食品工业科技

组别	K	n	R²
对照组	104.91±23.20	0.41±0.05	0.93995
TP-EWP-20%	1316.68±37.94	0.20±0.01	0.99951
TP-EWP-25%	1128.15±118.78	0.26±0.025	0.9922
TP-EWP-30%	462.20±25.40	0.20±0.01	0.99821
TP-EWP-35%	500.19±70.82	0.39±0.03	0.97668
TP-EWP-40%	230.17±16.83	0.44±0.02	0.99205

组别	K	n	R²
对照组	104.91±23.20	0.41±0.05	0.93995
TP-EWP-20%	1316.68±37.94	0.20±0.01	0.99951
TP-EWP-25%	1128.15±118.78	0.26±0.025	0.9922
TP-EWP-30%	462.20±25.40	0.20±0.01	0.99821
TP-EWP-35%	500.19±70.82	0.39±0.03	0.97668
TP-EWP-40%	230.17±16.83	0.44±0.02	0.99205

茶多酚-蛋清蛋白复合凝胶3D打印体系的构建及特性研究

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杨君慧 , 刘丽莉 ^* , 谢天怡 , 程伟伟 , 张新帅 , 丁玥

食品工业科技 | 研究与探讨 2026,47(13): 125-133

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食品工业科技 |研究与探讨 2026 , 47 (13) : 125 -133

茶多酚-蛋清蛋白复合凝胶3D打印体系的构建及特性研究

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杨君慧, 刘丽莉^*, 谢天怡, 程伟伟, 张新帅, 丁玥

作者信息

河南科技大学食品与生物工程学院，食品加工与安全国家级实验教学示范中心，河南省食品加工与质量安全控制国际联合实验室，河南省农产品加工装备工程研究中心，河南洛阳 471000

通讯作者:

刘丽莉（1974−），女，博士，教授，研究方向：畜产品科学与食品生物技术，E-mail：yangliuyilang@126.com。

作者简介:

杨君慧（2001−），女，硕士研究生，研究方向：畜产品科学与食品生物技术，E-mail：947865099@qq.com

Construction and Properties of Tea Polyphenols-Egg White Protein Composite Gel in 3D Printing Systems

Junhui YANG, Lili LIU^*, Tianyi XIE, Weiwei CHENG, Xinshuai ZHANG, Yue DING

Affiliations

College of Food and Bioengineering, Henan University of Science and Technology, National Experimental Teaching Demonstration Center for Food Processing and Security, Henan International Joint Laboratory of Food Processing and Quality and Safety Control, Henan Province Agricultural Product Processing Equipment Engineering Research and Development Center, Luoyang 471000, China

出版时间: 2026-07-01 doi: 10.13386/j.issn1002-0306.2025060346

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摘要

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茶多酚（Tea Polyphenols，TP）具有清除自由基等生物活性，其与蛋清蛋白（Egg White Protein，EWP）结合形成的TP-EWP复合物能增强蛋白质的结构稳定性和凝胶特性。本文以茶多酚、蛋清蛋白、玉米淀粉、黄原胶、明胶为原料，对不同TP-EWP添加量的3D打印凝胶体系的水分分布、流变学性质、二级结构、质构特性、微观结构和3D打印行为进行评价。结果表明TP-EWP能够通过分子间相互作用（如氢键、疏水作用等）与多糖结合，从而增强了3D打印凝胶体系的网络结构，降低了水分子的流动性，使部分游离水逐渐转化为不流动水，但TP-EWP超过25%会使凝胶过度交联或网络崩塌，导致孔隙率上升与水分流动性增强。TP-EWP的添加对3D打印凝胶体系的流变学特性有改善作用，凝胶体系均表现出假塑性行为，且所有样品的储存模量（G'）随着频率的升高而增加。随着TP-EWP添加量的增加，凝胶体系的损耗模量（G''）呈现减小的趋势，提高了凝胶体系的流动性。当TP-EWP添加量从20%增至25%时，凝胶体系的α-螺旋占比从17.11%升至25.29%，但TP-EWP添加量超过25%后，α-螺旋比例下降。不同TP-EWP添加量的加入对凝胶体系的强度、硬度、咀嚼性及黏性有显著影响（P<0.05）。该研究为多酚-蛋白质复合凝胶在功能性食品3D打印墨水开发中的应用提供了理论依据。

