Laser-induced breakdown spectroscopy (LIBS) combined with partial least squares (PLS) analysis has been applied for the quantitative analysis of the ash content of coal in this paper. The multivariate analysis method was employed to extract coal ash content information from LIBS spectra rather than from the concentrations of the main ash-forming elements. In order to construct a rigorous partial least squares regression model and reduce the calculation time, different spectral range data were used to construct partial least squares regression models, and then the performances of these models were compared in terms of the correlation coefficients of calibration and validation and the root mean square errors of calibration and cross-validation. Afterwards, the prediction accuracy, reproducibility, and the limit of detection of the partial least squares regression model were validated with independent laser-induced breakdown spectroscopy measurements of four unknown samples. The results show that a good agreement is observed between the ash content provided by thermo-gravimetric analyzer and the LIBS measurements coupled to the PLS regression model for the unknown samples. The feasibility of extracting coal ash content from LIBS spectra is approved. It is also confirmed that this technique has good potential for quantitative analysis of the ash content of coal.

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