Selective Design of Mesoporous Bi(2)Se(3) Films with Orthorhombic and Rhombohedral Crystals

具有正交晶系和菱面体晶系的介孔Bi(2)Se(3)薄膜的选择性设计

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Abstract

Materials with the same chemical composition can exhibit distinct properties depending on their crystal phases. Here, the synthesis of two types of mesoporous Bi(2)Se(3) films at different reduction potentials is reported and their application in electrochemical glucose sensing. Mesoporous Bi(2)Se(3) is synthesized by incorporating block copolymer micelle assemblies into the deposition solution and applying a reduction potential. To characterize the crystal phases accurately, Bi(2)Se(3) films are heat-treated at 200 °C for 1 h in a nitrogen atmosphere. The results reveal that the Bi(2)Se(3) films synthesized under different conditions exhibit clearly distinct phases: rhombohedral (R-Bi(2)Se(3)) and orthorhombic (O-Bi(2)Se(3)). The R-Bi(2)Se(3)-8 nm, featuring 8 nm pores and synthesized at a more negative reduction potential, outperforms its nonporous counterpart, achieving a glucose sensing sensitivity of 0.143 µA cm(-2) µM(-1) and a detection limit of 6.2 µM at pH 7.4 in 0.1 M phosphate-buffered saline solution. In contrast, the O-Bi(2)Se(3), prepared at a relatively positive potential, exhibits no glucose-sensing activity. The inactivity of O-Bi(2)Se(3) for glucose oxidation is likely due to the energetically unfavorable intermediates, as predicted by density functional theory calculations. These findings underscore the critical role of crystal phase control in porous nanomaterials and pave the way for developing innovative porous systems.

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