A Hydrolytically Stable Metal–Organic Framework for Simultaneous Desulfurization and Dehydration of Wet Flue Gas

Abstract Metal–organic frameworks (MOFs) have great prospects as adsorbents for industrial gas purification, but often suffer from issues of water stability and competitive water adsorption. Herein, we present a hydrolytically stable MOF that could selectively capture and recover trace SO 2 from flue gas, and exhibits remarkable recyclability in the breakthrough experiments under wet flue‐gas conditions, due to its excellent resistance to the corrosion of SO 2 and the water‐derived capillary forces. More strikingly, its SO 2 capture efficiency is barely influenced by the increasing humidity, even if the pore filling with water is reached. Mechanistic studies demonstrate that the delicate pore structure with diverse pore dimensions and chemistry leads to different adsorption kinetics and thermodynamics as well as segregated adsorption domains of SO 2 and H 2 O. Significantly, this non‐competitive adsorption mechanism enables simultaneous desulfurization and dehydration by a single adsorbent, opening an avenue toward cost‐effective and simplified processing flowcharts for flue gas purification.