Self-assembly Process Research Articles

Dimerization and liquid-liquid phase separation of the nonrepetitive domains of pyriform spidroin 1 controls the pyriform silk formation

Spiders spin high performance silks with diverse mechanical properties for specific biological functions. Of these spider silk types, pyriform silk stands out as a unique combination of wet glue and dry fibers. Investigation of self-assembly process of spider silk proteins is necessary for elucidating the silk formation mechanism. However, the functions of nonrepetitive domains in the silk formation of pyriform spidroins from liquid proteins to solid fibers are still unclear, making it difficult to achieve efficient biomimetic preparations of pyriform silk with good mechanical properties. In this study, we investigate the roles of the N-linker repeat (NLR) and both terminal domains of pyriform spidroin 1 (PySp1) in the silk formation. We demonstrate for the first time that the PySp1 NLR alone is sufficient to self-assemble into high strength fibers. Moreover, we showed that the ability to promote the pyriform silk formation by the addition of the NLR. We also found that the pH-sensitive dimerization property for N-terminal domain and the liquid-liquid phase separation (LLPS) coupled with acidification triggers the self-assembly mediated by the C-terminal domain. Overall, our results provide new insight into the role of nonrepetitive domains in the pyriform silk formation mechanism and the basis for producing new protein-based materials derived from spider pyriform silk.

A molecular synergy of non-covalent interactions facilitated via theobromine modifying the self-assembly process of type I collagen

Type I Collagen is a multifunctional fibrous protein present significantly in the connective tissues. Generally, fibril formation process of an interstitial collagen begins with a triple helix alignment to form a pentafibril, which sequentially self-assembles into a microfibril. Typically, this sequential formation can be achieved under an in vitro condition as well by maintaining certain specific physiological parameters to mimic the interstitial microenvironment of collagen. The necessity to study such a kinetically driven process is due to its implications in template fabrication particularly as a scaffold to enhance the growth of specific stem cells or accelerating nanoparticle synthesis. Drawing inspiration from this, theobromine, a methylxanthine that contributes towards the hydrogen bond network via dimerization and stacking interaction was used as a small molecule in modifying the molecular level interactions of a self-assembled collagen. Initially, rheological studies revealed certain variations in the viscous properties of collagen on addition of theobromine. Turbidity assay showed an increase in the rate of fibril formation and its topographical changes were observed through the high-resolution scanning electron microscope. The stability and probable physico-chemical interactions between collagen and theobromine were comprehended from the vibrational frequency changes recorded using (FT-IR) (ATR) and conformational changes using Circular Dichroism (CD) studies. Our results show possible multibinding sites on theobromine, which would compete to bind with the polar and non-polar residues exposed over the monomeric surfaces of triple helix causing a local conformational fluctuation modifying protein-protein interaction.

3D porous PEDOT/MXene scaffold toward high-performance supercapacitors

3D architectures of conductive polymer, especially PEDOT hold great promise in energy storage and conversion fields. However, the facile construction of 3D PEDOT and its functionalization have still been challenges due to its poor processability. Herein, the fabrication of 3D porous PEDOT:PSS and its functionalization with MXene are realized synchronously through a simple and low-cost self-assembly process. The prominent capacitive performance of MXene, excellent chemical stability of PEDOT:PSS and 3D porous architecture with inhibited aggregation of MXene nanosheets, large amount of active sites, and electrolyte storage chamber endow the PEDOT/MXene-based porous structure with superior capacitive performance than individual PEDOT:PSS or MXene porous and flat structures. Furthermore, the PEDOT/MXene-based porous structure can be applied as a flexible scaffold for the deposition of conductive polymer to construct excellent electrodes for supercapacitors (SCs). When polypyrrole (PPy) is deposited, the prepared porous PEDOT:PSS/MXene/PPy electrode exhibits a high gravimetric specific capacitance of 345 F g−1 at a current density of 0.5 A g−1 and a remarkable capacitance retention of 89 % over 5000 cycles. Based on it, an asymmetric supercapacitor (ASC) with a high energy density of 56.34 Wh kg−1 at the power density of 120 W kg−1, and a capacitance retention of 75 % after 5000 cycles is developed. Besides, the porous PEDOT:PSS/MXene/PPy can be constructed on various substrates in any pattern with high design freedom, thus enabling customizable electrochemical performance. When constructing on a flexible substrate, excellent deformation-tolerant performance is shown. This work provides a high-performance electrode for SCs, as well as a universal route for the construction and functionalization of 3D PEDOT-based structures.

