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Nanoconfinement Engineering over Hollow Multi-Shell Structured Copper towards Efficient Electrocatalytical C-C

Chunxiao Liu1, Menglu Zhang1, Jiawei Li1

  • 1Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, National Synchrotron Radiation Laboratory, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.

Angewandte Chemie (International Ed. in English)
|November 25, 2021
PubMed
Summary

Nanoconfinement in copper oxide hollow multi-shell structures enhances electrocatalytic carbon-carbon coupling for CO2 reduction. More shells improve selectivity for C2+ products, offering insights for catalyst design.

Keywords:
CO2 electroreductionC−C couplingDiffusion kineticsNanoconfinement

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Nanotechnology

Background:

  • Electrocatalytic C-C coupling is crucial for converting CO2 into valuable products.
  • Nanoconfinement strategies can enhance reaction kinetics and selectivity.
  • Developing efficient catalysts for CO2 electroreduction (CO2 RR) remains a significant challenge.

Purpose of the Study:

  • To investigate the effect of nanoconfinement in copper oxide hollow multi-shell structures (HoMSs) on electrocatalytic C-C coupling.
  • To optimize catalyst design for improved selectivity towards C2+ products in CO2 RR.
  • To elucidate the mechanistic role of nanoconfinement in enhancing carbon dimerization.

Main Methods:

  • Synthesis of Cu2O HoMSs with tunable shell numbers via Ostwald ripening.
  • Finite-element method (FEM) simulations to guide catalyst design.
  • Electrochemical CO2 reduction experiments in a neutral electrolyte.
  • In situ mechanistic studies to understand the confinement effect.

Main Results:

  • Cu HoMSs demonstrated a positive correlation between shell numbers and C2+ product selectivity.
  • Achieved a maximum C2+ Faradaic efficiency of 77.0±0.3% at 513.7±0.7 mA cm−2.
  • Mechanistic studies revealed enhanced CO adsorbate coverage due to shell superposition, promoting dimerization.

Conclusions:

  • Cu HoMSs effectively utilize nanoconfinement to promote electrocatalytic C-C coupling for CO2 RR.
  • Tunable shell numbers in HoMSs offer a pathway to optimize catalyst performance.
  • This work provides fundamental insights for designing advanced C-C coupling catalysts.