N and OH-Immobilized Cu 3 Clusters In Situ Reconstructed from Single-Metal Sites for Efficient CO 2 Electromethanation in Bicontinuous Mesochannels

Cu-based catalysts hold promise for electrifying CO2 to produce methane, an extensively used fuel. However, the activity and selectivity remain insufficient due to the lack of catalyst design principles to steer complex CO2 reduction pathways. Herein, we develop a concept to design carbon-supported Cu catalysts by regulating Cu active sites’ atomic-scale structures and engineering the carbon support’s mesoscale architecture. This aims to provide a favorable local reaction microenvironment for a selective CO2 reduction pathway to methane. In situ X-ray absorption and Raman spectroscopy analyses reveal the dynamic reconstruction of nitrogen and hydroxyl-immobilized Cu3 (N,OH-Cu3) clusters derived from atomically…

• NS
  National Science Foundation

  Awards: CBET-2223467, DMR 1905572, 1804326, CBET-1804326, 1905572
• UD
  U.S. Department of Energy

  Award: AC02-06CH11357
• NN
  National Natural Science Foundation of China

  Awards: No. AC02-06CH11357, 22071195
• NS
  Natural Science Foundation of Chongqing

  Award: CSTB2023NSCQ-MSX0429
• FR
  Fundamental Research Funds for the Central Universities
• DO
  Division of Materials Research

  Awards: DMR 1905572, 1905572
• DO
  Division of Chemical, Bioengineering, Environmental, and Transport Systems

  Awards: CBET-1804326, 1804326