Robust self-assembly of nonconvex shapes in two dimensions.

We present fast simulation methods for the self-assembly of complex shapes in two dimensions. The shapes are modeled via a general boundary curve and interact via a standard volume term promoting overlap and an interpenetration penalty. To efficiently realize the Gibbs measure on the space of possible configurations we employ the hybrid Monte Carlo algorithm together with a careful use of signed distance functions for energy evaluation. Motivated by the self-assembly of identical coat proteins of the tobacco mosaic virus which assemble into a helical shell, we design a nonconvex two-dimensional model shape and demonstrate its robust self-assembly into a unique final state. Our numerical experiments reveal certain essential prerequisites for this self-assembly process: blocking and matching (i.e., local repulsion and attraction) of different parts of the boundary, and nonconvexity and handedness of the shape.

Adoption of a Tetrahedral DNA Nanostructure as a Multifunctional Biomaterial for Drug Delivery.

DNA nanostructures have been widely researched in recent years as emerging biomedical materials for drug delivery, biosensing, and cancer therapy, in addition to their hereditary function. Multiple precisely designed single-strand DNAs can be fabricated into complex, three-dimensional DNA nanostructures through a simple self-assembly process. Among all of the synthetic DNA nanostructures, tetrahedral DNA nanostructures (TDNs) stand out as the most promising biomedical nanomaterial. TDNs possess the merits of structural stability, cell membrane permeability, and natural biocompatibility due to their compact structures and DNA origin. In addition to their inherent advantages, TDNs were shown to have great potential in delivering therapeutic agents through multiple functional modifications. As a multifunctional material, TDNs have enabled innovative pharmaceutical applications, including antimicrobial therapy, anticancer treatment, immune modulation, and cartilage regeneration. Given the rapid development of TDNs in the biomedical field, it is critical to understand how to successfully produce and fine-tune the properties of TDNs for specific therapeutic needs and clinical translation. This article provides insights into the synthesis and functionalization of TDNs and summarizes the approaches for TDN-based therapeutics delivery as well as their broad applications in the field of pharmaceutics and nanomedicine, challenges, and future directions.

Encapsulation and controlled delivery of curcumin by self-assembled cyclodextrin succinate/chitosan nanoparticles

Low aqueous dispersibility and poor stability severely restrict the bioaccessibility of curcumin in health-related products. Constructing highly effective delivery carriers is essential to overcome the limitation. In this study, a novel and simple self-assembly process driven by electrostatic interaction was developed to prepare cyclodextrin succinate/chitosan (SACD/CS) nanoparticles. Spherical SACD/CS nanoparticles were obtained by adjusting the ratio of SACD:CS to obtain an average size and ζ-potential of around 500 nm and 20 mV, respectively. By analyzing the intermolecular interactions and crystalline structure of SACD/CS nanoparticles, it is indicated that SACD could act as crosslinking nodes, and contributed to transformation of molecular arrangement in the nanoparticles. The noncytotoxic SACD/CS nanoparticles were further used as curcumin carriers and showed significant improvement on curcumin stability, with the retention index of curcumin under physiological conditions increased from 19% to 62%. Moreover, the Cur-SACD/CS nanoparticles displayed controlled release behavior of curcumin during in vitro digestion, with 9%, 22%, and 44% of curcumin released at the end of the oral, stomach, and small intestine stage, respectively. This study developed a novel and effective strategy for oral delivery of curcumin, showing promising potential for improving the bioaccessibility and bioavailability of bioactive compounds like curcumin.

