Soft gliadin nanoparticles at air/water interfaces: The transition from a particle-laden layer to a thick protein film.

HYPOTHESIS: Protein-based soft particles possess a unique interfacial deformation behavior, which is difficult to capture and characterize. This complicates the analysis of their interfacial properties. Here, we aim to establish how the particle deformation affects their interfacial structural and mechanical properties. EXPERIMENTS: Gliadin nanoparticles (GNPs) were selected as a model particle. We studied their adsorption behavior, the time-evolution of their morphology, and rheological behavior at the air/water interface by combining dilatational rheology and microstructure imaging. The rheology results were analyzed using Lissajous plots and quantified using the recently developed general stress decomposition (GSD) method. FINDING: Three distinct stages were revealed in the adsorption and rearrangement process. First, spherical GNPs (∼105 nm) adsorbed to the interface. Then, these gradually deformed along the interface direction to a flattened shape, and formed a firm viscoelastic 2D solid film. Finally, further stretching and merging of GNPs at the interface resulted in rearrangement of their internal structure to form a thick film with lower stiffness than the initial film. These results demonstrate that the structure of GNPs confined at the interface is controlled by their deformability, and the latter can be used to tune the properties of prolamin particle-based multiphase systems.

Microstrain-Stimulated Elastico-Mechanoluminescence with Dual-Mode Stress Sensing.

Elastico-mechanoluminescence technology has shown significant application prospects in stress sensing, artificial skin, remote interaction, and other research areas. Its progress mainly lies in realizing stress visualization and 2D or even 3D stress-sensing effects using a passive sensing mode. However, the widespread promotion of mechanoluminescence (ML) technology is hindered by issues such as high stress or strain thresholds and a single sensing mode based on luminous intensity. In this study, a highly efficient green-emitting ML with dual-mode stress-sensing characteristics driven by microscale strain is developed using LiTaO3:Tb3+. In addition to single-mode sensing based on the luminous intensity, the self-defined parameter (Q) is also introduced as a dual-mode factor for sensing the stress velocity. Impressively, the fabricated LiTaO3:Tb3+ film is capable of generating discernible ML signals even when supplied with strains as low as 500 µst. This is the current minimum strain value that can drive green-emitting ML. This study offers an ideal photonic platform for exploring the potential applications of rare-earth-doped elastico-ML materials in remote interaction devices, high-precision stress sensors, and single-molecule biological imaging.

Quantifying the interfacial triboelectricity in inorganic-organic composite mechanoluminescent materials.

Mechanoluminescence (ML) sensing technologies open up new opportunities for intelligent sensors, self-powered displays and wearable devices. However, the emission efficiency of ML materials reported so far still fails to meet the growing application requirements due to the insufficiently understood mechano-to-photon conversion mechanism. Herein, we propose to quantify the ability of different phases to gain or lose electrons under friction (defined as triboelectric series), and reveal that the inorganic-organic interfacial triboelectricity is a key factor in determining the ML in inorganic-organic composites. A positive correlation between the difference in triboelectric series and the ML intensity is established in a series of composites, and a 20-fold increase in ML intensity is finally obtained by selecting an appropriate inorganic-organic combination. The interfacial triboelectricity-regulated ML is further demonstrated in multi-interface systems that include an inorganic phosphor-organic matrix and organic matrix-force applicator interfaces, and again confirmed by self-oxidization and reduction of emission centers under continuous mechanical stimulus. This work not only gives direct experimental evidences for the underlying mechanism of ML, but also provides guidelines for rationally designing high-efficiency ML materials.

Bright Circularly Polarized Mechanoluminescence from 0D Hybrid Manganese Halides.

