Liquid-liquid biopolymers aqueous solution segregative phase separation in food: From fundamentals to applications-A review.

As a result of the spontaneous movement of molecules, liquid-liquid biopolymer segregative phase separation takes place in an aqueous solution. The efficacy of this type of separation can be optimized under conditions where variables such as pH, temperature, and molecular concentrations have minimal impact on its dynamics. Recently, interest in the applications of biopolymers and their segregative phase separation-associated molecular stratification has increased, particularly in the food industry, where these methods permit the purification of specific particles and the embedding of microcapsules. The present review offers a comprehensive examination of the theoretical mechanisms that regulate the liquid-liquid biopolymers aqueous solution segregative phase separation, the factors that may exert an impact on this procedure, and the importance of this particular separation method in the context of food science. These discussion points also address existing difficulties and future possibilities related to the use of segregative phase separation in food applications. This highlights the potential for the design of novel functional foods and the enhancement of food properties.

Nitrogen fertilization reduces plant diversity by changing the diversity and stability of arbuscular mycorrhizal fungal community in a temperate steppe.

Nitrogen (N) deposition resulting from anthropogenic activities poses threats to ecosystem stability by reducing plant and microbial diversity. However, the role of soil microbes, particularly arbuscular mycorrhizal fungi (AMF), as mediators of N-induced shifts in plant diversity remains unclear. In this study, we conducted 6 and 11 years of N addition field experiments in a temperate steppe to investigate AMF richness and network stability and their associations with plant species richness in response to N deposition. The N fertilization, especially in the 11 years of N addition, profoundly decreased the AMF richness and plant species richness. Furthermore, N fertilization significantly decreased the AMF network complexity and stability, with these effects becoming more enhanced with the increase in N addition duration. AMF richness and network stability showed positive associations with plant diversity, and these associations were stronger after 11 than 6 years of N addition. Our findings suggest that N deposition may lead to plant diversity loss via a reduction of AMF richness and network stability, with these effects strengthened over time. This study provides a better understanding of plant-AMF interactions and their response to the prevailing global N deposition.

Patterns of bacterial distance decay and community assembly in different land-use types as influenced by tillage management and soil layers.

Land use and cover change are major factors driving global change and greatly impact terrestrial organisms, especially soil microbial diversity. Little is known, however, about bacterial diversity, distribution patterns and assembly processes across different land use types. In this study, therefore, we conducted a large-scale field survey of 48 sampling sites, encompassing different land use types in Xuancheng city, China, with different degrees of soil disturbance and different soil horizons. The distance-decay relationships (DDRs), assembly processes and the spatial patterns of soil bacterial communities were investigated based on high-throughput sequencing data. We found that the DDRs might be weakened by anthropogenic disturbances, which were not observed in tilled soils, while a decreasing trend was observed along the soil horizon in untilled soils. The relative importance of environmental factors and geographic distance varied with soil tillage. Specifically, bacterial communities in tilled soils were driven by non-spatially autocorrelated environmental factors, while untilled soils were more susceptible to geographic distance. In addition, the heterogeneity of soil properties, as well as the differences in soil bacterial niche width and niche overlap, determined the assembly processes of the bacterial community, resulting in opposite trends along the soil layers in tilled and untilled soils. These findings expand the current understanding of the biogeography of soil bacterial communities across different land use types.

Engineering the formation of spin-defects from first principles.

The full realization of spin qubits for quantum technologies relies on the ability to control and design the formation processes of spin defects in semiconductors and insulators. We present a computational protocol to investigate the synthesis of point-defects at the atomistic level, and we apply it to the study of a promising spin-qubit in silicon carbide, the divacancy (VV). Our strategy combines electronic structure calculations based on density functional theory and enhanced sampling techniques coupled with first principles molecular dynamics. We predict the optimal annealing temperatures for the formation of VVs at high temperature and show how to engineer the Fermi level of the material to optimize the defect's yield for several polytypes of silicon carbide. Our results are in excellent agreement with available experimental data and provide novel atomistic insights into point defect formation and annihilation processes as a function of temperature.

Extremely Large Response of Phonon Coherence in Twisted Penta-NiN2 Bilayer.