Spherulite formation in green nonaqueous media: The impact of urea on gelation in glycerol

HypothesisLarge macroscopic assemblies formed by a surfactant, sodium dodecylsulfate (SDS), and glycerol, can be directed to assemble in a hierarchical manner by the addition of a strong hydrogen-bond donor/acceptor, such as urea. ContextSelf-assembly in complex media is important to a range of applications, for instance in biological media, which are multi-component, to industrial formulations, where additives are present for flavour, texture, and preservation. Here, the gelation and self-assembly of sodium dodecylsulfate (SDS) in glycerol is explored in the presence of an additive, urea. Urea was chosen due to its importance both fundamentally and industrially, but also because of its ability to form strong H-bonds and interact with both glycerol and SDS. ExperimentalTo cover the variety of length scales present in the gel-like phase, a combination of optical microscopy and small-angle X-ray scattering techniques were used to probe the micro- to nanoscale. FindingsOn the microscale, the formation of a spectacular spherulite phase, even at low urea contents - 0.1 wt%, upon cooling was observed, a stark difference to the microfibrillar phase observed in the absence of urea. Interestingly, the nanostructure of the two crystalline phases were similar and showed negligible differences. This suggests that urea is not involved in the SDS/glycerol microfibril formation but instead directs the assembly of spherulites by bundling the microfibrils. These ternary systems are also probed as a function of urea content, SDS concentration, and temperature. The observations in this work highlight the importance of small molecules in the self-assembly process, which is relevant both fundamentally but also industrially, where small molecules are often added to formulations.

Poly(Photosensitizer-Prodrug) Unimolecular Micelles for Chemo-Photodynamic Synergistic Therapy of Antitumor and Antibacteria.

It is crucial to use simple methods to prepare stable polymeric micelles with multiple functions for cancer treatment. Herein, via a "bottom-up" strategy, we reported the fabrication of β-CD-(PEOSMA-PCPTMA-PPEGMA)21 (βPECP) unimolecular micelles that could simultaneously treat tumors and bacteria with chemotherapy and photodynamic therapy (PDT). The unimolecular micelles consisted of a 21-arm β-cyclodextrin (β-CD) core as a macromolecular initiator, photosensitizer eosin Y (EOS-Y) monomer EOSMA, anticancer drug camptothecin (CPT) monomer, and a hydrophilic shell PEGMA. Camptothecin monomer (CPTMA) could achieve controlled release of the CPT due to the presence of responsively broken disulfide bonds. PEGMA enhanced the biocompatibility of micelles as a hydrophilic shell. Two βPECP with different lengths were synthesized by modulating reaction conditions and the proportion of monomers, which both were self-assembled to unimolecular micelles in water. βPECP unimolecular micelles with higher EOS-Y/CPT content exhibited more excellent 1O2 production, in vitro drug release efficiency, higher cytotoxicity, and superior antibacterial activity. Also, we carried out simulations of the self-assembly and CPT release process of micelles, which agreed with the experiments. This nanosystem, which combines antimicrobial and antitumor functions, provides new ideas for bacteria-mediated tumor clinical chemoresistance.

Incorporation strategy for organic dyes into gold nanoparticle supercrystals.

Ordered arrays of plasmonic nanoparticles, supercrystals can lead to the formation of plasmon-polaritons. Coupling light emitters with plasmon polaritons might allow the formation of exciton-plasmon polaritons with properties tuneable by the supercrystal design. To construct such optically active materials, the inclusion of emitters is imperative. The addition of organic dyes without affecting the periodic order of the nanocrystals is difficult, as post-formation protocols might dissolve the supercrystals, and pre-formation addition might affect the self-assembly process. Here, we present an exemplary strategy to functionalize gold nanoparticles prior to self-assembly with a cyanine isothiocyanate dye that was obtained by a straightforward reaction of the amine functionalized dye with carbon disulfide. In the second step, the nanoparticles are functionalized with a thiol-terminated polystyrene, which stabilizes the nanoparticles and governs the self-assembly process. The dye can be integrated in a quantitative fashion, and the nanoparticles can be self-assembled into supercrystals. The strategy should be applicable in general for amine functionalized dyes, which is a common modification.

