Predictive model of geographical origin discrimination of paper mulberry and handmade paper using ICP-AES/MS and multivariate statistical analysis

The fiber of paper mulberry, which is mostly grown in the East Asian region, varies in both length and width—even if from the same species—depending on the country, soil, and climate where it is grown. This accounts for differences in the quality of handmade paper between domestic and imported products. Once handmade paper is manufactured as sheets, its origin cannot be determined from a morphological perspective, regardless of macroscopic and microscopic observations. Therefore, this study attempted to determine the origin of Korean and imported products using mulberry bast fiber and handmade paper from a chemometrics perspective. The inorganic components of wood are absorbed from the soil and exist in the bark of trees; thus, metal and rare-earth elements in the bast fibers and handmade papers were quantitatively analyzed using inductively coupled plasma-atomic emission spectroscopy/mass spectrometry (ICP-AES/MS). Following this, a prediction model of their origin was constructed by applying multivariate statistical analysis, i.e., a partial least squares-discriminant analysis (PLS-DA) loading plot was constructed, which helped in identifying the discrimination factors resulting from their origin. According to the ICP-AES results, Pb was only detected in the Gyeongbuk Mungyeong dak sample of the Korean bast fibers. The Chinese bast fiber sample had high contents of Ca, and B and Zn were detected only in the Chinese bast fiber samples. Bast fiber samples from China, Japan, and Thailand showed relatively high contents of Al, Ca, and Na. Meanwhile, Cu and Zn were detected in the handmade paper manufactured from the imported materials. According to the ICP-MS results, among the Korean handmade papers, the products from Gyeongbuk Mungyeong, Andong, and Chungbuk Goesan exhibited a high U content and that from Gapyeong had high Sc, Rb, Sr, and Ba contents. Thus, the elemental analysis employed in this study effectively identified the origin of the papers. The origin prediction by PLS-DA for the domestic and imported products revealed an accuracy of 86.4% and 72.7% for ICP-AES and ICP-MS methods, respectively, which is deemed acceptable to assess the origin. We believe this method significantly contributes to determining the origin of paper mulberry bast fiber and handmade paper manufactured in East Asia.