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1.
Nat Commun ; 15(1): 3893, 2024 May 08.
Artigo em Inglês | MEDLINE | ID: mdl-38719799

RESUMO

Maintaining food safety and quality is critical for public health and food security. Conventional food preservation methods, such as pasteurization and dehydration, often change the overall organoleptic quality of the food products. Herein, we demonstrate a method that affects only a thin surface layer of the food, using beef as a model. In this method, Joule heating is generated by applying high electric power to a carbon substrate in <1 s, which causes a transient increase of the substrate temperature to > ~2000 K. The beef surface in direct contact with the heating substrate is subjected to ultra-high temperature flash heating, leading to the formation of a microbe-inactivated, dehydrated layer of ~100 µm in thickness. Aerobic mesophilic bacteria, Enterobacteriaceae, yeast and mold on the treated samples are inactivated to a level below the detection limit and remained low during room temperature storage of 5 days. Meanwhile, the product quality, including visual appearance, texture, and nutrient level of the beef, remains mostly unchanged. In contrast, microorganisms grow rapidly on the untreated control samples, along with a rapid deterioration of the meat quality. This method might serve as a promising preservation technology for securing food safety and quality.


Assuntos
Microbiologia de Alimentos , Conservação de Alimentos , Animais , Bovinos , Conservação de Alimentos/métodos , Microbiologia de Alimentos/métodos , Carne/microbiologia , Temperatura Alta , Carne Vermelha/microbiologia , Calefação , Inocuidade dos Alimentos/métodos
2.
Nat Mater ; 23(5): 579-580, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38702542
3.
Nat Nanotechnol ; 19(6): 782-791, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38499859

RESUMO

One possible solution against the accumulation of petrochemical plastics in natural environments is to develop biodegradable plastic substitutes using natural components. However, discovering all-natural alternatives that meet specific properties, such as optical transparency, fire retardancy and mechanical resilience, which have made petrochemical plastics successful, remains challenging. Current approaches still rely on iterative optimization experiments. Here we show an integrated workflow that combines robotics and machine learning to accelerate the discovery of all-natural plastic substitutes with programmable optical, thermal and mechanical properties. First, an automated pipetting robot is commanded to prepare 286 nanocomposite films with various properties to train a support-vector machine classifier. Next, through 14 active learning loops with data augmentation, 135 all-natural nanocomposites are fabricated stagewise, establishing an artificial neural network prediction model. We demonstrate that the prediction model can conduct a two-way design task: (1) predicting the physicochemical properties of an all-natural nanocomposite from its composition and (2) automating the inverse design of biodegradable plastic substitutes that fulfils various user-specific requirements. By harnessing the model's prediction capabilities, we prepare several all-natural substitutes, that could replace non-biodegradable counterparts as exhibiting analogous properties. Our methodology integrates robot-assisted experiments, machine intelligence and simulation tools to accelerate the discovery and design of eco-friendly plastic substitutes starting from building blocks taken from the generally-recognized-as-safe database.

4.
J Am Chem Soc ; 146(3): 2167-2173, 2024 Jan 24.
Artigo em Inglês | MEDLINE | ID: mdl-38214166

RESUMO

Due to the large multi-elemental space desired for property screening and optimization, high-entropy alloys (HEAs) hold greater potential over conventional alloys for a range of applications, such as structural materials, energy conversion, and catalysis. However, the relationship between the HEA composition and its local structural/elemental configuration is not well understood, particularly in noble-metal-based HEA nanomaterials, hindering the design and development of nano-HEAs in energy conversion and catalysis applications. Herein, we determined precise atomic-level structural and elemental arrangements in model HEAs composed of RhPtPdFeCo and RuPtPdFeCo to unveil their local characteristics. Notably, by changing just one constituent element in the HEA (Rh to Ru), we found dramatic changes in the elemental arrangement from complete random mixing to a local single elemental ordering feature. Additionally, we demonstrate that the local ordering in RuPtPdFeCo can be further controlled by varying the Ru concentration, allowing us to toggle between local Ru clustering and distinct heterostructures in multicomponent systems. Overall, our study presents a practical approach for manipulating local atomic structures and elemental arrangements in noble-metal-based HEA systems, which could provide in-depth knowledge to mechanistically understand the functionality of noble-metal-based HEA nanomaterials in practical applications.

