In situ XRD studies of ZnO/GaN mixtures at high pressure and high temperature

synthesis of Zn-rich (Ga1-xZnx)(N 1-xOx) photocatalysts

Haiyan Chen, Liping Wang, Jianming Bai, Jonathan C. Hanson, John B. Warren, James Muckerman, Etsuko Fujita, Jose A. Rodriguez

Research output: Contribution to journalArticle

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Abstract

The high-pressure, high-temperature conditions for the synthesis of Zn-rich (Ga1-xZnx)(N1-xOx) solid solutions from mixtures of ZnO/GaN were explored using synchrotron-based in situ time-resolved X-ray diffraction (XRD). Following a new synthetic path, (Ga 1-xZnxx)(N1-xOx) solid solutions with a Zn content up to ∼75% were prepared for the first time. The structures of the (Ga1-xZnx)(N1-xOx) solid solutions were characterized by XRD and X-ray absorption fine structure (XAFS) analyses and were in excellent agreement with the predictions of density functional calculations. These materials adopt a wurtzite crystal structure with metal-N or metal-O bond distances in the range of 1.95-1.98 Å. Although the (Ga1-xZnx)(N1-xOx) solid solutions seem to be stable over the full range of compositions, no ideal solid solution formation was observed. In all cases, the lattice parameters were larger than those of ideal solid solutions. The variation of the lattice parameter c showed an upward double bowing curve, as was predicted by theoretical calculations. Also, no ideal behavior was observed in the electronic properties of the (Ga1-xZnxx)(N1-xO x) solid solutions. X-ray absorption spectra at the Zn and Ga K-edges of the (Ga1-xZnxx)(N1-xOx) systems showed significant electronic perturbations with respect to ZnO and GaN. The synthesized (Ga1-xZnxx)(N1-xOx) solid solution with a Zn content of 50% displayed the ability to absorb visible light well above 500 nm. This material has a great potential for splitting water under visible light irradiation. The availability of (Ga1-xZn xx)(N1-xOx) solid solutions with a high Zn content opens the door to fully explore the application of these materials in photocatalysis.

Original languageEnglish
Pages (from-to)1809-1814
Number of pages6
JournalJournal of Physical Chemistry C
Volume114
Issue number4
DOIs
Publication statusPublished - Feb 4 2010

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Photocatalysts
Solid solutions
solid solutions
X ray diffraction
synthesis
diffraction
x rays
Temperature
temperature
X ray absorption
Lattice constants
lattice parameters
Metals
Bending (forming)
water splitting
Photocatalysis
Synchrotrons
electronics
Electronic properties
wurtzite

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry
  • Electronic, Optical and Magnetic Materials
  • Surfaces, Coatings and Films
  • Energy(all)

Cite this

In situ XRD studies of ZnO/GaN mixtures at high pressure and high temperature : synthesis of Zn-rich (Ga1-xZnx)(N 1-xOx) photocatalysts. / Chen, Haiyan; Wang, Liping; Bai, Jianming; Hanson, Jonathan C.; Warren, John B.; Muckerman, James; Fujita, Etsuko; Rodriguez, Jose A.

In: Journal of Physical Chemistry C, Vol. 114, No. 4, 04.02.2010, p. 1809-1814.

Research output: Contribution to journalArticle

Chen, Haiyan ; Wang, Liping ; Bai, Jianming ; Hanson, Jonathan C. ; Warren, John B. ; Muckerman, James ; Fujita, Etsuko ; Rodriguez, Jose A. / In situ XRD studies of ZnO/GaN mixtures at high pressure and high temperature : synthesis of Zn-rich (Ga1-xZnx)(N 1-xOx) photocatalysts. In: Journal of Physical Chemistry C. 2010 ; Vol. 114, No. 4. pp. 1809-1814.
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abstract = "The high-pressure, high-temperature conditions for the synthesis of Zn-rich (Ga1-xZnx)(N1-xOx) solid solutions from mixtures of ZnO/GaN were explored using synchrotron-based in situ time-resolved X-ray diffraction (XRD). Following a new synthetic path, (Ga 1-xZnxx)(N1-xOx) solid solutions with a Zn content up to ∼75{\%} were prepared for the first time. The structures of the (Ga1-xZnx)(N1-xOx) solid solutions were characterized by XRD and X-ray absorption fine structure (XAFS) analyses and were in excellent agreement with the predictions of density functional calculations. These materials adopt a wurtzite crystal structure with metal-N or metal-O bond distances in the range of 1.95-1.98 {\AA}. Although the (Ga1-xZnx)(N1-xOx) solid solutions seem to be stable over the full range of compositions, no ideal solid solution formation was observed. In all cases, the lattice parameters were larger than those of ideal solid solutions. The variation of the lattice parameter c showed an upward double bowing curve, as was predicted by theoretical calculations. Also, no ideal behavior was observed in the electronic properties of the (Ga1-xZnxx)(N1-xO x) solid solutions. X-ray absorption spectra at the Zn and Ga K-edges of the (Ga1-xZnxx)(N1-xOx) systems showed significant electronic perturbations with respect to ZnO and GaN. The synthesized (Ga1-xZnxx)(N1-xOx) solid solution with a Zn content of 50{\%} displayed the ability to absorb visible light well above 500 nm. This material has a great potential for splitting water under visible light irradiation. The availability of (Ga1-xZn xx)(N1-xOx) solid solutions with a high Zn content opens the door to fully explore the application of these materials in photocatalysis.",
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