Revolutionizing CO₂ Electrolysis: Fluent Gas Transportation within Hydrophobic Porous Cu₂O

Abstract

The success of electrochemical CO2 reduction at high current densities hinges on precise interfacial transportation and the local concentration of gaseous CO2. However, the creation of efficient CO2 transportation channels remains an unexplored frontier. In this study, we design and synthesize hydrophobic porous Cu2O spheres with varying pore sizes to unveil the nanoporous channel’s impact on gas transfer and triple-phase interfaces. The hydrophobic channels not only facilitate rapid CO2 transportation but also trap compressed CO2 bubbles to form abundant and stable triple-phase interfaces, which are crucial for high-current-density electrocatalysis. In CO2 electrolysis, in situ spectroscopy and density functional theory results reveal that atomic edges of concave surfaces promote C–C coupling via an energetically favorable OC-COH pathway, leading to overwhelming CO2-to-C2+ conversion. Leveraging optimal gas transportation and active site exposure, the hydrophobic porous Cu2O with a 240 nm pore size (P-Cu2O-240) stands out among all the samples and exhibits the best CO2-to-C2+ productivity with remarkable Faradaic efficiency and formation rate up to 75.3 ± 3.1% and 2518.2 ± 8.1 μmol h–1 cm–2, respectively. This study introduces a novel paradigm for efficient electrocatalysts that concurrently addresses active site design and gas-transfer challenges.

Customized CO2 electroreduction to methane or ethylene by manipulating *H and *CO adsorption on Cu/CeOx catalysts

“…57 In addition, a distinct *CHO peak, key intermediate for CH 4 , was further found at 1226 cm −1 . 58 In contrast, in the Cu/CuCeO x spectrum, the characteristic peak of *CHO is significantly weakened and replaced by *COCHO at 1550 and 1185 cm −1 , 59–62 indicating that Cu/CuCeO x catalysts are more inclined to produce C 2 , which is consistent with the results calculated by DFT.…”

Constructing Favorable Microenvironment on Copper Grain Boundaries for CO2 Electro-conversion to Multicarbon Products

“…Storing intermittent sustainable energy in valuable chemicals and fuels offers a promising approach to alleviating energy dilemmas while closing anthropogenic carbon cycles. Among various technologies, the electrochemical carbon dioxide reduction reaction (eCO 2 RR) stands out due to its moderate operational conditions and the diversity of products. − Compared with C 1 compounds, developing efficient electrocatalysts that achieve high selectivity for multicarbon (C 2+ ) product is particularly attractive, as these compounds hold greater economic value and market demand. − However, the eCO 2 RR involves multiple proton-coupled electron transfer steps, which generate sophisticated intermediates and overlapping reaction pathways, making the corresponding reaction mechanisms elusive. , To date, copper-based materials probably are recognized for their unique ability to favor the formation of C 2+ products, primarily due to the optimal binding energy with reaction intermediates. − Nonetheless, conventional bulk polycrystalline Cu catalysts still suffers from sluggish reaction kinetics and unsatisfactory C 2+ selectivity …”