Photoconductive Coordination Polymer with a Lead-Sulfur Two-Dimensional Coordination Sheet Structure

Area of Science:

• Materials Science
• Solid-State Chemistry
• Photocatalysis

Background:

• Coordination polymers with metal-sulfur (M-S) bonds exhibit promising optical properties and photocatalytic potential for water splitting.
• Limited structural data exists for these materials due to low crystallinity, hindering comprehension of their properties.
• Understanding the structure-property relationships is crucial for advancing M-S bond-containing materials.

Purpose of the Study:

• To conduct a structural investigation of a novel, highly crystalline coordination polymer featuring M-S bonds.
• To elucidate the photoconductivity mechanism of this material through theoretical calculations.
• To synthesize and characterize a new M-S coordination polymer for potential applications.

Main Methods:

• Synthesis and single-crystal X-ray diffraction of the coordination polymer [Pb(tadt)] (KGF-9).
• Spectroscopic analyses including diffuse-reflectance UV-Vis-NIR, time-resolved microwave conductivity, and photoelectron yield spectroscopy.
• First-principles calculations and direct-current photoconductivity measurements on single crystals.

Main Results:

• A novel, highly crystalline, three-dimensional coordination polymer, KGF-9 ([Pb(tadt)]), was successfully synthesized.
• Single-crystal X-ray diffraction revealed a 3D structure with an embedded 2D Pb-S framework.
• Experimental and theoretical studies elucidated the material's photoconductivity mechanism.

Conclusions:

• The synthesized KGF-9 represents a significant advancement in understanding crystalline M-S coordination polymers.
• The detailed structural and photoconductivity insights pave the way for designing advanced photocatalytic materials.
• This work overcomes previous limitations in structural characterization, enabling deeper exploration of M-S materials.