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Theory-Guided Synthesis of Stable Low-Nuclearity Cluster Catalysts via Atom-Stabilizer Locking
Leilei Wang1, Yuxing Xu1, Chuanqiang Wu2
1State Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Materials Science, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), University of Science and Technology of China, Hefei, Anhui 230026, P. R. China.
Low-nuclearity clusters (LNCs) are unstable for catalysis. Adding atom stabilizers, like Co or Cu, creates robust LNC catalysts with high stability in hydrogen, enabling practical applications.
Area of Science:
- Materials Science
- Catalysis
- Computational Chemistry
Background:
- Low-nuclearity clusters (LNCs) offer high atom utilization and unique electronic properties.
- Their practical application, particularly in heterogeneous catalysis, is limited by thermodynamic instability and high surface free energy.
Purpose of the Study:
- To develop a general synthesis strategy for stabilizing LNCs for catalytic applications.
- To investigate factors influencing LNC stability under hydrogen at elevated temperatures.
Main Methods:
- Computational modeling of single-atom and dimer configurations on nitrogen-doped carbon.
- Experimental verification using atom-by-atom fabrication.
- Testing catalyst stability in hydrogen at temperatures above 400 °C.
Main Results:
- High adsorption energies alone do not prevent LNC aggregation in hydrogen.
- Incorporating atom stabilizers (Co, Cu) that form robust support bonds is crucial for stability.
- Six dimeric and three trimeric LNC catalysts with exceptional stability were synthesized.
Conclusions:
- A theory-guided strategy for synthesizing ultrastable LNC catalysts has been established.
- Atom stabilizers are essential for preventing LNC aggregation in hydrogen-involved catalytic reactions.
- This approach facilitates the rational design of advanced LNC catalysts.
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