Universität zu Köln

Frank, Michael, Bulut, Yusuf ORCID: 0000-0003-0090-3990, Czympiel, Lisa, Weissing, Rene, Nahrstedt, Vanessa, Wilhelm, Michael ORCID: 0000-0002-4764-6955, Grosch, Matthias, Raauf, Aida, Verma, Anjneya, Fischer, Thomas and Mathur, Sanjay (2021). Piezo-enhanced activation of dinitrogen for room temperature production of ammonia. Nanotechnology, 32 (46). BRISTOL: IOP PUBLISHING LTD. ISSN 1361-6528

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Abstract

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.

Item Type:	Journal Article
Creators:	Creators Email ORCID ORCID Put Code Frank, Michael UNSPECIFIED UNSPECIFIED UNSPECIFIED Bulut, Yusuf UNSPECIFIED orcid.org/0000-0003-0090-3990 UNSPECIFIED Czympiel, Lisa UNSPECIFIED UNSPECIFIED UNSPECIFIED Weissing, Rene UNSPECIFIED UNSPECIFIED UNSPECIFIED Nahrstedt, Vanessa UNSPECIFIED UNSPECIFIED UNSPECIFIED Wilhelm, Michael UNSPECIFIED orcid.org/0000-0002-4764-6955 UNSPECIFIED Grosch, Matthias UNSPECIFIED UNSPECIFIED UNSPECIFIED Raauf, Aida UNSPECIFIED UNSPECIFIED UNSPECIFIED Verma, Anjneya UNSPECIFIED UNSPECIFIED UNSPECIFIED Fischer, Thomas UNSPECIFIED UNSPECIFIED UNSPECIFIED Mathur, Sanjay UNSPECIFIED UNSPECIFIED UNSPECIFIED
URN:	urn:nbn:de:hbz:38-561947
DOI:	10.1088/1361-6528/ac1a96
Journal or Publication Title:	Nanotechnology
Volume:	32
Number:	46
Date:	2021
Publisher:	IOP PUBLISHING LTD
Place of Publication:	BRISTOL
ISSN:	1361-6528
Language:	English
Faculty:	Unspecified
Divisions:	Unspecified
Subjects:	no entry
Uncontrolled Keywords:	Keywords Language NITROGEN REDUCTION REACTION; CRYSTAL-STRUCTURES; GOLD; COMPLEXES; FIXATION; CATALYST; SURFACE; PROGRAM; WATER; CVD Multiple languages Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied Multiple languages
URI:	http://kups.ub.uni-koeln.de/id/eprint/56194