The urgency to mitigate carbon dioxide (CO2) emissions and combat climate change has spurred the development of effective CO2 capture technologies. One of the industry’s most well-known CO2 collection processes is CO2 absorption utilizing amine solvents. However, designing a successful amine scrubbing system in power plants requires precise prediction of CO2 absorption in aqueous amine solutions under various operating circumstances. Using aqueous piperazine (PZ) solutions for chemical absorption is promising due to the favorable reactivity of PZ with CO2. In this study, a comprehensive evaluation of PZ solution performance in CO2 capturing, employing the white-box algorithms, namely, Genetic Programming (GP), Gene Expression Programming (GEP), and Group Method of Data Handling (GMDH), was performed. Through extensive experimentation and data analysis, several correlations were developed with high and acceptable R2 values, such as 0.933 for GP, 0.949 for GEP, and 0.889 for GMDH, which shows high accuracy and reliability in predicting the CO2 capture efficiency of PZ solutions under varying operating conditions. The results of sensitivity analysis revealed that CO2 partial pressure increased CO2 absorption, while PZ concentration and temperature had negative and decreasing effects. These insights provide essential guidance for optimizing process conditions to enhance the CO2 capture efficiency. Finally, the leverage method was used to assess the reliability of both experimental and predicted data from white-box algorithms. This analysis identified potential outliers and validated the accuracy of the model’s predictions, enhancing the credibility of developed correlations and demonstrating the robustness of the approach.