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A recent article reported a comparison study concerning compound-specificchlorine isotope analysis (CSIA-Cl) of organochlorines using gaschromatography- isotope ratio mass spectrometry (GC-IRMS) and gaschromatography-quadrupole mass spectrometry (GC-qMS). Comparable precisionsbetween the two instruments were achieved and trueness of the analysis resultswas confirmed. The CSIA-Cl method using GC-qMS was originally developed bySakaguchi-S\"oder et al.and further improved by several relevant studies,andhas been used to evaluate organic contaminant attenuation in the environment.The essential principle of the method is to calculate the chlorine isotoperatio (37Cl/35Cl) by using the first pair of neighboring chlorine isotopologues(two-mass apart) of either the molecular ion or a fragmental ion of a targetanalyte, or using all the first isotopologue pairs of all molecular andfragmental ions. These isotope-ratio calculation schemes using chlorineisotopologue pair(s) were based on the binomial theorem and the prerequisitehypothesis that the measured abundances of chlorine isotopologues of individualanalytes were binomially distributed. However, it is not true with thehypothesis.

Comparison and Evaluation of Isotope-Ratio Calculation Schemes for Compound-Specific Chlorine Isotope Analysis Using GC-EI-MS