多糖基天然高分子水凝胶的吸附性能: Comparison
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Please note this is a comparison between Version 2 by Jessie Wu and Version 1 by Wenxu Zhang.

淡水资源的污染和稀缺是对人类生活产生重大影响的全球性问题。去除水中的有害物质对于实现水资源的循环利用非常重要。水凝胶因其特殊的三维网状结构、较大的比表面积和孔隙而备受关注，显示出去除水中污染物的巨大潜力。在制备过程中，天然聚合物因其广泛的可用性、低成本和易热降解而成为首选材料之一。但是，当它直接用于吸附时，其性能并不理想，因此通常需要在制备过程中进行改性。

  • hydrogel
  • adsorption
  • natural polymer

1. 多糖基水凝胶的吸附机理与动力学Adsorption Mechanism and Kinetics of Polysaccharide-Based Hydrogels

水凝胶的吸附可分为化学吸附和物理吸附。化学吸附是一个不可逆的过程，主要是因为它的吸附剂和吸附剂在相互作用中是化学键合的The adsorption of the hydrogel can be divided into chemisorption and physisorption. Chemisorption is an irreversible process, mainly because its adsorbent and adsorbent are chemically bonded in the interaction;纽带的破坏是永久性的，一旦被破坏，将无法再次结合。相比之下，物理吸附是一个不可逆的过程，通常由物理力控制，如氢键、离子键、π-π堆积、疏水相互作用等，被破坏后可以恢复。在制备水凝胶时，物理作用通常与化学作用相结合，以加强其吸附性能和机械性能，例如在自修复水凝胶中，通常通过物理作用分散能量消耗，以确保内部化学键和机械性能的完整性得到改善;这种水凝胶广泛用于生物工程[39]。在吸附领域的水凝胶制备中，研究人员还选择将这两种作用模式结合起来。具体的吸附机理及其分类如下。 the destruction of the bond is permanent and, once destroyed, will not be able to bond again. In contrast, physisorption is an irreversible process, usually controlled by physical forces, such as hydrogen bonding, ionic bonding, π–π stacking, hydrophobic interactions, etc., and can be restored after being disrupted. In the preparation of hydrogels, physical action is usually combined with chemical action to strengthen their adsorption properties and mechanical properties, such as in self-healing hydrogels, which usually disperse energy consumption by physical action to ensure that the integrity of internal chemical bonds and mechanical properties is improved; such hydrogels are widely used in bioengineering [1]. In the preparation of hydrogels in the field of adsorption, researchers have also chosen to combine the two modes of action. The specific adsorption mechanisms and their classification are as follows.

1.1. 吸附机理Adsorption Mechanism

在吸附过程中，不同的官能团具有不同的吸附机理和不同的作用方式，官能团决定了分子间力的类型和强度以及分子的化学反应性。多糖基水凝胶材料吸附过程中涉及的主要官能团可分为三大类：含氧官能团、含氮官能团和含硫官能团。In the adsorption process, different functional groups have different adsorption mechanisms and different modes of action, and functional groups determine the type and strength of intermolecular forces and the chemical reactivity of molecules. The main functional groups involved in the adsorption process of polysaccharide-based hydrogel materials can be divided into three main categories: oxygen-containing functional groups, nitrogen-containing functional groups, and sulfur-containing functional groups. N，O和S类杂原子可以贡献一个或多个电子并与金属离子形成配位键，同时还进行离子交换或静电吸引以实现对各种污染物的吸附。在报道的水凝胶的各种金属吸附机制中，静电相互作用、离子交换和表面络合（包括配位和螯合）这三种方法被发现与表面官能团密切相关[6]。如图1所示，描述了通过这三种作用模式进行吸附时的作用过程，其中两种静电相互作用和离子交换的吸附机理大多是可逆的，吸附剂可以重复使用，属于物理吸附。, O, and S class heteroatoms can contribute to one or more electrons and form coordination bonds with metal ions while also undergoing ion exchange or electrostatic attraction to achieve the adsorption of a wide range of contaminants. Among the various metal adsorption mechanisms reported for hydrogels, the three methods of electrostatic interactions, ion exchange, and surface complexation (including coordination and chelation) have been found to be closely related to surface functional groups [2]. As shown in Figure 5, the process of action when adsorption is carried out by these three modes of action is depicted, among which most adsorption mechanisms of the two electrostatic interactions and ion exchange are reversible, and the adsorbents can be reused and belong to physical adsorption.
Gels 09 00249 g005 550
图1Figure 5.三种模式下的吸附过程示意图。 Schematic diagram of the adsorption process in three modes.

