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Boosting Selective Nitrogen Reduction via Geometric Coordination Engineering on Single-Tungsten-Atom Catalysts.

Yu Gu¹, Baojuan Xi¹, Wenzhi Tian¹

¹Key Laboratory of Colloid and Interface Chemistry, Ministry of Education, School of Chemistry and Chemical Engineering, State Key Laboratory of Crystal Materials, Shandong University, Jinan, 250100, P. R. China.

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|May 17, 2021

Summary

This study introduces novel tungsten single-atom catalysts (W SACs) with dual nitrogen and oxygen coordination. These catalysts demonstrate high efficiency for the electrochemical nitrogen reduction reaction (NRR) by optimizing intermediate binding energies.

Keywords:

coordination chemistry high loading nitrogen reduction reaction single tungsten atoms single-atom catalysts

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Area of Science:

Materials Science
Catalysis
Electrochemistry

Background:

Optimizing single-atom catalysts (SACs) performance relies on atomic interface regulation.
Understanding the structure-property correlation in SACs requires precise control over the coordination chemistry of individual atoms.

Purpose of the Study:

To develop and characterize a new class of tungsten single-atom catalysts (W SACs) with dual nitrogen and oxygen coordination.
To investigate the structure-property relationship for enhanced electrochemical nitrogen reduction reaction (NRR) performance.

Main Methods:

Facile synthesis of W SACs with high metal loading (>10 wt%) using an oxygen-bridged [WO4] tetrahedron precursor.
Characterization using high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), X-ray photoelectron spectroscopy (XPS), and extended X-ray absorption fine structure (EXAFS).
Electrochemical evaluation for the nitrogen reduction reaction (NRR) and density functional theory (DFT) calculations.

Main Results:

Successfully prepared W SACs with well-defined W-N/O coordination environments.
The W-NO/NC catalyst exhibited excellent selectivity and activity for the electrochemical NRR.
DFT calculations confirmed that the dual N and O coordination optimizes the binding energy of NRR intermediates.

Conclusions:

The developed W SACs with dual N and O coordination offer a promising strategy for efficient electrocatalytic NRR.
This work highlights the critical role of coordination chemistry in tuning SACs' properties.
Opens new avenues for designing advanced catalysts based on coordination structure-property correlations.