Twisting has recently been demonstrated as an effective strategy for tuning the interactions between particles or quasi-particles in layered materials. Motivated by the recent experimental synthesis of pentagonal NiN2 sheet [ACS Nano 2021, 15, 13539], for the first time, the response of phonon coherence to twisting in bilayer penta-NiN2 , going beyond the particle-like phonon transport is studied. By using the unified theory of phonon transport and high order lattice anharmonicity, together with the self-consistent phonon theory, it is found that the lattice thermal conductivity is reduced by 80.6% from 33.35 to 6.47 W m-1 K-1 at 300 K when the layers are twisted. In particular, the contribution of phonon coherence is increased sharply by an order of magnitude, from 0.21 to 2.40 W m-1 K-1 , due to the reduced differences between the phonon frequencies and enhanced anharmonicity after the introduction of twist. The work provides a fundamental understanding of the phonon interaction in twisted pentagonal sheets.

Thermal Conductivity of Water at Extreme Conditions.

Measuring the thermal conductivity (κ) of water at extreme conditions is a challenging task, and few experimental data are available. We predict κ for temperatures and pressures relevant to the conditions of the Earth mantle, between 1,000 and 2,000 K and up to 22 GPa. We employ close to equilibrium molecular dynamics simulations and a deep neural network potential fitted to density functional theory data. We then interpret our results by computing the equation of state of water on a fine grid of points and using a simple model for κ. We find that the thermal conductivity is weakly dependent on temperature and monotonically increases with pressure with an approximate square-root behavior. In addition, we show how the increase of κ at high pressure, relative to ambient conditions, is related to the corresponding increase in the sound velocity. Although the relationships between the thermal conductivity, pressure and sound velocity established here are not rigorous, they are sufficiently accurate to allow for a robust estimate of the thermal conductivity of water in a broad range of temperatures and pressures, where experiments are still difficult to perform.

Phase Stability, Strong Four-Phonon Scattering, and Low Lattice Thermal Conductivity in Superatom-Based Superionic Conductor Na3OBH4.

Superatom-based superionic conductors are of current interest due to their promising applications in solid-state electrolytes for rechargeable batteries. However, much less attention has been paid to their thermal properties, which are vital for safety and performance. Motivated by the recent synthesis of superatom-based superionic conductor Na3OBH4 consisting of superhalogen cluster BH4, we systematically investigate its lattice dynamics and thermal conductivity using the density functional theory combined with a self-consistent phonon approach. We reveal the bonding hierarchy features by studying the electron localization function and potential energy surface and further unveil the rattling effect of the BH4 superatom, which introduces strong quartic anharmonicity and induces soft phonon modes in low temperatures by assisting Na displacements, thus calling for the necessity of quartic renormalization and four-phonon scattering in calculating the lattice thermal conductivity. We find that the contribution of four-phonon processes to the lattice thermal conductivity increases from 13 to 32% when the temperature rises from 200 to 400 K. At room temperature (300 K), the phonon scattering phase space is enlarged by 133% due to the four-phonon interactions, and the lattice thermal conductivity is evaluated to be 5.34 W/mK, reduced by 24% as compared with a value of 6.99 W/mK involving three-phonon scattering only. These findings provide a better understanding of the lattice stability and thermal transport properties of superionic conductor Na3OBH4, shedding light on the role of strong quartic anharmonicity played in superatom-based materials.

Microbial Community Succession Associated with Poplar Wood Discoloration.

Microbes are common inhabitants of wood, but little is known about the relationship between microbial community dynamics during wood discoloration. This study uses simulation experiments to examine the changes in the microbial communities in poplar wood at different succession stages. The composition and structure of the microbial communities changed significantly in different successional stages, with an overarching pattern of bacterial diversity decreasing and fungal diversity increasing from the early to the late successional stages. Nevertheless, succession did not affect the composition of the microbial communities at the phylum level: Proteobacteria and Acidobacteria dominated the bacterial communities, while Ascomycota and Basidiomycota dominated the fungal communities. However, at the genus level, bacterial populations of Sphingomonas and Methylobacterium, and fungal populations of Sphaeropsis were significantly more prevalent in later successional stages. Stochastic assembly processes were dominant in the early successional stages for bacteria and fungi. However, variable selection played a more critical role in the assembly processes as succession proceeded, with bacterial communities evolving towards more deterministic processes and fungal communities towards more stochastic processes. Altogether, our results suggest that bacteria and fungi exhibit different ecological strategies in poplar wood. Understanding those strategies, the resulting changes in community structures over time, and the relationship to the different stages of poplar discoloration, is vital to the biological control of that discoloration.

Holocellulosic fibers and nanofibrils using peracetic acid pulping and sulfamic acid esterification.