Assembly of polysaccharide-based polymer brush for supramolecular hydrogel dressing

Extracted from Platycodon grandiflorum, platycodon grandiflorum polysaccharides (PGPs) with diverse biological functions have been extensively employed for modification and fabrication of hydrogels for biomedical applications, such as wound dressings. However, since the lack of effective structural design, the reported polysaccharide-based hydrogel dressings are still suffered from structural failures and limited bio-functionality. Herein, we demonstrate a facile and general strategy to fabricate a supramolecular hydrogel composed of PGP-based polymer brush as building blocks combined with a Ca2+-mediated self-assembly process. The specific polymer brush with high branch functionality was achieved with polyacrylamide arms evenly grown on the PGP (grafting efficiency as high as 80 %) with series of chemical modifications. With above structural merits, the resulting hydrogel with densely crosslinked polymer brush featured enhanced mechanical strength as well as self-healing, and shear-thinning behaviors. Further biocompatible investigation indicated the as-prepared hydrogels with admirable performances in self-adhesion (adhesive strength of 16.7–79.5 kPa), a pH-responsive swelling ratio as high as 44 at pH 5.4, and pH-responsive degradation. They also showed antioxidant capacity by scavenging DPPH activity of nearly 80 % in 20 min, hemocompatibility, cell viability and cell migration. Impressively, the PGP-based polymer brush hydrogel served as a wound dressing revealed significant acceleration on wound closure.

Directed Self-Assembly by Sparsely Prepatterned Substrates with Self-Responsive Polymer Brushes.

The guiding pattern in the chemoepitaxially directed self-assembly (DSA) of block copolymers is often fabricated by periodically functionalizing homogeneously random copolymer brushes tethered on a substrate. The prepatterned copolymer brushes constitute a soft penetrable surface, and their two components can in principle locally segregate in response to the overlying self-assembly process of block copolymers. To reveal how the self-responsive behavior of the copolymer brushes affects the directing effect, we develop a dissipative particle dynamics model to explicitly include the prepatterned polymer brushes and implement it to simulate the DSA of a cylinder-forming diblock copolymer melt on the sparse pattern of polymer brushes. Through large-scale dynamic simulations, we identify the windows of the content of the random copolymer, the film thickness, and the diameter of the patterned spot, for the formation of perfectly ordered hexagonal patterns composed of perpendicular cylinders. Our dynamic simulations reveal that the random copolymer brushes grafted on the unpatterned area exhibit a remarkable self-responsive ability with respect to the self-assembly of the diblock copolymers overlying them, which may widen the effective window of the content of the random copolymer. Within the processing windows of these key parameters, defect-free patterns are successfully achieved both in simulations and in experiments with sizes as large as a few micrometers for 4-fold density multiplications. This work demonstrates that highly efficient computer simulations based on an effective model can provide helpful guidance for experiments to optimize the critical parameters and even may promote the application of DSA.

Dynamic interfacial adsorption and emulsifying performance of self-assembled coconut protein and fucoidan mixtures

The functional properties of protein are affected by their aggregation behavior and morphology. In this study, the self-assembled coconut protein aggregates with specific morphology, including small amorphous aggregates (WLA), spherical-like aggregates (SLA) and rod-like aggregates (RLA), were regulated to form. The self-assembled process resulted in a decrease in fluorescence intensity and an increase in the surface hydrophobicity of coconut protein. Fucoidan was added to improve the stability of protein solutions, and the interfacial adsorption behavior was evaluated by dilatational rheology analysis. The results showed that the aggregation state of coconut protein affected its ability to reduce surface tension, and the interfacial layers mainly exhibited elastic property at oil-water interface (tanφ < 0.5). For macroscale analysis, the emulsions based on self-assembled coconut protein exhibited smaller droplet size, better rheological properties and centrifugal stability, especially WLA and RLA. This study may provide a reference to inspire the utilization of self-assembled coconut protein in the food industry.

