4.8 Article

Interface-Confined Surface Engineering via Photoelectrochemical Etching toward Solar Neutral Water Splitting

Journal

ACS CATALYSIS
Volume 12, Issue 3, Pages 1686-1696

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acscatal.1c05263

Keywords

interface and surface recombination; transition metal oxides; photoelectrochemical etching; charge transfer; solar neutral water splitting

Funding

  1. National Natural Science Foundations of China [51802320, 21965024]
  2. 111 project [D20033]
  3. Central Government Guiding Special Funds for the Development of Local Science and Technology [2020ZY0012]
  4. Inner Mongolia funding for Distinguished Young Scholars [2020JQ01]
  5. Young Science and Technology Talents Cultivation project of Inner Mongolia University [21221505]
  6. Inner Mongolia University [21300-5195102]
  7. opening project of Key Laboratory of Materials Processing and Mold from Zhengzhou

Ask authors/readers for more resources

This study demonstrates the importance of interface-confined surface modification in modulating charge transfer pathways for efficient solar energy conversion. By using a PEC reduction strategy, the interface-confined CoMoO4-x/BiVO4 system exhibits excellent photocorrosion resistance and long-term stability, showing potential for high-performance photoelectrode design in a neutral environment.
Photogenerated electron-hole recombination arising from the interface/surface among semiconductor/cocatalyst/electrolyte becomes prominent for photoelectrochemical (PEC) water splitting, which principally retards the charge transfer pathways and reduces the oxygen reaction kinetics, especially in a neutral environment. Herein, interface-confined surface engineering via a PEC reduction strategy was carried out on a semiconductor/transition metal oxide system in a neutral electrolyte, which can remove the interfacial charge recombination and mediate the charge transfer pathways, and importantly stabilize the semiconductor for a long-term operation. Surface-confined CoMoO4-x/BiVO4 exhibits a current density of 3.5 mA cm(-2) at 1.23 V-RHE under 1 sun irradiation with an excellent stability for 20 h in 0.5 M Na2SO4, showing one of the best photocorrosion resistance performances among BiVO4 photoelectrodes under near-neutral pH conditions. A comparable PEC activity and stability were achieved using pristine BVO, CoOx/BiVO4, and MoOx/BiVO4 with the PEC etching, which clarify the mechanism of the reduced barrier layer and the defected CoMoO4-x catalysts in boosting the charge transfer efficiency and stabilizing BiVO4. Meanwhile, CoOx acts as a promoter enhancing PEC activity and MoOx acts as a passivation layer protecting the semiconductor from photocorrosion. This work sheds light on that the interface-confined surface modification plays an essential role in modulating the charge transfer pathways, especially for a reaction occurring on a surface, which may lead to a new direction of using a neutral environment for high-performance photoelectrode design toward achieving efficient solar energy conversion.

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