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Multiscale Sampling of a Heterogeneous Water/Metal Catalyst Interface using Density Functional Theory and Force-Field Molecular Dynamics
Published on: April 12, 2019
Quantitative Active Hydrogen Modulation via Mastering Interfacial Water Over Single Rare Earth Atom on Copper for NO3
Yu-Cheng Liu1, Haolin Lu2, Xue-Zhi Song1
1School of Chemical Engineering, Ocean and Life Sciences, Dalian University of Technology, Panjin, China.
Angewandte Chemie (International Ed. in English)
|July 7, 2026
Summary
Engineered single-atom catalysts (CuYbSA@C, CuLaSA@C) enhance electrochemical nitrate reduction to ammonia by precisely controlling active hydrogen (H*). This breakthrough optimizes H* generation and utilization for sustainable ammonia synthesis.
Area of Science:
- Electrochemistry
- Catalysis
- Materials Science
- Sustainable Chemistry
Background:
- Electrochemical nitrate reduction to ammonia (NH3) is a sustainable synthesis route.
- Active hydrogen (H*) is crucial for NH3 synthesis, but its modulation and atomic-scale impact are poorly understood.
- Current catalyst design often focuses on active sites, neglecting the quantitative role of H*.
Purpose of the Study:
- To engineer single-atom catalysts for efficient nitrate-to-ammonia conversion.
- To quantitatively investigate the role of active hydrogen (H*) in the electrochemical reduction process.
- To establish a new paradigm for catalyst design based on H* spatiotemporal distribution and utilization.
Main Methods:
- Synthesis of single-atom rare earth catalysts in a copper matrix encapsulated within carbon (CuYbSA@C and CuLaSA@C).
- In situ Raman spectroscopy to study interfacial water structure and H* generation.
- Electrochemical measurements to assess catalytic performance (NH3 yield rate, Faradaic efficiency).
- Ab initio molecular dynamics simulations to elucidate reaction mechanisms and H* utilization.
Main Results:
- Isolated rare earth atoms (e.g., Yb, La) modulate interfacial water to promote H* generation and utilization.
- A quantitative positive correlation was found between interfacial K·H2O population, H* utilization, and catalytic performance.
- CuYbSA@C achieved an exceptional NH3 yield rate of 39.75 ± 1.03 mg·h-1·mgcat -1 and 94.5 ± 2.46% FE at -0.6 V vs. RHE.
- A tandem dual-site mechanism involving Yb single atoms and Cu sites was elucidated.
Conclusions:
- Single-atom rare earth catalysts effectively control interfacial water and H* for enhanced nitrate-to-ammonia conversion.
- This work establishes a quantitative H* concept for catalyst design, prioritizing its distribution and utilization.
- The findings shift the focus from active-site-centric design to a more comprehensive understanding of reaction intermediates.
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