Contributions of adsorption, bioreduction and desorption to uranium immobilization by extracellular polymeric substances

doi:10.1007/s11783-023-1707-z

Front. Environ. Sci. Eng.

2023, Vol. 17

Issue (9) : 107 https://doi.org/10.1007/s11783-023-1707-z

RESEARCH ARTICLE

Contributions of adsorption, bioreduction and desorption to uranium immobilization by extracellular polymeric substances

Chen Zhou¹, Ermias Gebrekrstos Tesfamariam², Youneng Tang²(

), Ang Li³(

)

¹. Biodesign Swette Center for Environmental Biotechnology, Arizona State University, Tempe, AZ 85281, USA
². Department of Civil and Environmental Engineering, FAMU-FSU College of Engineering, Florida State University, Tallahassee, FL 32310, USA
³. State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China

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Abstract

● EPS immobilizes U(VI) via adsorption, bioreduction and desorption.

● This work provides a framework to quantify the three immobilization processes.

● The non-equilibrium adsorption of U follows pseudo-second-order kinetics.

● The equilibrium adsorption of U followed Langmuir and Freundlich isotherms.

Hexavalent uranium (U(VI)) can be immobilized by various microbes. The role of extracellular polymeric substances (EPS) in U(VI) immobilization has not been quantified. This work provides a model framework to quantify the contributions of three processes involved in EPS-mediated U(VI) immobilization: adsorption, bioreduction and desorption. Loosely associated EPS was extracted from a pure bacterial strain, Klebsiella sp. J1, and then exposed to H₂ and O₂ (no bioreduction control) to immobilize U(VI) in batch experiments. U(VI) immobilization was faster when exposed to H₂ than O₂ and stabilized at 94% for H₂ and 85% for O₂, respectively. The non-equilibrium data from the H₂ experiments were best simulated by a kinetic model consisting of pseudo-second-order adsorption (k_a = 2.87 × 10⁻³ g EPS·(mg U)⁻¹·min⁻¹), first-order bioreduction (k_b = 0.112 min⁻¹) and first-order desorption (k_d = 7.00 × 10⁻³ min⁻¹) and fitted the experimental data with R² of 0.999. While adsorption was dominant in the first minute of the experiments with H₂, bioreduction was dominant from the second minute to the 50^th min. After 50 min, adsorption was negligible, and bioreduction was balanced by desorption. This work also provides the first set of equilibrium data for U(VI) adsorption by EPS alone. The equilibrium experiments with O₂ were well simulated by both the Langmuir isotherm and the Freundlich isotherm, suggesting multiple mechanisms involved in the interactions between U(VI) and EPS. The thermodynamic study indicated that the adsorption of U(VI) onto EPS was endothermic, spontaneous and favorable at higher temperatures.

Keywords Adsorption Bioreduction Desorption Kinetics Isotherm Uranium

Corresponding Author(s): Youneng Tang,Ang Li

Issue Date: 17 April 2023

Cite this article:

Chen Zhou,Ermias Gebrekrstos Tesfamariam,Youneng Tang, et al. Contributions of adsorption, bioreduction and desorption to uranium immobilization by extracellular polymeric substances[J]. Front. Environ. Sci. Eng., 2023, 17(9): 107.

URL:

https://academic.hep.com.cn/fese/EN/10.1007/s11783-023-1707-z
https://academic.hep.com.cn/fese/EN/Y2023/V17/I9/107

