4.6 Article

Piezo-enhanced activation of dinitrogen for room temperature production of ammonia

Journal

NANOTECHNOLOGY
Volume 32, Issue 46, Pages -

Publisher

IOP PUBLISHING LTD
DOI: 10.1088/1361-6528/ac1a96

Keywords

gold precursor; CVD; gold nanostructures; nitrogen reduction reaction

Funding

  1. German Science Foundation (DFG)

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The study demonstrates the catalytic conversion of dinitrogen into ammonia using efficient piezo-enhanced gold catalysis. The combination of gold nanostructures with piezoelectric materials provides a promising approach for sustained activation of dinitrogen molecules in chemical synthesis.
The catalytic conversion of nitrogen to ammonia remains an energy-intensive process, demanding advanced concepts for nitrogen fixation. The major obstacle of nitrogen fixation lies in the intrinsically high bond energy (941 kJ mol(-1)) of the N equivalent to N molecule and the absence of a permanent dipole in N-2. This kinetic barrier is addressed in this study by an efficient piezo-enhanced gold catalysis as demonstrated by the room temperature reduction of dinitrogen into ammonia. Au nanostructures were immobilized on thin film piezoelectric support of potassium sodium niobate (K0.5Na0.5NbO3, KNN) by chemical vapor deposition of a new Au(III) precursor [Me2Au(PyTFP)(H2O)] 1 (PyTFP = (Z)-3,3,3-trifluoro-1-(pyridin-2-yl)-prop-1-en-2-olate) that exhibited high volatility (60 degrees C, 10(-3) mbar) and clean decomposition mechanism to produce well adherent elemental gold films on KNN and Ti substrates. The gold-functionalized KNN films served as an efficient catalytic system for ammonia production with a Faradaic efficiency of 18.9% achieved upon ultrasonic actuation. Our results show that the spontaneous polarization of piezoelectric materials under external electrical fields augments the sluggish electron transfer kinetics by creating instant dipoles in adsorbed N-2 molecules to deliver a piezo-enhanced catalytic system promising for sustained activation of dinitrogen molecules.

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