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Atomic Defects Engineering Boosts Urea Synthesis toward Carbon Dioxide and Nitrate Coelectroreduction.

Zifan Xu1, Zhengwu Yang1, Huan Lu1

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Summary

Creating oxygen vacancies on indium hydroxide nanobelts significantly boosts urea electrosynthesis efficiency. This defect engineering enhances catalytic performance for producing urea, achieving record-high activity.

Keywords:
In(OH)3 nanobeltatomic defect engineeringcarbon dioxide and nitrate utilizationoxygen vacancyurea electrosynthesis

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Catalysis

Background:

  • Atomic defect engineering offers a pathway to tune material properties for enhanced catalytic performance.
  • Surface defects, specifically oxygen vacancies, can alter the chemical behavior of reaction intermediates.

Purpose of the Study:

  • To investigate the impact of oxygen vacancies on the surface of In(OH)3 nanobelts for urea electrosynthesis.
  • To enhance the efficiency and activity of urea electrosynthesis through defect engineering.

Main Methods:

  • Fabrication of In(OH)3 nanobelts with controlled oxygen vacancies.
  • Electrochemical characterization including Faradaic efficiency and partial current density measurements.
  • Density Functional Theory (DFT) calculations to understand reaction mechanisms.
  • In-situ spectroscopy to validate the role of oxygen vacancies.

Main Results:

  • Oxygen vacancies on In(OH)3 nanobelts led to a significant increase in urea Faradaic efficiency (80.1%) compared to pristine materials (20.7%).
  • The modified nanobelts demonstrated a record-high partial current density for urea electrosynthesis (-18.8 mA cm-2 at -0.8 V vs RHE).
  • DFT calculations indicated that unsaturated In sites adjacent to oxygen defects optimize intermediate adsorption and facilitate key reaction steps.
  • In-situ spectroscopy confirmed the promotional effect of oxygen vacancies on urea electrosynthesis.

Conclusions:

  • Oxygen vacancy engineering on In(OH)3 nanobelts is an effective strategy to enhance urea electrosynthesis.
  • The optimized electronic structure and adsorption properties due to oxygen defects are crucial for high catalytic activity.
  • This work provides a promising approach for developing efficient electrocatalysts for urea synthesis.