5.
Nano Lett ; 24(1): 245-253, 2024 Jan 10.
Artigo em Inglês | MEDLINE | ID: mdl-38157424

RESUMO

Mechanically strong and damage-tolerant corrosion protection layers are of great technological importance. However, corrosion protection layers with high modulus (>1.5 GPa) and tensile strength (>100 MPa) are rare. Here, we report that a 130 µm thick densified wood veneer with a Young's modulus of 34.49 GPa and tensile strength of 693 MPa exhibits both low diffusivity for metal ions and the ability of self-recovery from mechanical damage. Densified wood veneer is employed as an intermediate layer to render a mechanically strong corrosion protection structure, referred to as "wood corrosion protection structure", or WCPS. The corrosion rate of low-carbon steel protected by WCPS is reduced by 2 orders of magnitude than state-of-the-art corrosion protection layers during a salt spray test. The introduction of engineered wood veneer as a thin and mechanically strong material points to new directions of sustainable corrosion protection design.

6.
Nature ; 624(7992): 564-569, 2023 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-38123807

RESUMO

Medium- and high-entropy alloys (M/HEAs) mix several principal elements with near-equiatomic composition and represent a model-shift strategy for designing previously unknown materials in metallurgy1-8, catalysis9-14 and other fields15-18. One of the core hypotheses of M/HEAs is lattice distortion5,19,20, which has been investigated by different numerical and experimental techniques21-26. However, determining the three-dimensional (3D) lattice distortion in M/HEAs remains a challenge. Moreover, the presumed random elemental mixing in M/HEAs has been questioned by X-ray and neutron studies27, atomistic simulations28-30, energy dispersive spectroscopy31,32 and electron diffraction33,34, which suggest the existence of local chemical order in M/HEAs. However, direct experimental observation of the 3D local chemical order has been difficult because energy dispersive spectroscopy integrates the composition of atomic columns along the zone axes7,32,34 and diffuse electron reflections may originate from planar defects instead of local chemical order35. Here we determine the 3D atomic positions of M/HEA nanoparticles using atomic electron tomography36 and quantitatively characterize the local lattice distortion, strain tensor, twin boundaries, dislocation cores and chemical short-range order (CSRO). We find that the high-entropy alloys have larger local lattice distortion and more heterogeneous strain than the medium-entropy alloys and that strain is correlated to CSRO. We also observe CSRO-mediated twinning in the medium-entropy alloys, that is, twinning occurs in energetically unfavoured CSRO regions but not in energetically favoured CSRO ones, which represents, to our knowledge, the first experimental observation of correlating local chemical order with structural defects in any material. We expect that this work will not only expand our fundamental understanding of this important class of materials but also provide the foundation for tailoring M/HEA properties through engineering lattice distortion and local chemical order.

7.
ACS Nano ; 17(22): 22196-22226, 2023 Nov 28.
Artigo em Inglês | MEDLINE | ID: mdl-37934794

RESUMO

The cellulose industry depends heavily on water owing to the hydrophilic nature of cellulose fibrils and its potential for sustainable and innovative production methods. The emergence of nanocellulose, with its excellent properties, and the incorporation of nanomaterials have garnered significant attention. At the nanoscale level, nanocellulose offers a higher exposure of hydroxyl groups, making it more intimate with water than micro- and macroscale cellulose fibers. Gaining a deeper understanding of the interaction between nanocellulose and water holds the potential to reduce production costs and provide valuable insights into designing functional nanocellulose-based materials. In this review, water molecules interacting with nanocellulose are classified into free water (FW) and bound water (BW), based on their interaction forces with surface hydroxyls and their mobility in different states. In addition, the water-holding capacity of cellulosic materials and various water detection methods are also discussed. The review also examines water-utilization and water-removal methods in the fabrication, dispersion, and transport of nanocellulose, aiming to elucidate the challenges and tradeoffs in these processes while minimizing energy and time costs. Furthermore, the influence of water on nanocellulose properties, including mechanical properties, ion conductivity, and biodegradability, are discussed. Finally, we provide our perspective on the challenges and opportunities in developing nanocellulose and its interplay with water.