CTAB-induced synthesis of two-dimensional copper oxalate particles: using l-ascorbic acid as the source of oxalate ligand.

Copper oxalate is typically synthesized through a precipitation reaction involving copper salts mixed with oxalic acid or oxalate solutions. However, in this study, we were successful in synthesizing well-formed square-like copper oxalate particles under liquid-phase conditions at ambient temperature and pressure using ascorbic acid as the source of the oxalic acid ligand. The addition of cationic surfactant cetyltrimethylammonium bromide (CTAB) caused the morphology of copper oxalate particles to undergo a transition from three-dimensional to two-dimensional. And the inhibition of the assembly of primary copper oxalate nanocrystals along the [001] direction became stronger with the increase of CTAB concentration. The impact of CTAB on the crystallization, growth, and self-assembly processes of primary copper oxalate nanocrystals was analysed using various testing methods. Based on these analyses, the possible mechanism of CTAB-induced synthesis of two-dimensional copper oxalate particles was finally proposed.

The role of chelating agent in the self-assembly of amphoteric surfactants

Hypothesis: Limited research has been conducted on the influence of chelating agents on the self-assembly process in surfactant solutions. The traditional approach assumes the chelating agent only interferes as a salting-out ion, therefore promoting surfactant separation. However, the opposite behavior has been observed for iminodipropionate based surfactants, in which the presence of chelating agents of the aminopolycarboxylate type increases solubility of nonionic ethoxylated surfactants in mixed micellar systems. Specific interaction between chelating agents-surfactants can be an important parameter in the self-assembly processes.Experiments: Physicochemical properties of solutions containing amphoteric surfactant and tetrasodium glutamatediacetate have been investigated. Macroscopic properties, such as viscosity and cloud point, were evaluated in the presence of a non-water-soluble alkyl ethoxylated surfactant. Interactions between amphoteric surfactant and chelating agent were monitored by NMR spectroscopy, including 13C chemical shift and lineshape analysis as well as 1H diffusometry.Findings: The study reveals that there is an interaction between the head group of the surfactant and the chelating agent forming oligomeric surfactant analogues with larger hydrophilic moieties, which results in smaller, more spherical micelles. The combined interactions provide possibilities for tuning the aggregation behavior of systems containing surfactants and chelating agents, and with that, the macroscopic properties of the system.

Optimizing Double-Fibril Network Morphology via Solid Additive Strategy Enables Binary All-Polymer Solar Cells with 19.50% Efficiency.

Double-fibril network morphology (DFNM), in which the donor and the acceptor can self-assemble into a double-fibril structure, is beneficial for exciton dissociation and charge transport in organic solar cells. Herein, it is demonstrated that such DFNM can be constructed and optimized in all-polymer solar cells (all-PSCs) with the assistance of 2-alkoxynaphthalene volatile solid additives. It is revealed that the incorporation of 2-alkoxynaphthalene can induce a stepwise regulation in the aggregation of donor and acceptor molecules during film casting and thermal annealing processes. Through altering the alkoxy of 2-alkoxynaphthalene solid additives, both the intermolecular interactions and molecular miscibility with the host materials can be precisely tuned, which allows for the optimization of the molecular aggregation process and facilitation of molecular self-assembly, and thus leading to reinforced molecular packing and optimized DFNM. As a result, an unprecedented efficiency of 19.50% (certified as 19.1%) is obtained for 2-ethoxynaphthalene-processed PM6:PY-DT-X all-PSCs with excellent photostability (T80=1750h). This work reveals that the optimization of DFNM via solid additive strategy is a promising avenue to boosting the performance of all-PSCs.

