Anionic Condensation-Guided Synthesis of LaSi2N3O: A “Missing” Structure in the Ln–Si–N–O Series of Oxonitridosilicate Phosphor Materials
Source abstract
Abstract
Abstract The development of innovative luminescent materials for lighting and display applications is an important research field. In this work, we have employed an anionic condensation approach to discover a novel oxonitridosilicate synthesized via Li metal flux. LaSi2N3O crystallizes in the orthorhombic space group Pna21 (a = 7.82609(6), b = 18.24908(15), and c = 4.86567(5) Å) with a structure consisting of [Si6N12O2] ribbons cross-linked by [SiN3O] tetrahedra. This follows previously reported structural rules for a series of condensed rare-earth oxonitridosilicates, and discovery of this relatively simple composition verifies the design principles. Ce3+-doped LaSi2N3O is a highly efficient blue phosphor with peak emission at 450 nm under 390 nm excitation and a quantum yield of 72.0% and demonstrates strong potential for near-UV phosphor applications.
Source: crossref · Quality: baseline
Research context
OpenAlex topics: Luminescence Properties of Advanced Materials · Inorganic Chemistry and Materials · Microwave Dielectric Ceramics Synthesis
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
Affiliations
Shaanxi Normal University , , ,
University of Edinburgh , , ,
Institute of Nuclear Physics and Chemistry, China Academy of Engineering Physics , ,
Shaanxi Normal University , , , ,
Funding
Engineering and Physical Sciences Research Council · Chinese Government Scholarship · Fundamental Research Funds for the Central Universities · National Natural Science Foundation of China
References (65)
Show source-provided references
1. Advancing Reporting Guidelines for Optimal Characterization of Inorganic Phosphors10.1021/acs.chemmater.3c01743 ↗
2. Evolutionary Generation of Phosphor Materials and Their Progress in Future Applications for Light-Emitting Diodes10.1021/acs.chemrev.1c00952 ↗
3. New Polymorph of the Highly Efficient LED-Phosphor SrSi2O2N2:Eu2+ - Polytypism of a Layered Oxonitridosilicate10.1021/cm400461v ↗
4. Powder synthesis and luminescence of a novel yellow-emitting Ba5Si11Al7N25: Eu2+ phosphor discovered by a single-particle-diagnosis approach for warm w-LEDs10.1016/j.cej.2022.140932 ↗
5. Narrow-band red emitting oxonitridosilicate phosphor La4-xSr2+xSi5N12-xOx:Pr3+ (x ≈ 1.69)10.1039/D1CC00893E ↗
6. Narrow-Band Green-Emitting Phosphor Ba2LiSi7AlN12:Eu2+ with High Thermal Stability Discovered by a Single Particle Diagnosis Approach10.1021/acs.chemmater.5b01464 ↗
7. Unprecedented Deep-Red Ce3+ Luminescence of the Nitridolithosilicates Li38.7RE3.3Ca5.7[Li2Si30N59]O2F (RE = La, Ce, Y)10.1021/acs.chemmater.8b02604 ↗
8. Narrow-band blue emitting nitridomagnesosilicate phosphor Sr8Mg7Si9N22:Eu2+ for phosphor-converted LEDs10.1039/C8CC07218C ↗
9. Chemoproteomic Identification of Blue-Light-Damaged Proteins10.1021/jacs.2c07180 ↗
10. The Future Is Blue (LEDs): Why Chemistry Is the Key to Perovskite Displays10.1021/acs.chemmater.9b01650 ↗
11. Thermally Robust and Color-Tunable Blue-Green-Emitting BaMgSi4O10:Eu2+,Mn2+ Phosphor for Warm-White LEDs10.1021/acs.inorgchem.0c01803 ↗
12. Understanding the Local and Electronic Structures toward Enhanced Thermal Stable Luminescence of CaAlSiN3:Eu2+10.1021/acs.chemmater.6b02121 ↗