8.
Nature ; 623(7989): 964-971, 2023 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-38030779

RESUMO

Plasmas can generate ultra-high-temperature reactive environments that can be used for the synthesis and processing of a wide range of materials1,2. However, the limited volume, instability and non-uniformity of plasmas have made it challenging to scalably manufacture bulk, high-temperature materials3-8. Here we present a plasma set-up consisting of a pair of carbon-fibre-tip-enhanced electrodes that enable the generation of a uniform, ultra-high temperature and stable plasma (up to 8,000 K) at atmospheric pressure using a combination of vertically oriented long and short carbon fibres. The long carbon fibres initiate the plasma by micro-spark discharge at a low breakdown voltage, whereas the short carbon fibres coalesce the discharge into a volumetric and stable ultra-high-temperature plasma. As a proof of concept, we used this process to synthesize various extreme materials in seconds, including ultra-high-temperature ceramics (for example, hafnium carbonitride) and refractory metal alloys. Moreover, the carbon-fibre electrodes are highly flexible and can be shaped for various syntheses. This simple and practical plasma technology may help overcome the challenges in high-temperature synthesis and enable large-scale electrified plasma manufacturing powered by renewable electricity.

9.
Science ; 382(6671): 684-691, 2023 Nov 10.
Artigo em Inglês | MEDLINE | ID: mdl-37943922

RESUMO

Passive daytime radiative cooling materials could reduce the energy needed for building cooling up to 60% by reflecting sunlight and emitting long-wave infrared (LWIR) radiation into the cold Universe (~3 kelvin). However, developing passive cooling structures that are both practical to manufacture and apply while also displaying long-term environmental stability is challenging. We developed a randomized photonic composite consisting of a microporous glass framework that features selective LWIR emission along with relatively high solar reflectance and aluminum oxide particles that strongly scatter sunlight and prevent densification of the porous structure during manufacturing. This microporous glass coating enables a temperature drop of ~3.5° and 4°C even under high-humidity conditions (up to 80%) during midday and nighttime, respectively. This radiative "cooling glass" coating maintains high solar reflectance even when exposed to harsh conditions, including water, ultraviolet radiation, soiling, and high temperatures.

10.
Nano Lett ; 23(18): 8411-8418, 2023 Sep 27.
Artigo em Inglês | MEDLINE | ID: mdl-37677149

RESUMO

Bamboo composite is an attractive candidate for structural materials in applications such as construction, the automotive industry, and logistics. However, its development has been hindered due to the use of harmful petroleum-derived synthetic adhesives or low-bonding biobased adhesives. Herein, we report a novel bioadhesion strategy based on in situ lignin bonding that can process natural bamboo into a scalable and high-performance composite. In this process, lignin bonds the cellulose fibrils into a strong network via a superstrong adhesive interface formed by hydrogen bonding and nanoscale entanglement. The resulting in situ glued-bamboo (glubam) composite exhibits a record-high shear strength of ∼4.4 MPa and a tensile strength of ∼300 MPa. This in situ lignin adhesion strategy is facile, highly scalable, and cost-effective, suggesting a promising route for fabricating strong and sustainable structural bamboo composites that sequester carbon and reduce our dependence on petrochemical-based adhesives.