Cellulose provides promising alternatives to synthetic plastics to achieve a low carbon footprint and biodegradable materials, which have significant positive impacts on environmental protection and on human health. In this work, sulfated holocellulose fibers and sulfated holocellulose nanofibrils (SHCNFs) are prepared using a combination of delignification with derivatization to achieve high fiber yield, superior recycling performance, and less energy consumption of the final products by means of preserving hemicellulose. Derivatization of the surface with sulfate groups provides a further means to avoid excessive aggregation between adjacent cellulose surfaces. Interestingly, hemicellulose increases the accessibility of holocellulose fibers and reduces the embodied energy during sulfate esterification. The presence of hemicellulose imparts high optical transmittance, mechanical performance (ultimate strength, 390 MPa; Young's modulus, 33 GPa), and recyclability for SHCNFs. This combination of two treatments can unlock the greater potential of cellulose as a sustainable material over its entire life cycle.

Holocellulose nanofibrils assisted exfoliation of boron nitride nanosheets for thermal management nanocomposite films.

High-quality boron nitride nanosheets (BNNSs) were exfoliated via eco-friendly holocellulose nanofibrils (HCNFs) assisted ultrasound treatment in water. The resultant H-BNNSs possessed high yields (23.4%), few surface defects, a high aspect ratio (~134), and excellent dispersibility in water (Zeta potential, -53.5 mV). Furthermore, H-BNNSs were functionalized by liquid metal (Gallium, Ga) dominated interface engineering and assembled with cellulose fibers into Ga@H-BNNSs filled nanocomposite films. Owing to the well-designed interface engineering, the obtained nanocomposite films exhibited outstanding integrated performance, especially excellent in-plane thermal conductivity (11.78 W m-1 K-1), and had great potential in the thermal management of flexible electronics.

Facile preparation of lignin-containing cellulose nanofibrils from sugarcane bagasse by mild soda-oxygen pulping.

Lignin-containing cellulose nanofibrils (LCNFs) with tunable lignin contents from sugarcane bagasse were directly prepared by low-temperature soda­oxygen pulping combined with simple mechanical treatment. The residual lignin structure, morphology and physical dimensions of LCNFs, and properties of the relevant cellulose nanopapers (CNPs) were investigated. In situ 2D Heteronuclear Single Quantum Coherence (HSQC) NMR spectra showed ß-O-4 linkages, ferulate, and para-coumarate were well preserved in the LCNFs. Compared with the cellulose nanofibrils (CNFs), LCNFs displayed a more uniform size and narrow diameter distribution. The corresponding CNPs exhibited outstanding mechanical properties (tensile strength reached 152.9 MPa), and excellent combined optical properties both in the UV blocking and visible light transparency. Moreover, the water contact angles (50.0-80.2°) of LCNFs were much higher than that of CNFs (21.7°). Direct preparation of LCNFs under mild condition would unlock the full potential of cellulosic materials and provide enhanced opportunities for cellulose to fabricate multi-functional and high-value materials.

Photoelectron spectra of water and simple aqueous solutions at extreme conditions.

Determining the electronic structure of aqueous solutions at extreme conditions is an important step towards understanding chemical bonding and reactions in water under pressure (P) and at high temperature (T). We present calculations of the photoelectron spectra of water and a simple solution of NaCl under pressure at conditions relevant to the Earth's interior (11 GPa and 1000 K). We combine first-principles and deep-potential molecular dynamics with electronic structure calculations with dielectric-dependent hybrid functionals. These functionals are defined with a fraction of exact exchange determined from the dielectric constant of the liquid computed in extreme conditions. We find a broadening of the spectra relative to ambient conditions, particularly prominent in the merging of the two main peaks below the onset of the spectra. Furthermore we find an overall red shift at high pressure and temperature, which is however not constant over the whole energy range and varies between 1.1 and 2.4 eV. Our results also show that the anion energy levels are closer to the valence band maximum of the liquid than at ambient conditions, indicating that as P and T are increased, the defect levels of Cl- and OH- in water may eventually lie below the valence band maximum of water. Finally, we characterize the ionization potential of hydrated species deriving from rapid water dissociation, e.g. hydrated hydroxide and hydronium, and we elucidate the electronic states associated with proton transfer events at high pressure. Our results represent a first, important step in predicting the electronic properties of solutions in super-critical conditions.

Response of Fungal Sub-Communities in a Maize-Wheat Rotation Field Subjected to Long-Term Conservation Tillage Management.

