4.8 Article

Single-Site Ni-Grafted TiO2 with Diverse Coordination Environments for Visible-Light Hydrogen Production

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CHEMSUSCHEM
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WILEY-V C H VERLAG GMBH
DOI: 10.1002/cssc.202301041

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Anatase; Nickel Complexes; Surface Ligand Exchange; Water Splitting; Photocatalysis

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This study demonstrates the efficient photocatalytic hydrogen evolution reaction (HER) by constructing well-defined single-site Ni-grafted TiO2 photocatalysts with unique coordination environments. The T-Ni Bpy catalyst exhibits high catalytic activity, with a rate and turnover frequency 260 times higher than those of Ni-O-TiO2. The electron paramagnetic resonance and femtosecond transient IR absorption measurements indicate that the presence of fewer electron trapped oxygen vacancies and a larger portion of long-lived photogenerated electrons are essential for achieving excellent HER activity.
Solar hydrogen production at a high efficiency holds the significant importance in the age of energy crisis, while the micro-environment manipulation of active sites on photocatalysts plays a profound role in enhancing the catalytic performance. In this work, a series of well-defined single-site Ni-grafted TiO2 photocatalysts with unique and specific coordination environments, 2,2 '-bipyridine-Ni-O-TiO2 (T-Ni Bpy) and 2-Phenylpyridine-Ni-O-TiO2 (T-Ni Phpy), were constructed with the methods of surface organometallic chemistry combined with surface ligand exchange for visible-light-induced photocatalytic hydrogen evolution reaction (HER). A prominent rate of 33.82 mu mol . g(-1) . h(-1) and a turnover frequency of 0.451 h(-1) for Ni are achieved over the optimal catalyst T-Ni Bpy for HER, 260-fold higher than those of Ni-O-TiO2. Fewer electrons trapped oxygen vacancies and a larger portion of long-lived photogenerated electrons (>3 ns, similar to 52.9 %), which were demonstrated by the electron paramagnetic resonance and femtosecond transient IR absorption, correspond to the photocatalytic HER activity over the T-Ni Bpy. The number of long-lived free electrons injected from the Ni photoabsorber to the conduction band of TiO2 is one of the determining factors for achieving the excellent HER activity.

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