关键词

茶多酚 / 蛋清蛋白 / 玉米淀粉 / 黄原胶 / 明胶 / 3D打印

Abstract

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Tea polyphenols (TP) have biological activities such as scavenging free radicals. The TP-EWP complex formed by the combination of TP and egg white protein (EWP) can enhance the structural stability and gel properties of the protein. TP, EWP, corn starch, xanthan gum, and gelatin were used as raw materials in this paper. The moisture distribution, rheological properties, secondary structure, textural properties, microstructure, and 3D printing behaviours of 3D printed gel system with different TP-EWP additions were evaluated. The results showed that TP-EWP was able to bind to polysaccharides through intermolecular interactions (e.g., hydrogen bonding, hydrophobic interactions), which enhanced the network structure of the 3D printed gel system. The mobility of water molecules was reduced, with the result that some free water was gradually converted into immobile water. However, when TP-EWP was added in excess of 25%, it caused excessive cross-linking or network collapse, which increased porosity and improved water mobility. The inclusion of TP-EWP was enhanced the gels' rheological characteristics. The gels all showed pseudoplastic behavior and the G' of all samples increased with increasing frequency. With the increase of TP-EWP addition, the flowability of the gels improved and the G'' of the gels tended to decrease. When the amount of TP-EWP added was increased from 20% to 25%, the proportion of α-helices in the gel rose from 17.11% to 25.29%. However, when more than 25% of TP-EWP was added, the percentage of α-helices dropped. The strength, hardness, chewability, and viscosity of the gels were significantly impacted by the addition of various TP-EWP (P<0.05). This study provides a theoretical basis for the application of polyphenol-protein composite gel in the development of 3D printing ink for functional foods.

Key words

tea polyphenols / egg white protein / corn starch / xanthan gum / gelatin / 3D printing

引用本文

杨君慧, 刘丽莉, 谢天怡, 程伟伟, 张新帅, 丁玥. 茶多酚-蛋清蛋白复合凝胶3D打印体系的构建及特性研究. 食品工业科技, 2026 , 47 (13) : 125 -133 . DOI: 10.13386/j.issn1002-0306.2025060346

Junhui YANG, Lili LIU, Tianyi XIE, Weiwei CHENG, Xinshuai ZHANG, Yue DING. Construction and Properties of Tea Polyphenols-Egg White Protein Composite Gel in 3D Printing Systems[J]. Science and Technology of Food Industry, 2026 , 47 (13) : 125 -133 . DOI: 10.13386/j.issn1002-0306.2025060346

正文

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3D食品打印是增材制造的一种新兴应用，通过基于数字模型实现可食用材料的逐层沉积，改变了可食用产品的设计和生产方式^[1−2]。随着科技的不断发展，食品3D打印技术在材料、设备和工艺等方面都取得了显著的进展。在材料方面，研究人员不断开发适合3D打印的新型食品材料^[3]。除了传统的巧克力、面团等材料，越来越多的功能性食品材料，如富含营养成分的蛋白质凝胶、多糖凝胶和植物基材料等，被应用于食品3D打印^[4]。在食品3D打印中，蛋白基凝胶的流变特性对打印过程和打印产品的质量起着关键作用。蛋清蛋白（Egg White Protein，EWP）因其蛋白质含量高，氨基酸组成均衡而被广泛认为是一种优质蛋白质资源。EWP由于其独特的蛋白质组成，具有多种功能特性，包括乳化、发泡和凝胶特性^[5]。但是蛋清蛋白凝胶易受到pH、离子强度和多糖等各种因素的影响^[6]。目前，已经有研究表明，多酚的添加不仅能使蛋白质具有多酚的功能特性还能提高蛋清蛋白的凝胶特性^[5]。

茶多酚（Tea Polyphenols，TP）是茶叶中一种独特的重要活性物质，含有儿茶素、花青素、类黄酮和酚酸，具有清除自由基、延缓机体衰老、预防心血管疾病、预防癌症等功能^[4]。当TP与食物中的蛋白质共存时，TP和蛋白质能通过共价键或非共价键结合改变蛋白质结构从而增强蛋白质的凝胶特性。Wan等^[7]利用TP和磷酸盐协同改性鸭蛋白，发现磷酸盐和TP的协同作用改善了鸭蛋白质地和凝胶特性，缓解了磷酸化对鸭蛋白凝胶特性的恶化，降低了致敏性。周绪霞等^[8]研究不同添加量的TP改性对EWP凝胶特性的影响，发现TP的添加对EWP凝胶强度和持水性提高，凝胶网络结构更加有序，凝胶表面更加平滑均匀。尽管TP已被证明能够改善EWP蛋白凝胶性能，但纯TP-EWP凝胶在打印适性、结构支撑性和长期稳定性方面仍存在局限。