11.
iScience ; 26(10): 107775, 2023 Oct 20.
Artigo em Inglês | MEDLINE | ID: mdl-37736046

RESUMO

High-entropy alloys are claimed to possess superior stability due to thermodynamic contributions. However, this statement mostly lies on a hypothetical basis. In this study, we use on-line inductively coupled plasma mass spectrometer to investigate the dissolution of five representative electrocatalysts in acidic and alkaline media and a wide potential window targeting the most important applications. To address both model and applied systems, we synthesized thin films and carbon-supported nanoparticles ranging from an elemental (Pt) sample to binary (PtRu), ternary (PtRuIr), quaternary (PtRuIrRh), and quinary (PtRuIrRhPd) alloy samples. For certain metals in the high-entropy alloy under alkaline conditions, lower dissolution was observed. Still, the improvement was not striking and can be rather explained by the lowered concentration of elements in the multinary alloys instead of the synergistic effects of thermodynamics. We postulate that this is because of dissolution kinetic effects, which are always present under electrocatalytic conditions, overcompensating thermodynamic contributions.

12.
Nat Mater ; 22(11): 1294-1303, 2023 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-37500958

RESUMO

Textiles represent a fundamental material format that is extensively integrated into our everyday lives. The quest for more versatile and body-compatible wearable electronics has led to the rise of electronic textiles (e-textiles). By enhancing textiles with electronic functionalities, e-textiles define a new frontier of wearable platforms for human augmentation. To realize the transformational impact of wearable e-textiles, materials innovations can pave the way for effective user adoption and the creation of a sustainable circular economy. We propose a repair, recycle, replacement and reduction circular e-textile paradigm. We envisage a systematic design framework embodying material selection and biofabrication concepts that can unify environmental friendliness, market viability, supply-chain resilience and user experience quality. This framework establishes a set of actionable principles for the industrialization and commercialization of future sustainable e-textile products.

13.
Nano Lett ; 23(16): 7733-7742, 2023 Aug 23.
Artigo em Inglês | MEDLINE | ID: mdl-37379097

RESUMO

Electrochemical reduction of nitrate to ammonia (NH3) converts an environmental pollutant to a critical nutrient. However, current electrochemical nitrate reduction operations based on monometallic and bimetallic catalysts are limited in NH3 selectivity and catalyst stability, especially in acidic environments. Meanwhile, catalysts with dispersed active sites generally exhibit a higher atomic utilization and distinct activity. Herein, we report a multielement alloy nanoparticle catalyst with dispersed Ru (Ru-MEA) with other synergistic components (Cu, Pd, Pt). Density functional theory elucidated the synergy effect of Ru-MEA than Ru, where a better reactivity (NH3 partial current density of -50.8 mA cm-2) and high NH3 faradaic efficiency (93.5%) is achieved in industrially relevant acidic wastewater. In addition, the Ru-MEA catalyst showed good stability (e.g., 19.0% decay in FENH3 in three hours). This work provides a potential systematic and efficient catalyst discovery process that integrates a data-guided catalyst design and novel catalyst synthesis for a range of applications.

14.
Nature ; 616(7957): 488-494, 2023 04.
Artigo em Inglês | MEDLINE | ID: mdl-37076729

RESUMO

Depolymerization is a promising strategy for recycling waste plastic into constituent monomers for subsequent repolymerization1. However, many commodity plastics cannot be selectively depolymerized using conventional thermochemical approaches, as it is difficult to control the reaction progress and pathway. Although catalysts can improve the selectivity, they are susceptible to performance degradation2. Here we present a catalyst-free, far-from-equilibrium thermochemical depolymerization method that can generate monomers from commodity plastics (polypropylene (PP) and poly(ethylene terephthalate) (PET)) by means of pyrolysis. This selective depolymerization process is realized by two features: (1) a spatial temperature gradient and (2) a temporal heating profile. The spatial temperature gradient is achieved using a bilayer structure of porous carbon felt, in which the top electrically heated layer generates and conducts heat down to the underlying reactor layer and plastic. The resulting temperature gradient promotes continuous melting, wicking, vaporization and reaction of the plastic as it encounters the increasing temperature traversing the bilayer, enabling a high degree of depolymerization. Meanwhile, pulsing the electrical current through the top heater layer generates a temporal heating profile that features periodic high peak temperatures (for example, about 600 °C) to enable depolymerization, yet the transient heating duration (for example, 0.11 s) can suppress unwanted side reactions. Using this approach, we depolymerized PP and PET to their monomers with yields of about 36% and about 43%, respectively. Overall, this electrified spatiotemporal heating (STH) approach potentially offers a solution to the global plastic waste problem.

