Cu(II) oxo/hydroxides stabilized by ZSM-5 zeolite as an efficient and robust catalyst for chemical and photochemical water oxidation with Ru(bpy)33+

Описание

Тип публикации: статья из журнала

Год издания: 2020

Идентификатор DOI: 10.1016/j.cattod.2020.07.009

Ключевые слова: cu(ii)-hydroxides, one-electron oxidant, oxygen evolution reaction, photocatalytic water splitting, zeolites

Аннотация: Water oxidation is the bottleneck of the water splitting process. A novel highly efficient and stable for many cycles heterogeneous Cu-contained catalysts supported on MFI-type zeolite (1% Cu-ZSM-5) for water oxidation were prepared. Oxo/hydroxo complexes of copper (II) were stabilized in the zeolite channels via polycondensation. Показать полностьюThe analysis of the electron states of copper in the Cu-containing zeolite-based catalysts using EPR and UV–vis DR techniques revealed that the catalytic efficiency of Cu(II) state in zeolite grew up in the series: [Cu(NH3)4]2+ < isolated [Cu(H2O)6]2+ << Cu(OH)x-like and CuOx-like nanoclusters in mesopores << CuOx-like and Cu(OH)x-like complexes in channels < [Cu2(OH)2]2+ complexes in channels. The catalyst containing [Cu2(OH)2]2+ complexes in channels provided the yields of oxygen as high as 60 and 64 % of the stoichiometric quantity at pH 9.2–10.0 in the dark reaction with one-electron oxidant Ru(bpy)33+. Nevertheless, Cu(OH)x-like and [Cu2(OH)2]2+ complexes stabilized in the ZSM-5 channels decomposed easily under the conditions of the photocatalytic reaction. At the same time, the oxygen yield reached 92 % in photocatalytic system Ru(bpy)32+/S2O82− in the presence of 1%Cu-ZSM-5 containing CuOx-like complexes stabilized in the channels. The adsorption of Ru(bpy)32+ on the surface of 1%Cu-ZSM-5 containing CuOx-like complexes provided the increase of the reaction rate in 1.6 times and achieved the oxygen yield up to 98 % to stoichiometry. This indicated the strong effect of concurrent processes of Ru(bpy)32+ and Ru(bpy)33+ adsorption/desorption at the catalyst active site on the rate of oxygen evolution. © 2020

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Издание

Журнал: Catalysis Today

ISSN журнала: 09205861

Издатель: Elsevier B.V.

Персоны

  • Chikunov Andrey S. (RAS, SB, Boreskov Inst Catalysis, Lavrentieva Ave 5, Novosibirsk 630090, Russia)
  • Yashnik Svetlana A. (RAS, SB, Boreskov Inst Catalysis, Lavrentieva Ave 5, Novosibirsk 630090, Russia)
  • Taran Oxana P. (RAS, SB, Boreskov Inst Catalysis, Lavrentieva Ave 5, Novosibirsk 630090, Russia; RAS, SB, Inst Chem & Chem Technol, FRC,KSC, Akademgorodok St 50-24, Krasnoyarsk 660036, Russia; Siberian Fed Univ, Svobodny Ave 79, Krasnoyarsk 660041, Russia)
  • Kurenkova Anna Y. (RAS, SB, Boreskov Inst Catalysis, Lavrentieva Ave 5, Novosibirsk 630090, Russia)
  • Parmon Valentin N. (RAS, SB, Boreskov Inst Catalysis, Lavrentieva Ave 5, Novosibirsk 630090, Russia)