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

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.


Food Microbiology , Food Preservation , Animals , Cattle , Food Preservation/methods , Food Microbiology/methods , Meat/microbiology , Hot Temperature , Red Meat/microbiology , Heating , Food Safety/methods
2.
Nat Mater ; 23(5): 579-580, 2024 May.
Article En | MEDLINE | ID: mdl-38702542
3.
Nature ; 623(7989): 964-971, 2023 Nov.
Article En | MEDLINE | ID: mdl-38030779

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.

4.
Nat Commun ; 13(1): 6724, 2022 Nov 07.
Article En | MEDLINE | ID: mdl-36344574

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.

6.
Nature ; 605(7910): 470-476, 2022 05.
Article En | MEDLINE | ID: mdl-35585339

Conventional thermochemical syntheses by continuous heating under near-equilibrium conditions face critical challenges in improving the synthesis rate, selectivity, catalyst stability and energy efficiency, owing to the lack of temporal control over the reaction temperature and time, and thus the reaction pathways1-3. As an alternative, we present a non-equilibrium, continuous synthesis technique that uses pulsed heating and quenching (for example, 0.02 s on, 1.08 s off) using a programmable electric current to rapidly switch the reaction between high (for example, up to 2,400 K) and low temperatures. The rapid quenching ensures high selectivity and good catalyst stability, as well as lowers the average temperature to reduce the energy cost. Using CH4 pyrolysis as a model reaction, our programmable heating and quenching technique leads to high selectivity to value-added C2 products (>75% versus <35% by the conventional non-catalytic method and versus <60% by most conventional methods using optimized catalysts). Our technique can be extended to a range of thermochemical reactions, such as NH3 synthesis, for which we achieve a stable and high synthesis rate of about 6,000 µmol gFe-1 h-1 at ambient pressure for >100 h using a non-optimized catalyst. This study establishes a new model towards highly efficient non-equilibrium thermochemical synthesis.

7.
Nano Lett ; 22(10): 3931-3938, 2022 05 25.
Article En | MEDLINE | ID: mdl-35503740

Conventional plastic foams are usually produced by fossil-fuel-derived polymers, which are difficult to degrade in nature. As an alternative, cellulose is a promising biodegradable polymer that can be used to fabricate greener foams, yet such a process typically relies on methods (e.g., freeze-drying and supercritical-drying) that are hardly scalable and time-consuming. Here, we develop a fast and scalable approach to prepare cellulose-graphite foams via rapidly cross-linking the cellulose fibrils in metal ions-containing solution followed by ambient drying. The prepared foams exhibit low density, high compressive strength, and excellent water stability. Moreover, the cross-linking of the cellulose fibrils can be triggered by various metal ions, indicating good universality. We further use density functional theory to reveal the cross-linking effect of different ions, which shows good agreement with our experimental observation. Our approach presents a sustainable route toward low-cost, environmentally friendly, and scalable foam production for a range of applications.


Cellulose , Graphite , Ions , Polymers , Water
8.
Small ; 18(17): e2107951, 2022 Apr.
Article En | MEDLINE | ID: mdl-35355404

Silica glasses have wide applications in industrial fields due to their extraordinary properties, such as high transparency, low thermal expansion coefficient, and high hardness. However, current methods of fabricating silica glass generally require long thermal treatment time (up to hours) and complex setups, leading to high cost and slow manufacturing speed. Herein, to obtain high-quality glasses using a facile and rapid method, an ultrafast high-temperature sintering (UHS) technique is reported that requires no additional pressure. Using UHS, silica precursors can be densified in seconds due to the large heating rate (up to 102 K s-1 ) of closely placed carbon heaters. The typical sintering time is as short as ≈10 s, ≈1-3 orders of magnitude faster than other methods. The sintered glasses exhibit relative densities of > 98% and high visible transmittances of ≈90%. The powder-based sintering process also allows rapid doping of metal ions to fabricate colored glasses. The UHS is further extended to sinter other functional glasses such as indium tin oxide (ITO)-doped silica glass, and other transparent ceramics such as Gd-doped yttrium aluminum garnet. This study demonstrates an UHS proof-of-concept for the rapid fabrication of high-quality glass and opens an avenue toward rapid discovery of transparent materials.

9.
Small ; 18(11): e2104761, 2022 Mar.
Article En | MEDLINE | ID: mdl-35049145

High-entropy nanoparticles have received notable attention due to their tunable properties and broad material space. However, these nanoparticles are not suitable for certain applications (e.g., battery electrodes), where their microparticle (submicron to micron) counterparts are more preferred. Conventional methods used for synthesizing high-entropy nanoparticles often involve various ultrafast shock processes. To increase the size thereby achieving high-entropy microparticles, longer reaction time (e.g., heating duration) is usually used, which may also lead to undesired particle overgrowth or even densified microstructures. In this work, an approach based on Joule heating for synthesizing high-entropy oxide (HEO) microparticles with uniform elemental distribution is reported. In particular, two key synthesis conditions are identified to achieve high-quality HEO microparticles: 1) the precursors need to be loosely packed to avoid densification; 2) the heating time needs to be accurately controlled to tens of seconds instead of using milliseconds (thermal shock) that leads to nanoparticles or longer heating duration that forms bulk structures. The utility of the synthesized HEO microparticles for a range of applications, including high-performance Li-ion battery anode and water oxidation catalyst. This study opens up a new door toward synthesizing high-entropy microparticles with high quality and broad material space.

