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## Creator

Xun Liu, [Takeo Ohsawa](https://orcid.org/0000-0001-7528-8940), [Noriko Saito](https://orcid.org/0000-0002-8104-0172), [Kohsei Takahashi](https://orcid.org/0000-0002-6443-1534), [Takashi Takeda](https://orcid.org/0000-0003-2510-4562), Kenzo Deguchi, [Shinobu Ohki](https://orcid.org/0000-0002-7357-3833), Tetsuo Kishi, Tetsuji Yano, [Hiroyo Segawa](https://orcid.org/0000-0002-7198-8410), [Naoki Ohashi](https://orcid.org/0000-0002-4011-0031)

## Rights

© 2026 The Ceramic Society of Japan 

Abstract

Europium-doped oxynitride glass powder (Sr–Si–Al–O–N) was synthesized by a sol–gel method followed by ammonolysis to investigate the effect of the ammonolysis conditions on the structure and properties of the glass powder. In particular, the effect of the ammonia gas flow rate during nitridation was studied. The effective nitrogen concentration (Neff) in the obtained powder, analyzed by X-ray fluorescence, increased with an increase in the flow rate, and the results of X-ray photoemission, nuclear magnetic resonance, and Fourier transform infrared (FT-IR) spectroscopy measurements indicated that the population of Si–N bonds increased with an increase in Neff. However, the presence of hydrogen-terminated structures, such as –NHn, in the powder with high Neff was confirmed by FT-IR measurements. The presence of hydrogen-terminated structures, such as –Si–NHn, and the thermal stability of these hydrogen-related structures were further investigated by thermal analyses, including thermal desorption measurements, which suggested that hydrogen-terminated structures can be easily formed during the nitridation of the gel and that the formation of hydrogen-terminated structures inhibits the polymerization of the glass structures.
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## Other metadata

[Tracing nitridation reaction toward efficient production of oxynitride glasses as hosts for bright luminescence centers](https://mdr.nims.go.jp/datasets/c56e3e67-be15-426d-94b4-fb80ef29fcc4)

## Fulltext

S-1  Supporting information attached to   Tracing Nitridation Reaction Toward Efficient Production of Oxynitride Glasses as Hosts for Bright Luminescence Centers Xun Liu1,2, Takeo Ohsawa1, Noriko Saito1, Kohsei Takahashi1, Takashi Takeda1,  Kenzo Deguchi1, Shinobu Ohki1, Tetsuo Kishi3, Tetsuji Yano3, Hiroyo Segawa1,3,  Naoki Ohashi1,2,4 1 National Institute for Materials Science (NIMS), 1-1 Namiki, Tsukuba, Ibaraki 305-0044, Japan 2 Interdisciplinary Graduate School of Engineering Sciences, Kyusyu University, 6-1, Kasugakoen, Kasuga, Fukuoka 816-8580, Japan 3 Department of Chemistry and Materials Science, Graduate School of Science and Engineering, Institute of Science Tokyo, 2-12-1 Ookayama, Meguro-ku, Tokyo 152-8552, Japan 4 Materials DX Research Center for Element Strategy, Institute of Science Tokyo, 4259 Nagatsuta, Midori-ku, Yokohama 226-8503, Japan  I. Phase identification   Figure S1 X-ray diffraction pattern for the powder after ammonolysis with various ammonia flow rate. Sample IDs are show in main text. Crystalline phase, cristobalite, was formed in the P020 powder prepared by ammonolysis under small ammonia flow rate (20cm3/min).    S-2  II. Atmosphere in the furnace during ammonolysis  Figure S2 Composition of the exhaust gas from the furnace during ammonolysis. With smaller ammonia flow rate, actual ammonia concentration in the furnace was relatively low due to decomposition and the residual oxygen gas concentration due to out-gas from the furnace was relatively high. With very high flow rate, relatively high ammonia concentration was achieved.     S-3  III. Chemical composition analysis A. Typical results of XRF analyses  Table S1 Result of Xray fluorescence analysis for PwO powder (prepared by firing in the air). Charge compensation in the powder was considered by assuming formal charge (Q) of each element. Particularly, formal charge of europium was assumed to  be divalent. The summation of charge indicates slight excess of anion, likely presence of protons for compensation.  Element Mol% (M) Formal charge (Q) Charge (Q×M) N 0.0 -3 0.0 O 62.9 -2 -125.8 Al 4.2 3 12.6 Si 24.5 4 98.2 Sr 2.8 2 5.6 Eu 0.8 2 1.7   Sum. charge -7.8   Table S2 Result of Xray fluorescence analysis for P500SR powder (prepared by ammonolysis in ammonia flow rate at 500 ml/min). Charge compensation in the powder was considered by assuming formal charge (Q) of each element. Particularly, formal charge of europium was assumed to be divalent. The obvious excess of negative charge is an indication for the presence of proton in the powder.   Element Mol% (M) Formal charge (Q) Charge (Q×M) N 26.4 -3 -79.3 O 42.8 -2 -85.6 Al 4.1 3 12.4 Si 23.1 4 92.3 Sr 2.8 2 5.5 Eu 0.8 2 1.7   Sum. charge -53.1       S-4   B. Neff determined by XPS measurements  Figure S3 Effective nitrogen concentration (Neff) in the obtained powder as a function of ammonia flow rate on ammonolysis. In this figure, the results of X-ray photoemission (XPS) analyses are superimposed on the results of X-ray fluorescence (XRF) analyses show in the main text. The definition of Neff and sample IDs are also shown in main text.     S-5  IV. Microstructures A. Microstructure of the gel before ammonolysis  Figure S4 Secondary electron microscope image of the gel powder begore ammonolysis.    B. Microstructures of the powder after ammonolysis   Figure S5 Secondary electron microscope image of the gel powder after ammonolysis at the ammonia flow rate of 300 cm3/min (P300) and 500 cm3/min (P500).       I. Phase identification II. Atmosphere in the furnace during ammonolysis III. Chemical composition analysis A. Typical results of XRF analyses B. Neff determined by XPS measurements IV. Microstructures A. Microstructure of the gel before ammonolysis B. Microstructures of the powder after ammonolysis