Hybrid metal halides (HMHs) with efficient circularly polarized luminescence (CPL) have application prospects in many fields, due to their abundant host-guest structures and high photoluminescence quantum yield (PLQY). However, CPLs in HMHs are predominantly excited by light or electricity, limiting their use in multivariate environments. It is necessary to explore a novel excitation method to extend the application of chiral HMHs as smart stimuli-responsive optical materials. In this work, an enantiomeric pair of 0D hybrid manganese bromides, [H2(2R,4R)-(+)/(2S,4S)-(-)-2,4-bis(diphenylphosphino)pentane]MnBr4 [(R/S)-1] is presented, which exhibits efficient CPL emissions with near-unity PLQYs and high dissymmetry factors of ± 2.0 × 10-3. Notably, (R/S)-1 compounds exhibit unprecedented and bright circularly polarized mechanoluminescence (CPML) emissions under mechanical stimulation. Moreover, (R/S)-1 possess high mechanical force sensitivities with mechanoluminescence (ML) emissions detectable under 0.1 N force stimulation. Furthermore, this ML emission exhibits an extraordinary antithermal quenching effect in the temperature range of 300-380 K, which is revealed to originate from a thermal activation energy compensation mechanism from trap levels to Mn(II) 4T1 level. Based on their intriguing optical properties, these compounds as chiral force-responsive materials are demonstrated in multilevel confidential information encryption.

Modulating Smart Mechanoluminescent Phosphors for Multistimuli Responsive Optical Wood.

Mechanoluminescence is a smart light-emitting phenomenon in which applied mechanical energy is directly converted into photon emissions. In particular, mechanoluminescent materials have shown considerable potential for applications in the fields of energy and sensing. This study thoroughly investigates the mechanoluminescence and long afterglow properties of singly doped and codoped Sr2 MgSi2 O7 (SMSO) with varying concentrations of Eu2+ and Dy3+ ions. Subsequently, a comprehensive analysis of its multimode luminescence properties, including photoluminescence, mechanoluminescence, long afterglow, and X-ray-induced luminescence, is conducted. In addition, the density of states mapping is acquired through first-principles calculations, confirming that the enhanced mechanoluminescence properties of SMSO primarily stem from the deep trap introduced by Dy3+ . In contrast to traditional mixing with Polydimethylsiloxane, in this study, the powders are incorporated into optically transparent wood to produce a multiresponse with mechanoluminescence, long afterglow, and X-ray-excited luminescence. This structure is achieved by pretreating natural wood, eliminating lignin, and subsequently modifying the wood to overall modification using various smart phosphors and epoxy resin composites. After natural drying, a multifunctional composite wood structure with diverse luminescence properties is obtained. Owing to its environmental friendliness, sustainability, self-power, and cost-effectiveness, this smart mechanoluminescence wood is anticipated to find extensive applications in construction materials and energy-efficient displays.

Regulation of interfacial mechanics of soy protein via co-extraction with flaxseed protein for efficient fabrication of foams and emulsions.

Enrichment of plant proteins with functionality is of great importance for expanding their application in food formulations. This study proposed an innovation to co-enrich soy protein and flaxseed protein to act as efficient interfacial stabilizers for generating foams and emulsions. The structure, interfacial properties, and functionalities of the soy protein-flaxseed protein natural nanoparticles (SFNPs) obtained by alkali extraction-isoelectric precipitation (AE) and salt extraction-dialysis (SE) methods were investigated. Overall, the foamability of AE-SFNPs (194.67 %) was 1.45-fold that of SE-SFNPs, due to their more flexible structure, smaller particle size, and suitable surface wettability, promoting diffusion and adsorption at the air-water interface. AE-SFNPs showed higher emulsion stability (140.89 min), probably because the adsorbed AE-SFNPs with smaller size displayed soft particle-like properties and stronger interfacial flexibility, and therefore could densely and evenly arrange at the interface, facilitating the formation of a stiff and solid-like interfacial layer, beneficial for more stable emulsion formation. The findings may innovatively expand the applications of SFNPs as food ingredients.

Redesign of air/oil-water interface via physical fields coupled with pH shifting to improve the emulsification, foaming, and digestion properties of plant proteins.

The application of plant proteins in food systems is largely hindered by their poor foaming or emulsifying properties and low digestibility compared with animal proteins, especially due to the aggregate state with tightly folded structure, slowly adsorbing at the interfaces, generating films with lower mechanical properties, and exposing less cutting sites. Physical fields and pH shifting have certain synergistic effects to efficiently tune the structure and redesign the interfacial layer of plant proteins, further enhancing their foaming or emulsifying properties. The improvement mechanisms mainly include: i) Aggregated plant proteins are depolymerized to form small protein particles and flexible structure is more easily exposed by combination treatment; ii) Particles with appropriate surface properties are quickly adsorbed to the interfacial layer, and then unfolded and rearranged to generate a tightly packed stiff interfacial layer to enhance bubble and emulsion stability; and iii) The unfolding and rearrangement of protein structure at the interface may result in the exposure of more cutting sites of digestive enzymes. This review summarizes the latest research progress on the structural changes, interfacial behaviors, and digestion properties of plant proteins under combined treatment, and elucidates the future development of these modification technologies for plant proteins in the food industry.

