Research progress of biobased antibacterial hydrogels
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摘要: 致病微生物所引起的感染一直以来都威胁着全世界人类的健康，抗菌材料在某种情况下可以被视为抗生素的替代品，其中抗菌水凝胶就是一类重要的高分子抗菌材料。生物基抗菌水凝胶根据基体种类不同主要分为壳聚糖基、纤维素基、淀粉基、海藻酸钠基、蛋白质基等，这些基质在自然界具有高丰度，生物相容性及生物可降解性的优点，是制备抗菌水凝胶的理想材料。本文综述了近年来生物基抗菌水凝胶的发展现状及应用领域，着重从生物基抗菌水凝胶的种类、制备和应用3个方面来阐述，最后对生物基抗菌水凝胶所面临的挑战及未来的发展趋势进行了总结和展望。Abstract: Infections caused by pathogenic microorganisms have long been a threat to human health around the world. The development of antibacterial biomaterials can be regarded as a substitute for antibiotics in some cases, among which antibacterial hydrogels are an important class of macromolecular antibacterial agents. Bio-based antibacterial hydrogels can be divided into chitosan, cellulose, starch, sodium alginate and protein-based antibacterial hydrogels according to different matrix types. These substrates have high abundance, good biocompatibility and biodegradability in nature, and are ideal materials for preparing antibacterial hydrogels. In this paper, the development status and application fields of bio-based antibacterial hydrogels in recent years were reviewed, mainly from the types, preparation and application of bio-based antibacterial hydrogels. Finally, the challenges faced by bio-based antibacterial hydrogels and the future development trend were summarized and prospeced.
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图 1 (a) 壳聚糖(CS)-Ag+/NH3水凝胶机制示意图[17]；(b)对照组与CS-Ag+/NH3抗菌活性对比[17]；(c) 羧甲基壳聚糖/氧化右旋糖酐/γ-聚谷氨酸(COP)水凝胶交联机制及伤口涂覆示意图[20]；(d) COP水凝胶降解示意图[20]；(e) 水凝胶抗菌活性及促愈合示意图[20]
Figure 1. (a) Schematic diagram of chitosan (CS)-Ag+/NH3 hydrogel mechanism[17]; (b) Comparison of antibacterial activity between the control group and CS-Ag+/NH3[17]; (c) Schematic diagram of CMCS/OD/γ-PGA (COP) hydrogel crosslinking mechanism and wound coating[20]; (d) Schematic diagram of COP hydrogel degradation[20]; (e) Schematic diagram of hydrogel antibacterial activity and promoting healing[20]
CMCS—carboxymethyl chitosan; γ-PGA—γ-polyglutamic acid; OD—Oxidizing dextran; EDC—1-(3-dimethylaminopropyl)-3-ethylcarbodiimide hydrochloride; NHS—N-Hydroxy succinimide; CO—CMCS/OD; CP—CMCS/γ-PGA; CTS—chitosan;CTS0 —Samples without AgNO3; CTS13—Sample with optimal AgNO3 addition amount
图 2 (a) 羧甲基纤维素(CMC)基水凝胶制备示意图[23]；(b) 纤维素和季铵化纤维素(QC)在碱水溶液中与环氧氯丙烷(ECH)交联示意图[24]；(c) 细菌纤维素(BC)和3-氨基丙基三乙氧基硅烷(APTES)化学改性反应示意图[26]；(d) 菌落计数法检测样品对不同细菌抑制作用[26]
Figure 2. (a) Diagram of carboxymethyl cellulose (CMC)-based hydrogel preparation[23]; (b) Schematic diagram of cellulose and quaternary ammonium cellulose (QC) crosslinking with Epichlorohydrin (ECH) in alkaline water solution[24]; (c) Schematic of the chemical modification reactions of bacterial cellulose (BC) and 3-aminopropyl triethoxysilane (APTES)[26]; (d) Colony counting method was used to detect the inhibition of different bacteria[26]
PVA—Polyvinyl alcohol; EGDE—Ethylene glycol diglycidyl ethe; SPG—Schizophyllan;ECH—Epichlorohydrin
