Unraveling the Role of Lattice Substitutions on the Stabilization of the Intrinsically Unstable Pb2Sb2O7 Pyrochlore: Explaining the Lightfastness of Lead Pyroantimonate Artists’ Pigments,Chemistry of Materials

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Unraveling the Role of Lattice Substitutions on the Stabilization of the Intrinsically Unstable Pb2Sb2O7 Pyrochlore: Explaining the Lightfastness of Lead Pyroantimonate Artists’ Pigments
Chemistry of Materials ( IF 7.2 ) Pub Date : 2020-01-27 , DOI: 10.1021/acs.chemmater.9b04821
Andrea Marchetti _{1,

2} , Rolando Saniz _{2,

3} , Dileep Krishnan _{2,

4} , Laura Rabbachin ₅ , Gert Nuyts _{1,

2} , Steven De Meyer _{1,

2} , Johan Verbeeck _{2,

4} , Koen Janssens _{1,

2} , Claudia Pelosi ₆ , Dirk Lamoen _{2,

4} , Bart Partoens _{2,

3} , Karolien De Wael _{1,

2}

Affiliation

The pyroantimonate pigments Naples yellow and lead tin antimonate yellow are recognized as some of the most stable synthetic yellow pigments in the history of art. However, this exceptional lightfastness is in contrast with experimental evidence suggesting that this class of mixed oxides is of semiconducting nature. In this study the electronic structure and light-induced behavior of the lead pyroantimonate pigments were determined by means of a combined multifaceted analytical and computational approach (photoelectrochemical measurements, UV–vis diffuse reflectance spectroscopy, STEM-EDS, STEM-HAADF, and density functional theory calculations). The results demonstrate both the semiconducting nature and the lightfastness of these pigments. Poor optical absorption and minority carrier mobility are the main properties responsible for the observed stability. In addition, novel fundamental insights into the role played by Na atoms in the stabilization of the otherwise intrinsically unstable Pb₂Sb₂O₇ pyrochlore were obtained.

中文翻译：

阐明晶格取代在稳定本征不稳定的Pb ₂ Sb ₂ O ₇烧绿石上的作用：解释焦锑酸铅艺术家颜料的耐光性

焦锑酸颜料那不勒斯黄和锑酸铅锡黄被认为是艺术史上最稳定的合成黄色颜料。但是，这种优异的耐光性与实验证据相反，实验证据表明这类混合氧化物具有半导体性质。在这项研究中，通过组合的多方面分析和计算方法（光电化学测量，紫外可见漫反射光谱，STEM-EDS，STEM-HAADF和密度泛函法）确定了焦锑酸铅颜料的电子结构和光诱导行为。理论计算）。结果证明了这些颜料的半导体性质和耐光性。不良的光吸收和少数载流子迁移率是导致观察到的稳定性的主要特性。此外，有关钠原子在稳定本来不稳定的铅中的作用的新颖基本见解_获得2 Sb ₂ O ₇烧绿石。

更新日期：2020-01-27

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