4.8 Article

Blue-Emitting Sr3Si8-xAlxO7+xN8-xEu2+ Discovered by a Single-Particle-Diagnosis Approach: Crystal Structure, Luminescence, Scale-Up Synthesis, and Its Abnormal Thermal Quenching Behavior

期刊

CHEMISTRY OF MATERIALS
卷 27, 期 22, 页码 7689-7697

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.5b03252

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资金

  1. KAKENHI [15K06448]
  2. National Natural Science Foundation of China [61177050, 51272259]
  3. Grants-in-Aid for Scientific Research [15K06448] Funding Source: KAKEN

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The single-particle-diagnosis approach allows for the fast discovery of novel luminescent materials using powdered samples. This paper reports a new blue-emitting Sr3Si8-xAlxO7+xN8-x:Eu2+ phosphor for solid state lighting and its scale-up synthesis. The structure-, composition-, and temperature-dependent luminescence were investigated and discussed by means of various analytic techniques including single-crystal XRD diffractometer, single-particle fluorescence spectroscopy, FTIR spectra, decay time, low-temperature luminescence, and computed energy level scheme. Sr3Si8-xAlxO7+xN8-x crystallizes in the monoclinic system (space group C2/c, no. 15) with a = 18.1828 (13) angstrom, b = 4.9721 (4) angstrom, c = 15.9557 (12) angstrom, beta = 115.994 (10)(0), and Z = 2. The Sr atoms are coordinated to 8 and 6 O/N atoms and located in the voids along [010] formed by vertex-sharing (Si,Al)- (O,N)(4) tetrahedra. Phase-pure powder samples of Sr3Si8-xAlxO7+xN8-x:Eu2+ were synthesized from the chemical composition of the single particle by controlling the x value. Luminescence of both a single particle and powders show a broad Eu2+ emission band centered at similar to 465 nm and a fwhm of similar to 70 nm, under the UV light irradiation. The title phosphor has a band gap of 5.39 eV determined from the UV vis spectrum, absorption efficiency of 83%, internal quantum efficiency of 44.9%, and external quantum efficiency of 37.4% under the 355 nm excitation. An abnormal thermal quenching behavior is observed in Sr3Si8-xAlxO7+xN8-x:Eu2+ that has a high activation energy for thermal quenching (0.294 eV) but a low thermal quenching temperature (similar to 370 K), which is ascribed to the partial overlap between the Eu2+ excited energy level and the conduction band of the host.

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