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Procalcitonin (PCT) has been used to guide treatment in critically ill patients with sepsis, but whether PCT at intensive care unit (ICU) discharge can stratify risks of post-ICU readmission or mortality is unknown. This cohort study compared the ability of PCT with C-reactive protein (CRP) in predicting unexpected adverse post-ICU events. Of the 1877 patients admitted to the multidisciplinary ICU between 1 April 2012 and 31 March 2014, 1653 (88.1%) were discharged without treatment limitations. A total of 71 (4.3%) were readmitted and 18 patients (1%) died unexpectedly after ICU discharge during the same hospitalization. Both PCT (0.6 vs 0.4 μg/L, P = .002) and a high CRP concentration > 100 mg/L (58% vs 41%, P = .004) at ICU discharge were associated with an increased risk of adverse post-ICU events in the univariate analyses; however, the ability of PCT to discriminate between patients with and without adverse post-ICU outcomes was limited (area under the receiver operating characteristic curve = 0.61; 95% confidence interval, 0.55–0.66). In the multivariable analysis, only a high CRP concentration (odds ratio, 1.92; 95% confidence interval, 1.12–3.11; P = .008) was associated with an increased adverse post-ICU events. Elevated PCT concentration at ICU discharge was inadequate in its predictive ability to guide ICU discharge.