15.
Nat Nanotechnol ; 18(2): 168-176, 2023 02.
Artigo em Inglês | MEDLINE | ID: mdl-36585515

RESUMO

Cotton textiles are ubiquitous in daily life and are also one of the primary mediums for transmitting viruses and bacteria. Conventional approaches to fabricating antiviral and antibacterial textiles generally load functional additives onto the surface of the fabric and/or their microfibres. However, such modifications are susceptible to deterioration after long-term use due to leaching of the additives. Here we show a different method to impregnate copper ions into the cellulose matrix to form a copper ion-textile (Cu-IT), in which the copper ions strongly coordinate with the oxygen-containing polar functional groups (for example, hydroxyl) of the cellulose chains. The Cu-IT displays high antiviral and antibacterial performance against tobacco mosaic virus and influenza A virus, and Escherichia coli, Salmonella typhimurium, Pseudomonas aeruginosa and Bacillus subtilis bacteria due to the antimicrobial properties of copper. Furthermore, the strong coordination bonding of copper ions with the hydroxyl functionalities endows the Cu-IT with excellent air/water retainability and superior mechanical stability, which can meet daily use and resist repeated washing. This method to fabricate Cu-IT is cost-effective, ecofriendly and highly scalable, and this textile appears very promising for use in household products, public facilities and medical settings.


Assuntos
Antivirais , Cobre , Têxteis/microbiologia , Antibacterianos , Celulose
16.
Chem Rev ; 123(5): 1843-1888, 2023 Mar 08.
Artigo em Inglês | MEDLINE | ID: mdl-36260771

RESUMO

The building sector, including building operations and materials, was responsible for the emission of ∼11.9 gigatons of global energy-related CO2 in 2020, accounting for 37% of the total CO2 emissions, the largest share among different sectors. Lowering the carbon footprint of buildings requires the development of carbon-storage materials as well as novel designs that could enable multifunctional components to achieve widespread applications. Wood is one of the most abundant biomaterials on Earth and has been used for construction historically. Recent research breakthroughs on advanced engineered wood products epitomize this material's tremendous yet largely untapped potential for addressing global sustainability challenges. In this review, we explore recent developments in chemically modified wood that will produce a new generation of engineered wood products for building applications. Traditionally, engineered wood products have primarily had a structural purpose, but this review broadens the classification to encompass more aspects of building performance. We begin by providing multiscale design principles of wood products from a computational point of view, followed by discussion of the chemical modifications and structural engineering methods used to modify wood in terms of its mechanical, thermal, optical, and energy-related performance. Additionally, we explore life cycle assessment and techno-economic analysis tools for guiding future research toward environmentally friendly and economically feasible directions for engineered wood products. Finally, this review highlights the current challenges and perspectives on future directions in this research field. By leveraging these new wood-based technologies and analysis tools for the fabrication of carbon-storage materials, it is possible to design sustainable and carbon-negative buildings, which could have a significant impact on mitigating climate change.

17.
Sci Adv ; 8(49): eadd2031, 2022 Dec 09.
Artigo em Inglês | MEDLINE | ID: mdl-36490337

RESUMO

Supramolecular frameworks have been widely synthesized for ion transport applications. However, conventional approaches of constructing ion transport pathways in supramolecular frameworks typically require complex processes and display poor scalability, high cost, and limited sustainability. Here, we report the scalable and cost-effective synthesis of an ion-conducting (e.g., Na+) cellulose-derived supramolecule (Na-CS) that features a three-dimensional, hierarchical, and crystalline structure composed of massively aligned, one-dimensional, and ångström-scale open channels. Using wood-based Na-CS as a model material, we achieve high ionic conductivities (e.g., 0.23 S/cm in 20 wt% NaOH at 25 °C) even with a highly dense microstructure, in stark contrast to conventional membranes that typically rely on large pores (e.g., submicrometers to a few micrometers) to obtain comparable ionic conductivities. This synthesis approach can be universally applied to a variety of cellulose materials beyond wood, including cotton textiles, fibers, paper, and ink, which suggests excellent potential for a number of applications such as ion-conductive membranes, ionic cables, and ionotronic devices.

