TY - JOUR
T1 - Reduction of supported GaN and its application in methane conversion
AU - Trangwachirachai, K.
AU - Huang, A. L.
AU - Chen, H. K.
AU - Chen, C. L.
AU - Lee, J. F.
AU - Tian, H. K.
AU - Lin, Y. C.
N1 - Funding Information:
This study was supported by the National Science and Technology Council (Projects 109-2628-E-006-011-MY3 , 110-2221-E-006-165-MY3 , 110-2923-E-006-005-MY3 , 110-2222-E-006-014-MY3, and 110-2927-I-006-506 ) and by Higher Education Sprout Project, Ministry of Education to the Headquarters of University Advancement at National Cheng Kung University (NCKU). The authors thank the National Center for High-performance Computing (NCHC) for providing computational and storage resources. The authors also appreciate the use of Electron Spectroscopy for Chemical Analysis (ESCA00001006) belonging to the Precious Instrument Utilization Center at National Central University (NCU). The authors also acknowledge the support from the Hierarchical Green Energy Materials (Hi-GEM) Research Center at NCKU.
Funding Information:
This study was supported by the National Science and Technology Council (Projects 109-2628-E-006-011-MY3, 110-2221-E-006-165-MY3, 110-2923-E-006-005-MY3, 110-2222-E-006-014-MY3, and 110-2927-I-006-506) and by Higher Education Sprout Project, Ministry of Education to the Headquarters of University Advancement at National Cheng Kung University (NCKU). The authors thank the National Center for High-performance Computing (NCHC) for providing computational and storage resources. The authors also appreciate the use of Electron Spectroscopy for Chemical Analysis (ESCA00001006) belonging to the Precious Instrument Utilization Center at National Central University (NCU). The authors also acknowledge the support from the Hierarchical Green Energy Materials (Hi-GEM) Research Center at NCKU.
Publisher Copyright:
© 2023 Elsevier Ltd
PY - 2023/6
Y1 - 2023/6
N2 - The reduction of supported GaN using amorphous SiO2, silicalite-1 (S1), and HZSM-5 (HZ) as the carriers was investigated and tested for methane conversion to acetonitrile (ACN). Ammonia nitridation was used to synthesize GaN samples. The highest ammonia and ACN productivities (433 and 383 μmol/g, respectively) were obtained by using 5 wt% GaN on HZ (5GaN/HZ). The N–Ga interaction of 5GaN/HZ was discovered to be weakened due to the presence of a neighboring Brønsted acid. The oxidation state of gallium was reduced during methane conversion, implying the loss of nitrogen from GaN. The decreased activity could be rejuvenated by a renitridation step. The GaN surface structures, including the adsorption surface, 11¯0, and the side surfaces, (001), (110), (111), and 111¯, were calculated via first-principles calculations. Among them, the (001) side surface of GaN was likely to be the origin of mobile nitrogen, which is important in the conversion of methane to ACN.
AB - The reduction of supported GaN using amorphous SiO2, silicalite-1 (S1), and HZSM-5 (HZ) as the carriers was investigated and tested for methane conversion to acetonitrile (ACN). Ammonia nitridation was used to synthesize GaN samples. The highest ammonia and ACN productivities (433 and 383 μmol/g, respectively) were obtained by using 5 wt% GaN on HZ (5GaN/HZ). The N–Ga interaction of 5GaN/HZ was discovered to be weakened due to the presence of a neighboring Brønsted acid. The oxidation state of gallium was reduced during methane conversion, implying the loss of nitrogen from GaN. The decreased activity could be rejuvenated by a renitridation step. The GaN surface structures, including the adsorption surface, 11¯0, and the side surfaces, (001), (110), (111), and 111¯, were calculated via first-principles calculations. Among them, the (001) side surface of GaN was likely to be the origin of mobile nitrogen, which is important in the conversion of methane to ACN.
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U2 - 10.1016/j.mtchem.2023.101500
DO - 10.1016/j.mtchem.2023.101500
M3 - Article
AN - SCOPUS:85151546753
SN - 2468-5194
VL - 30
JO - Materials Today Chemistry
JF - Materials Today Chemistry
M1 - 101500
ER -