Construction of Sustainable Release Antimicrobial Microspheres Loaded with Potassium Diformate

doi:10.15541/jim20200131

Abstract

Abstract:

To prevent potassium diformate (KDF) from decomposing too quickly in an acidic environment, adjust the acidity and alkalinity of the gastrointestinal tract of the piglets and the colony balance, and realize the targeted release of KDF antibacterial, in this study, a kind of hydrogel microspheres were prepared by biodegradable chitosan (CS), carboxymethyl cellulose (CMC), and inorganic rigid material P-type molecular sieve (Zeolite P). Then the antibacterial drug potassium diformate was loaded so as to be controlled to release from this hydrogel microsphere. The results show that -NH₂ in CS and -COOH in CMC form a stable polyelectrolyte complex through ion interaction. Swelling rate test indicates that the CS/CMC/Zeolite P hydrogel microspheres display high pH-sensitivity. The addition of Zeolite P allows the hydrogel microspheres to maintain their original morphology at pH1.2 without being degraded or broken. The effective sustained-release KDF in pH7.4 phosphate buffer solution exhibits better sustained-release performance than that in pH1.2. When the concentration of CS/CMC/Zeolite P/KDF antimicrobial microspheres is 96 mg/mL, the maximum bacteriostatic rate of Escherichia coli is 83%, which effectively improves the utilization rate of KDF.

Key words: potassium diformate, hydrogel microsphere, sustained-release, antibacterial

CLC Number:

TB332

GUO Xiaowei, LI Yuyan, CHEN Nanchun, WANG Xiuli, XIE Qinglin. Construction of Sustainable Release Antimicrobial Microspheres Loaded with Potassium Diformate[J]. Journal of Inorganic Materials, 2021, 36(2): 181-187.

Figures/Tables 10

Fig. 1 Preparation of antibacterial microspheres loaded with KDF

Fig. 2 FT-IR spectra of CMC (a), CS (b), Zeolite P (c) and CS/CMC/Zeolite P (d) CS: chitosan; CMC: carboxymethyl cellulose; Zeolite P: Zeolite P molecular sieve

Fig. 3 Structures of CS/CMC/Zeolite/KDF microspheres

Fig. 4 TGA analysis of CS/CMC/Zeolite P(a), CS/CMC(b), CMC(c) and CS(d) CS: chitosan; CMC: carboxymethyl cellulose; Zeolite P: Zeolite P molecular sieve

Fig. 5 Internal SEM images of CS/CMC/Zeolite P

Fig. 6 Effect of Zeolite P concentration on swelling ratios of CS/CMC/Zeolite P in pH 7.4, pH 6.8 and pH 1.2

Fig. 7 Effect of Zeolite P concentration on KDF release profiles of CS/CMC/Zeolite P/KDF in pH 7.4 (a) and pH 1.2 (b)

Fig. 8 Kinetic equation of CS/CMC/Zeolite P/KDF in simulated gastric fluid with curves of Zero order kinetics (a),First order kinetics (b) and Higuchi equations (c)

Fig. 9 Kinetic equation of CS/CMC/Zeolite P/KDF in simulated intestinal fluid with curves of Zero order kinetics (a),First order kinetics (b), Higuchi equations (c)

Fig. 10 Antibacterial rates of antibacterial agents with different concentrations on Escherichia coli

