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摘要: 氧化石墨烯（GO）作为二维纳米材料石墨烯的衍生物，具有制备简单、成本低、官能团丰富、易于改性等特点。在GO二维纳米片层上引入褶皱，可改变其形貌和结构，带来特殊的物理、化学、生物等特性，在一些领域具有独特的应用优势。本文综述了国内外近年来在褶皱氧化石墨烯（WGO）的制备与应用方面的研究进展，重点讨论了预拉伸法、溶剂诱导法、快速干燥法和pH值调控法等制备WGO的原理和特点，同时总结了WGO在智能器件、生物医药和水处理方面的应用。还分析了当前在WGO制备和应用方面存在的问题，并展望了其未来发展趋势。Abstract: Graphene oxide (GO), as a derivative of two-dimensional graphene, has the characteristics of simple preparation, low cost, abundant functional groups and easy modification. The introduction of wrinkles in the two-dimensional GO nanosheets changes the morphology and structure, and thus can give GO special physical, chemical, biological and other characteristics, making it possible for use in many fields. Research progress on the preparation and applications of wrinkled GO (WGO) in recent years is reviewed, focusing on the preparation principles and characteristics of WGO, including pre-stretching, the solvent induction method, rapid drying, magnetic field induction, surfactant templating, electrophoretic deposition and pH adjustment methods. The applications of WGO in smart devices, biomedicine and water treatment are summarized. Current challenges in the preparation and use of WGO are discussed, and future development prospects are given.
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图 2 单轴预拉伸法制备WGO膜的制备过程和微观形貌：(a)制备流程示意图；(b)光学显微镜照片；(c) AFM照片；(d) SEM照片和(e)高倾斜的SEM横截面照片[42]
Figure 2. Preparation process and morphology characterization of WGO films prepared by uniaxial pre-stretching: (a) Schematic diagram of preparation process; (b) Optical microscope image; (c) AFM image; (d) SEM image; (e) High-tilt SEM cross section image[42]. Reprinted with permission.
图 3 溶剂诱导法制备的WGO膜的过程示意图和SEM微观形貌：(a)制备过程示意图；(b~d) GO的SEM照片；(e~g)WGO的SEM照片[48]
Figure 3. Preparation process and morphology characterization of WGO films prepared by solvent induction: (a) Schematic diagram of preparation process; (b-d) SEM images of GO; (e-f) SEM images of WGO[48]. Reprinted with permission.
图 4 溶剂诱导法制备的WGO膜的过程示意图和SEM微观形貌：(a)制备过程示意图；(b)GOMs-H的SEM照片；(c)GOMs的SEM照片；(d)GOMs-E的SEM照片[50]
Figure 4. Preparation process and morphology characterization of WGO films prepared by solvent induction method: (a) Schematic diagram of preparation process; (b) SEM image of GOMs-H; (c) SEM image of GOMs; (d) SEM image of GOMs-E[50]. Reprinted with permission.
图 5 快速干燥法制备WGO的制备过程和微观形貌：(a)实验装置示意图；(b)褶皱GO的形成机制；(c~f)不同快速干燥温度制备的GO颗粒的形貌的FESEM照片和(g~j) TEM照片：(c, g) 200 ℃；(d, h) 400 ℃；(e, i) 800 ℃；(f, j) 1000 ℃[54]
Figure 5. Preparation process and morphology characterization of WGO prepared by the rapid drying method: (a) Schematic diagram of experimental setup; (b) The possible formation mechanism of crumpled GO; Morphology of GO particles prepared at different rapid drying temperatures: (c-f) FESEM images and (g-j) corresponding TEM images. (c, g) 200 ℃; (d, h) 400 ℃; (e, i) 800 ℃; (f, j) 1000 ℃[54]. Reprinted with permission.
图 7 pH调控法制备的WGO：(a)GO的电离[59]；(b)不同pH条件下，单层GO水悬浮液的Zeta电位和悬浮液状态[58]；单层GO: (c, f) FQM; (d, g) SEM; (e, h) AFM[59]. 在受压条件下，(c~e)酸性条件下趋于起皱；(f~h)碱性条件下趋于重叠
Figure 7. Preparation of WGO by pH control method: (a) The ionization of GO; (b) Zeta potential and Suspension state of SLGO over pH range[58] ; Single-layer GO: (c, f) FQM; (d, g) SEM; (e, h) AFM[59] . Upon compression, GO sheets tend to (c-e) wrinkle on acidic subphase; and (f-h) overlap on basic subphase. Reprinted with permission.
图 8 GO膜的褶皱对正常透光率的影响：(a)未拉伸、单轴和双轴拉伸条件下的光学透射率；(b)不同双轴拉伸应变下的光学透射率[45]
Figure 8. Effect of wrinkling of GO films on normal light transmittance: (a) The optical transmittance under the conditions of no stretching, uniaxial and biaxial stretching; (b) The optical transmittance under different biaxial stretching strains[45]. Reprinted with permission.
图 9 AFM照片和相应交联的GO-ac膜的均方根粗糙度：(a) 1 mg mL−1；(b) 2 mg mL−1；(c) 4 mg mL−1；(d) 1 mg mL−1, 2 mg mL−1，4 mg mL−1 GO-ac的紫外吸光度[80]
Figure 9. AFM images and the corresponding RMS roughness of cross-linked GO-ac membrane formed at the concentration of: (a) 1 mg mL−1; (b) 2 mg mL−1; (c) 4 mg mL−1; (d) UV absorbance quantification of 1 mg mL−1, 2 mg mL−1, 4 mg mL−1 GO-ac[80]. Reprinted with permission.
表 1 WGO的制备方法与褶皱特征
Table 1. Preparation methods and wrinkle characteristics of WGO.
Methodss Substrates Wrinkle shape Characteristics References Pre-stretching Silicone rubber Film 1-25 μm in amplitude, 2-24 μm in height [42] Solvent induction Glass or PTFE Film Hierarchical wrinkles [48] Rapid drying Silicon Particle or film Particle diameter < 100 nm [55] PH adjustment Glass or silicon Film 3-10 nm in thickness [59] Magnetic field induction - Fiber Fiber diameter≈96.1 mm [60] Surfactant template method ODA Film Single layer [61] Electrophoretic deposition Titanium Film 31.4-84.5 nm in height [62] 
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