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In this paper, Ti/ZnO–Fe 2 O 3 composite derived from Ti/Schiff base intercalated ZnFe layered double hydroxides was used as thin film electrode in CO 2 photoelectroreduction. The influence of molar ratio of Ti/Fe and calcination temperature, which would affect the composites' physicochemical property and the photoelectrocatalytic performance for CO 2 reduction, were investigated in detail. The characterization results from XRD, SEM, TEM, UV-vis and BET showed that Ti/ZnO–Fe 2 O 3 composite with flower–like crystal from had small particle sizes, narrow band gap and excellent textural properties. The final product of CO 2 photoelectroreduction was methanol and the intermediates were formic acid and formaldehyde. The methanol field reached at 0.773 mmol/cm 2 after 3 h reaction with 0.5 V voltage by Ti/ZnO–Fe 2 O 3 composite with Ti/Fe = 1, calcined at 800 °C. In addition, the CO 2 photoelectroreduction pathway and the reason for highly efficient photoelectrocatalytic activity of the composite were also discussed. [ABSTRACT FROM AUTHOR]

Ethylene is particularly attractive due to its major importance as a feedstock for various applications including the polymer industry. As such, catalyst and electrolyzer developments are crucial to achieve industrially relevant ethylene production and efficiency levels. Here, a tandem electrocatalyst composed of copper nanocubes and nickel‐coordinated nitrogen‐doped carbon (NiNC) is presented, which is integrated into gas diffusion electrodes (GDEs) for direct conversion of vapor‐fed CO2 into ethylene. Evaluation of tandem GDEs in the vapor‐fed flow electrolyzer shows significantly increased ethylene selectivity in terms of faradaic efficiency and C2H4/CO ratio compared to a non‐tandem copper GDE. The enhancements are attributed to the increased local CO availability near the copper surface via effective CO2 to CO conversion on neighboring NiNC. The experimental results are validated by 3D resolved continuum simulations, which show increased flux of higher‐order products with the added CO flux from NiNC. The practical viability of Cu/NiNC catalyst is further evaluated in a membrane electrode assembly electrolyzer, achieving 40% FE toward ethylene at 150 mA cm−2 and 3.2 V. These findings highlight the high selectivity and formation rate of ethylene achieved by successful device integration of the Cu/NiNC catalyst, demonstrating the potential for implementation in large‐scale sustainable CO2 electrolyzers. [ABSTRACT FROM AUTHOR]