Synthesis and characterization of (Ga1-xZnx)(N1-xOx) nanocrystals with a wide range of compositions

Lee, Kyureon; Lu, Ying-Gang; Chuang, Chi-Hung; Ciston, Jim; Dukovic, Gordana

doi:10.1039/c5ta04314j

Title: Synthesis and characterization of (Ga_1-xZn_x)(N_1-xO_x) nanocrystals with a wide range of compositions

Journal Article · Thu Jul 28 00:00:00 EDT 2016 · Journal of Materials Chemistry. A

DOI:https://doi.org/10.1039/c5ta04314j· OSTI ID:1506251

Lee, Kyureon ^[1]; Lu, Ying-Gang ^[1]; Chuang, Chi-Hung ^[1]; Ciston, Jim ^[2]; Dukovic, Gordana ^[1]

Univ. of Colorado, Boulder, CO (United States). Dept. of Chemistry and Biochemistry
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Center for Electron Microscopy, Molecular Foundry

We describe the synthesis and characterization of wurtzite (Ga_1-xZn_x)(N_1-xO_x) nanocrystals with a wide range of compositions and a focus on properties relevant for solar fuel generation. (Ga_1-xZn_x)(N_1-xO_x), a solid solution of GaN and ZnO, is an intriguing material because it exhibits composition-dependent visible absorption even though the parent semiconductors absorb in the UV. When functionalized with co-catalysts, (Ga_1-xZn_x)(N_1-xO_x) is also capable of water splitting under visible irradiation. Here, we examine the synthesis of (Ga_1-xZn_x)(N_1-xO_x) nanocrystals to understand how they form by nitridation of ZnO and ZnGa₂O₄ nanocrystalline precursors. We find that the ZnO precursor is critical for the formation of crystalline (Ga_1-xZn_x)(N_1-xO_x) at 650 °C, consistent with a mechanism in which wurtzite (Ga_1-xZn_x)(N_1-xO_x) nucleates topotactically on wurtzite ZnO at an interface with ZnGa₂O₄. Using this information, we expand the range of compositions from previously reported 0.30 ≤ x ≤ 0.87 to include the low-x and high-x ends of the range. The resulting compositions, 0.06 ≤ x ≤ 0.98, constitute the widest range of (Ga_1-xZn_x)(N_1-xO_x) compositions obtained by one synthetic method. We then examine how the band gap depends on sample composition and find a minimum of 2.25 eV at x = 0.87, corresponding to a maximum possible solar-to-H₂ power conversion efficiency of 12%. Finally, we examine the photoelectrochemical (PEC) oxidation behavior of thick films of (Ga_1-xZn_x)(N_1-xO_x) nanocrystals with x = 0.40, 0.52, and 0.87 under visible illumination. (Ga_1-xZn_x)(N_1-xO_x) nanocrystals with x = 0.40 exhibit solar PEC oxidation activity that, while too low for practical applications, is higher than that of bulk (Ga_1-xZn_x)(N_1-xO_x) of the same composition. The highest photocurrents are observed at x = 0.52, even though x = 0.87 absorbs more visible light, illustrating that the observed photocurrents are a result of an interplay of multiple parameters which remain to be elucidated. This set of characterizations provides information useful for future studies of composition-dependent PEC properties of nanoscale (Ga_1-xZn_x)(N_1-xO_x).

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Research Organization:: Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22), Scientific User Facilities Division (SC-22.3 )

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1506251

Journal Information:: Journal of Materials Chemistry. A, Vol. 4, Issue 8; ISSN 2050-7488

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 34 works

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