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Carbon-dioxide Fixation01:28

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Carbon dioxide fixation in prokaryotes enables the assimilation of inorganic carbon into organic molecules, supporting biosynthetic pathways, sustaining ecosystems, and contributing to the global carbon cycle. It also has industrial applications in carbon capture and bioproduct synthesis. Autotrophic organisms rely on this process to utilize CO₂ as a carbon source in diverse environments.The Calvin CycleThe Calvin cycle is the most widespread carbon fixation mechanism, primarily used by...
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Enhancing Local CO2 Adsorption by L-histidine Incorporation for Selective Formate Production Over the Wide Potential

Yicheng Li1, Ernest Pahuyo Delmo2, Guoyu Hou1

  • 1School of Mechanical and Power Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai, 200237, China.

Angewandte Chemie (International Ed. in English)
|October 19, 2023
PubMed
Summary
This summary is machine-generated.

This study introduces bismuth-based (BH) catalysts modified with L-histidine for efficient electrochemical carbon dioxide reduction (CO2 RR). The new catalyst achieves high selectivity and activity over a wide potential range, offering a promising solution for CO2 conversion.

Keywords:
Bismuth-Based CatalystCO2 AdsorptionCO2 ReductionElectrocatalysisFormate

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Catalysis
  • Environmental Science

Background:

  • Electrochemical carbon dioxide reduction reaction (CO2 RR) is crucial for mitigating climate change and energy demands.
  • A key challenge in CO2 RR is balancing high Faradaic efficiency (FE) and current densities across a broad potential range.
  • Bismuth-based (BH) catalysts are explored for CO2 RR, but their performance often faces limitations in selectivity and activity.

Purpose of the Study:

  • To develop an effective strategy for enhancing the selectivity and activity of bismuth-based catalysts for CO2 RR.
  • To overcome the inherent trade-off between activity and selectivity in electrochemical CO2 reduction.
  • To investigate the role of L-histidine in modifying bismuth-based catalysts for improved CO2 RR performance.

Main Methods:

  • Synthesis and characterization of L-histidine-modified bismuth-based (BH) catalysts.
  • Electrochemical evaluation of CO2 RR performance, including Faradaic efficiency (FE) and current densities.
  • In situ ultraviolet-visible (UV-Vis) spectroscopy to study reaction mechanisms and onset potentials.
  • Long-term stability tests under various CO2 concentrations and potentials.

Main Results:

  • The L-histidine-modified BH catalyst demonstrated excellent FEformate (>90% within -0.1–1.8 V and >95% within -0.2–1.6 V vs. RHE).
  • High CO2 RR performance was maintained even with low-concentration CO2 feeding (20 vol.%).
  • An exceptionally low onset potential of -0.05 V RHE was observed, close to the theoretical value.
  • Stable operation exceeding 50 hours was achieved with a preserved FEformate of ~95% and a partial current density of 326.2 mA cm−2 at -1.0 V RHE.

Conclusions:

  • Incorporating L-histidine with bismuth-based catalysts is an effective strategy to enhance CO2 adsorption and electron richness, improving CO2 RR.
  • The modified BH catalyst overcomes the activity-selectivity trade-off, showing superior performance over a wide potential window.
  • This approach offers a promising pathway for practical applications of electrochemical CO2 conversion into valuable chemicals.