O nanowires prepared via galvanic replacement reaction. This catalyst enables CO2 reduction to ethylene and other C2+ products with a faradaic efficiency of 76%. Operando Raman spectroscopy reveals intermediate formation of CO at Ag sites which undergo subsequent spillover and hydrogenation on the Cu nanowires. Our Cu–Ag bimetallic design enables a ∼95% efficient spillover of intermediates from Ag to Cu, delivering an improved activity toward the formation of ethylene and other C2+ products. We also demonstrate a solar to ethylene conversion efficiency of 4.2% for the photoelectrochemical CO2 reduction using water as electron and proton donor, and solar power together with perovskite photovoltaics to drive the uphill reaction.

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Introduction of inorganic solid electrolytes is believed to be an ultimate strategy to dismiss dendritic Li in high-energy Li-metal batteries (LMBs), and garnet-type Li7La3Zr2O12 (LLZO) electrolytes are impressive candidates. However, the current density for stable Li plating/stripping in LLZO is still quite limited. Here, we create in situ formed Li-deficient shields by the high-temperature calcination at 900 °C. By this novel process, the formation of Li2CO3 on LLZO is restrained, and then we successfully obtain Li2CO3-free LLZO after removing the Li-deficient compounds. Without any surface modification, Li2CO3-free LLZO shows an intrinsic “lithiophilicity” characteristic. The contact angles of metallic Li on LLZO garnets are assessed by the first-principle calculation to confirm the lithiophilicity characteristic of LLZO electrolytes. The wetting of metallic Li on the Li2CO3-free LLZO surface leads to a continuous and tight Li/LLZO interface, resulting in an ultralow interfacial resistance of 49 Ω cm2 and a homogeneous current distribution in the charge/discharge processes of LMBs. Consequently, the current density for the stable Li plating/stripping in LLZO increases to 900 μA cm–2 at 60 °C, one of the highest current density for LMBs based on garnet-type LLZO electrolytes. Our findings not only offer insight into the lithiophilicity characteristics of LLZO electrolytes to suppress dendritic Li at high current densities but also expand the avenue toward high-performance, safe, and long-life energy-storage systems.