Highly Efficient Separation of Anionic Organic Pollutants from Water via Construction of Functional Cationic Metal-Organic Frameworks and Mechanistic Study

被引:15
作者
Zhao, Chaofeng [1 ]
Du, Yao [1 ]
Zhang, Jichuan [2 ]
Mi, Yongsheng [1 ]
Su, Hui [1 ]
Fei, Teng [1 ]
Li, Shenghua [1 ]
Pang, Siping [1 ]
机构
[1] Beijing Inst Technol, Sch Mat Sci & Engn, Beijing 100081, Peoples R China
[2] Chinese Acad Sci, Biomat Res Ctr, Zhuhai Inst Adv Technol, Zhuhai 519003, Peoples R China
基金
中国国家自然科学基金;
关键词
organic anionic pollutants; separation; metal-organic frameworks; function; construction; PICRIC ACID; ACTIVATED CARBON; REMOVAL; ADSORPTION; TRINITROPHENOL; DESIGN; 2,4,6-TRINITROPHENOL; ENCAPSULATION; COORDINATION; DEGRADATION;
D O I
10.1021/acsami.0c02624
中图分类号
TB3 [工程材料学];
学科分类号
0805 ; 080502 ;
摘要
Organic anions possess various functional properties; however, their presence in wastewater causes environmental pollution. Thus, coupling the separation of such species with the resultant function could be highly desirable. Herein, we propose a "killing two birds with one stone" strategy for highly efficient separation of organic pollutant anions from water at room temperature through direct construction of functional cationic metal-organic frameworks (CMOFs) based on the organic anions as charge-balancing anions. To illustrate this strategy, 2,4,6-trinitrophenolate anion (PA(-)) is chosen as a typical anion, while 4,4'-azo-triazole (atrz) is strategically chosen as a suitable neutral ligand. The resultant positive framework exhibits a high adsorption capacity and selectivity for PA(-). Remarkably, its adsorption capacity is 869.6 mg g(-1), which is more than 30 times that of multiwalled carbon nanotubes and 15 times that of activated carbon. Its capacity is even higher than that of BUT-13 (865 mg g(-1)), the highest adsorbent ever known. H-1 NMR and single-crystal X-ray diffraction show that the high capacity is attributed to strong electrostatic interaction between the positive framework and PA(-), which leads to all the pores being completely occupied by PA(-) anions. H-1 NMR titration reveals that the selectivity comes from stronger hydrogen-bonding interaction between the ligand of the positive framework and PA(-), which is confirmed from the eight times length of the shifted signal of atrz due to the addition of PA(-) compared with the competing anions. The stronger interaction is further confirmed from the high stability of the resultant CMOF in high-concentration salt solutions containing the competing anions, particularly in 100-fold molar NaNO3 and Na2SO4 solutions. Meanwhile, first-principles simulation shows that the high binding energy between the positive framework and PA(-) contributes to enhancing the selectivity. Moreover, the resultant CMOF is a potential energetic material with an improved oxygen balance, high heat of formation, and heat of detonation.
引用
收藏
页码:22835 / 22844
页数:10
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