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Photochemical Acceleration of Ammonia Production by Pt1-Ptn-TiN Reduction and N2 Activation.
Mao, Chengliang; Wang, Jiaxian; Zou, Yunjie; Shi, Yanbiao; Viasus, Camilo J; Loh, Joel Y Y; Xia, Meikun; Ji, Shufang; Li, Meiqi; Shang, Huan; Ghoussoub, Mireille; Xu, Yang-Fan; Ye, Jessica; Li, Zhilin; Kherani, Nazir P; Zheng, Lirong; Liu, Yanjiang; Zhang, Lizhi; Ozin, Geoffrey A.
Afiliación
  • Mao C; Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, P. R. China.
  • Wang J; Materials Chemistry and Nanochemistry Research Group, Solar Fuels Cluster, Department of Chemistry, University of Toronto, Toronto, Ontario M5S 3H6, Canada.
  • Zou Y; School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, China.
  • Shi Y; Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, P. R. China.
  • Viasus CJ; School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, China.
  • Loh JYY; Materials Chemistry and Nanochemistry Research Group, Solar Fuels Cluster, Department of Chemistry, University of Toronto, Toronto, Ontario M5S 3H6, Canada.
  • Xia M; Department of Materials Science and Engineering, University of Toronto, Toronto, Ontario M5S 3E4, Canada.
  • Ji S; Materials Chemistry and Nanochemistry Research Group, Solar Fuels Cluster, Department of Chemistry, University of Toronto, Toronto, Ontario M5S 3H6, Canada.
  • Li M; Materials Chemistry and Nanochemistry Research Group, Solar Fuels Cluster, Department of Chemistry, University of Toronto, Toronto, Ontario M5S 3H6, Canada.
  • Shang H; Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, P. R. China.
  • Ghoussoub M; Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, P. R. China.
  • Xu YF; Materials Chemistry and Nanochemistry Research Group, Solar Fuels Cluster, Department of Chemistry, University of Toronto, Toronto, Ontario M5S 3H6, Canada.
  • Ye J; Materials Chemistry and Nanochemistry Research Group, Solar Fuels Cluster, Department of Chemistry, University of Toronto, Toronto, Ontario M5S 3H6, Canada.
  • Li Z; Materials Chemistry and Nanochemistry Research Group, Solar Fuels Cluster, Department of Chemistry, University of Toronto, Toronto, Ontario M5S 3H6, Canada.
  • Kherani NP; Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, P. R. China.
  • Zheng L; Department of Materials Science and Engineering, University of Toronto, Toronto, Ontario M5S 3E4, Canada.
  • Liu Y; Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, P. R. China.
  • Zhang L; Ontario Centre for the Characterization of Advanced Materials, University of Toronto, 200 College Street, Toronto, Ontario M5S 3E5, Canada.
  • Ozin GA; Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, P. R. China.
J Am Chem Soc ; 145(24): 13134-13146, 2023 Jun 21.
Article en En | MEDLINE | ID: mdl-37278596
ABSTRACT
Stable metal nitrides (MN) are promising materials to fit the future "green" ammonia-hydrogen nexus. Either through catalysis or chemical looping, the reductive hydrogenation of MN to MN1-x is a necessary step to generate ammonia. However, encumbered by the formation of kinetically stable M-NH1─3 surface species, this reduction step remains challenging under mild conditions. Herein, we discovered that deleterious Ti-NH1─3 accumulation on TiN can be circumvented photochemically with supported single atoms and clusters of platinum (Pt1-Ptn) under N2-H2 conditions. The photochemistry of TiN selectively promoted Ti-NH formation, while Pt1-Ptn effectively transformed any formed Ti-NH into free ammonia. The generated ammonia was found to originate mainly from TiN reduction with a minor contribution from N2 activation. The knowledge accrued from this fundamental study could serve as a springboard for the development of MN materials for more efficient ammonia production to potentially disrupt the century-old fossil-powered Haber-Bosch process.
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Texto completo: 1 Base de datos: MEDLINE Idioma: En Revista: J Am Chem Soc Año: 2023 Tipo del documento: Article
Texto completo
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Texto completo: 1 Base de datos: MEDLINE Idioma: En Revista: J Am Chem Soc Año: 2023 Tipo del documento: Article