图 3 (a) AgNPs含量不同的羧甲基淀粉(CMS)/聚乙烯醇(PVA)/柠檬酸(CA)水凝胶对不同菌种的抑菌圈[29]；(b) 藻朊酸盐(Alg)/N-(2-羟基-3-三甲基铵)丙基壳聚糖(HTACC)水凝胶制备及作用示意图[31]；(c) HTACC制备示意图[31]
Figure 3. (a) Inhibition zone of carboxymethyl starch (CMS)/polyvinyl alcohol (PVA)/citric acid (CA) hydrogels with different AgNPs content on different strains[29]; (b) Preparation and action diagram of alginate (Alg) /N-(2-hydroxy-3-trimethylammonium) propyl chitosan (HTACC) hydrogel[31]; (c) Schematic diagram of HTACC preparation[31]
GTMEC—Glycidyl trimethylammonium chloride; S. aureus—Staphylococcus aureus; E. coli—Escherichia coli
图 4 (a) 海藻酸钠(SA)-壳寡糖(COS)-ZnO水凝胶制备及作用示意图[32]；(b) 对照组和SA-COS-ZnO水凝胶促进伤口愈合图[32]；(c) 水凝胶中ZnO纳米颗粒(NPs)随时间释放的百分比(SA47%表示SA被醛化程度)[32]；(d) 对照组(i)和SA-COS-ZnO(ii)水凝胶对不同菌种抑菌圈图片[32]；(e) 对照组和SA-COS-ZnO水凝胶对不同菌种的抑菌圈直径柱状图[32]
Figure 4. (a) Preparation and action diagram of sodium alginate (SA)-chito-oligosaccharides (COS)-ZnO hydrogel[32]; (b) Images of control group and SA-COS-ZnO hydrogel promoting wound healing[32]; (c) Percentage release of ZnO nano-particles (NPs) in hydrogel over time (SA47% indicates the degree to which SA is aldehyded)[32]; (d) Pictures of bacteriostatic zones of control group (i) and SA-COS-ZnO (ii) hydrogel for different species[32]; (e) Histogram of antibacterial zone diameter of control group and SA-COS-ZnO hydrogel for different species[32]
C.albicans—Candida albicans; B. subtilis—Bacillus subtilis; ASA—Amphiphilic sodium alginate
图 5 (a) 不同处理下耐甲氧西林金黄色葡萄球菌(MRSA)菌和SA菌的生长曲线[37]；(b) MRSA菌和SA菌与水凝胶共培养24 h后生长曲线[37]；(c) 水凝胶处理后MRSA和SA菌悬液图片[37]；(d) 小鼠皮肤伤口愈合图像[37]；(e) 不同水凝胶处理后伤口面积分布[37]；(f) 伤口愈合面积示意图[37]
Figure 5. (a) Growth curves of methicillin resistant staphylococcus aureus (MRSA) and SA strains under different treatments[37]; (b) Growth curves of MRSA and SA bacteria after 24 h of co-culture with the hydrogel[37]; (c) Pictures of MRSA and SA bacterial suspensions after hydrogel treatment[37]; (d) Images of wound healing in mouse skin[37]; (e) Wound area distribution after different hydrogel treatment[37]; (f) Schematic representation of the wound healing area[37]
THPS—Tetramethylphosphate sulfate; CFU—Colony-forming units; OD—Optical density; BSA—Bull serum albumin; B-Hydrogel—BSA hydrogel; G1—Control; G2—BSA; G3—THPS; G4—B-Hydrogel; CFU—Colony-forming units; OD—Optical density
图 6 (a) 前驱体溶液经紫外照射形成CS/聚甲基丙烯酰氧基乙基三甲基氯化铵(PMETAC)水凝胶示意图[40]；(b) 水凝胶交联示意图[40]；((c), (d)) 对照组与CS/PMETAC水凝胶不同菌种长期抗菌图片[40]
Figure 6. (a) Schematic diagram of CS/polymethylacryloxyethyl trimethyl ammonium chloride (PMETAC) hydrogel formed by UV irradiation of precursor solutionm[40]; (b) Schematic diagram of hydrogel cross-linking[40]; ((c), (d)) Long-term antibacterial pictures of different bacteria in control group and CS/PMETAC hydrogel[40]
图 7 (a) 羧甲基壳聚糖(CMCS)/低聚原花青苷(OPC)水凝胶形成及相互作用示意图[41]；(b) 水凝胶自愈机制示意图[41]；(c) 水凝胶对不同菌种杀菌率及抑菌圈照片及统计图[41]；(d) 空白组和水凝胶处理伤口、愈合率和定量分析肉芽组织厚度图片[42]
