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The purification of C2H4 from C2H6/C2H4/C2H2 mixtures is of great significance in the chemical industry for C2H4 production but remains a daunting task. Guided by powerful reticular chemistry principles, herein a systematic study is carried out to engineer pore dimensions and pore functionality of fcu‐type Y‐based metal–organic frameworks (Y‐MOFs) through the construction of a series of eight new...