10.
Sci Adv ; 8(4): eabm4322, 2022 Jan 28.
Article En | MEDLINE | ID: mdl-35089780

Nanoscale multi-principal element intermetallics (MPEIs) may provide a broad and tunable compositional space of active, high-surface area materials with potential applications such as catalysis and magnetics. However, MPEI nanoparticles are challenging to fabricate because of the tendency of the particles to grow/agglomerate or phase-separated during annealing. Here, we demonstrate a disorder-to-order phase transition approach that enables the synthesis of ultrasmall (4 to 5 nm) and stable MPEI nanoparticles (up to eight elements). We apply just 5 min of Joule heating to promote the phase transition of the nanoparticles into L10 intermetallic structure, which is then preserved by rapidly cooling. This disorder-to-order transition results in phase-stable nanoscale MPEIs with compositions (e.g., PtPdAuFeCoNiCuSn), which have not been previously attained by traditional synthetic methods. This synthesis strategy offers a new paradigm for developing previously unexplored MPEI nanoparticles by accessing a nanoscale-size regime and novel compositions with potentially broad applications.

11.
Adv Mater ; 34(9): e2106436, 2022 Mar.
Article En | MEDLINE | ID: mdl-34875115

Multi-elemental alloy (MEA) nanoparticles have recently received notable attention owing to their high activity and superior phase stability. Previous syntheses of MEA nanoparticles mainly used carbon as the support, owing to its high surface area, good electrical conductivity, and tunable defective sites. However, the interfacial stability issue, such as nanoparticle agglomeration, remains outstanding due to poor interfacial binding between MEA and carbon. Such a problem often causes performance decay when MEA nanoparticles are used as catalysts, hindering their practical applications. Herein, an interface engineering strategy is developed to synthesize MEA-oxide-carbon hierarchical catalysts, where the oxide on carbon helps disperse and stabilize the MEA nanoparticles toward superior thermal and electrochemical stability. Using several MEA compositions (PdRuRh, PtPdIrRuRh, and PdRuRhFeCoNi) and oxides (TiO2 and Cr2 O3 ) as model systems, it is shown that adding the oxide renders superior interfacial stability and therefore excellent catalytic performance. Excellent thermal stability is demonstrated under transmission electron microscopy with in situ heating up to 1023 K, as well as via long-term cycling (>370 hours) of a Li-O2 battery as a harsh electrochemical condition to challenge the catalyst stability. This work offers a new route toward constructing efficient and stable catalysts for various applications.

12.
Nano Lett ; 22(1): 255-262, 2022 01 12.
Article En | MEDLINE | ID: mdl-34932367

Chemically ordered intermetallic nanoparticles are promising candidates for energy-related applications such as electrocatalysis. However, the synthesis of intermetallics generally requires long annealing (several hours) to achieve the ordered structure, which causes nanoparticles agglomeration and diminished performance, particularly for catalysis. Herein, we demonstrate a new rapid Joule heating approach that can synthesize highly ordered and well-dispersed intermetallic nanoparticles. As a proof-of-concept, we synthesized fully ordered Pd3Pb intermetallic nanoparticles that feature small size distribution (∼6 nm). Computational analysis of the L12 Pd3Pb material suggests that this rapid atomic ordering transformation can be attributed to a vacancy-mediated diffusion mechanism. Moreover, the nanoparticles demonstrate excellent electrocatalytic activity and exceptional stability for the oxygen reduction reaction (ORR), retaining >95% of the current density over 10 h of chronoamperometry test with negligible structural and compositional changes. This study demonstrates a new strategy of providing a new direction for intermetallic synthesis and catalyst discovery.


Nanoparticles , Catalysis
13.
ACS Nano ; 15(9): 14928-14937, 2021 Sep 28.
Article En | MEDLINE | ID: mdl-34423972

High entropy alloy nanoparticles (HEA-NPs) are reported to have superior performance in catalysis, energy storage, and conversion due to the broad range of elements that can be incorporated in these materials, enabling tunable activity, excellent thermal and chemical stability, and a synergistic catalytic effect. However, scaling the manufacturing of HEA-NPs with uniform particle size and homogeneous elemental distribution efficiently is still a challenge due to the required critical synthetic conditions where high temperature is typically involved. In this work, we demonstrate an efficient and scalable microwave heating method using carbon-based materials as substrates to fabricate HEA-NPs with uniform particle size. Due to the abundant functional group defects that can absorb microwave efficiently, reduced graphene oxide is employed as a model substrate to produce an average temperature reaching as high as ∼1850 K within seconds. As a proof-of-concept, we utilize this rapid, high-temperature heating process to synthesize PtPdFeCoNi HEA-NPs, which exhibit an average particle size of ∼12 nm and uniform elemental mixing resulting from decomposition nearly at the same time and liquid metal solidification without diffusion. Various carbon-based materials can also be employed as substrates, including one-dimensional carbon nanofibers and three-dimensional carbonized wood, which can achieve temperatures of >1400 K. This facile and efficient microwave heating method is also compatible with the roll-to-roll process, providing a feasible route for scalable HEA-NPs manufacturing.