1.2. 吸附动力学Adsorption Kinetics

1.2.1. 伪一阶动力学Pseudo-First-Order Kinetic

伪一级动力学模型基于模态扩散理论，该理论假设吸附剂从溶液到达吸附剂表面受扩散步骤控制，并且吸附剂表面只有一个结合位点[40]。等式的形式如下：The pseudo-first-order kinetic model is based on the modal diffusion theory, which assumes that the arrival of the adsorbent from the solution to the adsorbent’s surface is controlled by the diffusion step and that the adsorbent’s surface has only one binding site [3]. The form of the equation is as follows:
ln q e − q t = lnq e − K 1 t ln(qe−qt)=lnqe−K1tlnqe−qt=lnqe−K1t
其中where qt是时间T的吸附容量（ is the adsorption capacity at time t (mg/g），), qe是吸附平衡时刻的吸附容量（ is the adsorption capacity at the moment of adsorption equilibrium (mg/g），), and K1是一阶动力学的速率常数。 is the rate constant of the first-order kinetic.
虽然一阶动力学模型已广泛用于各种吸附过程，但它具有局限性。它通常只适用于吸附初始阶段的动力学描述，不能准确描述整个吸附过程[41]。Although the first-order kinetic model has been widely used for various adsorption processes, it has limitations. It is often only suitable for the kinetic description of the initial stage of adsorption and cannot accurately describe the entire process of adsorption [4].

1.2.2. 伪二阶动力学Pseudo-Second-Order Kinetic

伪二阶动力学模型基于吸附限速步骤，包含吸附机理，如化学吸附，涉及吸附物和吸附剂之间的电子共享或电子转移[42]。与伪二阶动力学模型的一致性表明，吸附动力学主要由化学相互作用控制，而不是由材料传递步骤控制。等式的形式如下：The pseudo-second-order kinetic model is based on the adsorption rate-limiting step and contains the adsorption mechanism, such as chemisorption, which involves electron sharing or electron transfers between the adsorbate and the adsorbent [5]. The conformity to the pseudo-second-order kinetic model indicates that adsorption kinetics are mainly controlled by chemical interactions rather than by the material transport steps. The form of the equation is as follows:
t q t = 1 K 2 q e 2 + t q e tqt=1K2qe2+tqetqt=1K2qe2+tqe
其中where qt是时间T的吸附容量（ is the adsorption capacity at time t (mg/g），), qe是吸附平衡时刻的吸附容量（ is the adsorption capacity at the moment of adsorption equilibrium (mg/g），), and K2（ (g/mg·h） 是伪二阶速率常数。) is the pseudo-second-order rate constant.

