4.6 Article

Stacking design in photocatalysis: synergizing cocatalyst roles and anti-corrosion functions of metallic MoS2 and graphene for remarkable hydrogen evolution over CdS

Journal

JOURNAL OF MATERIALS CHEMISTRY A
Volume 9, Issue 3, Pages 1552-1562

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/d0ta10255e

Keywords

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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. Self-Topic Fund of Zhejiang Normal University [2020ZS04]
  5. Research Fund of the Department of Education of Zhejiang Province [Y201738697]
  6. Foundation of Science and Technology Bureau of Jinhua [20204185]
  7. Open Research Fund of Key Laboratory of the Ministry of Education for Advanced Catalysis Materials
  8. Zhejiang Key Laboratory for Reactive Chemistry on Solid Surfaces, Zhejiang Normal University

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The novel stacked nanostructure of CdS embedded at interfaces between graphene supports and metallic MoS2 overlayers significantly enhances the photocatalytic performance, achieving a high H-2 production rate and apparent quantum efficiency far exceeding pure CdS, mainly due to the synergistic effects of MoS2 and graphene.
CdS has been regarded as a promising visible-light-response photocatalyst in H-2 production while its practical application is often limited by low photoactivity and serious photocorrosion. To tackle these problems, traditional CdS based core-shell and supported photocatalysts have been widely developed but they also suffer from intrinsic structural drawbacks. Herein, a novel stacked nanostructure with CdS embedded at interfaces between graphene supports and metallic MoS2 overlayers has been designed to eliminate the shortages and achieve outstanding photocatalytic performance, which reaches an optimum H-2 production rate of 14.4 mmol gcat(-1) h(-1) and realizes an apparent quantum efficiency of 23.7% at 420 nm without obvious deterioration of activity in 20 h cyclic testing, far exceeding that of pure CdS by a factor of 17.9 times. The enhanced photocatalytic performance is mainly ascribed to the synergistic effects of MoS2 and graphene: (1) the intimate contact between the CdS core and MoS2 shell with a large interfacial area favors the transfer of photogenerated electrons to MoS2 cocatalysts, while a high-percentage 1T-phase provides an excellent electron mobility in the MoS2 cocatalysts and a high density of active sites for H-2 evolution; (2) CdS cores are protected by MoS2 and graphene from photocorrosion, in which photogenerated holes are quickly transferred to the MoS2 shell and isolated from the sulfide surface, while excessive electrons in CdS are shuttled to adjacent MoS2 outer layers by graphene supports for H-2 evolution in reducing their recombination with holes in the MoS2 shell and increasing the number of MoS2 sites available for the proton reduction reaction. The stacking design can be extended to the fabrication of other highly efficient photocatalytic systems.

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