Self-assembly Mechanism Research Articles

Solvent-dependent structural and electrochemical properties of zinc cobaltite via a self-assembled mechanism for battery-type supercapacitors

This paper reports the influence of the solvent’s properties on the growth mechanism of zinc cobaltite (ZnCo2O4) microstructures and their surface morphologies. We observed that the ZnCo2O4 microstructures (ZCO) offer a large number of interacting sites due to the solvent variation, influencing the phase purity and high crystallinity of the ZnCo2O4, which strongly affects its electrochemical conductivity. ZCO crystals were synthesized separately in water, ethanol, and isopropyl alcohol solvent at 180 °C for 12 h, governing the formation of 2D sheet-like morphology in water (ZCO-DIW), 3D flower-like and peanut-like morphologies in ethanol (ZCO-ETH), and isopropyl alcohol (ZCO-IPA), respectively. The successful formation of ZCO morphologies was confirmed through high-resolution scanning electron microscopy. Concerning the solvent variation, the specific surface area of the three ZCO electrodes varies in ascending order as ZCO-DIW (23.78 m2 g−1) < ZCO-IPA (27.19 m2 g−1) < ZCO-ETH (37.19 m2 g−1). We also proposed a model for this solvent-dependent formation mechanism of three ZCO electrodes via the self-assembly process. The electrochemical performance of the ZCO electrodes exhibits excellent battery-type behavior with a specific capacity of 98.89 mAh g−1 (for ZCO-ETH) owing to the highly porous flower-like morphology. These results revealed a simple and cost-effective synthesis strategy to fabricate micro/nano-structure with diverse morphology for a wide range of interfacial applications.

When Phased without Water: Biophysics of Cellular Desiccation, from Biomolecules to Condensates.

The molecular machinery that enables life has evolved in water, yet many of the organisms around us are able to survive even extreme desiccation. Especially remarkable are single-cell and sedentary organisms that rely on specialized biomolecular machinery to survive in environments that are routinely subjected to a near-complete lack of water. In this review, we zoom in on the molecular level of what is happening in the cellular environment under water stress. We cover the various mechanisms by which biochemical components of the cell can dysfunction in dehydrated cells and detail the different strategies that organisms have evolved to eliminate or cope with these desiccation-induced perturbations. We specifically focus on two survival strategies: (1) the use of disordered proteins to protect the cellular environment before, during, and in the recovery from desiccation, and (2) the use of biomolecular condensates as a self-assembly mechanism that can sequester or protect specific cellular machinery in times of water stress. We provide a summary of experimental work describing the critical contributions of disordered proteins and biomolecular condensates to the cellular response to water loss and highlight their role in desiccation tolerance. Desiccation biology is an exciting area of cell biology, still far from being completely explored. Understanding it on the molecular level is bound to give us critical new insights in how life adapted/can adapt to the loss of water, spanning from the early colonization of land to how we can deal with climate change in our future.

Self-assembling peptide biomaterials: Insights from spontaneous and enhanced sampling molecular dynamics simulations

Peptide self-assembly is the process by which peptide molecules aggregate into low dimensional (1D, 2D) or 3D ordered materials with potential applications ranging from drug delivery to electronics. Short peptides are particularly good candidates for forming supramolecular assemblies due to the relatively simple structure and ease of modulating their self-assembly process to achieve required material properties. The experimental resolution of fibrous peptide-based nanomaterials as 3D atomic coordinates remains challenging. For surface-mediated peptide assembly in particular, it is typically not feasible to resolve multiple conformationally distinct surface bound peptide structures by experiment. The mechanisms of peptide self-assembly also remain elusive due to the interchange of complex interactions and multiple time and length scales involved in the self-assembly process. Peptide self-assembly in solution, or mediated by surfaces, is driven by specific interactions between the peptides and water, competing interactions within the peptide and/or between peptide aggregate units and, in the latter case, an interplay of the interactions between peptides and solvent molecules for adsorption onto a proximal surface. Computational methodologies have proven beneficial in elucidating the structures formed during peptide self-assembly and the molecular mechanisms driving it, and hence have scope in facilitating the development of functional peptide-based nanomaterials for medical or biotechnological applications. In this perspective, computational methods that have provided molecular insights into the mechanisms of formation of peptide biomaterials, and the all-atom-resolved structures of peptide assemblies are presented. Established and recently emerged molecular simulation approaches are reviewed with a focus on applications relevant to peptide assembly, including all-atom and coarse-grained “brute force” molecular dynamics methods as well as the enhanced sampling methodologies: umbrella sampling, steered and replica exchange molecular dynamics, and variants of metadynamics. These approaches have been shown to contribute all-atom details not yet available experimentally, to advance our understanding of peptide self-assembly processes and biomaterial formation. The scope of this review includes a summary of the current state of the computational methods, in terms of their strengths and limitations for application to self-assembling peptide biomaterials.