1.3. 吸附等温线Adsorption Isotherms

1.3.1. 朗缪尔等温线方程Langmuir Isotherm Equation

The Langmuir吸附等温线模型是应用最广泛的分子吸附模型，它可以通过考虑吸附剂表面和温度的影响来预测吸附剂的最大吸附容量[43]。该理论是单分子层吸附理论，它要求具有相同吸附容量的均匀固体表面，并且吸附分子之间没有相互作用，但模型的假设与实际情况相去甚远，获得的信息有时非常不准确[44]。等式的形式如下： adsorption isotherm model is the most widely used molecular adsorption model, which can predict the maximum adsorption capacity of adsorbents by considering the influence of the adsorbent’s surface and temperature [6]. This theory is a single molecular layer adsorption theory, which requires a homogeneous solid surface with the same adsorption capacity and no interaction between the adsorbed molecules, but the assumptions of the model are far from the actual conditions, and the information obtained is sometimes highly inaccurate [7]. The form of the equation is as follows:
C e q Ceqe=Ce q qm+1qmK L LCeqe=Ceqm+1qmKL
其中where Ce是溶液的平衡浓度， is the equilibrium concentration of the solution, mg/L，, qm是最大吸附容量（饱和度）、 is the maximum adsorption capacity (saturation), mg/g 和, and KL是与键合位点的亲和力和吸附能 is the Langmuir constant related to the affinity and adsorption energy of the bonding site, L/g相关的朗缪尔常数。.

1.3.2. 弗氏等温线方程Freundlich Isotherm Equation

弗氏等温吸附方程是一个没有假设的经验方程。等式的形式如下：The Freundlich isothermal adsorption equation is an empirical equation with no assumptions. The form of the equation is as follows:
lnqe=lnK F+=lnKF+1nlnC lnCelnqe=lnKF+1nlnCelnqe=lnKF+1nlnCe
其中where qe是吸附达到平衡时的吸附量 is the adsorption amount, mg/g，, when adsorption reaches equilibrium, Ce是吸附平衡时溶液中吸附物的浓度， is the concentration of adsorbate in solution at adsorption equilibrium, mg/L，, KF是弗氏模型下与吸附容量和吸附强度相关的常数， is the constant related to adsorption capacity and adsorption strength under the Freundlich model, and 1/n为弗氏常数。 is the Freundlich constant. A large value of KF 值大F是吸附剂吸附性能更好的标志。弗氏吸附等温线可通过绘制is a sign of a better adsorption performance of the adsorbent. Freundlich adsorption isotherms can be obtained by plotting lnq得到e针对 against lnCe在不同温度下[45]。 at different temperatures [8].

2. Adsorption Applications 多糖基水凝胶的吸附应用of Polysaccharide-Based Hydrogels

2.1. 重金属离子吸附Heavy Metal Ion Adsorption

重金属离子剧毒、不可降解，在环境中具有生物蓄积性，在水和生物系统中通过食物链循环，严重影响食物链顶端的生物[59，60]。重金属是密度大于Heavy metal ions are highly toxic, non-degradable, and bioaccumulative in the environment and circulate through the food chain in water and biological systems, seriously affecting the organisms at the top of the food chain [9][10]. Heavy metals are metals with a density greater than 4.5克 g/厘米的金属cm3，主要包括金、银、铜、铅、锌、镍、钴、镉、汞、镉等, mainly including Au, Ag, Cu, Pb, Zn, Ni, Co, Cd, Hg, Cd, and more than 40多种金属[61]。对人体毒性最大的五种是铅、汞、铬、砷和镉。这些重金属在水中不能分解，进入人体时毒性被放大 other kinds of metals [11]. The five most toxic to humans are lead, mercury, chromium, arsenic, and cadmium. These heavy metals cannot be decomposed in water, and their toxicity is amplified when they enter the human body;因此，需要高效和特殊的方法来去除水系统中的重金属污染物[62]。重金属离子的吸附过程与吸附材料本身的官能团直接相关，目前的研究大多围绕二价重金属离子的吸附展开，其中 therefore, efficient and special methods are needed to remove heavy metal contaminants from water systems [12]. The adsorption process of heavy metal ions is directly related to the functional groups of the adsorbent materials themselves, and most current studies mainly revolve around the adsorption of divalent heavy metal ions, of which Cu2+，, 钯Pd2+和镉, and Cd2+占主导地位。表 are predominant. Table 1总结了过去两年多糖基吸附材料用于重金属离子吸附的应用。 summarizes the polysaccharide-based adsorbent materials in the last two years for this application of heavy metal ion adsorption.
表Table 1.不同多糖基复合水凝胶对重金属离子的吸附 Adsorption of heavy metal ions by different polysaccharide-based composite hydrogels.
多糖Polysaccharide

