4.8 Article

Emerging Stacked Photocatalyst Design Enables Spatially Separated Ni(OH)2 Redox Cocatalysts for Overall CO2 Reduction and H2O Oxidation

Journal

SMALL
Volume 18, Issue 9, Pages -

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/smll.202104681

Keywords

CO; (2) reduction; H; O-2 oxidation; photocatalysis; redox cocatalysts; stacked design

Funding

  1. National Natural Science Foundation of China [21603191]
  2. Zhejiang Provincial Natural Science Foundation of China [LY20B030003, LQ16B010001]
  3. Public Welfare Technology Application Research Plan Project of Zhejiang Province [2017C37024]
  4. Foundation of Science and Technology Bureau of Jinhua [20204185]
  5. Self-Topic Fund of Zhejiang Normal University [2020ZS04]
  6. Open Research Fund of Key Laboratory of the Ministry of Education for Advanced Catalysis Materials
  7. Zhejiang Key Laboratory for Reactive Chemistry on Solid Surfaces, Zhejiang Normal University

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The study demonstrates a strategy for spatial separation of redox cocatalysts on various semiconductors through a unique stacked photocatalyst design, showing superior activity and stability. This smart design helps mitigate charge recombination, provide highly active and selective sites, and protect semiconductors from photocorrosion.
Construction of photocatalytic systems with spatially separated dual cocatalysts is considered as a promising route to modulate charge separation/transfer, promote surface redox reactivities, and prevent unwanted reverse reactions. However, past efforts on the loading of spatially separated double-cocatalysts are limited to hollow structured semiconductors with inner/outer surface and monocrystalline semiconductors with different exposed facets. To overcome this limitation, herein, enabled by a unique stacked photocatalyst design, a facile and versatile strategy for spatial separation of redox cocatalysts on various semiconductors without structural and morphological restriction is demonstrated. The smart design begins with the deposition of light-harvesting semiconductors on reduced graphene oxide (rGO) nanosheets, followed with the coverage of Ni(OH)(2) outer layer. The ternary photocatalysts exhibit superior activities and stabilities of H2O oxidation and selective CO2-to-CO reduction, remarkably surpassing other counterparts. The origin of the enhanced performance is attributed to the synergistic interplay of rGO@Ni(OH)(2) reduction cocatalysts surrounding the semiconductors and Ni(OH)(2) oxidation cocatalysts directly supported by the semiconductors, which mitigates the charge recombination, supplies highly active and selective sites for overall reactions, and preserves the semiconductors from photocorrosion. This work presents a new approach to regulating the position of dual cocatalysts and ameliorating the net efficiency of photoredox catalysis.

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