Parameter	Description
I. Constants
M_w	Atomic weight of uranium (238.03 g/mol)
R	Ideal gas constant (8.314 J/(K·mol))
K_H	Dimensionless Henry’s Law constant for H₂ ( $1.91 × 10 − 2$ )
II. Parameters obtained from experiments
C₀	Initial concentration of U(VI) in the solution (mg U/L)
C_e	Equilibrium concentration of U(VI) in the solution (mg U/L)
C_t	Concentration of U(VI) in the solution at time t (mg U/L)
N	Number of measurements made during the isotherm experiments
n_a	Number of moles of dissolved H₂ gas in the aqueous medium (mol)
n_g	Number of moles of H₂ gas in the headspace of the serum bottles (mol)
n_T	Total number of moles of H₂ in the serum bottles (mol)
P	Partial pressure in the headspace of the serum bottles (Pa)
q_e	Amount of U(VI) adsorbed by EPS at equilibrium (mg U/g EPS)
q_t	Amount of U(VI) adsorbed by EPS at time t (mg U/g EPS)
T	Absolute temperature (K)
t	Time (min)
V_a	Volume of the aqueous medium in the serum bottles (L)
V_g	Volume of the headspace of the serum bottles (L)
X	Concentration of EPS used as an adsorbent (g EPS /L)
ε	Polanyi adsorption potential (J/mol)
III. Unknown parameters obtained from model simulation
b	Langmuir’s affinity constant associated with adsorption energy (L/mg U)
B	Initial adsorption for intraparticle diffusion model (mg U/g EPS)
k	Dubinin-Radushkevich isotherm constant related to adsorption energy (mol²/J²)
k₁	Pseudo-first-order rate constant of adsorption (min⁻¹)
k₂	Pseudo-second-order rate constant of adsorption (g EPS/(mg U·min))
k_a	Second-order adsorption constant (g EPS/(mg U·min))
k_b	First-order bioreduction constant (min⁻¹)
k_d	First-order desorption constant (min⁻¹)
K_F	Freundlich distribution coefficient for adsorption (mg U/g EPS)·(L/mg U)^1/n
k_id	Intraparticle diffusion rate constant (min^−1/2)
n	Freundlich isotherm constant indicating adsorption intensity
q_m	Langmuir isotherm constant for maximum adsorption capacity (mg U/g EPS)
q_s	Saturation capacity related to Dubinin-Radushkevich isotherm (mg U/g EPS)
R_L	Langmuir’s separation factor
SSRR	Sum of squared relative residuals
ΔG°	Gibbs free energy (J/mol)
ΔH°	Enthalpy change (J/mol)
ΔS°	Entropy change (J/(mol·K))

Tab.1 Description of parameters used in this study

Fig.1 Kinetics of U(VI) adsorption by EPS exposed to O₂: (a) pseudo-first-order, (b) pseudo-second-order, and (c) intraparticle diffusion.

Kinetic model	Parameter	Value
Pseudo-first-order	q_e (mg U/g EPS)	21.3
	k₁ (min⁻¹)	$8.48 × 10 − 3$
	R²	0.732
Pseudo-second-order	q_e (mg U/g EPS)	46.1
	k₂ (g EPS / (mg U·min))	$2.87 × 10 − 3$
	R²	0.999
Intraparticle diffusion	B (mg U/g EPS)	22.9
	k_id (min^−1/2)	2.08
	R²	0.768

Tab.2 Kinetic constants of pseudo-first-order, pseudo-second-order and intraparticle diffusion models for U(VI) adsorption by EPS exposed to O₂

Fig.2 Comparison of U(VI) immobilization by EPS exposed to O₂ and H₂.

Fig.3 Contribution of three processes to U(VI) immobilization by EPS exposed to H₂.

Fig.4 Rates of U(VI) immobilization by EPS exposed to H₂.

Fig.5 Comparison of experimental and simulated H₂ partial pressures in the headspace.

Isotherm model		T (°C)
Isotherm model		22	30	37
Langmuir	q_m (mg U/g EPS)	169	67.1	62.5
	b (L/ mg U)	$4.02 × 10 − 3$	$1.43 × 10 − 2$	$1.66 × 10 − 2$
	R_L	0.805	0.553	0.519
	R²	0.982	0.936	0.927
	SSRR	0.077	0.153	0.158

Freundlich	K_F (mg U/g EPS)	0.623	1.14	1.30
	n	1.01	1.19	1.24
	R²	0.982	0.954	0.944
	SSRR	0.043	0.080	0.087

Dubinin-Radushkevich	q_s (mg U/g EPS)	29.9	29.6	29.5
	k (mol²/J²)	$2.50 × 10 − 5$	$2.66 × 10 − 5$	$3.34 × 10 − 5$
	R²	0.660	0.666	0.735
	SSRR	1.053	0.628	0.518

Tab.3 Constants of the Langmuir, Freundlich and Dubinin-Radushkevich isotherms for U(VI) adsorption by EPS exposed to O₂

Fig.6 Langmuir (a), Freundlich (b), and Dubinin-Radushkevich (c) isotherms for U(VI) adsorption by EPS exposed to O₂ at various temperatures.

Tab.4 Thermodynamic parameters for U(VI) adsorption by EPS exposed to O₂

Fig.7 (a) Effect of temperature on U(VI) adsorption by EPS exposed to O₂ and (b) determination of enthalpy change and entropy change.

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