Jung Won-Sik, Park Soo-Hyeon, Kadam Abhijit Nanaso, Kim Hansang, Lee Sang-Wha
Department of Chemical and Biological Engineering, Gachon University, 1342 Seongnamdaero, Seongnam-si 13120, Republic of Korea.
Department of Mechanical Engineering, Gachon University, Seongnamdaero 1342, Seongnam-si, Korea.
Dalton Trans. 2020 Mar 3;49(9):2924-2932. doi: 10.1039/c9dt04611a.
Cubic-shaped hematite (C-Fe2O3) functionalized with amine groups was directly prepared via one-pot hydrothermal reaction of Fe3+ with 1,12-diaminododecane (DA-12) in aqueous solution (50% ethanol). Herein, DA-12 (as a Lewis acid) promoted the aggregation of α-FeOOH nanorods with Lewis base sites, leading to the rapid recrystallization and conversion into uniform C-Fe2O3. C-Fe2O3 was subsequently deposited with nanosized Au via sonochemical reduction of 1.0 wt% HAuCl4 (0.1-0.8 mL), hereafter referred to as Au-deposited C-Fe2O3 (C-Fe2O3@Au). X-ray diffraction patterns of C-Fe2O3@Au confirmed the hexagonal crystalline phases of hematite and crystalline Au (111) and showed a weak broad band attributed to the amorphous carbon of DA-12. C-Fe2O3@Au was tested as a visible-light photocatalyst towards the degradation of methylene blue (MB) dye. C-Fe2O3@Au (0.1-0.4 mL of 1.0 wt% HAuCl4) exhibited 6-8 times higher photocatalytic activity than the Au-free counterpart (C-Fe2O3). The enhanced photocatalysis was mainly attributed to the improved separation efficiency of photo-excited charge carriers, i.e., the facilitated transport of electrons from the conduction band to the lower lying Fermi level of Au. However, the photocatalytic activity of C-Fe2O3@Au (0.8 mL of 1.0 wt% HAuCl4) was decreased probably due to the reduction of active sites for MB adsorption by the high coverage of the Au layer. The combined hydrothermal and sonochemical methods provided the direct synthetic route to cubic-shaped hematite decorated with nanosized Au and surface amine functionality as a promising visible-light photocatalyst.
通过在水溶液(50%乙醇)中使Fe³⁺与1,12 - 二氨基十二烷(DA - 12)进行一锅水热反应,直接制备了胺基官能化的立方体形赤铁矿(C - Fe₂O₃)。在此,DA - 12(作为路易斯酸)促进了具有路易斯碱位点的α - FeOOH纳米棒的聚集,导致快速重结晶并转化为均匀的C - Fe₂O₃。随后通过超声化学还原1.0 wt%的HAuCl₄(0.1 - 0.8 mL)将纳米尺寸的Au沉积在C - Fe₂O₃上,此后称为Au沉积的C - Fe₂O₃(C - Fe₂O₃@Au)。C - Fe₂O₃@Au的X射线衍射图谱证实了赤铁矿的六方晶相和结晶Au(111),并显示出归因于DA - 12无定形碳的弱宽带。测试了C - Fe₂O₃@Au作为可见光光催化剂对亚甲基蓝(MB)染料的降解性能。C - Fe₂O₃@Au(1.0 wt% HAuCl₄的0.1 - 0.4 mL)表现出比无Au对应物(C - Fe₂O₃)高6 - 8倍的光催化活性。光催化增强主要归因于光激发电荷载流子的分离效率提高,即电子从导带向Au的较低费米能级的促进传输。然而,C - Fe₂O₃@Au(1.0 wt% HAuCl₄的0.8 mL)的光催化活性可能由于Au层的高覆盖率降低了MB吸附的活性位点而降低。水热法和超声化学法相结合提供了一种直接合成路线,用于制备装饰有纳米尺寸Au和表面胺官能团的立方体形赤铁矿,作为一种有前景的可见光光催化剂。