Experimental Correlation between Apparent pKa and Gelation Propensity in Amphiphilic Hydrogelators Derived from l-Dopa.

We report the gelation propensity of three gelators derived from l-dihydroxyphenylalanine (l-Dopa), where the amino group is derivatized with three different fatty acids (lauric acid, palmitic acid, and azelaic acid). The long aliphatic side chains should introduce additional van der Waals interactions among the molecules, contributing to the self-assembly process. The hydrogels have been prepared with the pH change method, and both the hydrogels and the corresponding aerogels have been analyzed using several techniques. In any case, Lau-Dopa provides stronger hydrogels compared with the other gelators. This property may be ascribed to its tendency to efficiently form supramolecular β-sheet structures, as outlined by the ECD, IR, and SEM analyses. Moreover, the preliminary measurement of the apparent pKa displays for Lau-Dopa two plateaux, as previously observed for, one at about pH 12 and a second one at pH 7.5. Thus, its pKa results in two apparent pKa shifts of ∼8.5 and ∼4 pH units above the theoretical pKa, as a consequence of a multistep self-assembly pathway that correlates, in the final β-sheet-based hydrogel, with a high degree of order and stability.

Self-assembly metal phenolic network coating improves the controlled release and bacteriostatic properties of Litsea cubeba essential oil-loaded ε-polylysine-pectin nanoparticles

Pectin and ε-polylysine (ε-PL) nanoparticles loaded with Litsea cubeba essential oil (LEO) (PP-LNPs) were prepared through the electrostatic interaction. Metal phenol network (MPN) coatings, designated as MPN@PP-LNPs, were fabricated on the surface of the nanoparticles via self-assembly process of tannic acid (TA) and FeIII to develop food preservative materials with pH-responsive controlled release. The morphology, encapsulation efficiency, and pH-responsive release characteristics of MPN@PP-LNPs were investigated. The results showed that the particle size of MPN@PP-LNPs was 432.5 ± 58.6 nm. Furthermore, the encapsulation efficiencies of ε-PL and LEO were 83.26 ± 2.21% and 30.78 ± 3.92%, respectively. TA was rapidly released at low pH, while LEO exhibited controlled release over a wide pH range (pH 1.2–9.0). In addition, the MPN coating has been demonstrated to enhance antioxidant activity and inhibit the growth of E. coli and S. aureus under acidic conditions. Furthermore, preliminary evidence suggests that MPN@PP-LNPs are not cytotoxic. In conclusion, MPN@PP-LNPs, prepared through the self-assembled surface modification of TA and FeIII, was an effective material for food preservation.

Regulatory mechanisms of phosphorylation in ovalbumin self-assembly for aggregates formation: Insights into size, structure, and morphology

In this study, the impact of different phosphorylation degrees on ovalbumin (OVA) assemblies was investigated by introducing negatively charged phosphorylated groups as driving forces at pH 9.0 and 85 °C for 2, 4, 6, 10, and 12 h to examine their turbidity, zeta-potential, and average particle size during phosphorylation-mediated aggregation. The presence of phosphate groups in the aggregates was confirmed by 31P NMR and FTIR spectra. The aggregation process, including amyloid formation, was analyzed by evaluating active thiol groups, intrinsic fluorescence spectra, surface hydrophobicity, circular dichroism, and thioflavin T (THT) fluorescence. TEM and small-angle scattering analysis of the morphological evolution of the self-assembly process over time revealed a structural progression from flexible to longer and thicker flexible fibrils, with the formation of shorter, more rigid semiflexible aggregates after 10h of phosphorylation. When phosphorylated for 12 h, the OVA aggregates exhibited a compact core primarily composed of cross β-structures and surrounded by loosely packed protein segments with random coil structures. Overall, this study highlighted the enhancement of OVA self-assembly by phosphorylation, where electrostatic and hydrophobic interactions play pivotal roles in regulating the formation of protein self-assembly aggregates.

