Activated Sludge Incineration Ash Derived Fenton-like Catalyst: Preparation and Degradation Performance on Methylene Blue

doi:10.15541/jim20230580

Abstract

Abstract:

Fe@zeolite materials are widely applied in the production of ·OH by catalyzing Fenton-like reactions for degradation of recalcitrant organic pollutants due to their comprehensive sources, simple preparation and low environmental impact. However, the high cost of Fe@zeolite synthesis and the lack of Fe²⁺ regeneration strategy are serious issues that limit the application of Fe@zeolite as a Fenton-like catalyst in industrial-scale systems. In this study, the ash generated from activated sludge incineration treatment was utilized as raw material to selective recover Si, Al and Fe, preparing Fe²⁺-sodalite (FSD) material. Consequently, it was used as a Fenton-like catalyst to activate peroxyacetic acid (PAA) for the degradation of methylene blue (MB) in wastewater. Results indicated thatFSD was capable of effectively catalyzing PAA to generate various active oxygen species such as ·OH, ¹O₂ and R-O· in a wide pH range, thereby degrading MB through hydroxylation and sulfonation pathways. MB can be completely removed during 20 min under optimized conditions of 0.3 mmol/L PAA and 0.3 g/L FSD prepared with 0.5 mol/L Fe²⁺. In addition, the reductive S species in FSD can maintain its catalytical activity by enhancing Fe²⁺ regeneration, and the FSD/PAA system has been proven to be effective in the degradation of various organic pollutants under practical and complex environmental conditions.

Key words: activated sludge, sodalite, Fenton-like degradation, peroxyacetic acid, methylene blue

CLC Number:

X705

CAI Mengyu, LI-YANG Hongmiao, YANG Caiyun, ZHOU Yuting, WU Hao. Activated Sludge Incineration Ash Derived Fenton-like Catalyst: Preparation and Degradation Performance on Methylene Blue[J]. Journal of Inorganic Materials, 2024, 39(10): 1135-1142.

Figures/Tables 12

Fig. 1 XRD patterns of SD, FSD and RFSD

Fig. 2 SEM images of (a, b) SD and (c, d) FSD before and after loading Fe2+

Fig. 3 MB degradation performances in different systems

Fig. 4 Effects of (a) concentration of Fe2+ loading solution, (b) oxidant dosage and (c) catalyst dosage on degradation of MB by FSD/PAA system

Fig. 5 Effect of different quenchers on degradation of MB by the optimized FSD/PAA system

Fig. 6 (a, b) Total and (c, d) Fe2p XPS spectra of (a, c) FSD and (b, d) RFSD before and after catalytical reaction

Fig. 7 Degradation pathways and intermediates of MB in the FSD/PAA system

Fig. 8 Effects of co-existed substrates and water conditions on the degradation of MB by the optimized FSD/PAA system (a-d) Effects of (a) NO3-, (b) SO42-, (c) CO32-, and (d) HA on MB degradation by the optimized FSD/PAA system; (e) Effect of deionic water (DW), tap water (TW) and lake water (LW) on the degradation performance of MB by the optimized FSD/PAA system; (f) Performance of the optimized FSD/PAA system in actual wastewater; Colorful figures are available on website

Fig. 9 Degradation performance of different pollutants by FSD/PAA system during 20 min

Table S1 Characterizations of different water samples

Item	TW	LW	Wastewater
TOC/(mg·L^-1)	16.7	28.8	188.1
F^-/(mg·L^-1)	0.1	0.1	0.2
Cl^-/(mg·L^-1)	23.2	24.3	51.1
K⁺/(mg·L^-1)	30.9	35.6	64.4
Mg²⁺/(mg·L^-1)	16.7	21.4	96.5

Table S2 HPLC conditions for phase gradient elution measuring concentrations of organic contaminants

Compound	Column temperature/℃	Flow rate/ (mL·min^-1)	Wavelength/ nm	Phase mobile phase	Phase elution gradient
MB	40	0.2	254	Ammonium acetate (A)+ acetonitrile (B)	0-1-9-14 min, 10%B-10%B-90%B-90%B
SMX	40	0.3	275	0.1% Formic acid solution (A)+ methanol (B)	0-1-1-3.5-5 min, 20%B-20%B-51.25%B-51.25%B
GM	40	0.3	278	0.1% Formic acid solution (A)+ acetonitrile (B)	0-0.5-1-4-6 min, 5%B-5%B-30%B-30%B
MDZ	40	0.8	318	Ultrapure water (A)+ acetonitrile (B)	0-0.5-3-5 min, 6%B-5%B-20%B-90%B
CIP	40	0.3	278	Ultrapure water (A)+ acetonitrile (B)	0-0.5-3-5 min, 6%B-5%B-20%B-90%B
RHB	40	0.2	554	0.1% Formic acid solution (A)+ acetonitrile (B)	0-5-8 min, 5%B-95%B-95%B
TC	40	0.3	360	Ultrapure water (A)+ acetonitrile (B)	0-0.5-3-5 min, 6%B-5%B-20%B-90%B

Fig. S1 Effect of pH on the degradation of MB by the FSD/PAA system

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