Prussian Blue Modified Biochar: Preparation and Adsorption of Ammonia Nitrogen from Sewage

doi:10.15541/jim20220432

Abstract

Abstract:

Eutrophication caused by nitrogen, phosphorus and organic pollutants is a common problem which has attracted much attention in China. Ammonia nitrogen, as a main pollutant, should be removed efficiently to avoid the extension of eutrophication. In this research, Prussian Blue (PB), which can not only capture ammonia nitrogen by vacancy in crystal cell but also degrade organic pollutants by Fenton oxidation, was combined with modified biochar to increase efficiency of ammonia nitrogen removal. Several characterization methods were used to investigate the structure and morphologies of the biochar composite. Adsorption capacity of biochar composite material (BC700-PB) was tested by NH₄Cl solution. The results show that the maximum adsorption capacity to ammonia nitrogen is 24.4 mg/g and the removal efficiency is over 95% within 60 min under the condition of pH 8, which is 101.3% higher than that of the unmodified biochar. The adsorption mechanism of BC700-PB was investigated with Langmuir model and pseudo-second-order kinetic equation which reveal that the adsorption including physical adsorption by biochar and coordination adsorption by PB. Meanwhile, Fenton oxidation process is conducted by PB nanoparticles in the biochar composite material with existence of H₂O₂. The biochar composite material could catalyze H₂O₂ to generate •OH, and achieve degradation of organic pollutants and adsorption of ammonia nitrogen. The PB/biochar composite material can be recycled easily by NaCl solution for several times. In conclusion, the PB/biochar composite is a promising material for eliminating multi-component eutrophication wastewater.

Key words: biochar material, prussian blue nanoparticles, ammonia nitrogen adsorption, Fenton oxidation process

CLC Number:

TQ424

YU Yefan, XU Ling, NI Zhongbing, SHI Dongjian, CHEN Mingqing. Prussian Blue Modified Biochar: Preparation and Adsorption of Ammonia Nitrogen from Sewage[J]. Journal of Inorganic Materials, 2023, 38(2): 205-212.

Figures/Tables 9

Fig. 1 SEM images of BC700 (a) and BC700-PB (b), and TEM images of BC700 (c) and BC700-PB (d)

Fig. 2 N2 adsorption-desorption curves (a) and pore size distributions (b) of BC700 and BC700-PB

Fig. 3 XRD patterns (a) and FT-IR spectra (b) of BC700-PB and BC700

Fig. 4 Full XPS spectra (a) of BC700 and BC700-PB, core-level XPS spectra of the elemental C1s (b, c) and O1s (d, e) of BC700 (b, d) and BC700-PB (c, e), and N1s (f) of BC700-PB Colorful figures are available on website

Fig. 5 Effect of dosage on the removal of NH3-N by of BC700 and BC700-PB (pH 8, C0=50 mg/L, t=60 min) (a), effects of pH (dosage=5 g/L, C0=50 mg/L, t=60 min) (b), initial concentration and coexisting ions (C0=50 mg/L, dosage=5 g/L, pH 8, t=60 min) (c), and reaction time(dosage=5 g/L, pH 8, C0=50 mg/L) (d) on the removal of NH3-N by BC700-PB

Fig. 6 Schematic diagram of adsorption and catalysis removal of ammonia nitrogen by BC700-PB

Fig. 7 Langmuir (a) and Freundlich models (b) of NH3-N on BC700-PB, and pseudo-first-order kinetic (c) and pseudo-second-order kinetic (d) models of NH3-N on BC700-PB

Fig. 8 Recycling removal property of BC700-PB (pH 8, dosage=5 g/L, C0=50 mg/L)

Fig. 9 Effects of adsorbents and additive on the removal efficiency for mixed solution of NH3-N and HA(pH 2, dosage=5 g/L, C0=50 mg/L) (a), and EPR spectra of DMPO-OH (b) adducts in the systems of BC700-PB

