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Published on: December 6, 2021
An Atomically Precise Ru1Au6(TBBT)6(PPh3)6 Cluster Catalyst for Ammonia Production
Jinzhi Lu1, Chenyang Shen1, Yiqi Tian1
1State Key Laboratory of Coordination Chemistry, Key Laboratory of Mesoscopic Chemistry of Ministry of Education, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, 210093, China.
A new ruthenium-gold cluster catalyst enhances electrocatalytic nitrate reduction. This multi-functional catalyst uses separate sites for water activation and nitrate reduction, boosting efficiency 19-fold.
Area of Science:
- Catalysis
- Materials Science
- Electrochemistry
Background:
- Single-site catalysts struggle with complex reactions requiring multiple steps.
- Multi-functional catalysts with complementary units are needed for efficient multitasking.
- The Au(TBBT)PPh3 complex shows limited efficiency in electrocatalytic nitrate reduction due to dual-role active sites.
Purpose of the Study:
- To design a multi-functional catalyst that decouples water activation and nitrate reduction.
- To improve the efficiency of electrocatalytic nitrate reduction.
- To investigate the cooperative effects in a multi-site catalytic system.
Main Methods:
- Synthesis of a Ru1Au6(TBBT)6(PPh3)6 cluster catalyst.
- Bridging of gold complexes with sulfur atoms.
- Utilizing distinct Ru and Au sites for complementary catalytic functions.
Main Results:
- The Ru site facilitates water dissociation, providing protons.
- The Au sites sequentially reduce nitrate.
- Proton hopping from Ru to Au over sulfur bridges enhances catalytic activity.
- A 19-fold increase in efficiency was observed compared to the single-complex catalyst.
Conclusions:
- The Ru1Au6 cluster effectively separates catalytic roles, enhancing nitrate electroreduction.
- Proton transfer dynamics between Ru and Au sites are crucial for high efficiency.
- This work demonstrates a strategy for designing cooperative multi-site catalysts.
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