18.
Nat Commun ; 13(1): 6724, 2022 Nov 07.
Artigo em Inglês | MEDLINE | ID: mdl-36344574

RESUMO

Multi-principal element alloys (MPEA) demonstrate superior synergetic properties compared to single-element predominated traditional alloys. However, the rapid melting and uniform mixing of multi-elements for the fabrication of MPEA structural materials by metallic 3D printing is challenging as it is difficult to achieve both a high temperature and uniform temperature distribution in a sufficient heating source simultaneously. Herein, we report an ultrahigh-temperature melt printing method that can achieve rapid multi-elemental melting and uniform mixing for MPEA fabrication. In a typical fabrication process, multi-elemental metal powders are loaded into a high-temperature column zone that can be heated up to 3000 K via Joule heating, followed by melting on the order of milliseconds and mixing into homogenous alloys, which we attribute to the sufficiently uniform high-temperature heating zone. As proof-of-concept, we successfully fabricated single-phase bulk NiFeCrCo MPEA with uniform grain size. This ultrahigh-temperature rapid melt printing process provides excellent potential toward MPEA 3D printing.

20.
Acc Chem Res ; 55(20): 3020-3031, 2022 Oct 18.
Artigo em Inglês | MEDLINE | ID: mdl-36173244

RESUMO

ConspectusHoley graphene (hG) is a structural derivative of graphene with arrays of through-thickness holes of a few to tens of nanometers in diameter, randomly distributed across the nanosheet surfaces. In most bulk preparation methods, the holes on hG sheets are preferentially generated from the pre-existing defects on graphene. Therefore, contrary to intuitive belief, hG is not necessarily more defective than the intact graphene. Instead, it retains essential parent properties, including high electrical conductivity, high surface area, mechanical robustness, and chemical inertness. Furthermore, the added holey structural motif imparts unique properties that are not present in unmodified graphene, making hG advantageous in numerous applications such as sensing, membranes, reinforcements, and electrochemical energy storage. In particular, the presence of holes enhances the mass transport through the nanosheet plane and thus significantly reduces tortuosity. This difference is a key advantage for using hG in energy storage applications where the transport of ions through the thickness becomes more hindered as the electrode thickness increases to meet practical energy density requirements.An unexpected discovery is that the holes of the hG sheets enable the dry hG powder to be directly compressed into robust monoliths. hG not only can be pressed into monoliths by itself but also can host other electrochemically active materials as a compressible matrix. This important yet unique property, which is not available for other carbon materials including intact graphene, significantly broadens the application horizon in energy storage applications. With the dry compressibility, electrodes with ultrahigh mass loading and thus ultrahigh areal capacity may be conveniently fabricated without toxic solvents or parasitic binders, which are required in conventional slurry-based approaches for electrode fabrication. The dry-press electrode preparation process can be completed within minutes regardless of mass loading. In comparison, high-mass-loading electrodes for advanced battery chemistries using conventional fabrication methods often need stringent and time-consuming process control. hG can also be combined with electrochemically active battery materials while maintaining dry compressibility. This has allowed the unprecedented, convenient manipulation of a wide variety of thick electrode compositions and architectures, which provides not only outstanding performance but also new physical insights for various battery chemistries.In this Account, we first present some basic observations on the dry compressibility of hG as well as the mechanistic investigations from atomistic modeling rationalizing this unique property. We then showcase the applications of neat and composite dry-pressed hG electrodes for various energy storage platforms including supercapacitors, lithium (Li) ion batteries, Li-O2 batteries, and Li-S/Se batteries. The preparation and performance of thick electrodes with practical mass loadings and unique electrode architecture manipulation, both enabled by the dry compressibility of hG, are highlighted and discussed.

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