Monodisperse Ni-clusters anchored on carbon nitride for efficient photocatalytic hydrogen evolution

doi:10.1016/S1872-2067(21)63865-2

Abstract

Abstract:

The active sites of monodisperse transition metal Ni-clusters were anchored on carbon nitride (CN) by an in situ photoreduction deposition method to promote the efficient separation of photogenerated charges and achieve high-efficiency photocatalytic activity for hydrogen evolution. The Ni-cluster/CN exhibited a photocatalytic hydrogen production rate of 16.5 mmol·h ^-1·g ^-1 and a total turnover frequency (TOF (H₂)) value of 461.14 h ^-1. X-ray absorption spectroscopy based on synchrotron radiation indicated that CN had two reaction centers to form stable interface interactions with monodispersed Ni-clusters, in which carbon can act as an electron acceptor, while nitrogen can act as an electron donor. Meanwhile, the hybrid electronic structure of the Ni-cluster/CN system was constructed, which was favorable for photocatalytic activity for hydrogen production. An in-depth understanding of the interfacial interaction between CN and Ni-clusters will have important reference significance on the mechanistic study of development based on the cocatalyst.

Key words: Monodisperse Ni-clusters, Carbon nitride, Interface interaction, Photocatalytic hydrogen evolution

Liang Jian, Huizhen Zhang, Bing Liu, Chengsi Pan, Yuming Dong, Guangli Wang, Jun Zhong, Yongjie Zheng, Yongfa Zhu. Monodisperse Ni-clusters anchored on carbon nitride for efficient photocatalytic hydrogen evolution[J]. Chinese Journal of Catalysis, 2022, 43(2): 536-545.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)63865-2

https://www.cjcatal.com/EN/Y2022/V43/I2/536

Figures/Tables 5

Fig. 1. HRTEM (a) and HAADF-STEM (b,c) images of Ni-cluster/CN; (d) Elemental mapping.

Fig. 2. (a) XPS spectrum of Ni-cluster/CN; (b) High-resolution XPS spectrum of Ni 2p; (c) XANES curves of Ni-cluster/CN at the edge of Ni-K and Ni(OH)2 reference spectrum; (d) Corresponding Fourier transform curve of EXAFS spectrum.

Fig. 3. High-resolution XPS spectra of C 1s (a) and N 1s (b) of CN, Ni-cluster/CN and Ni(OH)2NPs/CN; XAS spectra of Ni-cluster/CN and reference samples are located at edge of C K (c) and edge of N K (d); (e) Top view of the model structure calculated by DFT: Ni-N3C2 (Note: DFT calculation was performed on the model structure established by a single Ni atom in Ni-lusters); (f) Differential charge density distribution of Ni-cluster/CN (Note: the yellow and blue areas indicate electron accumulation and consumption, respectively).

Fig. 4. (a) Schematic diagram of the Mott-Schottky contact of Ni-cluster/CN (Φ: work function, EF: Fermi level, EC: conduction band, EV: valence band); (b) Measured work functions via UV photoelectron spectroscopy analysis; (c) Ni 2p high-resolution XPS spectra of Ni(OH)2NPs/CN and Ni-cluster/CN; (d) Photocatalytic HER rate of CN, Ni(OH)2NPs/CN, and Ni-cluster/CN; (e) Cyclic stability experiment of photocatalytic hydrogen evolution; (f) Photocatalytic hydrogen evolution of Ni-cluster/CN driven by sunlight.

Fig. 5. (a) PL spectra of CN and Ni-cluster/CN at 375 nm; (b) Time-resolved photoluminescence spectra; (c) Transient photocurrent response; (d) EIS Nyquist EIS’; (e) Schematic diagram of the interface interaction between Ni-clusters and CN and Ni-cluster/CN photocatalytic reaction hydrogen production mechanism.

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