In situ investigation of decomposing ammonia and ammonobasic solutions under supercritical conditions via UV/vis and Raman Spectroscopy

Autor: Thomas G. Steigerwald, Johannes Balouschek, Eberhard Schluecker, Anna-Carina L. Kimmel, Nicolas S. A. Alt, Benjamin Hertweck
Rok vydání: 2018
Předmět:
Zdroj: The Journal of Supercritical Fluids. 134:96-105
ISSN: 0896-8446
Popis: An optical cell was used in this work, which allows spectroscopic measurements of fluids up to 600 °C and 300 MPa. The maximum pressure reached in this work was 254 MPa and the internal cell temperature was a maximum of 563 °C at a heating temperature of 617 °C. In the following, a combination of Raman and UV/vis spectroscopy was used for in situ investigation of the breakdown of sodium azide above 300 °C combined with the formation of sodium amide. It was verified that the breakdown of NaN3 occurs before the formation of NaNH2 starts. In a second step the decomposition of supercritical ammonia under ammonothermal conditions was investigated solely via Raman spectroscopy. The study comprises four different fluid compositions: pure ammonia, ammonia with a ruthenium catalyst, ammonia and mineralizer (sodium azide) and last ammonia, mineralizer and gallium nitride (GaN). By this, it was possible to proof that with pure ammonia and without a proper catalyst the decomposition of ammonia stops quite far before chemical equilibrium is reached.
Databáze: OpenAIRE