Conservation tillage is an advanced agricultural technology that seeks to minimize soil disturbance by reducing, or even eliminating tillage. Straw or stubble mulching in conservation tillage systems help to increase crop yield, maintain biodiversity and increase levels of exogenous nutrients, all of which may influence the structure of fungal communities in the soil. Currently, however, the assembly processes and co-occurrence patterns of fungal sub-communities remain unknown. In this paper, we investigated the effects of no-tillage and straw mulching on the composition, assembly process, and co-occurrence patterns of soil fungal sub-communities in a long-term experimental plot (15 years). The results revealed that combine straw mulching with no-tillage significantly increased the richness of fungi but not their diversity. Differential abundance analysis and principal component analysis (PCA) indicated that tillage management had a greater effect on the fungal communities of abundant and intermediate taxa than on the rare taxa. Available phosphorus (AP) and total nitrogen (TN) were the major determinants of fungal sub-communities in NT treatment. The abundant fungal sub-communities were assembled by deterministic processes under medium strength selection, while strong conservation tillage strength shifts the abundant sub-community assembly process from deterministic to stochastic. Overall, the investigation of the ecological network indicated that no-tillage and straw mulching practices decreased the complexity of the abundant and intermediate fungal networks, while not significantly influencing rare fungal networks. These findings refine our knowledge of the response of fungal sub-communities to conservation tillage management techniques and provide new insights into understanding fungal sub-community assembly.

Lithium Bonds Enable Small Biomass Molecule-Based Ionoelastomers with Multiple Functions for Soft Intelligent Electronics.

Lipoic acid (LA), which originates from animals and plants, is a small biomass molecule and has recently shown great application value in soft conductors. However, the severe depolymerization of LA places a significant limitation on its utilization. A strategy of using Li-bonds as both depolymerization quenchers and dynamic mediators to melt transform LA into high-performance ionoelastomers (IEs) is proposed. They feature dry networks while simultaneously combining transparency, stretchability, conductivity, self-healing ability, non-corrosive property, re-mouldability, strain-sensitivity, recyclability, and degradability. Most of the existing soft conductors' drawbacks, such as the tedious synthesis, non-renewable polymer networks, limited functions, and single-use only, are successfully solved. In addition, the multi-functions allow IEs to be used as soft sensors in human-computer interactive games and wireless remote sports assistants. Notably, the recycled IE also provides an efficient conductive filler for transparent ionic papers, which can be used to design soft transparent triboelectric nanogenerators for energy harvesting and multidirectional motion sensing. This work creates a new direction for future research involving intelligent soft electronics.

Four-Phonon Scattering Effect and Two-Channel Thermal Transport in Two-Dimensional Paraelectric SnSe.

In recent years, increased attention has been paid to the study of four-phonon interactions and diffusion transport in three-dimensional (3D) thermoelectric materials because they play an essential role in understanding the thermal transport process. In this work, we study four-phonon scattering and diffusion transport in two-dimensional (2D) thermoelectric materials using the paraelectric phase of 2D SnSe as an example. The inherent soft phonon modes are treated by the self-consistent phonon theory, which considers the temperature-induced renormalization of the phonons. Based on density functional theory and the Peierls-Boltzmann transport equation for phonons, we show that the four-phonon interactions can reduce the thermal conductivity of the 2D SnSe sheet by nearly 40% due to the collapse of soft optical modes, and the contribution of diffusion transport to the total thermal conductivity accounts for 14% at a high temperature of 800 K due to the short phonon mean free path approaching the Ioffe-Regel limit, suggesting the two-channel transport in this system. The results are further confirmed by using the machine learning-assisted molecular dynamics simulations. This work provides a new insight into the physical mechanisms for thermal transport in 2D systems with strong anharmonic effects.

High strength holocellulose paper from bamboo as biodegradable packaging tape.

As the fast-growing of package business in express delivery industry, replacing traditional scotch tapes with degradable materials has attracted extensive attention. Herein, holocellulose paper (H-paper) was prepared by an efficient delignification and papermaking process from bamboo. The structure and properties of resultant holocellulose fibers and H-paper were characterized and compared with those from other pulping methods, such as Kraft pulping, enzyme treated, sulfite and alkaline sulfite process. The yield of holocellulose pulp (55%) increased by about 10% compared with that of other fibers. Compared to that of Kraft paper (38 MPa), the strength of H-paper increased by nearly 60% at similar density, reaching a maximum of 65 MPa. The total transmittance of H-paper was about 20% higher than Kraft paper. Moreover, H-papers displayed high mechanical properties, good printability, and degradability, which was important for the application as paper tape.

Holocellulose nanofibrils assisted exfoliation to prepare MXene-based composite film with excellent electromagnetic interference shielding performance.