Molecular Mechanisms of Amyloid-β Self-Assembly Seeded by In Vivo-Derived Fibrils and Inhibitory Effects of the BRICHOS Chaperone.

Self-replication of amyloid-β-peptide (Aβ) fibril formation is a hallmark in Alzheimer's disease (AD). Detailed insights have been obtained in Aβ self-assembly in vitro, yet whether similar mechanisms are relevant in vivo has remained elusive. Here, we investigated the ability of in vivo-derived Aβ fibrils from two different amyloid precursor protein knock-in AD mouse models to seed Aβ42 aggregation, where we quantified the microscopic rate constants. We found that the nucleation mechanism of in vivo-derived fibril-seeded Aβ42 aggregation can be described with the same kinetic model as that in vitro. Further, we identified the inhibitory mechanism of the anti-amyloid BRICHOS chaperone on seeded Aβ42 fibrillization, revealing a suppression of secondary nucleation and fibril elongation, which is strikingly similar as observed in vitro. These findings hence provide a molecular understanding of the Aβ42 nucleation process triggered by in vivo-derived Aβ42 propagons, providing a framework for the search for new AD therapeutics.

Mechanism of Cross-Linking, Self-Assembly, Controlled Release, and Applications of Nanogels in Drug Delivery System

Drug delivery system has been very important for achieving the last goal of precision medicine, also, among various drug carrier materials, nanogel is considered a promising one. Nanogels are a kind of material that have been proven very effective and specialized on targeted controlled release of drugs in medical therapies. Many researches and applications have used nanogels as an efficient drug carrier through its properties of loading and high capacity, and very high future expectations has been given to this material as a future idealized material in nano medical areas. This paper mainly discusses the key features of the nanogels including degradability and high drug capacity, as well as the mechanism of cross- linking mechanism and self assembly of nanogels in both physical and chemical ways. In addition, this paper explains how nanogels can carry different drugs and control-release the drug under different stimuli to aim the goal at targeted drugs delivery. Finally current research situations and future expectations of this topic are also proposed.

Applying dynamic light scattering to investigate the self-assembly process of DNA nanostructures

Understanding the dynamic assembly process of DNA nanostructures is important for developing novel strategy to design and construct functional devices. In this work, temperature-controlled dynamic light scattering (DLS) strategy has been applied to study the global assembly process of DNA origami and DNA bricks. Through the temperature dependent size and intensity profiles, the self-assembly process of various DNA nanostructures with different morphologies have been well-studied and the temperature transition ranges could be observed. Taking advantage of the DLS information, rapid preparation of the DNA origami and the brick assembly has been realized through a constant temperature annealing. Our results demonstrate that the DLS-based strategy provides a convenient and robust tool to study the dynamic process of forming hieratical DNA structures, which will benefit understanding the mechanism of self-assembly of DNA nanostructures.

Atomic-Scale Insights into the Self-Assembly of Alternating AlN/TiN Lamellar Nanostructures via Spinodal Decomposition in AlTiN Coating.

The self-assembly mechanism of alternating AlN/TiN nano-lamellar structures in AlTiN coating is still a mystery, though this coating has been widely used in industry. Here, by using the phase-field crystal method, we studied the atomic-scale mechanisms of the formation of nano-lamellar structures during spinodal decomposition transformation of an AlTiN coating. The results show that the formation of a lamella is characterized by four distinct stages including the generation of dislocations (stage I), formation of islands (stage II), merging of islands (stage III), and flattening of lamellae (stage IV). The locally periodic fluctuation of the concentration along the lamella leads to the generation of periodically distributed misfit dislocations and then AlN/TiN islands, while the fluctuation of the composition in the direction normal to the lamella is responsible for the merging of islands and flattening of a lamella and more importantly the cooperative growth between neighboring lamellae. Moreover, we found that misfit dislocations play a crucial role in all the four stages, promoting the cooperative growth of TiN and AlN lamellae. Our results demonstrate that the TiN and AlN lamellae could be produced through the cooperative growth of AlN/TiN lamellae in spinodal decomposition of the AlTiN phase.

