Photochemical Acceleration of Ammonia Production by Pt1-Ptn-TiN Reduction and N2 Activation.
J Am Chem Soc
; 145(24): 13134-13146, 2023 Jun 21.
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| 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-NH1â3 surface species, this reduction step remains challenging under mild conditions. Herein, we discovered that deleterious Ti-NH1â3 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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J Am Chem Soc
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2023
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