説明:
(abstract)Mixed-anion compounds offer unique functionalities unattainable with single-anion materials, yet rational morphology control remains largely unexplored. Here, we report a Lewis acid–base-driven strategy that enables low-temperature, solution-phase morphology control of the oxyfluoride photocatalyst Pb2Ti2O5.4F1.2 (PTOF). A microwave-assisted solvothermal method with monoethanolamine (MEA) was used to tune the particle morphology and size via the precursor-solution pH, which was adjusted by the addition of formic acid or acetic acid. PTOF, an A2B2X6X′0.5-type pyrochlore with intrinsic anion vacancies (X′2, 4d site), has exposed {111} facets composed of alternating Pb-rich and Ti-rich layers. Lewis basic MEA is proposed to bind selectively to undercoordinated, strongly acidic Pb2+ sites adjacent to Ti4+ and vacancies on Ti-rich {111} facets, suppressing growth along the surface direction and stabilizing these facets, thereby driving anisotropic crystal growth and forming plate-like nanoparticles. At pH 10 (formic acid), PTOF nanoparticles (∼30 nm) with a specific surface area of 37 m2 g–1 were obtained. Compared with an analogous PTOF synthesized by a conventional solid–state reaction, the optimized sample exhibited ∼29-fold higher H2 evolution activity in an aqueous solution containing dissolved disodium ethylenediaminetetraacetate under visible-light (λ > 400 nm) with the aid of a Pt cocatalyst. Lewis acid–base-directed facet stabilization is thus shown to be a promising approach for the rational morphological design of mixed-anion oxyfluorides via solution processing.
権利情報:
キーワード: Catalytic activity, Nanoparticles, Organic acids, pH, Photocatalysis
刊行年月日: 2026-02-24
出版者: American Chemical Society (ACS)
掲載誌:
研究助成金:
原稿種別: 出版者版 (Version of record)
MDR DOI:
公開URL: https://doi.org/10.1021/acs.chemmater.5c03153
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更新時刻: 2026-04-13 09:22:40 +0900
MDRでの公開時刻: 2026-04-13 10:23:12 +0900
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lewis-acid-base-driven-anisotropic-crystal-growth-of-pyrochlore-pb2ti2o5-4f1-2-with-enhanced-visible-light-h2-evolution.pdf
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サイズ | 7.67MB | 詳細 |