Highly Efficient Photocatalytic Hydrogen Evolution Using a Self‐Assembled Octupolar Molecular System. Issue 1 (6th October 2022)

• Record Type: Journal Article
• Authors: Lee, Hyun‐Jun; Abudulimu, Abasi; Roldao, Juan Carlos; Nam, Hyunwoo; Gierschner, Johannes; Lüer, Larry; Park, Soo Young
• Is Part Of: ChemPhotoChem. Volume 7:Issue 1(2023)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2022-10-06
• Subjects: hydrogen evolution -- intersystem crossing -- photocatalysis -- self-assembly -- water splitting; Photochemistry -- Periodicals; Periodicals; Electronic journals; 541.35
• DOI: 10.1002/cptc.202200177
• Languages: English
• ISSNs: 2367-0932

Abstract

Abstract: A highly efficient photocatalytic hydrogen evolution system was prepared by using an octupolar molecule as a building block of self‐assembled nanoparticles. The photocatalytic system showed an enhanced hydrogen evolution reaction (HER) rate upon the addition of halide ions, which was attributed to an external heavy atom effect enhancing intersystem crossing. The HER rate of the photocatalytic system was proportional to the atomic weight and concentration of halide ion additives, and its maximum HER rate reached 460 mmol/g ⋅ h in the presence of iodide ions and a metal co‐catalyst. Further, the photocatalytic system without any halide ion additives generated hydrogen gas utilizing seawater and stimulated sunlight with remarkable efficiency (apparent quantum yield∼3.8 %). Abstract : An octupolar molecule with excellent visible light absorption and strong intramolecular charge transfer characteristics was designed and synthesized. In aqueous solution, the molecules self‐assemble into positively charged nanoparticles. The optimized self‐assembled system (composed of nanoparticles with platinum and halide additives) reached a maximum hydrogen evolution rate of 460 mmol/g ⋅ h.