Citation:
Imran Khan, Xiaoyu Chu, Yanduo Liu, Salman Khan, Linlu Bai, Liqiang Jing. Synthesis of Ni2+ cation modified TS-1 molecular sieve nanosheets as effective photocatalysts for alcohol oxidation and pollutant degradation[J]. Chinese Journal of Catalysis,
;2020, 41(10): 1589-1602.
doi:
10.1016/S1872-2067(20)63555-0
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Improvement of the charge separation of titanosilicate molecular sieves is critical to their use as photocatalysts for oxidative organic transformations. In this work, MFI TS-1 molecular sieve nanosheets (TS-1 NS) were synthesized by a low-temperature hydrothermal method using a tailored diquaternary ammonium surfactant as the structure-directing agent. Introducing Ni2+ cations at the ion-exchange sites of the TS-1 NS framework significantly enhanced its photoactivity in aerobic alcohol oxidation. The optimized Ni cation-functionalized TS-1 NS (Ni/TS-1 NS) provide impressive photoactivity, with a benzyl alcohol (BA) conversion of 78.9% and benzyl aldehyde (BAD) selectivity of 98.8% using O2 as the only oxidant under full light irradiation; this BAD yield is approximately six times greater than that obtained for bulk TS-1, and is maintained for five runs. The excellent photoactivity of Ni/TS-1 NS is attributed to the significantly enlarged surface area of the two-dimensional morphology TS-1 NS, extra mesopores, and greatly improved charge separation. Compared with bulk TS-1, Ni/TS-1 NS has a much shorter charge transfer distance. The as-introduced Ni species could capture the photoelectrons to further improve the charge separation. This work opens the way to a class of highly selective, robust, and low-cost titanosilicate molecular sieve-based photocatalysts with industrial potential for selective oxidative transformations and pollutant degradation.
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