References 25

[1]	LIN S, SHEN S L, ZHOU A, et al. Assessment and management of lake eutrophication: a case study in Lake Erhai, China. Science of The Total Environment, 2020, 751(1): 141618. DOI URL
[2]	SHENG K, ZHANG P, OU S J, et al. Spatiotemporal nutrient patterns, composition, and implications for eutrophication mitigation in the Pearl River Estuary, China. Estuarine, Coastal and Shelf Science, 2022, 266(5): 107749. DOI URL
[3]	HUANG W, ZHANG Y, LI D. Adsorptive removal of phosphate from water using mesoporous materials: a review. Journal of Environmental Management, 2017, 193(15): 470. DOI PMID
[4]	ZHANG M, SONG G, GELARDI D L, et al. Evaluating biochar and its modifications for the removal of ammonium, nitrate, and phosphate in water. Water Research, 2020, 186(1): 116303. DOI URL
[5]	LU Y, CAI Y, ZHANG S, et al. Application of biochar-based photocatalysts for adsorption-(photo)degradation/reduction of environmental contaminants: mechanism, challenges and perspective. Biochar, 2022, 4: 45. DOI URL
[6]	QIU M, LIU L, LING Q, et al. Biochar for the removal of contaminants from soil and water: a review. Biochar, 2022, 4: 19. DOI URL
[7]	LIANG L, XI F, TAN W, et al. Review of organic and inorganic pollutants removal by biochar and biochar-based composites. Biochar, 2021, 3(1): 255. DOI URL
[8]	GONG Y P, NI Z Y, XIONG Z Z, et al. Phosphate and ammonium adsorption of the modified biochar based on Phragmites australis after phytoremediation. Environmental Science & Pollution Research, 2017, 24(9): 8326.
[9]	YI A, MP A, MVSA B, et al. A SAXS study of the pore structure evolution in biochar during gasification in H₂O, CO₂ and H₂O/CO₂. Fuel, 2021, 292: 120384. DOI URL
[10]	XIAO Y, WU Z J, CUI M, et al. Co-modification of biochar and bentonite for adsorption and stabilization of Pb²⁺ ions. Journal of Inorganic Materials, 2021, 36(10): 1083. DOI
[11]	ANDREAS L. Prussian blue, an inorganic evergreen. Journal of Chemical Education, 1981, 58(12): 1013. DOI URL
[12]	LIN H, FANG Q, WANG W, et al. Prussian blue/PVDF catalytic membrane with exceptional and stable Fenton oxidation performance for organic pollutants removal. Applied Catalysis B: Environmental. 2020, 273(15): 119047. DOI URL
[13]	TAKAHASHI A, TANAKA H, PARAJULI D, et al. Historical pigment exhibiting ammonia gas capture beyond standard adsorbents with adsorption sites of two kinds. Journal of the American Chemical Society, 2016, 138(20): 6376. DOI PMID
[14]	TAKAHASHI A, MINAMI K, NODA K, et al. Trace ammonia removal from air by selective adsorbents reusable with water. ACS Applied Materials and Interfaces, 2020, 12(13): 15115. DOI URL
[15]	WAN S, QIU L, TANG G, et al. Ultrafast sequestration of cadmium and lead from water by manganese oxide supported on a macro-mesoporous biochar. Chemical Engineering Journal, 2020, 387(1): 124095. DOI URL
[16]	HUFF M D, LEE J W. Biochar-surface oxygenation with hydrogen peroxide. Journal of Environmental Management, 2016, 165(1): 17. DOI PMID
[17]	ZHAO G, FENG J J, ZHANG Q L, et al. Synthesis and characterization of Prussian blue modified magnetite nanoparticles and its application to the electrocatalytic reduction of H₂O₂. Journal of Materials Chemistry, 2005, 17(12): 3154. DOI URL
[18]	FENG S S, CAO X, ZHENG W, et al. In-situ formed Prussian blue nanoparticles supported by porous biochar as highly efficient removal of cesium ions. Journal of Environmental Chemical Engineering, 2022, 10(3): 107972. DOI URL
[19]	AI J, LU C, BERG F, et al. Biochar catalyzed dichlorination-which biochar properties matter. Journal of Hazardous Materials, 2021, 406(15): 124724. DOI URL
[20]	CHEN L, CHEN X L, ZHOU C H, et al. Environmental-friendly montmorillonite-biochar composites: facile production and tunable adsorption-release of ammonium and phosphate. Journal of Cleaner Production, 2017, 156(10): 648. DOI URL
[21]	SIZMUR T, FRESNO T, AKGUL G, et al. Biochar modification to enhance sorption of inorganics from water. Bioresource Technology, 2017, 246: 34. DOI PMID
[22]	CUI X, HAO H, HE Z, et al. Pyrolysis of wetland biomass waste: potential for carbon sequestration and water remediation. Journal of Environmental Management, 2016, 173(15): 95. DOI PMID
[23]	YIN L A, NT A, TKL A, et al. Microwave assisted hydrothermal preparation of rice straw hydrochars for adsorption of organics and heavy metals. Bioresource Technology, 2019, 273: 136. DOI PMID
[24]	LI L, LAI C, HUANG F, et al. Degradation of naphthalene with magnetic bio-char activate hydrogen peroxide: synergism of bio-char and Fe-Mn binary oxides. Water Research, 2019, 160(1): 238. DOI PMID
[25]	SUN Y M, ZHOU P, ZHANG P, et al. New insight into carbon materials enhanced Fenton oxidation: a strategy for green iron(III)/ iron(II) cycles. Chemical Engineering Journal, 2022, 450(15): 138423. DOI URL