水凝胶Hydrogel

吸附Adsorption		 吸附物Adsorbates 吸附容量（毫克Adsorption Capacity (mg/克）g) 吸附Adsorption

等温线Isotherm		 吸附Adsorption

动力学Kinetics		 Kinetics裁判。Ref.
Ref.
上午AM/AA 铜Cu2+ 157.51 朗缪尔Langmuir PSO定位器 [
C/SA/FeMB63]105.93[Langmuir13PSO]
[88] 钯Pd2+ 393.28 朗缪尔Langmuir PSO定位器
CarboxymethylcelluloseMB756FreundlichPSO[12] 镉Cd2+ 289.97 朗缪尔Langmuir PSO定位器
纳米纤维素Nanocellulose/碳点Carbon dot 铬Cr6+ 599.9 弗罗恩德利希Freundlich PSO定位器 [64][14]
秸秆纤维素Straw cellulose 镉Cd2+
Pineapple peel

cellulose/diatomite		MB101.94LangmuirPSO[89]95.62
PCMC-PVAMB172.14LangmuirPSO[90] 朗缪尔Langmuir PSO定位器 [65][15]
All-lignocelluloseMB145LangmuirPSO[72] 纳米纤维素Nanocellulose/南非SA 铅
Millettia speciosa Champ cellulose-CSPb2+ 318.47 朗缪尔Langmuir PSO定位器 [66][16]
CR221.43FreundlichPSO[71] 去GO-PVA-CS 镉
PAM-Fe3O4Cd2+ 172.11 朗缪尔Langmuir PSO定位器 -CS[67]MB[17]
1603LangmuirPFO[91] 镍Ni2+ 70.37 朗缪尔Langmuir PSO
Montmorillonite-CS定位器
MB530LangmuirPSO[92] 中国国际铜矿CYCS/数控CNC 铅Pb2+ 334.92 朗缪尔Langmuir PSO
GO-CS-Fe3O4MB289定位器 [68][18]
LangmuirPSO[93] 壳聚糖低聚糖Chitosan oligosaccharide 铬Cr6+ 148.1 朗缪尔Langmuir EBT292PSOLangmuir定位器 [69][19]
PSO[94] α-酮戊二酸ketoglutaric acid–PAM-氨基戊二酸-丙烯酸CS 铜Cu2+ 72.39 朗缪尔Langmuir PSO定位器 [50][20]
钯Pd2+ 61.41 朗缪尔Langmuir PSO定位器
Jute cellulose nanocrystalMB131.58LangmuirPSO
Succinic anhydride-SNCsMB84.00FreundlichPSO[31] 锌Zn2+ 51.89 朗缪尔Langmuir PSO定位器
Reptilite-StarchMB277.0LangmuirPSO CPCS-PAM-PVA 铬Cr6+ 95.31 朗缪尔Langmuir 全氟辛烷磺酸PFO [70][21]
[81]
PAM-cassava starchMB2000LangmuirPSO[ Millettia speciosa Champ cellulose-CS Cu2+ 23.37 Freundlich PFO [71][22]
95]
MXene-SAMB92.17LangmuirPSO[96] All-lignocellulose Cu2+ 350 Langmuir PSO [72][23]
AA-GO-SAMG628.93LangmuirPSO[97] Caffeic acid starch Cr6+ 96.45 Langmuir PSO [73][24]
Flax seed ash-SAMB333.3LangmuirPSO[98] Starch-FMBO As3+ 161.29 Langmuir PSO [74][25]
Starch nanoparticle Pb2+
PEI-SAMB400LangmuirPSO[47] 40.52 Langmuir PSO [27][26]
AM-HEMA-StarchMG164LangmuirPFO[71] Cu2+ 32.88 Langmuir PSO
MV156Freundlich dibenzo-18-crown-6 starch Cd2+ 368.5 Freundlich PSO [75][27]
Ni2+ 182.5 Freundlich PSO
Zn2+ 377.5 Freundlich PSO
Cu2+ 385 Freundlich PSO
Succinic anhydride-SNCs Cu2+ 84.07 Freundlich PSO [31][28]
PVA-SA Pb2+ 784.97 Langmuir PSO [76][29]
ZIF-67-SA Cu2+ 153.63 Langmuir PSO [77][30]
AM-GO-SA Cu2+ 68.76 Langmuir PSO [78][31]
Pb2+ 240.69 Langmuir PSO
Zeolite-PVA-SA Pb2+ 99.5 Langmuir PFO [79][32]
Cd2+ 99.2 Langmuir PFO
Sr2+ 98.8 Langmuir PFO
Cu2+ 97.2 Langmuir PFO
Zn2+ 95.6 Langmuir PFO
Ni2+ 93.1 Langmuir PFO
Mn2+ 92.4 Langmuir PFO
Starch ether-SA Cu2+ 25.81 Langmuir PSO [80][33]
Reptilite-Starch Pb2+ 180.8 Langmuir PSO [81][34]
NCDs-CNF/CS Cu2+ 148.3 Langmuir PSO [82][35]
Cr6+ 294.46 Langmuir PSO
CTS/CA/BT Pb2+ 434.89 Freundlich PSO [83][36]
Cu2+ 115.30 Freundlich PSO
Cd2+ 102.38 Freundlich PSO
GO-SA As5+ 277.39 Langmuir PSO [55][37]
PAN-PPY-SA-GO Cu2+ 133.7 Redlich–Peterson PFO [84][38]
Cr6+ 87.2 Redlich–Peterson PFO