13. Super-Tunable LaSi3N5 Structure Type: Insights into the Structure and Luminescence of SrSi2PN5:Eu2+10.1021/acs.chemmater.4c00459 ↗
14. Synthesis, crystal structure, and photoluminescence of new strontium barium nitrido-alumino-silicate phosphor, Sr27.9Ba22.8Al61.4Si174.6N328.4:Eu2+10.1016/j.jallcom.2023.171982 ↗
15. Toward New Phosphors for Application in Illumination-Grade White pc-LEDs: The Nitridomagnesosilicates Ca[Mg3SiN4]:Ce3+, Sr[Mg3SiN4]:Eu2+, and Eu[Mg3SiN4]10.1021/cm500610v ↗
16. Zeolite-like Topology Oxonitridosilicate La3.6Ba1.7Si5N10O2.1 with Potential Applications in Nonlinear Optical Materials10.1021/acs.inorgchem.3c03376 ↗
17. Promising Oxonitridosilicate Phosphor Host Sr3Si2O4N2: Synthesis, Structure, and Luminescence Properties Activated by Eu2+ and Ce3+/Li+ for pc-LEDs10.1021/ic202340q ↗
18. Efficient Yellow-Orange Phosphor Lu4Ba2[Si9ON16]O:Eu2+ and Orange-Red Emitting Y4Ba2[Si9ON16]O:Eu2+: Two Oxonitridosilicate Oxides with Outstanding Structural Variety10.1021/acs.chemmater.7b02900 ↗
19. La3BaSi5N9O2:Ce3+ - A Yellow Phosphor with an Unprecedented Tetrahedra Network Structure Investigated by Combination of Electron Microscopy and Synchrotron X-ray Diffraction10.1021/acs.chemmater.5b01702 ↗
20. Crystal Structures and Luminescence Properties of RE6Si11N20O:Ce3+ (RE = Lu, Y)10.1149/2162-8777/ace995 ↗
21. Nitridosilicates and Oxonitridosilicates: From Ceramic Materials to Structural and Functional Diversity10.1002/anie.201005755 ↗
22. Oxonitridosilicate Oxides RE26Ba6[Si22O19N36]O16:Eu2+ (RE = Y, Tb) with a Unique Layered Structure and Orange-Red Luminescence for RE = Y10.1021/acs.inorgchem.7b03124 ↗
23. BaYbSi4N7-Unexpected Structural Possibilities in Nitridosilicates10.1002/anie.199619831 ↗
24. From Minor Side Phases to Bulk Samples of Lanthanum Oxonitridosilicates: An Investigation with Microfocused Synchrotron Radiation10.1021/acs.inorgchem.6b00143 ↗
25. Data-Driven Discovery of Full-Visible-Spectrum Phosphor10.1021/acs.chemmater.9b02505 ↗
26. Discovery of New Nitridosilicate Phosphors for Solid State Lighting by the Single-Particle-Diagnosis Approach10.1021/cm501866x ↗
27. Activator - host structure relations of applied optical materials: a review10.1515/zkri-2025-0019 ↗
28. The Metal Flux: A Preparative Tool for the Exploration of Intermetallic Compounds10.1002/anie.200462170 ↗
29. Nitridophosphates: A Success Story of Nitride Synthesis10.1002/anie.201812791 ↗
30. Recent progress on discovery of novel phosphors for solid state lighting10.1016/j.jre.2020.01.016 ↗
31. Narrow-band red-emitting Sr[LiAl3N4]:Eu2+ as a next-generation LED-phosphor material10.1038/nmat4012 ↗
32. Nitridomagnesosilicate Ba[Mg3SiN4]:Eu2+ and Structure-Property Relations of Similar Narrow-Band Red Nitride Phosphors10.1021/cm504604d ↗
33. A New Paradigm for Materials Discovery: Heuristics-Assisted Combinatorial Chemistry Involving Parameterization of Material Novelty10.1002/adfm.201102118 ↗
34. Discovery of a Phosphor for Light Emitting Diode Applications and Its Structural Determination, Ba(Si,Al)5(O,N)8:Eu2+10.1021/ja409865c ↗
35. A Strategy for the Synthesis of Oxonitridosilicate Phosphors from Anionic Condensation10.1021/acs.chemmater.3c03045 ↗
36. Highly Humidity-Resistant Oxynitride Phosphor BaSi6N8O:Ce3+ for pc-LEDs10.1021/acs.inorgchem.4c04463 ↗
37. Ln3[SiON3]O (Ln = La, Ce, Pr) - Three Oxonitridosilicate Oxides with Crystal Structures Derived from the Anti-Perovskite Structure Type10.1002/zaac.200900274 ↗