本研究创新性地将TP-EWP复合物与玉米淀粉、黄原胶和明胶进行复配优化TP-EWP复合凝胶的3D打印性能。其中，玉米淀粉作为填充剂和刚性支撑骨架，糊化后可显著增强凝胶硬度和形状保持性^[9]；黄原胶是一种高效假塑性多糖，能够显著改善墨水的挤出流动性和挤出后的自支撑能力^[10]；明胶则可在低温下形成热可逆凝胶网络，有效增强凝胶体系的弹性和打印产品的精确度^[9]。通过多组分协同策略设计适用于挤出式打印的功能性凝胶墨水，有望构建出兼具良好打印精度、结构稳定性和功能特性的新型凝胶体系。通过系统研究TP-EWP添加量对复合体系水分分布、流变行为、蛋白质二级结构、质构特性及微观结构的影响，为多酚-蛋白-多糖复合体系在食品3D打印中的开发与应用提供了新的见解，并为TP-EWP在食品3D打印中的应用奠定了基础。

1　材料与方法

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1.1　材料与仪器

EWP（蛋白质含量≥90%）　食品级，河南鑫瑞生物科技有限公司；TP　食品级，河南中辰生物科技有限公司；玉米淀粉　食品级，繁峙县懿康土特产有限公司；明胶　食品级，河南高宝实业有限公司；黄原胶　食品级，新疆梅花氨基酸有限公司；溴化钾　色谱纯，天津市科密欧化学试剂有限公司。

LC-FA1004电子分析天平　上海力辰邦西仪器科技有限公司；85-2A数显恒温测速磁力搅拌器　常州荣华仪器制造有限公司；FJ200-SH数显高速分散均质机　上海标本模型厂；AMTD-4000电热恒温水浴锅　北京市永光明医疗仪器有限公司；NMI20-015V-I低场核磁共振成像分析仪　上海纽迈电子科技有限公司；DHR-2流变仪　美国TA公司；VERTEX70傅里叶变换红外光谱仪　德国Bruker公司；SMS TA.XT Epress Enhanced食品物性分析仪　英国SMS公司；TM3030Plus电子扫描显微镜　日本岛津公司；FOODBOT 3D打印机　杭州时印科技有限公司。

1.2　实验方法

1.2.1　TP-EWP复合凝胶体系的制备

按最终TP-EWP复合凝胶体系总质量100 g计，首先分别制备TP-EWP添加量为20%、25%、30%、35%、40%的TP-EWP凝胶，参考Wan等^[7]的方法并稍作修改，TP添加量为EWP添加量的0.6%（w/w），用磁力搅拌器充分搅拌10 min。将混合物在65 ℃下加热20 min，得到的凝胶在4 ℃下保存。为构建具有适宜3D打印特性的TP-EWP复合凝胶体系，在制备的TP-EWP凝胶中加入0.5%黄原胶、0.5%明胶和15%玉米淀粉得到相应TP-EWP添加量的TP-EWP复合凝胶体系。参考Liu等^[11]的方法并稍作修改制备凝胶体系，用均质机在5000 r/min下均质5 min，将混合物在90 ℃下水浴加热30 min，制得TP-EWP添加量为20%、25%、30%、35%、40%的复合凝胶体系，得到的凝胶体系在4 ℃下保存，用于后续的水分分布、流变特性、质构等测定。以不添加黄原胶、明胶和玉米淀粉的30%的TP-EWP凝胶作为对照组。

1.2.2　凝胶体系水分分布测定

凝胶的低频核磁共振测定参照Zhang等^[12]的方法并稍作修改。将装有蛋白凝胶的小瓶放入核磁共振玻璃管中，用核磁共振分析仪进行测定。在Carr-Purcell-Meiboom-Gill模式下，使用1~15 mm探头在32 ℃温度和19 MHz质子共振频率下对样品进行评估。具体参数为：回波数=1500，扫描数=32，等待时间=1500 ms。采样后，反演分析迭代次数设定为10⁵。每个样本重复测定三次。

