Metal-organic framework (MOF) activation is crucial for the use of MOFs in several applications and solvent-exchange process is a necessary step in many activation methods. In this contribution, we have explored in situ MOF monolayer film formation at the air-water interface. Nanoparticles (NPs) of the Al trimesate MIL-96(Al) retain chloroform into their micropores, which considerably diminishes the CO2 adsorption capacity of MOF films. However, a solvent-exchange process between chloroform and water increases CO2 film adsorption capacity by 30%. Total Reflection X-Ray Fluorescence (TRXF) allows studying the kinetics of this process at the air-water interface, that strongly depends on the NP size. The conclusions derived from in situ studies allow optimizing the ex situ activation procedure of MIL-96(Al) films deposited onto quartz crystal microbalance (QCM) substrates in order to maximize CO2 and methanol adsorption. (C) 2021 Elsevier Inc. All rights reserved.