38. Solid-solution transformation and photoluminescence control in Ce3+-doped Ln4Si2-xMxO7+xN2-x (Ln= Y, Lu; M= B, Al, P) oxonitridosilicate phosphors10.1016/j.jallcom.2018.10.271 ↗
39. Ca[Si2O2N2]─A Novel Layer Silicate10.1002/anie.200460098 ↗
40. Ce16Si15O6N32─An Oxonitridosilicate with Silicon Octahedrally Coordinated by Nitrogen10.1002/(SICI)1521-3773(19990201)38:3<357::AID-ANIE357>3.0.CO;2-D ↗
41. The Role of Cerium Orthosilicate in the Densification of Si3N410.1111/j.1151-2916.1979.tb18795.x ↗
42. Crystal Structure of La4Si2O7N2 Analyzed by the Rietveld Method Using the Time-of-Flight Neutron Powder Diffraction Data10.1021/cm020930c ↗
43. A crystallographic study of a new compound of lanthanum silicon nitride, LaSi3N510.1007/BF00550562 ↗
44. Preparation, Electronic Structure, and Photoluminescence Properties of Eu2+- and Ce3+/Li+-Activated Alkaline Earth Silicon Nitride MSiN2 (M = Sr, Ba)10.1021/cm701875e ↗
45. Structure elucidation of BaSi2O2N2 - A host lattice for rare-earth doped luminescent materials in phosphor-converted (pc)-LEDs10.1016/j.solidstatesciences.2008.06.014 ↗
46. Real structure of SrSi2O2N210.1016/j.solidstatesciences.2006.11.009 ↗
47. A short history of SHELX10.1107/S0108767307043930 ↗
48. OLEX2: a complete structure solution, refinement and analysis program10.1107/S0021889808042726 ↗
49. 2014
50. Coelho · 2003
51. First-principles computation of material properties: the ABINIT software project10.1016/s0927-0256(02)00325-7 ↗
52. The structures of the Ce and La N-phases RE3Si8-xAlxN11-xO4+x (x≈1.75 for RE = Ce, x≈1.5 for RE = La), determined by single-crystal X-ray and time-of-flight neutron powder diffraction, respectively10.1039/b102340n ↗
53. Ce-Doped La3Si6.5Al1.5N9.5O5.5, a Rare Highly Efficient Blue-Emitting Phosphor at Short Wavelength toward High Color Rendering White LED Application10.1021/acsami.7b03909 ↗
54. Die neuen Schichtsilicate Ba3Si6O9N4 und Eu3Si6O9N410.1002/zaac.200500452 ↗
55. Satoshi Shimooka, Kyota Uheda, Hiroyuki Imura, and Naoto Kijima. New Green Phosphor Ba3Si6O12N2:Eu for White LED: Crystal Structure and Optical Properties10.4028/www.scientific.net/kem.403.11 ↗
56. The 5d level positions of the trivalent lanthanides in inorganic compounds10.1016/S0022-2313(00)00229-5 ↗
57. Inverse-tunable Red Luminescence and Electronic Properties of Nitridoberylloaluminates Sr2-xBax[BeAl3N5]:Eu2+ (x = 0–2)10.1002/chem.202104121 ↗
58. Phosphors in phosphor-converted white light-emitting diodes: Recent advances in materials, techniques and properties10.1016/j.mser.2010.07.001 ↗
59. Ca2Al3O6F:Eu2+: a green-emitting oxyfluoride phosphor for white light-emitting diodes10.1039/c2jm32733c ↗
60. Energy transfer in oxidic phosphors10.1016/0375-9601(68)90486-6 ↗
61. A Theory of Sensitized Luminescence in Solids10.1063/1.1699044 ↗
62. Synthesis, structure and luminescence properties of new blue-green-emitting garnet-type Ca3Zr2SiGa2O12:Ce3+ phosphor for near-UV pumped white-LEDs10.1039/C5RA22953G ↗
63. Temperature dependent studies of cathodoluminescence of green band of ZnO crystals10.1007/BF01730729 ↗
64. Generating cyan emission via ammonia-thermal nitridation: Na18-xCa13+xMg5(PO4-yNy)18: Eu2+10.1039/D5TC01824B ↗
65. Colossal Chromatic Shift in the Ba2Ca2B4O10:Ce3+ Phosphor10.1021/acs.chemmater.3c01465 ↗