Surface etching induced ultrathin sandwich structure realizing enhanced photocatalytic activity

Bo Yang; Wentuan Bi; Yangyang Wan; Xiaogang Li; Mingcan Huang; Ruilin Yuan; Huanxin Ju; Wangsheng Chu; Xiaojun Wu; Linghui He; Changzheng Wu; Yi Xie

doi:10.1007/s11426-018-9314-4

SCIENCE CHINA Chemistry

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SCIENCE CHINA Chemistry, Volume 61, Issue 12: 1572-1580(2018) https://doi.org/10.1007/s11426-018-9314-4

Surface etching induced ultrathin sandwich structure realizing enhanced photocatalytic activity

Bo Yang¹, Wentuan Bi¹, Yangyang Wan^1,2, Xiaogang Li¹, Mingcan Huang¹, Ruilin Yuan¹, Huanxin Ju³, Wangsheng Chu³, Xiaojun Wu^1,2, Linghui He¹, Changzheng Wu^1,*, Yi Xie¹

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ReceivedMay 10, 2018
AcceptedJun 20, 2018
PublishedSep 21, 2018

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Abstract

Photocatalytic conversion efficiency is limited by serious charge carrier recombination. Efficient carrier separation is usually achieved by elegantly-designed multi-component structures connected by directional electric field. Herein, we developed a two-dimensional (2D) sandwich structure, as a new photocatalytic system, to realize high-efficiency carrier separation. This strategy integrated multifunction into a single structure for the first time, which successfully introduces a stable built-in electric field, realizing high-effective carrier separation. Besides, the carrier concentration is dramatically increased due to dimensional confinement. Benefiting from above synergic advantages, 2D sandwich photocatalyst achieves the highest nitrogen fixation rate (435?μmol?g^?1?h^?1) in inorganic solid photocatalysts under visible light irradiation. We anticipate that 2D sandwich photocatalyst holds promises for the application and expansion of 2D materials in photocatalysis research.

Funded by

the National Basic Research Program of China(2015CB932302)

the National Natural Science Foundation of China(U1432133,11321503,21701164)

the National Young Top-Notch Talent Support Program

the Chinese Academy of Sciences(XDB01020300)

the Fok Ying-Tong Education Foundation(141042)

the Fundamental Research Funds for the Central Universities(WK2060190027,WK2060190058)

Acknowledgment

This work was supported by the National Basic Research Program of China (2015CB932302), the National Natural Science Foundation of China (U1432133, 11321503, 21701164), the National Young Top-Notch Talent Support Program, the Chinese Academy of Sciences (XDB01020300), the Fok Ying-Tong Education Foundation (141042), the Fundamental Research Funds for the Central Universities (WK2060190027, WK2060190058). We would like to thank beamline BL14W1 (Shanghai Synchrotron Radiation Facility) and the Catalysis and Surface Science Endstation (National Synchrotron Radiation Laboratory) for providing the beam time.

Interest statement

The authors declare that they have no conflict of interest.

Contributions statement

These authors contributed equally to this work.

Supplement

Supporting Information

The supporting information is available online at http://chem.scichina.com and http://link.springer.com/journal/11426. The supporting materials are published as submitted, without typesetting or editing. The responsibility for scientific accuracy and content remains entirely with the authors.

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Figure 1
Characterizations for the pristine and etching BiOBr nanosheet. (a) XRD pattern. (b) Raman spectra. (c, d) Top and side view of HR-TEM image for pristine sample. (e, f) Top and side view of HR-TEM image for sandwiched sample, there is a very thin layer observed on the surface of the nanosheets after irradiation (color online).
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Scheme 1
(a) Sandwich structure of two-dimensional (2D) photocatalyst. (b) The preparation process of the sandwich structure of two-dimensional photocatalyst using the facile surface etching technique. Photo-assisted surface etching with partial Br ion removal, leads to the formation of the structure of surface Bi-O layer (color online).
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Figure 2
High-resolution synchrotron radiation photoelectron spectroscopy (HR-SRPES) spectra of sandwiched samples. (a) Br 3d, (b) Bi 4f. High-resolution X-ray photoelectron spectroscopic (HR-XPS) spectra. (c) Br 3d, (d) Bi 4f (color online).
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Figure 3
Extended X-ray absorption fine spectroscopy. (a) The Bi L₂-edge extended EXAFS oscillation, and (b) corresponding Fourier transform (FT) for the pristine and sandwiched BiOBr nanosheet (color online).
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Figure 4
Photo and electrical properties for the pristine and sandwiched BiOBr nanosheet. (a) UV-vis absorption spectra (inset is the plots of (αhν)^1/2 vs. the photon energy (hν)). (b) Valence-band spectra measured by SRPES. (c) Schematic illustration of the band structure. (d) The charge density difference for sandwiched BiOBr. The yellow and blue isosurfaces represent charge accumulation and depletion in the space, respectively (color online).
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Figure 5
Charge transport properties for the pristine and sandwiched BiOBr nanosheet. (a) Room-temperature steady-state PL spectra. (b) Time-resolved PL spectra for the pristine and sandwiched BiOBr nanosheet. (c) Surface photovoltage spectra. (d) EIS Nyquist plots. (e) Mott-Schottky plots. (f) Transient OCVD measurements after exposure to visible light irradiation. (g) Average lifetimes of the photogenerated carriers (τ_n) obtained from the OCVD measurements (color online).
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Figure 6
(a) Photocatalytic N₂ reduction performance comparisons for the pristine and sandwiched BiOBr nanosheet. (b) Comparison of visible light nitrogen fixation rate for the pristine and sandwiched BiOBr nanosheet. (c) Comparison of NH₃ and O₂ yield on sandwiched BiOBr. (d) Multicycle N₂ fixation with sandwiched BiOBr nanosheet (color online).