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The release of anthropogenic toxic pollutants into the atmosphere is a worldwide threat of growing concern. In this regard, it is possible to take advantage of the high versatility of MOFs materials in order to develop new technologies for environmental remediation purposes. Consequently, one of the main scientific challenges to be achieved in the field of MOF research should be to maximize the performance of these solids towards the sensing, capture and catalytic degradation of harmful gases and vapors by means of a rational control of size and reactivity of the pore walls that are directly accessible to guest molecules.