Rational Construction of Two-Dimensional Conjugated Metal-Organic Frameworks for Electronics and Beyond

Two-dimensional conjugated metal-organic frameworks (2D c-MOFs) have emerged as a novel class of multifunctional materials, attracting increasing attention due to their highly customizable chemistry yielding programmable and unprecedented structures and properties. In this talk, we summarize and discuss our efforts to achieve full control at the atomic level over the structure of 2D c-MOFs and their applications in electronics and spintronics, thereby providing distinct evidence on 2D c-MOFs as a promising platform for exploring novel quantum phenomena. Firstly, we unravel the key role played by the rational design of the ligands to decrease the boundary defects, achieve atomically precise large single crystals, and investigate the intrinsic charge transport properties of 2D c-MOFs. The advantages and disadvantages of the current structural elucidation strategies will be discussed. Secondly, the fundamental challenge in 2D c-MOF charge transport studies is to decouple the in-plane and interlayer charge transport pathways and achieve precise tuning of the charge transport properties in 2D c-MOFs. To address this challenge, we propose a design concept for the 2^nd-generation conjugated ligands, termed "programmable conjugated ligands," to replace the current 1^st-generation ligands which lack modifiability as they mainly consist of <i>sp</i>² hybridization atoms. Our efforts also extend to controlling the spin dynamics properties of 2D c-MOFs as "spin concentrated assemblies" using a bottom-up strategy.<br/><br/>Reference：<br/>1. <i>Angew. Chem. Int. Ed. </i><b>2022,</b> <i>61</i> (39), e202208163.；<br/>2. <i>Nat. Commun. </i><b>2022,</b> <i>13</i> (1), 7240.；<br/>3. <i>J. Am. Chem. Soc. </i><b>2024,</b> <i>146</i> (4), 2574-2582..