Uncovering the mechanisms of cyclic peptide self-assembly in membranes with the chirality-aware MA(R/S)TINI forcefield

Cyclic peptides (CPs) formed by alternation of D- and L-amino acids (D,L-CPs) can self-assemble into nanotubes (SCPNs) by parallel or/and antiparallel stacking. Different applications have been attributed to these nanotubes, including the disruption of lipid bilayers of specific compositions and the selective transport of ions throughout membranes. Molecular dynamics (MD) simulations have significantly contributed to understand the interaction between CPs, including the structural, dynamic and transport properties of their supramolecular aggregates. The high computational cost of atomic resolution forcefields makes them impractical for simulating the self-assembly of macromolecules, so coarse-grained (CG) models might represent a more feasible solution for this purpose. However, general CG models used for the simulation of biomolecules such as the MARTINI forcefield do not explicitly consider the non-covalent interactions leading to the formation of secondary structure patterns in proteins. This becomes particularly important in the case of CPs due to the D- and L-chirality alternation in their sequence, leading to opposite orientations of the backbone polar groups on both sides of the cyclic ring plane. In order to overcome this limitation, we have extended the MARTINI forcefield to introduce chirality in each residue of the CPs. The new parametrization, which we have called MA(R/S)TINI, reproduces the expected self-assembly patterns for several CP sequences in the presence of different membrane models, explicitly considering the chirality of the CPs and with no significant extra computational cost. Our simulations provide new mechanistic information of how these systems self-assemble in presence of different lipid scenarios, showing that the CP-CP and CP-membrane interactions are sensitive to the peptide sequence chirality. This opens the door to design new bioactive CPs based on CG-MD simulations. A web-based tool for the automatic parameterization of new CP sequences using MA(R/S)TINI, among other functionalities, is under construction (see http://cyclopep.com).

Meniscus-confined electrochemical additive manufacturing of copper microstructures: Design, fabrication, characterization, and decorative art technology

For the first time, a room-temperature meniscus-confined electrochemical additive manufacturing (MC-ECAM) process is evaluated as a potential decorative art technology for fabricating copper metal. The MC-ECAM has proven to be an excellent method for large-scale printing of decorative copper artworks such as warli art, plant leaves, and paintings. The inherent nature of the MC-ECAM process has the potential to eliminate the traditional time-consuming route to producing such copper microstructures and provide a one-step and efficient solution. The TEM and FE-SEM results revealed that well-oriented microstructures are prepared without surfactant, indicating the ECAM self-assembly mechanism. A small amount of zinc is added to the copper system to prevent corrosion. The XRD analysis also revealed the formation of copper metal, which barely changed even after 10 months of atmospheric ageing with the addition of 2% zinc. The XPS results show that zinc provides excellent stability for the ECAM-printed copper microstructure, further examined by an electrochemical corrosion study. Zinc act as a barrier to corrosion, and the results show that the Cu-Zn 2% exhibits excellent corrosion resistance than the pure copper microstructures.

Efficient Purification of Cowpea Chlorotic Mottle Virus by a Novel Peptide Aptamer

The cowpea chlorotic mottle virus (CCMV) is a plant virus explored as a nanotechnological platform. The robust self-assembly mechanism of its capsid protein allows for drug encapsulation and targeted delivery. Additionally, the capsid nanoparticle can be used as a programmable platform to display different molecular moieties. In view of future applications, efficient production and purification of plant viruses are key steps. In established protocols, the need for ultracentrifugation is a significant limitation due to cost, difficult scalability, and safety issues. In addition, the purity of the final virus isolate often remains unclear. Here, an advanced protocol for the purification of the CCMV from infected plant tissue was developed, focusing on efficiency, economy, and final purity. The protocol involves precipitation with PEG 8000, followed by affinity extraction using a novel peptide aptamer. The efficiency of the protocol was validated using size exclusion chromatography, MALDI-TOF mass spectrometry, reversed-phase HPLC, and sandwich immunoassay. Furthermore, it was demonstrated that the final eluate of the affinity column is of exceptional purity (98.4%) determined by HPLC and detection at 220 nm. The scale-up of our proposed method seems to be straightforward, which opens the way to the large-scale production of such nanomaterials. This highly improved protocol may facilitate the use and implementation of plant viruses as nanotechnological platforms for in vitro and in vivo applications.