Mechanoluminescent Materials Enable Mechanochemically Controlled Atom Transfer Radical Polymerization and Polymer Mechanotransduction.

Organic mechanophores have been widely adopted for polymer mechanotransduction. However, most examples of polymer mechanotransduction inevitably experience macromolecular chain rupture, and few of them mimic mussel's mechanochemical regeneration, a mechanically mediated process from functional units to functional materials in a controlled manner. In this paper, inorganic mechanoluminescent (ML) materials composed of CaZnOS-ZnS-SrZnOS: Mn2+ were used as a mechanotransducer since it features both piezoelectricity and mechanolunimescence. The utilization of ML materials in polymerization enables both mechanochemically controlled radical polymerization and the synthesis of ML polymer composites. This procedure features a mechanochemically controlled manner for the design and synthesis of diverse mechanoresponsive polymer composites.

Mechanoluminescence and Photoluminescence Heterojunction for Superior Multimode Sensing Platform of Friction, Force, Pressure, and Temperature in Fibers and 3D-Printed Polymers.

Endowing a single material with various types of luminescence, that is, exhibiting a simultaneous optical response to different stimuli, is vital in various fields. A photoluminescence (PL)- and mechanoluminescence (ML)-based multifunctional sensing platform is built by combining heterojunctioned ZnS/CaZnOS:Mn2+ mechano-photonic materials using a 3D-printing technique and fiber spinning. ML-active particles are embedded in micrometer-sized cellulose fibers for flexible optical devices capable of emitting light driven by mechanical force. Individually modified 3D-printed hard units that exhibit intense ML in response to mechanical deformation, such as impact and friction, are also fabricated. Importantly, they also allow low-pressure sensing up to ≈100 bar, a range previously inaccessible by any other optical sensing technique. Moreover, the developed optical manometer based on the PL of the materials demonstrates a superior high-pressure sensitivity of ≈6.20 nm GPa-1 . Using this sensing platform, four modes of temperature detection can be achieved: excitation-band spectral shifts, emission-band spectral shifts, bandwidth broadening, and lifetime shortening. This work supports the possibility of mass production of ML-active mechanical and optoelectronic parts integrated with scientific and industrial tools and apparatus.

Mechanically induced photons from ultraviolet-C to near-infrared in Tm3+-doped MgF2.

Mechanoluminescence (ML) plays a vital role in various fields, and has gained increasing popularity over the past two decades. The widely studied materials that are capable of generating ML can be classified into two groups, self-powered and trap-controlled. Here, we demonstrate that both self-powered ML and trap-controlled ML can be achieved simultaneously in MgF2:Tm3+. Upon stimulation of external force, the 1I6→3H6 and 3H4→3H6 transitions of Tm3+ are observed, ranging from the ultraviolet-C to near-infrared. After exposure to X-rays, MgF2:Tm3+ presents a stronger ML than the uncharged sample. After cleaning up at high temperatures, the ML returns to the initial level, which is a typical characteristic of trap-controlled ML. In the end, we demonstrate the potential applications of MgF2:Tm3+ in dynamic anti-counterfeiting, and structure inspection.

Two Organic-Inorganic Manganese(II) Halide Hybrids Showing Compelling Photo- and Mechanoluminescence as well as Rewritable Anticounterfeiting Printing.