2.2. Dye Adsorption

There are many methods for removing dyes from wastewater: biological dye removal, acoustic chemical degradation, electrocatalytic degradation, cation exchange membrane technology, etc. However, these processes produce toxic residues that cause secondary pollution and are costly to implement. In contrast, the gel’s adsorption method is simple, efficient, and inexpensive to operate. Hydrogels have a strong dye removal capability, and dyes are more easily diffused in the dissolved hydrogel, which enhances the adsorption capacity via electrostatic interactions with oppositely charged dyes [85][39].
There is a wide range of adsorbed dyes, among which methylene blue (MB), malachite green (MG), and methyl orange (MO) fuels are more widely adsorbed. MB is a phenothiazine cationic dye, an alkali, that is used to treat methemoglobinemia in histology and microscopy to identify and detect bacteria, to treat fungal infections by staining tissues [21][40], and to stain cotton and wood. The waste dye discharged into the environment after use can be harmful, causing dizziness, headaches, tremors, and mental confusion, among other symptoms [86][41]. Malachite green (MG) is a toxic trityl methane chemical, both as a dye and as a bactericidal and parasiticidal chemical, is an alkali, and is prohibited for use in aquaculture. In industries, it is used to color leather, paper, cotton, and silk. However, it is potentially carcinogenic, teratogenic, and mutagenic and is difficult to remove from water [87][42]. Table 2 summarizes polysaccharide-based adsorbent materials used in the past two years for this application of dye adsorption.
Table 2. Adsorption of dyes by different polysaccharide-based composite hydrogels.
Adsorption of dyes by different polysaccharide-based composite hydrogels.
Polysaccharide

Hydrogels

Adsorption		AdsorbatesAdsorption Capacity (mg/g)Adsorption

Isotherm		Adsorption

PFO
Polysaccharide

Hydrogels

Adsorption		AdsorbatesAdsorption Capacity (mg/g)Adsorption

Isotherm		Adsorption

Kinetics		Ref.
C/SA/FeMB105.93
Table 3. Adsorption of drug antibiotics by different polysaccharide-based composite hydrogels.
Table 3. Adsorption of drug antibiotics by different polysaccharide-based composite hydrogels.
多糖Polysaccharide

