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Low-Temperature Initiation Enhances HCN and NH3 Formation From Methane and NO Over Pt/Al2O3.
Emika Yamashita1, Kyoko K Bando2, Toshitaka Kubo3
1Department of Chemistry and Life Science, Graduate School of Engineering Science, Yokohama National University, Yokohama, Japan.
Low-temperature methane activation for hydrogen cyanide (HCN) synthesis is improved by optimizing nitrogen monoxide (NO) concentration and temperature. Dynamic control of surface intermediates, like Pt-CO, enhances HCN and ammonia (NH3) yield.
Area of Science:
- Catalysis
- Chemical Engineering
- Materials Science
Background:
- Methane (CH4) activation at low temperatures is difficult due to its strong C-H bond.
- Hydrogen cyanide (HCN) synthesis from methane offers a promising route under milder conditions.
Purpose of the Study:
- Investigate HCN and ammonia (NH3) formation from CH4 and NO over a Pt/Al2O3 catalyst.
- Determine the impact of NO concentration, temperature, and reaction-start conditions on HCN synthesis.
Main Methods:
- Utilized a commercial Pt/Al2O3 catalyst for methane and nitrogen monoxide reactions.
- Employed in situ Fourier Transform Infrared (FTIR) spectroscopy and dispersive X-ray absorption fine structure (DXAFS) analysis.
- Compared ramping versus constant-temperature reaction conditions and implemented temperature-swing operation.
Main Results:
- Increased NO concentration up to 4.5% enhanced HCN production to a 3.5% carbon-based yield.
- Optimal HCN yield of 4.8% was achieved at 475°C.
- Ramping the temperature from 300°C significantly boosted CH4 conversion and HCN formation.
- Pt-CO correlated positively with HCN production, while Pt-CN acted as an inhibitor.
- Temperature-swing operation improved HCN and NH3 yields by promoting desorption of inhibiting species.
Conclusions:
- Dynamic control of surface intermediates is crucial for enhancing low-temperature HCN synthesis.
- Optimizing NO concentration, temperature, and reaction profiles improves catalyst performance.
- Understanding surface species dynamics (e.g., Pt-CO, Pt-CN) is key to catalyst design and process optimization.
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