Two organic-inorganic manganese(II) halide hybrids (OIMHs) with formulas of [(TEA)(TMA)]MnCl4 (1) and [(TPA)(TMA)3](MnCl4)2 (2) (TEA = tetraethylammonium, TMA = tetramethylammonium, and TPA = tetrapropylammonium) were synthesized by a mixed-ligand strategy. Both compounds crystallize in the acentric space group and are composed of isolated [MnCl4]2- tetrahedral units separated by two types of organic cations. They show high thermal stability and emit strong green light with different emission bandwidths, quantum yields, and high-temperature photostability. Remarkably, the quantum yield of 1 can reach up to 99%. Due to the high thermal stability and quantum yield of 1 and 2, green light-emitting diodes (LEDs) were fabricated. Furthermore, mechanoluminescence (ML) was observed in 1 and 2 when stress was applied. The ML spectrum of 1 is similar to the photoluminescence (PL) spectrum, suggesting ML and PL emissions come from the same transition of Mn(II) ions. Finally, rewritable anticounterfeiting printing and information storage were achieved by utilizing the outstanding photophysical properties and ionic features of the products. The printed images still remain clear after several cycles, and the information stored on the paper can be read out by a UV lamp and commercial mobile phones.

Co-Extraction of Flaxseed Protein and Polysaccharide with a High Emulsifying and Foaming Property: Enrichment through the Sequence Extraction Approach.

A new focus with respect to the extraction of plant protein is that ingredient enrichment should target functionality instead of pursuing purity. Herein, the sequence aqueous extraction method was used to co-enrich five protein-polysaccharide natural fractions from flaxseed meal, and their composition, structure, and functional properties were investigated. The total recovery rate of flaxseed protein obtained by the sequence extraction approach was more than 80%, which was far higher than the existing reports. The defatted flaxseed meal was soaked by deionized water to obtain fraction 1 (supernatant), and the residue was further treated to get fraction 2 (supernatant) and 3 (precipitate) through weak alkali solubilization. Part of the fraction 2 was taken out, followed by adjusting its pH to 4.2. After centrifuging, the albumin-rich supernatant and precipitate with protein content of 73.05% were gained and labeled as fraction 4 and fraction 5. The solubility of fraction 2 and 4 exceeded 90%, and the foaming ability and stability of fraction 5 were 12.76 times and 9.89 times higher than commercial flaxseed protein, respectively. The emulsifying properties of fractions 1, 2, and 5 were all greater than that of commercial sodium caseinate, implying that these fractions could be utilized as high-efficiency emulsifiers. Cryo-SEM results showed that polysaccharides in fractions were beneficial to the formation of network structure and induced the formation of tighter and smoother interfacial layers, which could prevent emulsion flocculation, disproportionation, and coalescence. This study provides a reference to promote the high-value utilization of flaxseed meals.

Smart Mechanoluminescent Phosphors: A Review of Strontium-Aluminate-Based Materials, Properties, and Their Advanced Application Technologies.

Mechanoluminescence, a smart luminescence phenomenon in which light energy is directly produced by a mechanical force, has recently received significant attention because of its important applications in fields such as visible strain sensing and structural health monitoring. Up to present, hundreds of inorganic and organic mechanoluminescent smart materials have been discovered and studied. Among them, strontium-aluminate-based materials are an important class of inorganic mechanoluminescent materials for fundamental research and practical applications attributed to their extremely low force/pressure threshold of mechanoluminescence, efficient photoluminescence, persistent afterglow, and a relatively low synthesis cost. This paper presents a systematic and comprehensive review of strontium-aluminate-based luminescent materials' mechanoluminescence phenomena, mechanisms, material synthesis techniques, and related applications. Besides of summarizing the early and the latest research on this material system, an outlook is provided on its environmental, energy issue and future applications in smart wearable devices, advanced energy-saving lighting and displays.

Modulating interfacial structure and lipid digestion of natural Camellia oil body by roasting and boiling processes.

Oil body (OB) is the lipid-storage organelle in oilseed, and its stability is crucial for oilseed processing. Herein, effects of roasting and boiling on the structure, stability, and in vitro lipid digestion of Camellia OB were studied. The interfacial structure and physical stability of the extracted OB were investigated by electrophoresis, confocal-Raman spectroscopy, zeta-potential, and surface hydrophobicity, etc. Boiling caused protein loss on the OB surfaces, forming a stable phospholipid interface, which resulted in coalescence of the droplets (d > 100 µm) and negative ζ-potential (-3 âˆ¼ -8 mV) values at a pH of 2.0. However, roasting partially denatured the proteins in the seeds, which were adsorbed on the OB surfaces. The random coil structure of interfacial protein increased to ∼20 % after thermal treatment. Besides, heating decreased the surface hydrophobicity of OB and improved lipid digestion. After boiling 60 min, the extent of lipolysis increased from 41.7 % (raw) to 57.4 %.

