Ultra-deep removal of Pb by functionality tuned UiO-66 framework: A combined experimental, theoretical and HSAB approach

Ali，Shafqat1; Zuhra，Zareen1; Ali，Sajjad2; Han，Qi1; Ahmad，Muhammad3; Wang，Zhongying1

2021-12-01

10.1016/j.chemosphere.2021.131305

CHEMOSPHERE   影响因子和分区

0045-6535

1879-1298

A specific functionality in the adsorbent materials plays a significant role for the selective capture of heavy metals based on Pearson's Hard-Soft-Acid-Base (HSAB) concept. Herein, we introduced single and double amino- and thiol-functionalities into the UiO-66 framework, which acted as hard and soft base sites for heavy metal adsorption, respectively. The synthesized adsorbents (labelled as NH-UiO-66, (NH)-UiO-66, SH-UiO-66 and (SH)-UiO-66) were applied for the selective removal of lead (Pb) ions from contaminated water. The removal efficiency of Pb was about 64, 85, 75 and 99% (pH = 6, T = 30 °C, sample dosage = 10 mg, Pb concentration = 100 mg L), respectively, based on available number of interacting sites in the respective adsorbent. To elaborate HSAB concept, the interacting sites of these functional groups towards Pb were explored by identifying their possible types of interactions in terms of soft acid-base affinity, coordinate and covalent bonding, chelation, π-π interactions and synergetic effect of bonding. Density functional theory (DFT) simulation was used to confirm these interactions and to help the better understanding of adsorption mechanism. Model fitting and characterization of Pb-sorbed adsorbents were also performed to reveal kinetics, order of adsorptive reaction, thermodynamics and adsorption mechanism. Moreover, the optimization of adsorptive removal was performed by controlled parameters including time, initial concentration, pH and temperature. The reusability and selectivity of these adsorbents along with recovery of Pb(II) were also assessed. This study presents the conceptual framework for the design of functional adsorbents in the removal of heavy metals using the HSAB principle as an intended guideline.

Changed functionality DFT simulation Hard-soft-acid-base Mechanism MOF Pb(II) adsorption

SCI ; EI

英语

第一 ; 通讯

WOS:000703197100001

20213010685985

Chemical bonds ; Density functional theory ; Design for testability ; Heavy metals ; Lead compounds ; Mechanisms ; Reaction kinetics ; Reusability ; Thermodynamics ; Water pollution

Water Pollution:453 ; Metallurgy and Metallography:531 ; Mechanisms:601.3 ; Thermodynamics:641.1 ; Physical Chemistry:801.4 ; Chemical Reactions:802.2 ; Chemical Operations:802.3 ; Probability Theory:922.1 ; Atomic and Molecular Physics:931.3 ; Quantum Theory; Quantum Mechanics:931.4

ENVIRONMENT/ECOLOGY

2-s2.0-85111052252

Scopus

1.Guangdong Provincial Key Laboratory of Soil and Groundwater Pollution Control,School of Environmental Science and Engineering,Southern University of Science and Technology,Shenzhen,1088 Xueyuan Blvd, Nanshan District,518055,China
2.Department of Physics,Southern University of Science and Technology,Shenzhen,1088 Xueyuan Blvd, Nanshan District,518055,China
3.Department of Mechanical Engineering,City University of Hong Kong,Kowloon,83 Tat Chee Avenue,Hong Kong

Ali，Shafqat,Zuhra，Zareen,Ali，Sajjad,et al. Ultra-deep removal of Pb by functionality tuned UiO-66 framework: A combined experimental, theoretical and HSAB approach[J]. CHEMOSPHERE,2021,284.

Ali，Shafqat,Zuhra，Zareen,Ali，Sajjad,Han，Qi,Ahmad，Muhammad,&Wang，Zhongying.(2021).Ultra-deep removal of Pb by functionality tuned UiO-66 framework: A combined experimental, theoretical and HSAB approach.CHEMOSPHERE,284.

Ali，Shafqat,et al."Ultra-deep removal of Pb by functionality tuned UiO-66 framework: A combined experimental, theoretical and HSAB approach".CHEMOSPHERE 284(2021).