A high-yield and straightforward method is proposed to obtain an electromagnetic interference (EMI) shielding film based on multilayered Ti3C2Tx (m-Ti3C2Tx). Holocellulose nanofibrils modified by sulfamic acid (SHCNF) with unique "core-shell" structure can act as a dispersant and a binder to assist in exfoliating m-Ti3C2Tx into delaminated-Ti3C2Tx (d-Ti3C2Tx) and fabricate flexible Ti3C2Tx/SHCNF composite films with a high-yield value. The "brick-and-mortar" composite films exhibit a superior electromagnetic interference (EMI) shielding effectiveness (SE) of 45.02 dB with an ultrathin thickness of 40 µm at the 12.4 GHz. Moreover, these flexible and strong integrated Ti3C2Tx/SHCNF composite films also display excellent specific EMI SE of SSE/t (4437 dB cm2 g-1) and high EMI shielding efficiency (99.996%). Therefore, the SHCNF-assisted method provides a cost-effective approach to fabricate a strong and flexible MXene-based nanocomposite films toward EMI shielding application.

Holocellulose Nanofibril-Assisted Intercalation and Stabilization of Ti3C2Tx MXene Inks for Multifunctional Sensing and EMI Shielding Applications.

2D transition-metal carbide/nitride (MXene)-based conductive inks have received tremendous attention due to their high electrical conductivity and other fascinating properties. However, the unstability of MXene-based inks, low fabrication yield of MXene flakes, and poor mechanical properties of printed products strongly limit the proper and large-scale printing of MXene patterns. Here, functioning as a dispersant, an intercalation agent, and reinforcement, sulfated holocellulose nanofibrils (HCNFs) with a unique "core-shell" structure are conducive to the fabrication, storage, and subsequent printing of MXene inks. The MXene/HCNF (MH) ink with high yield (97.2%), good stability, and good homogeneity exhibits excellent printing performance (high resolution and good coverage). It could print various products with adjustable thicknesses and electrical conductivity properties on different substrates. The products printed by the MH ink can be applied as multifunctional sensing materials responding to multiple external stimuli, such as stress/strain, blowing, humidity, and temperature. Furthermore, the resulting products also display a high electromagnetic interference (EMI) shielding effectiveness (SE) of 54.3 dB at a shallow thickness of 100 µm and an excellent specific EMI SE of SSE/t of 7159 dB cm2 g-1.

Recent progress in cellulose-based electrospun nanofibers as multifunctional materials.

Cellulose, the most abundant natural polymer, has good biocompatibility, biodegradability, and non-toxicity, which make it and its derivatives promising candidates for the fabrication of multifunctional materials, while maintaining sustainability and environmental friendliness. The combination of electrospinning technology and cellulose (and its derivatives) provides a feasible approach to produce nanostructured porous materials with promising functionalities, flexibility, renewability and biodegradability. At the same time, it enables value-added applications of cellulose and its derivatives that are derived from nature or even biomass waste. This review summarizes and discusses the latest progress in cellulose-based electrospun nanofibers, including their construction methods and conditions, various available raw materials, and applications in multiple areas (water treatment, biomaterials, sensors, electro-conductive materials, active packaging, and so on), which are followed by the conclusion and prospects associated with future opportunities and challenges in this active research area.

Long-term nitrogen fertilization shaped the nifH, nirK, and nosZ gene community patterns in red paddy soil in south China.

To understand the diversities of diazotrophs and denitrifiers in red paddy soil under long-term fertilization conditions, nifH, nirK, and nosZ libraries were constructed by PCR-RFLP. nirK gene diversity proved to be lower than that of nosZ and nifH, and nirK and nosZ genes were more sensitive to different fertilization treatments than the nifH gene was. The 3 libraries were dominated by diverse microbes, including the Alpha, Beta, Gamma, and Delta subclasses of the Proteobacteria. Long-term addition of urea with straw mulch and azophoska increased the abundance of nonsymbiotic diazotrophs, which indicated that nonsymbiotic diazotrophs were responsible for the majority of the nitrogen-fixing ability in paddy soil. In addition, a potential link between nifH and nosZ was found due to the existence of nitrogen fixers, such as Bradyrhizobium and Ralstonia, in the nosZ library. The main chemical factors affecting the 3 genes were identified: pH was the most important factor of the nifH community; the nirK gene was more affected by pH and organic matter; available potassium and the carbon-to-nitrogen ratio significantly influenced the community structure of the nosZ gene.