Construction of crystal defect sites in N-coordinated UiO-66 via mechanochemical in-situ N-doping strategy for highly selective adsorption of cationic dyes

被引:121
作者
Hu, Peng [1 ]
Zhao, Zhongxing [1 ,2 ]
Sun, Xiaodan [1 ]
Muhammad, Yaseen [2 ,3 ]
Li, Jing [1 ]
Chen, Shibo [1 ]
Pang, Chunjiao [1 ]
Liao, Tingting [1 ]
Zhao, Zhenxia [1 ]
机构
[1] Guangxi Univ, Sch Chem & Chem Engn, Nanning 530004, Peoples R China
[2] Guangxi Univ, Guangxi Key Lab Electrochem Energy Mat, Nanning 530004, Peoples R China
[3] Univ Peshawar, Inst Chem Sci, Peshawar 25120, KP, Pakistan
基金
中国国家自然科学基金;
关键词
Mechanochemical in-situ N-coordination strategy; UiO-66; modification; Selective adsorption; Cationic dyes; Textural characterization; DFT simulation; METAL-ORGANIC FRAMEWORKS; ROOM-TEMPERATURE SYNTHESIS; COMPETITIVE ADSORPTION; COMPOSITE MEMBRANES; CARBON NANOTUBES; CO2; ADSORPTION; REACTIVE DYES; HIGH-CAPACITY; WATER-VAPOR; P-XYLENE;
D O I
10.1016/j.cej.2018.09.060
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Alkaline N-compounds (pyrrole, dopamine and 2-methylimidazole) were applied to induce crystal defects on UiO-66 via mechanochemical in-situ N-doping strategy and their role on its selective adsorption for cationic dyes i.e. rhodamine B (RhB) and safranine T (ST) were investigated systematically. Alkaline N-compounds coordination were proved to simultaneously modulate pore sizes and intensify surface alkalinity of the original UiO-66. The crystal defects constructed 3-D multi-point adsorption structure, which dramatically enhanced specific adsorption for RhB and ST in binary system. Results showed that pyrrole coordinated UiO-66 possessed 30% enhancement in surface area (1549.1 m(2)/g) with micropores at 9 and 12 angstrom (larger defects in UiO-66). Furthermore, temperature programmed desorption (H2O and NH3) and corrosion resistance test concluded that N-doped UiO-66 possessed improved alkali-resistance and higher alkaline surface compared to pristine UiO-66. Separation performance revealed that pyrrole-doped UiO-66 showed two times enhanced adsorption capacity for RhB (384.1 mg/g), and 223 times higher selectivity for equimolar RhB/ST than that of parent UiO-66. Textural characterization, DFT simulation and electronic factors concluded that proper defect size and alkaline surface endow the novel defective UiO-66 excellent selectivity, adsorption and recycling performances. Thus, our in-situ N-doping strategy has guiding significance to design MOFs with special and useful defects for unique selective adsorption system beyond the circle of organic dyes on industrial level.
引用
收藏
页码:329 / 340
页数:12
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