Our group has recently shown that thermolabile crosslinkers can be used to template pairs of functional groups in metal-organic framework pores at specific relative distances and orientations. For example, we have used tertiary ester and tertiary carbamate-based crosslinkers to template pairs of carboxylic acids and pairs of amines in the terphenyl-expanded MOF-74 framework, also known as Mg2dotpdc (dotpdc 4-= 4,4″-dioxido-[1,1′:4′,1″-terphenyl]-3,3″-dicarboxylate) (Fig. ). This framework contains large, one-dimensional hexagonal channels (~3 nm) framed by tightly packed ligand struts (~7 Å apart). Mg2dotpdc (abbreviated 1) and other frameworks with similar 1D channels are attractive supports for bifunctional catalysis, as they provide large pore diameters while still maintaining short distances between adjacent ligands.