1.2.3　凝胶体系流变特性测定

采用Kan等^[13]的方法并稍作修改，取按1.2.1方法制备的凝胶样品对凝胶体系的流变特性进行测定。

1.2.3.1　应力扫描

通过测定应变与储能模量（G'）和损耗模量（G"）的变化关系，确定样品的线性黏弹性区。将频率设为1 Hz，应变为0.1%~1000%。

1.2.3.2　频率扫描

设置扫描频率范围为0.1~100 rad/s，应变为2%，在25 ℃下测定凝胶体系的G'、G"和损耗因子（tanδ=G"/G'）随角频率的变化。

1.2.3.3　稳态流变测定

在25 ℃下测定凝胶样品表观黏度随剪切速率的变化，剪切速率参数为0.01~300 s⁻¹。用幂函数模型分析了不同剪切速率下的表观黏度数据^[14]。

$ \mathit{\eta } \mathrm{=K}\cdot \mathit{\gamma } ^{ \mathrm{n-1}} $

式中，η为凝胶的黏度（Pa·s），γ为剪切速率（s⁻¹），n为流动特性指数，K为稠度（Pa·s）。

1.2.4　凝胶体系二级结构测定

参考Jafari等^[15]的方法并稍作修改测定傅里叶变换红外光谱。将冻干材料制成细粉末，并与KBr粉末（1:100，v/v）充分混合，从而获得样品的红外光谱。以KBr空白压片作为对照，扫描样品在25 ℃波数为4000~400 cm⁻¹之间的光谱。

1.2.5　凝胶体系质构分析测定

参照Li等^[16]的方法稍作修改，使用P/0.5圆柱形探头，测试前速度2.0 mm/s，测试速度1.0 mm/s，测试后速度2.0 mm/s，压缩率40%，停留时间5 s，触发力5 g，记录复合凝胶体系的凝胶强度、硬度、咀嚼性和黏性。

1.2.6　凝胶体系扫描电镜分析

参照Man等^[17]的测定方法稍作修改。将凝胶样品切成小块冷冻干燥48 h。将冻干后的凝胶块固定在贴有导电双面胶的样品台上，并用洗耳球吹去未牢固黏附的颗粒。样品经离子溅射喷金处理后，置于扫描电镜样品室中观察样品的微观形态。

1.2.7　凝胶体系的3D打印分析

参考Tomczyńska-Mleko等^[18]的方法稍作修改。打印模型设定为直径30 mm、高15 mm的圆柱体。使用挤压式食品3D打印机打印。在25 ℃下进行，并在打印完成时使用游标卡尺测定打印形状的尺寸，然后进行计算，以确定打印精度。印刷参数为：印刷喷嘴直径1.2 mm，印刷速度15 mm/s，印刷填充密度50%。根据打印准确度数据，选出打印精确度最佳的TP-EWP凝胶体系打印爱心、金字塔、小猪、乌龟、海豹等模型，观察其能否打印复杂结构。

$ \mathrm{打印准确度}({\text{%}})=(1-|({\mathrm{L}}_{\mathrm{s}}-{\mathrm{L}}_{\mathrm{m}})/{\mathrm{L}}_{\mathrm{m}}|) \times 100$

式中，L_s为打印样本的实际边长，mm；L_m为打印模型设定的边长，mm。

1.3　数据处理

所有指标每次测定进行三次，结果以平均值±标准差（SD）表示。采用SPSS 19.0进行单因素方差分析以及Origin 2022进行其他分析和制图，P<0.05表示差异显著。

