Intrinsic hydrogen evolution capability and a theoretically supported reaction mechanism of a paddlewheel-type dirhodium complex

Dalton Transactions : an International Journal of Inorganic Chemistry
Yusuke KataokaTatsuya Kawamoto

Abstract

The intrinsic capability of the paddlewheel-type dirhodium tetraacetate complex, [Rh2(O2CCH3)4(H2O)2] ([1(H2O)2]), as a hydrogen evolution catalyst (HEC) for photochemical hydrogen evolution from aqueous solution was illustrated. This was achieved by using an optimized artificial photosynthesis (AP) system with a cyclometalated iridium complex [Ir(ppy)2(bpy)](PF6) ([Ir-PS-1]) and triethylamine (TEA) serving as a photosensitizer (PS) and a sacrificial donor, respectively. The total amount of hydrogen evolution and the turnover number (TON) of catalysis using this AP system were 385.7 μmol and 3857 (per Rh ion), respectively; these values are higher than those of [Rh(dtBubpy)3](PF6)3, which is the most efficient HEC among the mononuclear rhodium complexes, and RhCl3. Moreover, the catalytic performance of [1(H2O)2] was further accelerated by using [Ir(ppy)2(dtBubpy)](PF6) [Ir-PS-3] as a PS; 9886 TON (H2 per Rh ion) was verified after 12 h of irradiation. In addition, the detailed mechanism of hydrogen evolution catalyzed by [1(H2O)2] was clarified by combining electro- and photochemical analyses and DFT calculations. The optimized geometries of [1(H2O)2], [1], hydride intermediates [H-Rh2(O2CCH3)4] ([H-1]), and their reduced spec...Continue Reading

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Citations

Feb 6, 2020·Dalton Transactions : an International Journal of Inorganic Chemistry·Giarita FerraroAntonello Merlino
Aug 26, 2020·Dalton Transactions : an International Journal of Inorganic Chemistry·Yusuke KataokaTatsuya Kawamoto
Jul 3, 2019·Dalton Transactions : an International Journal of Inorganic Chemistry·Yusuke KataokaMakoto Handa
Jan 20, 2021·Chemical Communications : Chem Comm·Hemanthi D ManamperiClaudia Turro
Feb 6, 2021·International Journal of Molecular Sciences·Domenico LoretoAntonello Merlino
Jul 17, 2021·Inorganic Chemistry·Pondchanok ChinapangShigeyuki Masaoka

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Methods Mentioned

BETA
dynamic light scattering
X-ray

Software Mentioned

TEA
Gaussian

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