Figure 7. (a) Carboxymethyl chitosan (CMCS)/oligoproanthocyanidin (OPC) hydrogel formation and interaction diagram[41]; (b) Schematic diagram of the self-healing mechanism of hydrogel[41]; (c) Photos and statistical charts of bactericidal rate and bacteriostatic zone of hydrogel against different strains[41]; (d) Images of wounds, healing rates and quantitative granulation tissue thickness in blank and hydrogel dressing treatments[41]
CCS—Catechol modified chitosan ; CCHOs—aldehyde-modified cellulose nanocrystals; x in CMCS/OPCx—Content of OPC is x%
图 8 (a) 水凝胶膜形成机制及抗菌作用示意图[46]；((b), (c)) 贮藏10天期间使用聚乙烯(PE)膜、再生纤维素(RC)膜和试验组(N-3)包装猪肉中细菌总数和总挥发性氮(TVB-N)[46]；(d) 膜对两种菌落覆盖的琼脂图片[46]；(e) 25℃不同膜对奶酪包装影响图片[46]
Figure 8. (a) Schematic diagram of hydrogel film formation mechanism and antibacterial action[46]; ((b), (c)) Total bacterial count and total volatile nitrogen (TVB-N) in pork packaged with polyethylene (PE) film, regenerated cellulose (RC) film and experimental group (N-3) during 10 days of storage[46]; (d) AGAR images of the membrane covering both colonies[46]; (e) Pictures of the effects of different films on cheese packaging at 25℃[46]
CNC—Cellulose nanocrystal; r-CNC—Rosin-grafted CNCs; PVC—Polyvinyl chloride
图 9 (a) 多功能电子皮肤制备示意图[53]；(b) 菌落溶液培养24 h后图片[53]；(c) 腕部脉搏随运动实时I-t曲线[53]；(d) 弯曲手指关节的实时I-t曲线[53]；(e) 行走时电子皮肤的实时I-t曲线[53]
Figure 9. (a) Schematic diagram of multifunctional e-skin preparation[53]; (b) Pictures after 24 h of colony solution culture[53]; (c) Real-time I-t curves of wrist pulse with movement[53]; (d) Real-time I-t curve of bending finger joint[53]; (e) Real-time I-t curve of the electronic skin during walking[53]
TOCN—TEMPO oxidized cellulose nanofibers; t—Incubation time
表 1 不同生物基抗菌水凝胶作用机制、基底材料对比分析
Table 1. Comparative analysis of action mechanism and substrate materials of different biological - based antibacterial hydrogels
Action Substrate Antimicrobial agent Antimicrobial ability Citation Other properties References Metal coordination CS Ag+ 5 mm inhibition zone Wound dressing Tensile strength (0.17 MPa) [17] Schiff base DCS, PEGSH — Lethal rate for E. coli and
S. aureus exceeds 95%Medical adhesive Blood absorption performance
((1300±50)%)[19] Metal coordination CMC, PVA AgNPs 15 mm inhibition zone against UTI pathogens Antibacterial material — [23] Silicon-oxygen
covalent bondBC SPG Inhibitory against E. coli and
S. aureusAntibacterial film — [26] Metal coordination CMS, PVA AgNPs 6 mm inhibition zone Wound dressing Swelling index 243% [29] Schiff base ASA, COS ZnO NPs 3.1 cm inhibition zone against
B. subtilisWound dressing Water vapor permeability
682 g/m2/24 h[32] Hydrogen bond ASA PL Lethal rate for E. coli and S. aureus exceeds 91.01% and 84.97% Wound healing materials PL broad-sectrum
and efficient[33] Mannich reaction BSA THPS 15 mm inhibition zone Wound healing dressing Wide alicability [37] Electrostatic
InteractionGel, CS, NF CA Lethal rate for E. coli and S. aureus exceeds 90% Wound dressing Tensile strength (0.85±0.02) MPa [38] Notes: PL—Polylysine; NF—Non-woven fabrics; SPG—Schizophyllan. 
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