水凝胶Hydrogels

吸附Adsorption		 吸附物Adsorbates 吸附容量（毫克Adsorption Capacity (mg/克）g) 吸附Adsorption

等温线Isotherm		 吸附Adsorption

动力学Kinetics		 裁判。Ref.
LangmuirPSO
铁Fe3O4-[43]
淀粉Starch 萘Naphthalene 24.752 朗缪尔Langmuir PSO定位器 [99][56] CarboxymethylcelluloseMB756FreundlichPSO[44]
Pineapple peel

cellulose/diatomite		MB101.94Langmuir
CS-壳聚糖薄膜Chitosan filmPSO[45]
] PCMC-PVAMB172.14
氨基Amino/GO-SALangmuirPSO[46]
环丙沙星Ciprofloxacin 301.36 朗缪尔Langmuir PSO定位器 [101][58] All-lignocellulose
腐植酸Humicacid-CS-生物炭MBBiochar145LangmuirPSO[23]
环丙沙星Ciprofloxacin 154.89 朗缪尔Langmuir PSO定位器 [102][59Millettia speciosa Champ cellulose-CSCR[48]
]
生物炭Biochar221.43-CSFreundlichPSO[22]
环丙沙星Ciprofloxacin 106.038 朗缪尔Langmuir PSO定位器 [103][60] PAM-Fe3O4-CSMB1603LangmuirPFO[47]
恩诺沙星Enrofloxacin 100.433 朗缪尔Langmuir PSO定位器 Montmorillonite-CSMB530LangmuirPSO
戈萨GO-SA 氟沙星Fluoxacin 4.11 朗缪尔Langmuir PSO定位器 [104][61] GO-CS-Fe3O4MB289Langmuir
莫西沙星Moxifloxacin 3.43 朗缪尔Langmuir PSOPSO定位器[49]
EBT
铁Fe3292LangmuirPSOO4-SA 四环素Tetracycline 454.54 朗缪尔Langmuir[50]
PSO定位器 [105][62] Jute cellulose nanocrystalMB131.58LangmuirPSO
阿莫西林Amoxicillin 400 朗缪尔Langmuir PSO定位器 Succinic anhydride-SNCsMB84.00FreundlichPSO
三甲基氯化铵Trimethylammonium chloride-CS 四环素[28]
Tetracycline 22.42 朗缪尔Langmuir 全氟辛烷磺酸PFO [106][63] Reptilite-StarchMB277.0LangmuirPSO[
聚氯乙烯PVA-SA-铜Cu2+34]
四环素Tetracycline 231.431 朗缪尔Langmuir PSO定位器 [107][64] PAM-cassava starchMB2000LangmuirPSO[51]
MXene-SAMB92.17LangmuirPSO[52]
AA-GO-SAMG628.93LangmuirPSO[53]
Flax seed ash-SAMB333.3LangmuirPSO[54]
PEI-SAMB400LangmuirPSO[55]
AM-HEMA-StarchMG164LangmuirPFO[22]
MV156FreundlichPFO

2.3. Drug Antibiotics Adsorption

In the treatment of contaminants in water, attention has been focused mainly on the adsorption of textile dyes and heavy metals. However, the harmful effects of these emerging contaminants, such as pesticides, herbicides, fungicides, pharmaceutical compounds, and personal care products, on the water environment cannot be ignored. Once the toxic substances of pharmaceutical and medical waste enter the soil, they will be adsorbed by the soil, pollute the soil, kill microorganisms and protozoa in the soil, and destroy the microecology in the soil, which in turn will reduce the soil’s ability to degrade pollutants. Furthermore, the acid, alkali, and salts in the substances will change the nature and structure of the soil, leading to the acidification, alkalization, and hardening of the soil, affecting the development and growth of plant roots, and damaging the ecological environment; meanwhile, many harmful drug pollutants can cause serious damage to the liver and nervous systems. Table 3 summarizes the polysaccharide-based adsorption materials used for antibiotic adsorption in the past two years.
头孢噻肟钠
Cefotaxime Sodium
1003.64 弗罗恩德利希Freundlich PSO定位器 [100][57]
戈萨GO-SA 四环素Tetracycline 477.9 弗罗恩德利希Freundlich PSO定位器 [55][37

 

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