Enhancing Photocatalytic Attributes of Perovskite Nanocrystals in Aqueous Media via Ligand Engineering

Abstract

The remarkable catalytic potential of perovskite nanocrystals (NCs) remains underutilized due to their limited stability in polar media, resulting from the vulnerability of their structure to disruption by polar solvents. In this study, we address this challenge by employing the bolaamphiphilic NKE-12 ligand, which features multiple denticities to effectively shield the surface of CsPbBr 3 NCs from polar solvent interactions without compromising their light-harvesting properties. Our research, utilizing electrochemical impedance and photocurrent response measurements, highlights efficient charge separation and charge transfer enabled by NKE-12 ligands, which feature multiple ionic groups and peptide bonds, compared to conventional oleylamine/oleic acid ligands on CsPbBr 3 NCs. Through the utilization of purely ligand-derived water-dispersed CsPbBr 3 /NKE-12 NCs, we successfully showcased their photocatalytic activity for acrylamide polymerization. A series of control experiments unveil a radical-based reaction pathway and suggest the synergistic involvement of photogenerated electrons and holes in producing the O 2•− and OH • free radicals, respectively. Our findings emphasize the crucial role of ligand engineering in stabilizing perovskites in water and harnessing their exceptional photocatalytic attributes. This study opens new avenues for applying perovskite NCs in various catalytic processes in polar media.

Metal Halide Perovskite Nanocrystals for C–X Activation: Role of Halide Vacancies

“…This delicate balance necessitates careful optimization to maximize the efficiency of C–X bond activation. Recent studies have explored this concept, aiming to strike a balance between ligands promoting adsorption while simultaneously allowing access to active sites. ,− …”

Insights into interfacial mechanisms: CsPbBr3 nanocrystals as sustainable photocatalysts for primary amine oxidation

“…1,2 Recent studies have unveiled their potential as photocatalysts in reactions such as water splitting, CO 2 reduction, dye degradation, polymerization, and organic synthesis. 3–12 However, LHPs face challenges due to their structural instability in polar solvents. To address this, various strategies, including ligand engineering, surface encapsulation, and heterojunction formation, have been explored.…”