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Electron Injection From B4C to Sn Sites Optimizes *OOH Adsorption Enabling Efficient H2O2 Electrosynthesis
Haochong Zhong1, Jinglei Si1, Yuanan Li1
1State Key Laboratory of Green Chemical Synthesis and Conversion, Zhejiang Key Laboratory of Surface and Interface Science and Engineering for Catalysts, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, People's Republic of China.
A new tin/boron carbide (Sn/B4C) composite catalyst efficiently produces hydrogen peroxide (H2O2) via a two-electron oxygen reduction reaction (2e- ORR). This sustainable catalyst shows high selectivity and stability, enabling effective microbial disinfection.
Area of Science:
- Materials Science
- Electrochemistry
- Catalysis
Background:
- Developing efficient non-precious metal electrocatalysts is crucial for sustainable hydrogen peroxide (H2O2) electrosynthesis.
- The two-electron oxygen reduction reaction (2e- ORR) pathway is key for selective H2O2 production.
Purpose of the Study:
- To construct and evaluate a novel Sn/B4C composite catalyst for efficient and selective H2O2 electrosynthesis.
- To investigate the catalytic mechanism and long-term stability of the Sn/B4C catalyst.
- To demonstrate the practical application of in situ generated H2O2 for microbial disinfection.
Main Methods:
- Low-temperature pyrolysis under a hydrogen atmosphere to synthesize the Sn/B4C composite catalyst.
- Rotating disk electrode (RRDE) measurements to assess H2O2 selectivity and Faradaic efficiency.
- Operando X-ray Photoelectron Spectroscopy (XPS) and in situ Attenuated Total Reflection Surface-Enhanced Infrared Reflection Absorption Spectroscopy (ATR-SEIRAS) for mechanistic studies.
- Density Functional Theory (DFT) calculations to understand the electronic structure and reaction pathways.
- Continuous operation in a neutral flow cell and microbial inactivation tests.
Main Results:
- The optimized Sn/B4C-3 catalyst achieved high H2O2 selectivity (93.69% in KOH, 91.9% in Na2SO4) and a production rate of 13.33 mol gcat-1 h-1 with 91.38% Faradaic efficiency in a flow cell.
- The catalyst demonstrated excellent stability, operating continuously for 130 hours.
- Mechanistic studies revealed that electron transfer from B4C to Sn creates electron-rich Sn centers that optimize the adsorption of the *OOH intermediate, facilitating the 2e- ORR pathway.
- In situ generated H2O2 effectively inactivated E. coli and S. griseus with 99% sterilization efficiency within 40 minutes.
Conclusions:
- The Sn/B4C composite catalyst, designed via metal-carbide synergy, offers a promising pathway for sustainable H2O2 production.
- The catalyst's performance is attributed to modulated electronic properties of Sn centers, enhancing the 2e- ORR selectivity.
- This work provides a new design strategy for electrocatalysts and highlights the potential of electrogenerated H2O2 for disinfection applications.
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