2　结果与分析

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2.1　凝胶水分分布分析

T₂弛豫时间与水分子的运动密切相关，通过LF-NMR分析了不同TP-EWP添加量凝胶体系的水分分布，得到了凝胶体系中水分子不同组分的水分分布特征、结构特征和流动性等信息。水分分布对3D打印产品的支撑性能和挤出过程的平稳性起着重要作用^[19]。由图1可知，在凝胶体系的LF-NMR曲线中有两个峰，集中在约0.1~10 ms（T₂₁）和10~100 ms（T₂₂）。T₂₁通常与固定化水有关，固定化水包括分布在水分子单层之外的、与离子基团或离子连接的水^[20]。T₂₂表示自由流动的水，与凝胶体系的分子结构无关，这部分水与材料结合的能力较弱，更容易迁移和被去除^[21]。T₂的变化依赖于质子的环境。该值越低，样品与水的结合能力越强^[22]。由图1A和图1B可知，对照组凝胶有最大的T₂反演谱总积分面积，说明自由流动水含量最高。当TP-EWP添加量从20%增至25%时，T₂总信号强度呈现下降趋势，且弛豫时间T₂₁与T₂₂均向左移动，这表明凝胶体系中的结合水含量增加，自由水含量减少，从而提升了水分束缚能力。可能是TP-EWP浓度的升高促进了TP-EWP与多糖之间的分子间相互作用（如氢键等），从而增强了凝胶网络的结构，降低了水分子的流动性，使部分游离水逐渐转化为不流动水。同时，TP-EWP和多糖与游离水分子形成氢键，增强了整体TP-EWP和多糖与水分子之间的相互作用^[20]。Xie等^[23]在大豆分离蛋白（SPI）-螯合可溶性果胶（CSP）复合凝胶的研究中发现SPI-CSP网络结构能够捕获更多结合水，与本文有相似的实验结果。TP-EWP添加量从25%增至40%时，结合水含量减少，自由水含量增加。说明过量TP-EWP引发过度交联或网络崩塌，导致孔隙率上升与水分流动性增强^[24]。因此，TP-EWP添加量为25%时结合水含量最高且自由水最少，凝胶网络稳定性最优。

2.2　凝胶流变特性分析

凝胶体系的流变特性决定了其是否适用于3D打印油墨。为了确定TP-EWP对复合凝胶体系的这些流变性质的影响，通过应变扫描、表观黏度、频率扫描对打印凝胶体系的流变性质进行表征^[25]。

存储模量（G'）与材料的弹性和固体行为有关。损耗模量（G''）与材料的黏性或液体行为有关。由图2A可知，在应变扫描中，对照组的G'和G''远低于其他凝胶体系，表明单一蛋白凝胶网络结构较弱，对外界应变的抵抗能力较差。当应变较小时，G'和G''不随剪切应力的变化而变化的应变范围，称为线性黏弹性区域（LVR）^[26]。通过应变扫描确定了凝胶体系的LVR，LVR范围结束G'和G''开始变化的临界应变为γ_c。如图2A所示，当TP-EWP添加量为20%、25%、30%、35%和40%时，γ_c分别为18.71%、30.41%、18.71%、15.57%和11.54%。如图所示，所有样品的G'在低应变范围内均高于G''，表明体系以弹性行为为主导，具有典型凝胶特征，有益于打印凝胶通过喷嘴挤出并提高3D打印的精确度^[25]。随着应变增大，G'逐渐下降并最终与G''相交，该交点对应的应力即为屈服应力^[21]，当凝胶应变超过屈服应力，G''超过G'，凝胶网络开始破裂，进一步增加的应变通过破坏分子间氢键和降低链缠结程度来破坏凝胶网络，导致样品流动^[27]。TP-EWP-25%样品表现出最宽的LVR和最高的临界应变，说明其凝胶网络结构最为稳定，可承受更大变形而不被破坏，这主要归因于茶多酚与蛋清蛋白通过疏水相互作用和氢键交联形成的致密且均匀的三维网络。过高TP-EWP添加量（>25%）则因分子间空间位阻增大和静电排斥作用导致网络均匀性下降、结构稳定性减弱。Xian等^[28]将蛋白质添加至玉米淀粉中，复合凝胶的自支撑力增加，与本文的研究结果相似。

动态频率试验凝胶体系的G'和G''有助于评估其在挤出过程中的流动特性^[15]。图2B和图2C显示出了在恒定应变下G'和G''随频率的变化。对照组的G'和G''值均为最低，且随频率升高增长缓慢，表明其网络结构较弱，对外部频率变化的响应不敏感，弹性储能能力较差。随着角频率增加，所有实验组G'呈缓慢上升趋势，说明凝胶网络具备良好的结构稳定性和抗变形能力^[29]。同时，TP-EWP复合凝胶的G'始终高于G''，证实了TP-EWP和多糖的相互作用显著增强了体系的固体弹性行为。在TP-EWP添加量在20%~40%范围内，凝胶体系G'和G''随着添加量的增加逐渐降低，说明TP-EWP的添加量对凝胶体系的流变特性有显著影响。可能是TP-EWP颗粒填充了多糖网络，降低了分子间的摩擦^[30]。本文与崔亚雪等^[31]对卡拉胶-变性淀粉-蛋清蛋白凝胶的流变特性研究结果相似，相较于单一多糖凝胶，蛋清蛋白-多糖复配系统提高了复合凝胶的黏弹特性和流变性能。研究发现，在一定范围内G'较高时，3D打印油墨的形状保持能力越好。但当G'过大时，3D打印油墨可挤出性差，容易使线条断裂，与预期结构的偏差较大^[32]。因此，适当的G'和G''确保了3D打印产品的结构稳定性和挤出连续性^[33]。最优添加量的确定不能仅依据G'和G''的单调变化，而应结合其在3D打印过程中的实际性能进行综合判断。