Influence of supramolecular self-assembly of oppositely charged Co- and Sn-porphyrins on the their spectral-luminescent properties in aqueous and aqueous micellar media of ionic surfactants

The processes of supramolecular self-assembly of Co(III)-meso-tetra-(4-trimethylammoniophenyl)porphyrin (CoP) and bis-(4-(1-imidazolyl)-phenol)-Sn(IV)-meso-tetra(4-sulfophenyl)porphyrin (SnP) were studied using electronic, steady-state and time-resolved fluorescence, one- and two-dimensional NMR spectroscopy in aqueous media. The main product of such interaction at a 2:1 M ratio of Co and Sn porphyrinates was found to be supramolecular porphyrin trimer CoP–SnP–CoP formed due to donor-acceptor, hydrogen and electrostatic interactions. The distinctive features of the resulting trimer are: significant distortion of the spatial structure of the Co-porphyrin fragments and strong quenching of the Sn-porphyrin macrocycles fluorescence (by 70 %). The distortion of the spatial structure of Co porphyrinates is in good agreement with the quantum chemical calculations as well as with the electronic and NMR spectroscopy data. Adding surfactants – both anionic (Cetyltrimethylammonium bromide - CTAB) and cationic (Sodium dodecyl sulfate - SDS) – even at concentrations below the critical micelle concentration (CMC) leads to the supramolecular trimer destruction. In solutions of ionic surfactants, supramolecular trimer destruction is caused by the interaction of either the peripheral macrocycles of the trimer (CoP) with SDS micelles (premicellar aggregates) or the central macrocycle (SnP) with CTAB micelles (premicellar aggregates). This process is prolonged and the rate of trimer destruction depends on the surfactant concentration. The sizes of the CTAB and SDS micelles solubilized with porphyrin molecules were established by dynamic light scattering. In general, surfactant additions lead to an increase in the SnP fluorescence at least due to the destruction of the supramolecular self-assembly, as well as due to the changes in the state of its microenvironment.

Preparation of β-cyclodextrin-reduced graphene oxide aerogel and its application for adsorption of herbicides

Herbicides are the primary pesticides that can easily pollute water bodies, attracting significant attention from researchers regarding the effective removal of herbicide residues from the water environment. In this study, a β-cyclodextrin-reduced graphene oxide (β-CD-BTCA-rGO) aerogel was prepared following the self-assembly hydrothermal method using 1,2,3,4-butane tetracarboxylic acid (BTCA) as crosslinkers. The self-assembly process involved the cross-linking of “soft” β-cyclodextrin (β-CD) with “hard” graphene oxide (GO) nanosheets, forming a stable β-CD-BTCA-rGO aerogel. The prepared β-CD-BTCA-rGO aerogel demonstrated excellent adsorption performance. The adsorption capacities were 62.3 and 46.8 mg/g for sulfentrazone and quinclorac, respectively, surpassing the traditional reduced graphene oxide (rGO) aerogel and citric acid cross-linked (β-CD-CA-rGO) aerogel. Correspondingly, its adsorption capacity for quinclorac was 1.8 times and 12 times that of rGO aerogel and β-CD-CA-rGO aerogel, respectively. Quantum chemical calculations at the density functional theory (DFT) level, utilizing the Fukui function to predict chemical reaction sites, indicated that BTCA, as crosslinkers, formed stable chemical bonds (ester bonds) with GO through hydroxyl and carboxyl surface functional groups, leading to the formation of stable porous aerogels. Furthermore, the highest occupied molecular orbital-lowest unoccupied molecular orbital (HOMO-LUMO) energy gap was quantitatively measured for various adsorption mechanisms, revealing that electrostatic adsorption was the main force of the adsorption on the aerogels. The β-CD-BTCA-rGO aerogels prepared in this study demonstrated economic feasibility as adsorbents and exhibited good reproducibility. Consequently, β-CD-BTCA-rGO aerogels hold promising application prospects in the remediation of pesticide pollution in water systems.