Rational Modulation of Single Atom Coordination Microenvironments in a BCN Monolayer for Multifunctional...

Area of Science:

• Materials Science
• Catalysis
• Computational Chemistry

Background:

• Single-atom catalysts (SACs) exhibit high performance in electrocatalysis.
• Controlling the coordination microenvironment of active sites is crucial for optimizing SACs.
• Existing nanocarbon platforms offer limited coordination diversity.

Purpose of the Study:

• To systematically investigate the impact of diverse coordination microenvironments on single-atom catalyst performance.
• To explore the potential of boroncarbon-nitride (BCN) monolayers as a versatile platform for SACs.
• To identify structure-property relationships for designing efficient BCN-based SACs.

Main Methods:

• High-throughput density functional theory (DFT) calculations were employed.
• Investigated 400 transition metal-BCN moieties with varying coordination environments.
• Evaluated structural stability, electrochemical properties, catalytic activity, and selectivity.

Main Results:

• Discovered that specific single-atom coordination environments in BCN monolayers significantly enhance stability and selectivity.
• Identified unique coordination possibilities offered by the ternary BCN structure compared to binary systems.
• Developed a universal descriptor to guide the experimental synthesis of BCN-SACs.

Conclusions:

• The coordination microenvironment is a critical factor in tuning the performance of single-atom catalysts.
• BCN monolayers provide a promising and tunable platform for developing highly efficient and selective SACs.
• The findings offer valuable guidance for rational catalyst design and accelerate experimental discovery.