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ISSN 0036-0244, Russian Journal of Physical Chemistry A, 2019, Vol. 93, No. 8, pp. 1455–1459. © Pleiades Publishing, Ltd., 2019.
Russian Text © The Author(s), 2019, published in Zhurnal Fizicheskoi Khimii, 2019, Vol. 93, No. 8, pp. 1159–1163.
Low-Temperature Synthesis of Zirconium Carbonitrode via the
Reduction of Zirconia with Magnesium in the Presence of Sodium
Carbonate in a Nitrogen Atmosphere
R. A. Shishkin
a,
* and V. S. Kudyakova
a
a
Institute of Physics and Technology, Ural Federal University, Yekaterinburg, 620078 Russia
*e-mail: roman.shishkin@urfu.ru
Received November 9, 2018; revised November 9, 2018; accepted November 20, 2018
Abstract—Physicochemical transformations that occur during the low-temperature synthesis of zirconium
carbonitride via the reduction of zirconia with magnesium in the presence of sodium carbonate in a nitrogen
atmosphere are studied. Both reactions leading to the formation of Zr
2
CN and side processes occurring in the
charge are studied by means of differential scanning calorimetry. Based in the results, it is concluded that zir-
conium carbonitride can be synthesized in the temperature range of 600–675°C. It is shown that using graph-
ite does not lead to the formation of zirconium carbide or zirconium carbonitride in the investigated range of
temperatures, while the use of urea has hardly any effect on the final product.
Keywords: co-reduction, mechanism, zirconium carbonitride, zirconium nitride, sodium carbonate, low-
temperature synthesis
DOI: 10.1134/S0036024419080272
INTRODUCTION
Carbides, nitrides, and carbonitrides of group III–
V transition metals are of considerable interest, due to
such remarkable physicochemical properties of these
materials [1] as high melting temperatures, hardness,
chemical resistance, strength, wear resistance, and
thermal stability [2, 3]. Zr
2
CN is therefore used as
wear-resistant coatings and barrier layers.
A number of ways of synthesizing transition metal
carbonitrides, particularly zirconium carbonitride,
have been developed. These include the pyrolysis of
organic precursors [4–6], solvothermal synthesis [7,
8], chemical vapor deposition [9], carbothermal
reduction in a nitrogen-containing gas medium [10,
11], and combustion [11, 12]. In recent years, particu-
lar attention has been given to means based on the co-
reduction of inorganic compounds containing transi-
tion metals and alkali or alkaline-earth metal carbon-
ates with metallic magnesium [13–15]. However, the
possibility of conducting synthesis in a nitrogen-con-
taining atmosphere has yet to be explored. The use of
this technique would appear to be promising, since it
provides both a source of nitrogen and an additional
reducing agent.
The zirconium carbonitride formation reaction can
be written as
(1)
However, it is still unclear which chemical transforma-
tions occur during the co-reduction of zirconia and an
alkali metal carbonate with metallic magnesium in a
nitrogen-containing atmosphere. Studies of the pro-
cesses that occur in the charge will allow us not only to
select the optimum temperatures of synthesis, but to
abandon the steel autoclaves and long periods of syn-
thesis (8–12 h) that are conventionally used in these
technologies as well.
EXPERIMENTAL
The precursors in this work were zirconia (special
purity grade 9-2), sodium carbonate (reagent grade), a
metallic magnesium powder (MPF-1 stored in kero-
sene), powdered graphite (GII-A), and urea (analyti-
cal grade). The composition of the four samples is
given in Table 1. The samples were placed in an alun-
dum crucible and subjected to simultaneous analysis
via thermogravimetry and differential scanning calo-
rimetry on a Sentsys EVO 1600 unit upon heating to
1200°C in a special purity grade nitrogen atmosphere
(99.999%). The resulting product was washed with
0.1 M hydrochloric acid and isopropyl alcohol on a
white ribbon filter and then dried at 90°C for 4 h.
X-ray diffraction analysis was conducted on an
Xpert PRO MRD diffractometer equipped with a ver-
tical goniometer and a nickel filter on the secondary
beam using CuK
α
radiation in Bragg–Brentano focus-
+ + +
= + +
(g)
2 2 3 2
2 2
2ZrO Na CO 6Mg 0.5N
Zr CN 6MgO Na O.
CHEMICAL KINETICS
AND CATALYSIS