References 30

[1]	MARQUARDT R R, LI S Z. Antimicrobial resistance in livestock: advances and alternatives to antibiotics. Animal Frontiers, 2018,8(2):30-37.
[2]	CANIÇA M, MANAGEIRO V, ABRIOUEL H, et al. Antibiotic resistance in foodborne cacteria. Trends in Food Science & Technology, 2019,84:41-44.
[3]	LIN W S, WANG H X, LI Q B, et al. Optimization of green synthesis of potassium diformate and its potential as a mold inhibitor for animal feed. Industrial and Engineering Chemistry Research, 2010,49(13):5981-5985.
[4]	XIA S S, YAO W, ZOU B, et al. Effects of potassium diformate on the gastric function of weaning piglets. Animal Production Science, 2016,56:1161-1166.
[5]	CANIBE N, STEIEN S H, OVERLAND M, et al. Effect of K-diformate in starter diets on acidity, microbiota, and the amount of organic acids in the digestive tract of piglets, and on gastric alterations. Journal of Animal Science, 2001,79(8):2123-2333. URL PMID
[6]	PAULICKS B R, ROTH F X, KIRCHGESSNER M. Effects of potassium diformate (Formi® LHS) in combination with different grains and energy densities in the feed on growth performance of weaned piglets. Journal of Animal Physiology and Animal Nutrition, 2000,84(3/4):102-111.
[7]	MROZ Z, REESE D E, OVERLAND M. The effects of potassium diformate and its molecular constituents on the apparent ileal and fecal digestibility and retention of nutrients in growing-finishing pigs. Journal of Animal Science, 2002,80(3):681-690. URL PMID
[8]	ZHANG X H, CHEN N C, TANG Q, et al. Slow releasing behaviors of potassium diformate from zeolite A. Journal of the Chinese Ceramic Society, 2013,41(2):245-250.
[9]	HU Y, GUO X W, PEI Y C, et al. Zeolite X with potassium diformate as a sustained-release antibacterial agent. Bulletin of Materials Science, 2019,42(2):66-70.
[10]	RASOULZADEH M, NAMAZI H. Carboxymethyl cellulose/ graphene oxide bio-nanocomposite hydrogel beads as anticancer drug carrier agent. Carbohydrate Polymers, 2017,168:320-326.
[11]	SHARIATINIA Z. Pharmaceutical applications of chitosan. Advances in Colloid and Interface Science, 2019,263:131-194.
[12]	WANG S J, ZHANG Q, TAN B, et al. pH-sensitive poly(vinyl alcohol)/sodium carboxymethyl cellulose hydrogel beads for drug delivery. Journal of Macromolecular Science, Part B: Physics, 2011,50(12):2307-2317.
[13]	MITSUMATA T, SUEMITSU Y, FUJII K, et al. pH-response of chitosan, κ-carrageenan, carboxymethyl cellulose sodium salt complex hydrogels. Polymer, 2003,44(23):7103-7111.
[14]	ZHU Y L, GU Y, CHEN K P, et al. Research progress in synthesis and application of microcapsules with organic-inorganic hybrid shell. Journal of Functional Materials, 2015,46(19):19007-19013.
[15]	ZHAI Q Z. Preparation and controlled release of mesoporous MCM-41/propranolol hydrochloride composite drug. Journal of Microencapsulation, 2013,30(2):173-180. URL PMID
[16]	ZHANG L, PENG Y X, ZHANG J, et al. Adsorptive and catalytic properties in the removal of volatile organic compounds over zeolite-based materials. Chinese Journal of Catalysis, 2016,37(6):800-809.
[17]	KHODAVERDI E, HONARMANDI R, ALIBOLANDI M, et al. Evaluation of synthetic zeolites as oral delivery vehicle for anti- inflammatory drugs. Iranian Journal of Basic Medical Sciences, 2014,17(5):337-343. URL PMID
[18]	GAO S S, CHEN N C, PEI Y C, et al. Hydrothermal reaction conditions for preparation of zeolite P from natural stilbite as raw material. Journal of Synthetic Crystals, 2018,47(6):1096-1101.
[19]	ZHANG C Y, CHEN N C, ZHANG X H, et al. In situ preparation and structure of zeolites A, X and P. Journal of the Chinese Ceramic Society, 2014,42(10):1332-1336.
[20]	ZHANG X H. Study on preparation of zeolite antibacterial agents and antibacterial properties. Guilin: Master's thesis of Guilin University of Technology, 2013.
[21]	JIN X X, WANG J T, BAI J. Synthesis of Schiff base from chitosan and cinnamaldehyde and its antimicrobial activity. Journal of Chemical Engineering of Chinese Universities, 2010,24(4):645-650.
[22]	YADOLLAHI M, NAMAZI H. Synthesis and characterization of carboxymethyl cellulose/layered double hydroxide nanocomposites. Journal of Nanoparticle Research, 2013,15(4):2-9.
[23]	YADOLLAHI M, NAMAZI H, BARKHORDARI S. Preparation and properties of carboxymethyl cellulose/layered double hydroxide bionanocomposite films. Carbohydrate Polymers, 2014,108(1):83-90.
[24]	BEHIN J, KAZEMIAN H, ROHANI S. Sonochemical synthesis of zeolite NaP from clinoptilolite. Ultrasonics Sonochemistry, 2016,28:400-408. DOI URL PMID
[25]	DONG X X, HONG J H, HE G. Synthesis of zeolite NaP from low-grade kaolin with high silica content. Journal of Synthetic Crystals, 2016,45(16):2650-2654.
[26]	WANG R, SHOU D, LÜ O Y, et al. pH-controlled drug delivery with hybrid aerogel of chitosan, carboxymethyl cellulose and graphene oxide as the carrier. International Journal of Biological Macromolecules, 2017,103:248-253.
[27]	LEE J H, CHOI Y M, PAIK U, et al. The effect of carboxymethyl cellulose swelling on the stability of natural graphite particulates in an aqueous medium for lithium ion battery anodes. Journal of Electroceramics, 2006,17(2):657-660.
[28]	YU W L, LIU W H, ZHANG L, et al. Preparation of B-vitamins microcapsules and studies on its slow-release kinetics. Journal of Chinese Institute of Food Science and Technology, 2019,19(12):122-132.
[29]	WANG R, SHOU D, LV O Y, et al. pH-controlled drug delivery with hybrid aerogel of chitosan, carboxymethyl cellulose and graphene oxide as the carrier. International Journal of Biological Macromolecules: Structure, Function and Interactions, 2017,103:248-253.
[30]	KORSMEYER R W, GURNY R, DOELKER E, et al. Mechanisms of solute release from porous hydrophilic polymers. International Journal of Pharmaceutics, 1983,15(1):25-35.