TY - JOUR

T1 - Investigation of the Photocatalytic Hydrogen Production of Semiconductor Nanocrystal-Based Hydrogels

AU - Schlenkrich, Jakob

AU - Lübkemann-Warwas, Franziska

AU - T. Graf, Rebecca

AU - Wesemann, Christoph

AU - Schoske, Larissa

AU - Rosebrock, Marina

AU - D. J. Hindricks, Karen

AU - Behrens, Peter

AU - Банеманн, Детлеф Вернер

AU - Dorfs, Dirk

AU - C. Bigall, Nadja

PY - 2023/5/24

Y1 - 2023/5/24

N2 - Destabilization of a ligand-stabilized semiconductor nanocrystal solution withan oxidizing agent can lead to a macroscopic highly porous self-supportingnanocrystal network entitled hydrogel, with good accessibility to the surface.The previously reported charge carrier delocalization beyond a singlenanocrystal building block in such gels can extend the charge carrier mobilityand make a photocatalytic reaction more probable. The synthesis of ligandstabilizednanocrystals with specific physicochemical properties is possible,thanks to the advances in colloid chemistry made in the last decades. Combiningthe properties of these nanocrystals with the advantages of nanocrystalbasedhydrogels will lead to novel materials with optimized photocatalyticproperties. This work demonstrates that CdSe quantum dots, CdS nanorods,and CdSe/CdS dot-in-rod-shaped nanorods as nanocrystal-based hydrogelscan exhibit a much higher hydrogen production rate compared to their ligandstabilizednanocrystal solutions. The gel synthesis through controlled destabilizationby ligand oxidation preserves the high surface-to-volume ratio, ensuresthe accessible surface area even in hole-trapping solutions and facilitatesphotocatalytic hydrogen production without a co-catalyst. Especially with suchself-supporting networks of nanocrystals, the problem of colloidal (in)stabilityin photocatalysis is circumvented. X-ray photoelectron spectroscopy and photoelectrochemicalmeasurements reveal the advantageous properties of the 3Dnetworks for application in photocatalytic hydrogen production.

AB - Destabilization of a ligand-stabilized semiconductor nanocrystal solution withan oxidizing agent can lead to a macroscopic highly porous self-supportingnanocrystal network entitled hydrogel, with good accessibility to the surface.The previously reported charge carrier delocalization beyond a singlenanocrystal building block in such gels can extend the charge carrier mobilityand make a photocatalytic reaction more probable. The synthesis of ligandstabilizednanocrystals with specific physicochemical properties is possible,thanks to the advances in colloid chemistry made in the last decades. Combiningthe properties of these nanocrystals with the advantages of nanocrystalbasedhydrogels will lead to novel materials with optimized photocatalyticproperties. This work demonstrates that CdSe quantum dots, CdS nanorods,and CdSe/CdS dot-in-rod-shaped nanorods as nanocrystal-based hydrogelscan exhibit a much higher hydrogen production rate compared to their ligandstabilizednanocrystal solutions. The gel synthesis through controlled destabilizationby ligand oxidation preserves the high surface-to-volume ratio, ensuresthe accessible surface area even in hole-trapping solutions and facilitatesphotocatalytic hydrogen production without a co-catalyst. Especially with suchself-supporting networks of nanocrystals, the problem of colloidal (in)stabilityin photocatalysis is circumvented. X-ray photoelectron spectroscopy and photoelectrochemicalmeasurements reveal the advantageous properties of the 3Dnetworks for application in photocatalytic hydrogen production.

UR - https://doi.org/10.1002/smll.202208108

U2 - 10.1002/smll.202208108

DO - 10.1002/smll.202208108

M3 - Article

VL - 19

JO - Small

JF - Small

SN - 1613-6810

IS - 21

M1 - 2208108

ER -