Laser-Induced Fabrication of Electrodes on Graphene Oxide–MXene Composites for Planar Supercapacitors

Graphene-based supercapacitors are powerful devices for supporting smart wearable electronics. However, the properties of the as-prepared graphene and its analogues differ from the expected characteristics, which hinder the development of graphene-based energy storage devices. Herein, we demonstrated the fabrication of planar supercapacitors based on laser-induced electrostatic self-assembled graphene oxide–MXene (GO–M) composites. Owing to the synergetic effect of the laser–matter interaction and electrostatic self-assembly, the as-prepared reduced GO–M (R-GO–M) showed good conductivity and a better layered micro-/nanostructure than reduced graphene oxide (RGO). Moreover, in this laser-induced process, MXene was introduced in R-GO–M, which offered more active sites. Therefore, the supercapacitor based on R-GO–M exhibited noticeable capacity enhancement, five times more than the value of the RGO-based supercapacitor. Furthermore, after comprehensive electrochemical performance analysis, the proper electrostatic self-assembly ratio was confirmed to be 10:1. We believe that the laser fabrication technique combined with a simple electrostatic self-assembly mechanism will promote the development of graphene-based energy storage devices using a simple but effective method.

Molecular Insights into Cyclodextrin-Adamantane-Modified Copolymer Host-Guest Interactions.

Supramolecular polymer flooding has great potential in solving the problems of difficult injection and low recovery in low-permeability polymer reservoirs. However, the self-assembly mechanism of supramolecular polymers is not yet to be fully understood at the molecular level. In this work, molecular dynamics simulations were used to explore the formation of cyclodextrin and adamantane-modified supramolecular polymer hydrogels; the self-assembly mechanism was summarized; and the effect of concentration on the oil displacement index was evaluated. The assembly mechanism of supramolecular polymers can be attributed to the "node-rebar-cement" mode of action. At the same time, Na+ can form intermolecular and intramolecular salt bridges with supramolecular polymers, and together with the "node-rebar-cement" mode of action, the supramolecular polymers can form a more compact 3D network structure. When the polymer concentration was increased, especially up to its critical association concentration (CAC), the association increased significantly. Besides, the construction of a 3D network was promoted, which results in a higher viscosity. This work investigated the assembly process of supramolecular polymers from the molecular scale and explained its mechanism of action, which makes up for the deficiencies of other research methods and provides a theoretical basis for screening out functional units that can be used for the supramolecular polymer assembly.

Fast Self-Assembly Dynamics of a β-Sheet Peptide Soft Material.

Peptide-based hydrogels are promising biocompatible materials for wound healing, drug delivery, and tissue engineering applications. The physical properties of these nanostructured materials depend strongly on the morphology of the gel network. However, the self-assembly mechanism of the peptides that leads to a distinct network morphology is still a subject of ongoing debate, since complete assembly pathways have not yet been resolved. To unravel the dynamics of the hierarchical self-assembly process of the model β-sheet forming peptide KFE8(Ac-FKFEFKFE-NH2 ), high-speed atomic force microscopy (HS-AFM) in liquid is used. It is demonstrated that a fast-growing network, based on small fibrillar aggregates, is formed at a solid-liquid interface, while in bulk solution, a distinct, more prolonged nanotube network emerges from intermediate helical ribbons. Moreover, the transformation between these morphologies has been visualized. It is expected that this new in situ and in real-time methodology will set the path for the in-depth unravelling of the dynamics of other peptide-based self-assembled soft materials, as well as gaining advanced insights into the formation of fibers involved in protein misfolding diseases.

The development of a smart gel for CO2 mobility control in heterogeneity reservoir

CO2 flooding is regarded as one of the most effective ways to enhance oil recovery for unconventional oil and gas reservoirs, that is also conducive to the capture and storage of CO2. However, due to the heterogeneity of the reservoir, the gas channeling of CO2 becomes more serious, limiting the sweep efficiency of CO2 flooding. Herein, to make the most use of CO2 flooding, a CO2-responsive smart gel system is designed to improve the formation profile and control the mobility of CO2. Through rheological tests, the basic properties, such as shear resistance, viscoelasticity and responsiveness, are evaluated. The system has good viscoelastic and shear resistance, and can quickly form high strength gel within 150 s. At the same time, the self-assembly mechanism of the system is revealed by SEM. The influence of permeability, injection concentration and volume of smart gel on the plugging performance of the CO2-responsive smart gel system are also explored. Finally, the mobility control ability and EOR performance of the CO2-responsive smart gel system are revealed by the double pipes flooding experiments. This work puts forward a new idea of enhancing oil recovery for CO2 flooding with the aid of CO2-responsive smart gel.

