Odd-membered cyclic hetero-polyoxotitanate nanoclusters with high stability and photocatalytic H2 evolution activity

doi:10.1016/S1872-2067(20)63648-8

Abstract

Abstract:

We investigated the hydrolysis of TiIV along with naturally abundant AlIII ions and reported the formation of a stable and semiconducting nanocluster. Interestingly, this compound exhibits an unusual odd-membered ring structure and also represents the largest Al-containing polyoxotitanium cluster (PTC) observed thus far. The presence of a shell of organic ligands as well as the incorporation of hetero-Al ^III ions endowed the nanocluster with high air, thermal, and pH stabilities. The present compound exhibited a record photocatalytic hydrogen evolution of 402.88 μmol g ^-1 h ^-1 among PTC materials. This work not only paves the way towards stable PTC materials but also provides new insights into the design of novel photocatalysts.

Key words: Polyoxotitanate, Heterometallic cluster, Nanocluster, Water-splitting H₂ production

Ya-Jie Liu, Lin Geng, Yao Kang, Wei-Hui Fang, Jian Zhang. Odd-membered cyclic hetero-polyoxotitanate nanoclusters with high stability and photocatalytic H₂evolution activity[J]. Chinese Journal of Catalysis, 2021, 42(8): 1332-1337.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(20)63648-8

https://www.cjcatal.com/EN/Y2021/V42/I8/1332

Figures/Tables 3

Fig. 1. (a) Summary of reported Al-containing PTCs: inorganic cores of Ti3Al, Ti3Al2, Ti3Al3, Ti6Al, and Ti7Al clusters; (b) core-shell wheel nanocluster of compound 1. Hydrogen atoms and guest acetonitrile molecules are omitted for clarity.

Fig. 2. (a) Ball-and-stick representation of the [Ti14O21]14+ ring. (b) Ball-and-stick representation of the {Ti14Al7} heterometallic ring. (c,d) Top/side views of ball-and-stick representations of 1. (e) 3-D supramolecular packing of 1 viewed along the b axis. (f) Simplified 3-D supramolecular packing of 1. Hydrogen atoms and guest acetonitrile molecules are omitted for clarity.

Fig. 3. (a) PXRD patterns of 1 (simulated or immersed in aqueous solution at pH = 1, 3, 5, 7, 9, and 12 (adjusted with H2SO4 or NaOH) for 12 h). (b) Comparison of H2 evolution profiles under UV-visible (UV-vis) light, obtained with or without 1. (c) Cycling tests of H2 evolution from 1 under UV-vis light irradiation. (d) Transient photocurrent responses of 1 under +0.2 V bias potential and UV-vis light irradiation with and without lactic acid.

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Odd-membered cyclic hetero-polyoxotitanate nanoclusters with high stability and photocatalytic H₂evolution activity

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