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Maintaining human thermal comfort and extensive power consumption of the conventional heating ventilating and air-conditioning systems drive the researchers to look for an alternative dehumidification system. Among the potential alternatives, the liquid desiccant dehumidification system has evolved as a long-term renewable and less power consuming system due to its effective controlling capability of humidity. In the present study, an experimental investigation is carried out to demonstrate the performance of lithium bromide (LiBr) and potassium formate (HCOOK) desiccant solution mixture in a spray type counterflow-packed bed adiabatic dehumidifier. Subsequently, ternary plots and 3D-contour trade-off paradigms are patterned to assess the performance parameters using an optimal mixture design methodology. Additionally, empirical correlations are developed to pattern the performance parameters (moisture removal rate (MRR), enthalpy effectiveness (ξh) and moisture effectiveness (ξm)) as a function of blend combinations. Further, the present study endeavours to explore the application of offline calibration methods based on a balanced optimum mixture design-centred desirability approach for optimizing the mixture proportion to obtain the optimal performance parameters (i.e., MRR, ξh and ξm). The wettability area is explained based on the static contact angle on a plane glass. The results showed that the contact angle was decreased from 47.3° to 44.1° for the optimum mixture of LiBr solution (37.2%-LiBr +17.8%-HCOOK), which further confirmed the higher MRR. Lastly, the tuning effect of the liquid to gas flow rate on the dehumidifier performance and economic viability of LiBr-HCOOK blends are studied.