In situ self-assembled macroporous interconnected nanosheet arrays of Ni-1,3,5-benzenetricarboxylate metal − organic framework on Ti mesh as high-performance oxygen evolution electrodes

Highly efficient metal–organic framework (MOF)-based oxygen evolution reaction (OER) catalysts are desirable for water splitting, but their development remains challenging due to poor accessibility of coordinatively unsaturated metal (cum) sites and low intrinsic activity. A large-area three-dimensional (3-D) macroporous interconnected nanosheet array of Ni-1,3,5-benzenetricarboxylate has been in situ self-assembled on Ti mesh (TM) by using ethanol as the solvent and high-affinity oxide layer on TM to promote in situ nucleation. The obtained nanoarchitecture exhibits much superior catalytic activity compared to most reported catalysts including MOF-based catalysts, other precious-metal-free ones, and Ir/Ru-based ones. Additionally, this electrode undergoes no current decay after 300 cyclic voltammetry (CV) cycles and can maintain at 250 mA cm−2 for over 266 h. The excellent catalytic performance is mainly due to the 3-D macroporous and interconnected nanosheet array structure improving cum site exposure and charge transport and in situ activated cum cations enhancing OH− adsorption. This work not only develops a facile and economical approach to synthesize 3-D macroporous interconnected MOF nanosheet arrays to simultaneously increase the number, exposure, and intrinsic activity of active sites and facilitate charge transport for high-performance eletrocatalysis, but provides scientific insights into the mechanisms for self-assembly of this unique nanoarchitecture and for the high OER performance.

Self-assembly of nanoflower-like MIL-125(Ti)/Bi2O2CO3 hierarchical tandem heterojunctions for enhanced visible-light degradation of antibiotic contamination

A high-efficiency photocatalytic composite with nano-flower-like structure was self-assembly constructed with Bi2O2CO3 as the main body to solve the problem of antibiotic pollution. Considering the high surface area and porous structure of MOFs, solvothermal method was used to introduce the porous band-matched n-type semiconductor MIL-125 into Bi2O2CO3 compound to construct a Self-assembly hierarchical tandem heterojunction, the tight binding of MIL-125(Ti) nanoparticles and Bi2O2CO3 nanoparticles facilitated charge transfer and separation under illumination. In the photocatalytic degradation experiment, the concentration of tetracycline was 20 mg/L, and the content of MIL-125(Ti) was 20 %, the composite photocatalyst has the best degradation rate of tetracycline that can reach 92.2 % after 60 min irradiation. In addition, the effects of different mass ratios of MIL-125(Ti)/Bi2O2CO3 composite photocatalysts on the photocatalytic performance were also discussed. Compared with the Bi2O2CO3 monomer, the degradation efficiency of the composites increased gradually with the addition of MIL-125(Ti) from 10 % to 20 %. Through electrochemical characterization, the self-assembly Z-type electron transfer mechanism of MIL-125(Ti)/Bi2O2CO3 composite photocatalyst is expounded, and the problem of overcoming the mismatch of electron and hole mobility is revealed, which solves the wide band gap defect of Bi2O2CO3, according to the first-order kinetic curve, the reaction rate of 20 % MIL-125/Bi2O2CO3 is 4.9 times that of pure Bi2O2CO3.

Regulatory Mechanism of Opposite Charges on Chiral Self-Assembly of Cellulose Nanocrystals.

The charge plays an important role in cellulose nanocrystal (CNC) self-assembly to form liquid crystal structures, which has rarely been systematically explored. In this work, a novel technique combining atomic force microscopy force and atomistic molecular dynamics simulations was addressed for the first time to systematically investigate the differences in the CNC self-assembly caused by external positive and negative charges at the microscopic level, wherein sodium polyacrylate (PAAS) and chitosan oligosaccharides (COS) were used as external positive and negative charge additives, respectively. The results show that although the two additives both make the color of CNC films shift blue and eventually disappear, their regulatory mechanisms are, respectively, related to the extrusion of CNC particles by PAAS and the reduction in CNC surface charge by COS. The two effects both decreased the spacing between CNC particles and further increased the cross angle of CNC stacking arrangement, which finally led to the color variations. Moreover, the disappearance of color was proved to be due to the kinetic arrest of CNC suspensions before forming chiral nematic structure with the addition of PAAS and COS. This work provides an updated theoretical basis for the detailed disclosure of the CNC self-assembly mechanism.

