Development of functional conjugated two-dimensional metal-organic frameworks
Metal-organic frameworks (MOFs) have been highlighted for catalysis, gas storage and separation. However, due to low conductivity (<1E-8 S/cm), weak magnetic interaction as well as difficult device integration, the application of bulk 3D MOFs in (spin-)electronics is challenging. Recent advances disclose that the designs of conjugated 2D MOFs (C2DMOFs) have led to improved intrinsic conductivity (up to 1000 S/cm). However, the related research remains immature due to lack of high-quality film samples, very limited structural types and elusive transport mechanism. In this project, we will develop unprecedented magnetic (semi-)conductive C2DMOFs and accomplish electronic/magnetic structure engineering for functions in electronics and spintronics. Here, we will synthesize novel conjugated monomers to tune geometries and pore sizes of C2DMOFs, thus achieving in-plane engineering on charge and spin distribution. We will develop versatile synthesis strategies towards highly crystalline C2DMOF films/nanosheets: (1) develop solvothermal synthesis and subsequent electrochemical exfoliation of layer-stacked bulk samples into 2D nanosheets; (2) develop air/liquid and liquid/liquid interfacial synthesis of large-area single-/few-layer films; (3) particularly establish a ground-breaking chemical vapor deposition (CVD) synthesis route for “clean” single-crystalline films. We will further establish unprecedented C2DMOF-based 2D-2D van der Waals heterostructures (vdWHs) with other inorganic 2D crystals to realize out-of-plane engineering on band gaps and unique interfacial transport characteristics. By employing the developed C2DMOFs and vdWHs, we will explore magnetism and temperature-/magnetic field-depended charge transport properties. As the key achievements, we expect to establish novel electronic/magnetic structures and general synthesis strategies, delineation of reliable structure-transport relationships and superior device performance of C2DMOFs.