Carbon nanodots for all-in-one photocatalytic hydrogen generation

Jana, Bikash; Reva, Yana; Scharl, Tobias; Strauß, Volker; Cadranel, Alejandro; Guldi, Dirk M.

doi:10.1021/jacs.1c07049

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Carbon nanodots for all-in-one photocatalytic hydrogen generation

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Strauß, Volker
Volker Strauß, Kolloidchemie, Max Planck Institute of Colloids and Interfaces, Max Planck Society;

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引用

Jana, B., Reva, Y., Scharl, T., Strauß, V., Cadranel, A., & Guldi, D. M. (2021). Carbon nanodots for all-in-one photocatalytic hydrogen generation. Journal of the American Chemical Society, 143(48), 20122-20132. doi:10.1021/jacs.1c07049.

引用: https://hdl.handle.net/21.11116/0000-0009-9543-3

要旨

Carbon nanodots (CNDs) were photochemically altered to produce dihydrogen under light irradiation. Within the complex structure of CNDs, photo-oxidation takes place at citrazinic acid molecular fluorophore sites. Important is the fact that the resulting CND materials have a dual function. On one hand, they absorb light, and on the other hand, they photo- and electrocatalytically produce dihydrogen from water and seawater, without any external photosensitizer or cocatalyst. Record HER activities of 15.15 and 19.70 mmol(H₂) g(catalyst)⁻¹ h^–1 were obtained after 1 h of 75 mW/cm² Xe lamp illumination, from water and seawater, respectively. This impressive performance outweighs the remaining structural uncertainties. A full-fledged physicochemical investigation based on an arsenal of steady-state and time-resolved spectroscopic characterizations together with microscopy enabled a comprehensive look into the reaction mechanism. For an efficient dihydrogen formation, a precatalytic activation by means of reduction with a sacrificial electron donor is imperative.