Insight into the adsorption behavior and mechanism of trace impurities from H<sub>2</sub>O<sub>2</sub> solution on functionalized zirconia by tuning the structure of amino groups

doi:10.1007/s11705-024-2415-3

2024, Vol. 18

Issue (5) : 56 https://doi.org/10.1007/s11705-024-2415-3

Insight into the adsorption behavior and mechanism of trace impurities from H₂O₂ solution on functionalized zirconia by tuning the structure of amino groups

Yu Meng¹, Yitong Wang¹, Guozhu Li^1,², Guozhu Liu^1,², Li Wang^1,²(

)

¹. Key Laboratory for Green Chemical Technology of Ministry Education, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China
². Haihe Laboratory of Sustainable Chemical Transformations, Tianjin 300192, China

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Abstract

Primary, secondary and tertiary amino-functionalized zirconia (ZrO₂−NH₂, ZrO₂−NH and ZrO₂−N) was synthesized by the postgrafting method for the adsorption removal of typical metallic ions, phosphate and total oxidizable carbon from a real H₂O₂ solution. ZrO₂−NH₂, ZrO₂−NH and ZrO₂−N exhibited similar pore sizes and sequentially increased zeta potentials. The adsorption results of single and binary simulated solutions showed that the removal efficiency increased in the order of Fe³⁺ > Al³⁺ > Ca²⁺ > Na⁺. There is competitive adsorption between metallic ions, and Fe³⁺ has an advantage over the other metals, with a removal efficiency of 90.7%. The coexisting phosphate could promote the adsorption of metallic ions, while total oxidizable carbon had no effect on adsorption. The adsorption results of the real H₂O₂ solution showed that ZrO₂−NH₂ exhibited the best adsorption affinity for metallic ions, as did phosphate and total oxidizable carbon, with a total adsorption capacity of 120.9 mg·g^–1. Density functional theory calculations revealed that the adsorption process of metallic ions involves electron transfer from N atoms to metals and the formation of N-metal bonds.

Keywords adsorption metallic ion phosphate total oxidizable carbon zirconia H₂O₂

Corresponding Author(s): Li Wang

Just Accepted Date: 24 January 2024 Issue Date: 23 April 2024

Cite this article:

Yu Meng,Yitong Wang,Guozhu Li, et al. Insight into the adsorption behavior and mechanism of trace impurities from H₂O₂ solution on functionalized zirconia by tuning the structure of amino groups[J]. Front. Chem. Sci. Eng., 2024, 18(5): 56.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-024-2415-3
https://academic.hep.com.cn/fcse/EN/Y2024/V18/I5/56

Fig.1 (a) XRD patterns, (b) FTIR spectra, (c) nitrogen adsorption-desorption isotherms and (d) pore size distributions of ZrO₂, ZrO₂?NH₂, ZrO₂?NH and ZrO₂?N.

Tab.1 Textural properties of the adsorbents

Fig.2 XPS spectra of (a–d) O 1s and (e–g) N 1s and (h) zeta potentials for ZrO₂, ZrO₂?NH₂, ZrO₂?NH and ZrO₂?N.

Fig.3 Removal efficiency of metallic ions on ZrO₂, ZrO₂?NH₂, ZrO₂?NH and ZrO₂?N from (a) a single-impurity simulated solution, (b) a binary-impurity solution of Al³⁺?M (M = Na⁺, Ca²⁺ and Fe³⁺ ) and (c) Al³⁺?phosphate and Al³⁺?TMB (initial content:

C A l 3 +

= 1.96 mg·L^–1,

C N a +

= 1.83 mg·L^–1,

C C a 2 +

= 1.80 mg·L^–1,

C F e 3 +

= 2.09 mg·L^–1, C_phosphate = 108.1 mg·L^–1, C_TMB = 46.9 mg·L^–1; time = 1 h; temperature = 30 °C; solution/adsorbent = 20 mL/20 mg).

Fig.4 Removal efficiency of (a) metallic ions and (b) phosphate and TOC from real H₂O₂ solution (initial concentration of H₂O₂ = 30.28%; initial value of pH = 2.26; contents of various impurities are shown in Tables S1 and S2; time = 1 h; temperature = 30 °C; solution/adsorbent = 20 mL/20 mg).

Adsorbent	$C H 2 O 2$ ^a)/%	$C Z r 4 +$ ^b)/(× 10^?3 mg·L^–1)	q_e^c)/(mg·g^–1)
ZrO₂	29.33	6.2	63.7
ZrO₂?NH₂	28.83	10.3	120.9
ZrO₂?NH	28.93	7.6	112.0
ZrO₂?N	28.98	6.5	107.8

Tab.2 Concentration of the H₂O₂ solution and content of Zr⁴⁺after adsorption and total adsorption capacity

Fig.5 Adsorption isotherms of Al³⁺ at 30 °C (time = 1 h and solution/adsorbent = 20 mL/20 mg): (a) Langmuir model, (b) Freundlich model and (c) Sips model; adsorption kinetics of Al³⁺ at 30 °C and 6 mg·L^–1 (solution/adsorbent = 20 mL/20 mg), (d) pseudo-first-order model, (e) pseudo-second-order model, (f) Elovich model and (g) Weber-Morris model.

Tab.3 Adsorption energy and N–M (M = Al, Na, Ca and Fe) bond length of the optimal configurations

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