Benignly-fabricated supramolecular poly(amidoxime)-alginate-poly(acrylic acid) beads synergistically enhance uranyl capture from seawater

Ahmad，Zia1,2; Li，Yun1; Ali，Sajjad3; Yang，Jiajia1,4; Jan，Faheem5; Fan，Yun1; Gou，Xiaoyi6; Sun，Qingye4; Chen，Jiping1

2022-08-01

10.1016/j.cej.2022.136076

CHEMICAL ENGINEERING JOURNAL   影响因子和分区

1385-8947

1873-3212

Design of amidoxime-based adsorbents in a cooperative and synergistic manner together with a concept of facile and green fabrication is becoming highly desirable to harvest uranium from seawater. Herein, taking benefit of supramolecular ionic-crosslinking and hydrogen bonding interactions, we have reported a simple and environmentally benign approach to construct novel bifunctional poly(amidoxime)-alginate-poly(acrylic acid) (PAO-A-PAA) composite beads. As a result of synergistic uranyl binding, the PAO-A-PAA composite beads reached a high adsorption capacity of 735.1 mg g for uranium aqueous solution (36 ppm), which is 2.24 and 1.46 times that of monofunctional Alg-PAA (328.1 mg g) and Alg-PAO (502.2 mg g), respectively. More importantly, the PAO-A-PAA exhibits excellent selectivity towards U(VI) in the presence of natural organic matter and multiple coexisting metal ions in simulated seawater. The XPS analysis reveals the utilization and coordination of both amidoxime and carboxylate ligands of PAO-A-PAA for uranyl binding, which results in energetically more stable synergistic uranyl complexes (E = −9.45 to −10.34 eV) as proved by the density functional theory study. The adsorption efficiency of PAO-A-PAA is further supported by its ability to extract µg L-level uranium in real seawater (94.7–99.5%). The PAO-A-PAA also demonstrates good mechanical and chemical stability over a wide pH range, as well as good reusability. These findings provide insight into the significance of designing efficient sorbent material for enhanced uranyl capture via a supramolecular strategy.

Amidoxime Carboxyl Seawater Supramolecular synergistic Uranium Extraction

SCI ; EI

英语

其他

National Natural Science Foundation of China[21705149];National Natural Science Foundation of China[21777159];

Engineering

Engineering, Environmental ; Engineering, Chemical

WOS:000795645400003

ELSEVIER SCIENCE SA

20221411884022

Carboxylation ; Carboxylic acids ; Chemical stability ; Coordination reactions ; Crosslinking ; Density functional theory ; Fabrication ; Hydrogen bonds ; Metals ; Reusability ; Supramolecular chemistry ; Uranium compounds

Metallurgy:531.1 ; Chemistry:801 ; Physical Chemistry:801.4 ; Chemical Reactions:802.2 ; Organic Compounds:804.1 ; Probability Theory:922.1 ; Atomic and Molecular Physics:931.3 ; Quantum Theory; Quantum Mechanics:931.4

ENGINEERING

2-s2.0-85127157663

Scopus

1.Key Laboratory of Separation Sciences for Analytical Chemistry,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian,116023,China
2.University of Chinese Academy of Science,Beijing,100049,China
3.Department of Physics,Southern University of Science and Technology,Shenzhen,518055,China
4.College of Materials Science and Engineering,Hebei University of Engineering,Handan,19 Taiji Road,056038,China
5.Shenyang National Laboratory for Materials Science,Institute of Metal Research,Chinese Academy of Sciences,Shenyang,Liaoning,110016,China
6.School of Materials Science and Engineering,Dalian Jiaotong University,Dalian,116028,China

Ahmad，Zia,Li，Yun,Ali，Sajjad,et al. Benignly-fabricated supramolecular poly(amidoxime)-alginate-poly(acrylic acid) beads synergistically enhance uranyl capture from seawater[J]. CHEMICAL ENGINEERING JOURNAL,2022,441.

Ahmad，Zia.,Li，Yun.,Ali，Sajjad.,Yang，Jiajia.,Jan，Faheem.,...&Chen，Jiping.(2022).Benignly-fabricated supramolecular poly(amidoxime)-alginate-poly(acrylic acid) beads synergistically enhance uranyl capture from seawater.CHEMICAL ENGINEERING JOURNAL,441.

Ahmad，Zia,et al."Benignly-fabricated supramolecular poly(amidoxime)-alginate-poly(acrylic acid) beads synergistically enhance uranyl capture from seawater".CHEMICAL ENGINEERING JOURNAL 441(2022).