MgF2:Mn2+: novel material with mechanically-induced luminescence.

Mechanoluminescent (ML) materials can directly convert external mechanical stimulation into light without the need for excitation from other forms of energy, such as light or electricity. This alluring characteristic makes ML materials potentially applicable in a wide range of areas, including dynamic imaging of force, advanced displays, information code, storage, and anti-counterfeiting encryption. However, current reproducible ML materials are restricted to sulfide- and oxide-based materials. In addition, most of the reported ML materials require pre-irradiation with ultraviolet (UV) lamps or other light sources, which seriously hinders their practical applications. Here, we report a novel ML material, MgF2:Mn2+, which emits bright red light under an external dynamic force without the need for pre-charging with UV light. The luminescence properties were systematically studied, and the piezophotonic application was demonstrated. More interestingly, unlike the well-known zinc sulfide ML complexes reported previously, a highly transparent ML film was successfully fabricated by incorporating MgF2:Mn2+ into polydimethylsiloxane (PDMS) matrices. This film is expected to find applications in advanced flexible optoelectronics such as integrated piezophotonics, artificial skin, athletic analytics in sports science, among others.

Self-Charging Persistent Mechanoluminescence with Mechanics Storage and Visualization Activities.

Persistent mechanoluminescence (ML) with long lifetime is highly required to break the limits of the transient emitting behavior under mechanics stimuli. However, the existing materials with persistent ML are completely trap-controlled, and a pre-irradiation is required, which severely hinders the practical applications. In this work, a novel type of ML, self-charging persistent ML, is created by compositing the Sr3 Al2 O5 Cl2 :Dy3+ (SAOCD) powders into flexible polydimethylsiloxane (PDMS) matrix. With no need for any pre-irradiation, the as-fabricated SAOCD/PDMS elastomer could exhibit intense and persistent ML under mechanics stimuli directly, which greatly facilitates its applications in mechanics lighting, displaying, imaging, and visualization. By investigating the matrix effects as well as the thermoluminescence, cathodoluminescence, and triboelectricity properties, the interfacial triboelectrification-induced electron bombardment processes are demonstrated to be responsible for the self-charged energy in  SAOCD under mechanics stimuli. Based on the unique self-charging processes, the SAOCD/PDMS further exhibits mechanics storage and visualized reading activities, which brings novel ideas and approaches to deal with the mechanics-related problems in the fields of mechanical engineering, bioengineering, and artificial intelligence.

Ultrasonic-assisted pH shift-induced interfacial remodeling for enhancing the emulsifying and foaming properties of perilla protein isolate.

In order to expand the applications of plant protein in food formulations, enhancement of its functionalities is meaningful. Herein, the effects of ultrasonic (20 KHz, 400 W, 20 min)-assisted pH shift (pH 10 and 12) treatment on the structure, interfacial behaviors, as well as the emulsifying and foaming properties of perilla protein isolate (PPI) were investigated. Results showed that the solubility of PPI treated by ultrasonic-assisted pH shift (named UPPI-10/12) exceeded 90 %, which was at least 2 and 1.4 times that of untreated PPI and ultrasound-based PPI. Meanwhile, UPPI-10/12 possessed higher foamability (increasing by at least 1.2 times) and good emulsifying stability. Ultrasonic-assisted pH shift treatment decomposed large PPI aggregates into tiny particles, evident from the dynamic light scattering (DLS) and atomic force microscopy results. Besides, this approach induced a decrease in α-helix of PPI and an increase in ß-sheet, which might result in the exposure of the hydrophobic group on the structural surface of PPI, thus leading to the increase of surface hydrophobicity. The smaller size and higher hydrophobicity endowed UPPI-10/12 faster adsorption rate, tighter interfacial structure, and higher elastic modulus at the air- and oil-water interfaces, evident from the cryo-SEM and interfacial dilatational rheological results. Thus, the emulsifying and foaming properties could evidently enhance. This study demonstrated that ultrasonic-assisted pH shift technique was a simple approach to effectively improve the functional performance of PPI.