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A XANES study of cobalt speciation state in blue-and-white glazes from 16th to 17th century Chinese porcelains

机译:XANES研究16至17世纪中国瓷器的青釉和白釉中钴的形态

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The composition of cobalt blue pigments used in ancient blue-and-white Chinese glazes is known to have changed between the 14th and the 17th century and ratios of some main chemical components plus trace elements are relevant guide-lines to establish the porcelain manufacture period. Once archaeological findings of Chinese porcelains can contribute to set up dating processes, a study of blue-and-white porcelain shards recovered during recent excavations in Lisbon Old-City was carried out by non-destructive laboratory X-ray fluorescence spectrometry for chemical characterization, combined with X-ray absorption spectroscopy (XAS) using synchrotron radiation to ascertain the formal valence and coordination of pigmenting cobalt ions. Following a preliminary extended X-ray absorption fine-structure study that revealed a coordination of divalent cobalt ions slightly above four, a detailed analysis of the near-edge region of Co 1s X-ray absorption spectra (XANES) was carried out on the blue-and-white glazes from those archaeological Chinese porcelain fragments. Pre-edge features and edge details are discussed in comparison with XANES spectra obtained from model compounds with well known crystal structure - Co _3O _4, CoAl _2O _4 and Co _2SiO _4, plus a cobalt-based blue pigment (cerulean). Present chemical data validate the manufacture period of studied Chinese porcelains advanced by Art Historians on the single basis of stylistic features (late 16th and medium 17th century). Spectroscopic results confirm a coordination environment of pigmenting Co ~(2+) ions close to tetrahedral and substantiate the dual role of cobalt as network former plus modifier in the glaze of ancient Chinese porcelains.
机译:众所周知,在古代青花瓷釉中使用的钴蓝色颜料的成分在14至17世纪间发生了变化,某些主要化学成分与微量元素的比例是确定瓷器制造时期的相关准则。一旦中国瓷器的考古发现有助于建立测年过程,便通过无损实验室X射线荧光光谱法对里斯本旧城最近发掘的青花瓷碎片进行了研究,以进行化学表征,与X射线吸收光谱法(XAS)结合使用同步加速器辐射来确定色素钴离子的形式价和配位。在初步的扩展X射线吸收精细结构研究表明二价钴离子的配位稍高于4之后,对蓝色的Co 1s X射线吸收光谱(XANES)的近边缘区域进行了详细分析。那些考古中国瓷器碎片制成的黑白釉。与从具有已知晶体结构的模型化合物Co _3O _4,CoAl _2O _4和Co _2SiO _4以及钴基蓝色颜料(天青石)获得的XANES光谱进行比较,讨论了前边缘特征和边缘细节。目前的化学数据证实了艺术史学家仅根据风格特征(16世纪中叶和17世纪中叶)所研究的中国瓷器的生产时期。光谱结果证实了接近四面体的Co〜(2+)离子着色的配位环境,并证实了钴在中国古代瓷釉中作为网络形成剂和改性剂的双重作用。

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