动态损耗角正切（tanδ=G''/G'）通常用于评价食品材料的不同黏弹性行为，当tanδ大于1表示较好的流体性质，而tanδ小于1表示较好的固体性质^[33]。由图2D可知，在0.1~100 rad/s的范围内，所有样品的tanδ均小于1，进一步表明凝胶体系主要表现出弹性、固体特性。在TP-EWP添加量在20%~40%范围内，随着TP-EWP添加量的增加，凝胶体系tanδ值先减小后增大。当TP-EWP添加量为25%时，凝胶体系tanδ值最小。说明TP-EWP添加量为25%的凝胶体系网络结构更致密，固体特性更好。图2E显示了含有不同TP-EWP添加量凝胶体系的复数黏度随频率的变化。复数黏度是3D打印中材料流动性的关键指标。所有样品的复数黏度均随着角频率的增加而逐渐降低，表明存在典型的剪切变稀行为，有助于凝胶体系进行3D打印^[34]。添加40%TP-EWP的凝胶体系复数黏度较低，这表明该组的凝胶体系3D打印的机械强度较弱，形状保持性降低。

表观黏度是指在特定剪切条件下的黏度，适当的黏度有利于凝胶体系通过打印喷嘴^[35]。图2F是剪切速率在0.01~300 s⁻¹范围内时，不同TP-EWP添加量对凝胶体系的表观黏度的影响。所有样品都随着剪切速率的增加而逐渐降低。这表明凝胶体系具有剪切稀化特性。这可能是由于在低剪切速率下，凝胶体系内部的分子间作用力发生了破坏，导致分子链的定向和伸展。在高剪切速率下，分子链的缠结完全瓦解，导致表观黏度下降速率的降低^[36]。随着TP-EWP添加量的增加，凝胶体系的初始表观黏度逐渐减小。这表明TP-EWP改变了凝胶体系的网络结构，从而降低体系内多糖与多糖之间的相互作用，导致凝胶体系强度降低，同时提高了凝胶体系的流动性。寇锟等^[37]发现3D打印结构的形状稳定性与打印油墨的黏度之间存在一定的相关性。用幂函数模型对稳态流变进行拟合分析，如表1所示，所有凝胶样品的相关系数R²在0.93995~0.99951之间，该模型适用于所有样品。所有凝胶样品的n值都小于1，证实了它们的非牛顿流体特性。此外，TP-EWP复合凝胶体系的K值均高于对照组。通常，较高的K值表示可能形成了更为致密或交联程度更高的网络结构^[14]。

2.3　FT-IR分析

FT-IR被广泛用于研究凝胶的有机官能团，不同的吸收峰对应于特定的官能团。图3A显示了不同TP-EWP添加量的3D打印凝胶体系在400~4000 cm⁻¹波段的红外吸收光谱。所有样品表现出相似的吸收峰，其中在波数2930 cm⁻¹处的特征谱带表示多糖分子的-CH伸缩，在1540 cm⁻¹和1650 cm⁻¹处的吸收峰是蛋白质酰胺Ⅰ带的C-O伸缩振动和N-H弯曲振动^[38]。通常，3000~3700 cm⁻¹主要与-OH伸缩振动有关，并且代表分子间氢键^[39]。与对照组相比，所有TP-EWP复合凝胶体系在2930 cm⁻¹和3000~3700 cm⁻¹处的吸收峰发生蓝移，这可能是由于TP-EWP与多糖之间的相互作用增强以及凝胶网络结构的变化。酰胺Ⅰ带（1590~1710 cm⁻¹）和酰胺Ⅱ带（1490~1590 cm⁻¹）相关的吸收峰向更低的波数移动，表明凝胶网络更加有序。此外，当TP-EWP添加量为25%时，与分子内氢键相关的1000 cm⁻¹附近的吸收峰强度最大。这可能是因为当TP-EWP添加量为25%，多糖与TP-EWP之间的协同作用达到最佳状态，使得分子内的氢键作用更加显著，进一步提高了吸收峰的强度^[40]。这与Xie等^[23]的研究结果相似。

