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A series of anion‐functionalized pillararenes were prepared and applied in the capture of SO2 through incorporating an anion with different basicity into pillararenes. A high SO2 absorption capacity up to 15.9 mmol g−1 and excellent reversibility were achieved by tuning the basicity of the anion and the size of the cavity. Spectroscopic investigations and DFT calculations indicated that high SO2 capacity...
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