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Solar-Driven Electrochemical Green Fuel Production from CO2 and Water Using Ti3C2Tx MXene-Supported CuZn and NiCo Catalysts
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Published on: November 7, 2025

Coordination-Engineered Interfacial Pathway Partitioning for Electrocatalytic CO2 Conversion and Downstream

Kangyu Lou1,2, Libin Zeng2,3, Qingshuang Xu2

  • 1China-Uzbekistan Joint Laboratory on Advanced Porous Materials, State Key Laboratory of Bio-based Fiber Materials, School of Materials Science and Engineering, Zhejiang Sci-Tech University, Hangzhou, China.

Angewandte Chemie (International Ed. in English)
|June 9, 2026
PubMed
Summary
This summary is machine-generated.

This study uses tunable Cu-Sn catalysts to control electrochemical CO2 reduction (eCO2RR) pathways, directing synthesis towards formate or CO. This coordination-engineered approach enables efficient downstream product conversion.

Keywords:
CO2 electroreductionC–N couplinghydrogen‐bond networklocal coordination environmentpathway differentiation

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Catalysis
  • Chemical Engineering

Background:

  • Electrochemical CO2 reduction (eCO2RR) shows promise for producing valuable carbon products.
  • Understanding the interfacial factors governing pathway selection in eCO2RR is crucial for catalyst design.
  • Current eCO2RR systems often lack control over product selectivity and downstream processing.

Purpose of the Study:

  • To investigate the role of catalyst coordination environment in controlling eCO2RR pathway selectivity.
  • To elucidate the interfacial mechanisms dictating the formation of formate versus CO.
  • To demonstrate integrated eCO2RR with efficient downstream product upgrading.

Main Methods:

  • Synthesis and characterization of coordination-environment-tunable Cu-Sn catalysts.
  • In situ spectroscopy (e.g., FTIR, Raman) to study adsorbed intermediates and interfacial water.
  • H/D kinetic isotope analysis and in situ electrochemical impedance spectroscopy-distribution of relaxation times (EIS-DRT) to probe reaction kinetics.
  • Density functional theory (DFT) calculations to understand energetic origins of pathway bifurcation.

Main Results:

  • Cu-Sn catalysts effectively partitioned CO2 electrosynthesis between Sn-centered (formate) and Cu-centered (CO) pathways.
  • Coordination environment influenced adsorbed intermediates and interfacial water structures, correlating with pathway selection.
  • DFT calculations revealed energetic differences in adsorption and interfacial energetics based on coordination.
  • Downstream electrodialysis achieved 98.1% HCOOK-to-HCOOH conversion; CO2-NH3 route yielded formamide with 45.2% FE.

Conclusions:

  • Catalyst coordination engineering is a viable strategy for controlling interfacial partitioning in eCO2RR.
  • This approach enables selective synthesis of downstream-compatible carbon products like formate and formamide.
  • Integrated eCO2RR with downstream upgrading offers a pathway for efficient carbon utilization.