Citation: Lei Wang, A-Ni Wang, Zhen-Zhen Xue, Yan-Ru Wang, Song-De Han, Guo-Ming Wang. In situ growth of polyoxometalate-based metal-organic framework nanoflower arrays for efficient hydrogen evolution[J]. Chinese Chemical Letters, ;2023, 34(4): 107414. doi: 10.1016/j.cclet.2022.04.012 shu

In situ growth of polyoxometalate-based metal-organic framework nanoflower arrays for efficient hydrogen evolution

College of Chemistry and Chemical Engineering, Qingdao University, Qingdao 266071, China

wangani@qdu.edu.cn

gmwang_pub@163.com

Received Date: 21 March 2022
Revised Date: 2 April 2022
Accepted Date: 7 April 2022
Available Online: 11 April 2022

Figures(4)

The conversion of traditional polymolybdate-based metal-organic frameworks (POMOFs) crystals to well-aligned nanoarrays are highly attractive for electrocatalytic hydrogen evolution but remains significant challenge. Herein, we demonstrated that the POMOFs nanoarrays as self-supported electrode toward hydrogen evolution with high catalytic activity and stability. Single-crystal X-ray analysis reveal the {ε-PMo₈^VMo₄^VIO₃₇Zn₄} (Zn-ε-Keggin) serve as secondary building blocks and directly connected to BPB organic ligands (BPB = 1, 4-bis(pyrid-4-yl)benzene) to obtain novel [ε-PMo₈^VMo₄^VIO₃₇(OH)₃Zn₄][BPB]₃ (named as ZnMo-POMOF). Particularly, ZnMo-POMOF nanoflower arrays grown in-situ on a Ni foam substrate exhibiting excellent electrocatalytic hydrogen evolution performance of 180 mV at a current density of 10 mA/cm² with the Tafel slope of 66 mV/dec, thus among one of the best POMOF-based electrocatalysts reported so far. DFT calculations reveal that the bridging oxygen active sites (O_a) significantly optimizes Gibbs free energy of H^* adsorption for Zn-ε-Keggin polymolybdate units (−0.07 eV), thereby increasing the intrinsic activity of the ZnMo-POMOF.
- Polyoxometalate,
- Metal-organic framework,
- Nanoflower arrays,
- Hydrogen evolution,
- DFT calculations
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