Bioinspired Interfacial Chelating-like Reinforcement Strategy toward Mechanically Enhanced Lamellar Materials

Abstract

Many biological organisms usually derived from the ordered assembly of heterogeneous, hierarchical inorganic/organic constituents exhibit outstanding mechanical integration, but have proven to be difficult to produce the combination of excellent mechanical properties, such as strength, toughness, and light weight, by merely mimicking their component and structural characteristics. Herein, inspired by biologically strong chelating interactions of phytic acid (PA) or IP6 in many biomaterials, we present a biologically interfacial chelating-like reinforcement (BICR) strategy for fabrication of a highly dense ordered "brick-and-mortar" microstructure by incorporating tiny amounts of a natural chelating agent ( e. g., PA) into the interface or the interlamination of a material ( e. g., graphene oxide (GO)), which shows joint improvement in hardness (∼41.0%), strength (∼124.1%), maximum Young's modulus (∼134.7%), and toughness (∼118.5%) in the natural environment. Besides, for different composite matrix systems and artificial chelating agents, the BICR strategy has been proven successful for greatly enhancing their mechanical properties, which is superior to many previous reinforcing approaches. This point can be mainly attributed to the stronger noncovalent cross-linking interactions such as dense hydrogen bonds between the richer phosphate (hydroxyl) groups on its cyclohexanehexol ring and active sites of GO, giving rise to the larger energy dissipation at its hybrid interfaces. It is also simple and environmentally friendly for further scale-up fabrication and can be readily extended to other material systems, which opens an advanced reinforcement route to construct structural materials with high mechanical performance in an efficient way for practical applications.

Tough Polyelectrolyte Hydrogels with Antimicrobial Property via Incorporation of Natural Multivalent Phytic Acid

“…In addition, the characteristic absorption peak of P-O-C at 1064 cm -1 appears in pTMAEMA-PA spectra, indicating the success of docking PA on pTMAEMA polymer chains as reported in literature [59]. In Figure 7b, the change in the peak position of OH bands (3445 cm -1 to 3401 cm -1 ) between as-prepared pTMAEMA and pTMAEMA-PA confirms the formation of hydrogen-bonding within pTMAEMA-PA hydrogels [33]. Furthermore, no peak shift in OH band was observed in the spectra of pTMAEMA-PP 6-.…”

“…These secondary metabolites have not only shown substantial antimicrobial capability against wide range of pathogenic bacteria, fungi and yeast via growth and protease inhibition and cell wall disruption, but also provide additional benefit for the body such as anti-inflammatory, antithrombotic and antioxidant [29][30][31]. Among these plant derivatives, phytic acid (PA), a natural chelating agents extracted from legumes, has been broadly applied in a variety of purposes, ranging from enhancing mechanical properties of materials [32][33] to therapeutic uses such as anticancer drug [34].…”

Tough Polyelectrolyte Hydrogels with Antimicrobial Property via Incorporation of Natural Multivalent Phytic Acid

“…Inspired by the compelling characteristics of a plant-based protocatechualdehyde in the formation of imide and coordinative bonds, Cheng′s group has recently introduced a novel approach to fabricate a supramolecular multistimuli-responsive hydrogel with antibacterial capability [32]. Another plant derivative, phytic acid (PA) has been broadly applied in a variety of purposes, ranging from enhancing mechanical properties of materials [33,34] to therapeutic uses such as anticancer drug [35]. Yet, to our knowledge, the fabrication of an antibacterial hydrogel incorporating with PA has not been explored.…”

Tuning the Mechanical Behavior of Metal–Phenolic Networks through Building Block Composition

“…[1][2][3] Coordination-based cross-linking is a rapid process 4,5 and can impart unique functionalities to materials such as adhesion, load-bearing, and abrasion resistance. [6][7][8][9][10][11] For example, Fe III -catechol complexes in mussel byssus threads and Zn II -histidine complexes in wandering spider fangs have remarkable mechanical properties (e.g., low density, and high extensibility and hardness). 2,6 Fundamental studies on metal complexation provide vital insights not only for understanding the hierarchical structuring and mechanical behavior of biological organisms, but also for designing bio-inspired materials for industrial and biomedical applications.…”

“…2,6 Fundamental studies on metal complexation provide vital insights not only for understanding the hierarchical structuring and mechanical behavior of biological organisms, but also for designing bio-inspired materials for industrial and biomedical applications. [4][5][6][7][8][9][10][11][12][13][14] The roles of metal ions and their coordination states have been extensively studied in biological and bio-inspired materials, including borate cross-linking in the cell walls of plants 12 and metal ion complexation in proteins, 7 peptides, 11 and synthetic materials. 8,10,11,13 However, systematic studies on the influence of metal ions and organic ligands on the physical properties of biological and bio-inspired materials are scant, likely because researchers either focus on a specific ligand (e.g., dopamine, histidine) or a specific metal ion (e.g., Fe III , Zn II ).…”