Halogen Bond-Driven Aggregation-Induced Emission Skeleton: N-(3-(Phenylamino)allylidene) Aniline Hydrochloride.

Aggregation-induced emission (AIE) is a unique photophysical process, and its emergence brings a revolutionary change in luminescence. However, AIE-based research has been limited to a few classical molecular skeletons, which is unfavorable for in-depth studies of the photophysical characteristics of AIE and the full exploitation of their potential values. There is an urgent need to develop new skeletons to rise to the challenges of an insufficient number of AIE core structures and difficult modification. Here, we report a novel dumbbell AIE skeleton, in which two phenyls are connected through (E)-3-iminoprop-1-en-1-amine. This skeleton shows extremely strong solid-state emission with an absolute quantum yield up to 69.5%, a large Stokes shift, and typical AIE characteristics, which well resolves the challenge of difficult modification and low luminous efficiency of the traditional AIE skeletons. One-step reaction, high yield, and diversified modification endow the skeleton with great scalability from simple to complicated, or from symmetrical to asymmetrical structures, which establishes the applicability of the skeleton in various scenarios. These molecules self-assemble into highly ordered layer-, rod-, petal-, hollow pipe-, or helix-like nanostructures, which contribute to strong AIE emission. Crystallographic data reveal the highly ordered layer structures of the aggregates with different substituents, and a novel halogen bond-driven self-assembly mechanism that restricts intramolecular motion is clearly discovered. Taking advantage of these merits, a full-band emission system from green to red is successfully established, which displays great potential in the construction of light-emitting films and advanced light-emitting diodes. The discovery of this AIE skeleton may motivate a huge potential application value in luminescent materials and lead to hitherto impossible technological innovations.

Self-Healing, Robust, Liquid-Repellent Coatings Exploiting the Donor-Acceptor Self-Assembly.

Liquid-repellent coatings with rapid self-healing and strong substrate adhesion have tremendous potential for industrial applications, but their formulation is challenging. We exploit synergistic chemistry between donor-acceptor self-assembly units of polyurethane and hydrophobic metal-organic framework (MOF) nanoparticles to overcome this challenge. The nanocomposite features a nanohierarchical morphology with excellent liquid repellence. Using polyurethane as a base polymer, the incorporated donor-acceptor self-assembly enables high strength, excellent self-healing property, and strong adhesion strength on multiple substrates. The interaction mechanism of donor-acceptor self-assembly was revealed via density functional theory and infrared spectroscopy. The superhydrophobicity of polyurethane was achieved by introducing alkyl-functionalized MOF nanoparticles and post-application silanization. The combination of the self-healing polymer and nanohierarchical MOF nanoparticles results in self-cleaning capability, resistance to tape peel and high-speed liquid jet impacts, recoverable liquid repellence over a self-healed notch, and low ice adhesion up to 50 icing/deicing cycles. By exploiting the porosity of MOF nanoparticles in our nanocomposites, fluorine-free, slippery liquid-infused porous surfaces with stable, low ice adhesion strengths were also achieved by infusing silicone oil into the coatings.

Maturation of demineralized arabinogalactan-proteins from Acacia seyal gum in dry state: Aggregation kinetics and structural properties of aggregates

The aggregation in dry state of mineral-loaded arabinogalactan-proteins (AGPs) from Acacia seyal gum (GA) generally occurs above 70 °C. This study focuses on the aggregation sensitivity of AGPs after their demineralization. The dry incubation in mild temperature (25 °C to 70 °C) of demineralized AGPs induced the formation of aggregates, not observed with GA. AGPs aggregated following a self-assembly mechanism for which temperature only modulated the aggregation rate. The activation energy was around 90–100 kJ·mol−1 that could correspond to chemical condensation reactions induced by the AGPs surface dehydration. The aggregation kinetics were characterized by the formation of soluble aggregates during the first times of incubation, whose molar mass increased from 1 · 106 g·mol−1 to 6.7 · 106 g·mol−1 (SEC MALS) or 12 · 106 g·mol−1 (AF4 MALS) after 1.66 days of dry heating at 40 °C. These soluble aggregates revealed they adopted a similar conformation to that of not aggregated AGPs with a νh value around 0.45. Above 1.66 days at 40 °C, the soluble aggregates grew up to form microparticles with sizes ranging from 10 to around 200 μm. This study highlighted the protective role of cations from AGPs whose demineralization increased their sensibility to dry heating and their chemical reactivity for aggregation.