对1600~1700 cm⁻¹范围内的FT-IR光谱进行去卷积和峰拟合，以获得蛋白质形成的二级结构，不同TP-EWP添加量的3D打印凝胶体系的二级结构相对含量如图3B所示。一般而言，β-折叠和α-螺旋结构被认为是凝胶体系中有序且稳定的二级结构，而β-转角和无规卷曲被认为是无序结构。当TP-EWP添加量为25%时，凝胶体系的β-折叠和α-螺旋相对含量分别是32.08%和25.29%。TP-EWP添加量超过25%后，α-螺旋比例下降，表明TP-EWP与多糖作用稳定了凝胶体系构象，促进有序螺旋结构的形成，但过量的TP-EWP与多糖竞争结合位点或引发局部脱水，导致螺旋结构部分解旋^[41]。这种变化趋势可能与TP-EWP与多糖之间的相互作用有关。TP-EWP添加量从20%增至25%，凝胶体系中TP-EWP与多糖之间的相互作用增强，促进了凝胶体系间的有序排列，使得β-折叠和α-螺旋结构增加。过量的TP-EWP可能引发凝胶体系结构重排与无序化，从而导致凝胶体系结构的破坏，影响凝胶的性能^[42]。

2.4　质构分析

凝胶体系质构分析是评价凝胶在广泛食品应用中适用性的关键指标之一^[43]。咀嚼性是将凝胶体系咀嚼至可吞咽状态所需能量的量度^[44]。黏性反映凝胶在剪切力下的流动阻力，与分子链的延展性及水合状态密切相关。适宜的黏性可提升产品的顺滑口感或成型能力^[45]。若黏性过高，可能导致加工困难或口感黏腻。图4显示了不同凝胶体系的质构特性变化。与对照组相比，所有TP-EWP复合凝胶体系的添加可显著改善复合凝胶的各项质构参数。不同TP-EWP添加量的加入对凝胶体系的强度、硬度、咀嚼性及黏性有显著影响（P<0.05）。由图4所示，不同TP-EWP添加量对凝胶体系性能的影响呈现先增强后减弱的趋势。当TP-EWP添加量25%时，凝胶体系强度、硬度、咀嚼性及黏性达到最大值。说明此时凝胶形成致密且稳定的三维网络结构，机械性能最优。可能是由于TP-EWP与多糖之间的氢键、疏水相互作用增强，形成了更为紧密和稳定的凝胶网络结构，使得凝胶体系的质地性能得到改善^[46]。然而，当TP-EWP添加量继续增加到40%时，凝胶体系的强度、硬度、咀嚼性和弹性均显著下降（P<0.05）。可能是过量的TP-EWP引入凝胶体系可能会导致凝胶体系内分子间空间位阻增加，抑制有效交联，过量带电荷基团引发静电排斥，破坏凝胶网络稳定性^[39]，TP-EWP与多糖竞争结合水分子，导致凝胶持水性下降，结构松散，以至于TP-EWP添加量超过25%时削弱了凝胶体系的机械强度。Liu等^[47]研究了玉米淀粉对银耳多糖-蛋清蛋白凝胶的影响，结果表明复合凝胶的硬度、弹性、粘聚性和胶粘性均高于纯蛋白凝胶，与本文结论一致。

2.5　微观结构分析

扫描电镜能直观地观察到凝胶体系的微观结构。随着TP-EWP添加量的增加，凝胶体系的微观结构发生显著变化。从图5中可以看出，单一TP-EWP凝胶表现出多孔结构和相对较大的直径，具有较大的孔洞且分布不均匀，拥有更大空腔的网络结构，而添加多糖的TP-EWP复合凝胶孔洞较小。当TP-EWP添加量从20%（图5B）增加到25%（图5C）时，凝胶的微观结构变得更加致密和均匀，孔隙结构有所减少。当添加量进一步增加到30%（图5D）时，凝胶的微观结构保持致密，但局部出现不均匀结构。当添加量增加到35%（图5E）和40%（图5F）时，凝胶的微观结构变得相对疏松，孔隙结构再次增多，表明凝胶网络结构的稳定性有所下降。这种微观结构的变化可能与TP-EWP与多糖之间的相互作用有关^[22]。当TP-EWP添加量为25%时，TP-EWP之间的氢键和疏水相互作用增强，促进了凝胶体系中的TP-EWP与多糖之间的均匀交联，使凝胶体系形成了致密且稳定的凝胶网络。这种网络结构限制了分子链的运动，使得微观结构更加均匀和致密^[41]。然而，当TP-EWP添加量过多时，可能会导致蛋白质过度聚集或网络结构的局部破坏，从而使得微观结构出现不均匀性，并且随着添加量的进一步增加，凝胶网络的稳定性下降，孔隙结构增多^[30]。崔亚雪等^[31]研究了卡拉胶-变性淀粉-蛋清蛋白凝胶，发现多糖-蛋白三元复合凝胶具有稳定互连、良好的网络结构，能增强复合体系的有序稳定性，与本文研究结果一致。

2.6　3D打印分析

单一的TP-EWP凝胶无法进行3D打印，不同TP-EWP添加量的凝胶体系打印如图6所示。随着TP-EWP添加量的增加，凝胶体系的打印准确度和打印效果呈现出明显的先增加后降低的变化趋势。从图6A可以看出，当TP-EWP添加量从20%增加到25%，3D打印准确性略有升高。TP-EWP添加量超过25%时，凝胶体系打印油墨的打印准确性显著降低（P<0.05）。总体而言，TP-EWP添加量为25%时，凝胶体系打印油墨的打印效果最佳，打印准确性为99.67%，而TP-EWP添加量为40%时的打印准确性降至71.87%。

图6B展示了不同添加量下的打印效果，打印效果与打印准确性的变化相一致。当TP-EWP添加量为25%时，打印产品的边缘较为整齐，内部结构均匀，表明凝胶的微观结构较为致密和均匀。但随着TP-EWP添加量从25%增加到40%，打印模型的边缘变得不规则，内部出现更多的孔隙和不均匀结构，产品形状甚至坍塌，表明凝胶的微观结构变得疏松。此外，图6C展示了TP-EWP添加量为25%时的不同图案打印效果图，进一步证明了在这一添加量下，凝胶体系具有良好的打印性能和较高的准确性。不同形状的模型（爱心、金字塔、小猪、乌龟、海豹）均能清晰地打印出来，表明在25%添加量时，凝胶的微观结构和物理性能达到了最佳状态，能够支持复杂结构的精确打印。

3　结论

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本研究探讨了茶多酚-蛋清蛋白复合物（TP-EWP）添加量对复合凝胶体系特性及3D打印性能的影响，TP-EWP添加量对TP-EWP复合凝胶体系的流变学特性、质构特性、二级结构、微观结构以及3D打印均有影响，在TP-EWP添加量为25%时凝胶综合性能最优，其α-螺旋占比达25.29%，微观结构致密均匀，质构特性（硬度、咀嚼性、黏性）显著增强，打印精度高达99.67%，能实现复杂结构的稳定打印。TP-EWP通过氢键和疏水作用与多糖网络协同交联，增强了凝胶持水性和机械强度，但过量添加（>25%）会导致网络崩塌、水分流动性增加和打印质量下降。与以往研究相比，本研究创新性地构建了TP-EWP-玉米淀粉-黄原胶-明胶多元复合体系，更真实地模拟食品配方的复杂性，明确了该体系在3D打印功能性食品墨水中的应用潜力。

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2026年第47卷第13期

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doi: 10.13386/j.issn1002-0306.2025060346

接收时间：2025-06-29
首发时间：2026-10-24
出版时间：2026-07-01

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收稿日期：2025-06-29

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刘丽莉（1974−），女，博士，教授，研究方向：畜产品科学与食品生物技术，E-mail：yangliuyilang@126.com。

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2种不同金属材料的力学参数

科 Family	属数 Number of genus	种数 Number of species	占总种数比例 Percentage of total species (%)	属 Genus	种数 Number of species	占总种数比例 Percentage of total species (%)
鹅膏菌科Amanitaceae	2	11	5.26	鹅膏菌属 Amanita	10	4.78
小菇科 Mycenaceae	2	12	5.74	丝盖伞属 Inocybe	5	2.39
多孔菌科 Polyporaceae	8	14	6.70	蜡蘑属 Laccaria	5	2.39
红菇科 Russulaceae	3	23	11.00	小皮伞属 Marasmius	6	2.87
				小菇属 Mycena	11	5.26
				光柄菇属 Pluteus	5	2.39
				红菇属 Russula	17	8.13
				栓菌属 Trametes	5	2.39

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