14.
Adv Mater ; 33(34): e2100726, 2021 Aug.
Article En | MEDLINE | ID: mdl-34288146

Solid-state batteries (SSBs) promise better safety and potentially higher energy density than the conventional liquid- or gel-based ones. In practice, the implementation of SSBs often necessitates 3D porous scaffolds made by ceramic solid-state electrolytes (SSEs). Herein, a general and facile method to sinter 3D porous scaffolds with a range of ceramic SSEs on various substrates at high temperature in seconds is reported. The high temperature enables rapid reactive sintering toward the desired crystalline phase and expedites the surface diffusion of grains for neck growth; meanwhile, the short sintering duration limits the coarsening, thus accurately controlling the degree of densification to preserve desired porous structures, as well as reducing the loss of volatile elements. As a proof-of-concept, a composite SSE with a good ionic conductivity (i.e., ≈1.9 × 10-4 S cm-1 at room temperature) is demonstrated by integrating poly(ethylene oxide) with the 3D porous Li6.5 La3 Zr1.5 Ta0.5 O12 scaffold sintered by this method. This method opens a new door toward sintering a variety of ceramic-SSE-based 3D scaffolds for all-solid-state battery applications.

15.
Nano Lett ; 21(11): 4517-4523, 2021 Jun 09.
Article En | MEDLINE | ID: mdl-34018760

The conventional thermal treatment systems typically feature low ramping/cooling rates, which lead to steep thermal gradients that generate inefficient, nonuniform reaction conditions and result in nanoparticle aggregation. Herein, we demonstrate a continuous fly-through material synthesis approach using a novel high-temperature reactor design based on the emerging thermal-shock technology. By facing two sheets of carbon paper with a small distance apart (1-3 mm), uniform and ultrahigh temperatures can be reached up to 3200 K within 50 ms by simply applying a voltage of 15 V. The raw materials can be continuously fed through the device, allowing the final products to be rapidly collected. As a proof-of-concept demonstration, we synthesized Pt nanocatalysts (∼4 nm) anchored on carbon black via this reactor at ∼1400 K. Furthermore, we find it features excellent electrocatalytic activities toward methanol oxidation reaction. This work offers a highly efficient platform for nanomaterials synthesis at high temperatures.

16.
Small ; 17(18): e2008011, 2021 05.
Article En | MEDLINE | ID: mdl-33759326

The huge consumption of single-use plastic straws has brought a long-lasting environmental problem. Paper straws, the current replacement for plastic straws, suffer from drawbacks, such as a high cost of the water-proof wax layer and poor water stability due to the easy delamination of the wax layer. It is therefore crucial to find a high-performing alternative to mitigate the environmental problems brought by plastic straws. In this paper, all natural, degradable, cellulose-lignin reinforced composite straws, inspired by the reinforcement principle of cellulose and lignin in natural wood are developed. The cellulose-lignin reinforced composite straw is fabricated by rolling up a wet film made of homogeneously mixed cellulose microfibers, cellulose nanofibers, and lignin powders, which is then baked in oven at 150 °C. When baked, lignin melts and infiltrates the micro-nanocellulose network, acting as a polyphenolic binder to improve the mechanical strength and hydrophobicity performance of the resulting straw. The obtained straws demonstrate several advantageous properties over paper straws, including 1) excellent mechanical performance, 2) high hydrostability, and 3) low cost. Moreover, the natural degradability of the cellulose-lignin reinforced composite straws makes them promising candidates to replace plastic straws and suggests possible substitutes for other petroleum-based plastics.


Lignin , Nanofibers , Cellulose , Hydrophobic and Hydrophilic Interactions , Wood
17.
Sci Adv ; 7(5)2021 Jan.
Article En | MEDLINE | ID: mdl-33571122

Transparent wood is considered a promising structural and light management material for energy-efficient engineering applications. However, the solution-based delignification process that is used to fabricate transparent wood generally consumes large amounts of chemicals and energy. Here, we report a method to produce optically transparent wood by modifying the wood's lignin structure using a solar-assisted chemical brushing approach. This method preserves most of the lignin to act as a binder, providing a robust wood scaffold for polymer infiltration while greatly reducing the chemical and energy consumption as well as processing time. The obtained transparent wood (~1 mm in thickness) demonstrates a high transmittance (>90%), high haze (>60%), and excellent light-guiding effect over visible wavelength. Furthermore, we can achieve diverse patterns directly on wood surfaces using this approach, which endows transparent wood with excellent patternability. Combining its efficient, patternable, and scalable production, this transparent wood is a promising candidate for applications in energy-efficient buildings.

18.
Adv Mater ; 33(8): e2001588, 2021 Feb.
Article En | MEDLINE | ID: mdl-33470483

Lignin serves as a binder that forms strong matrices of the cell walls of wood. However, it has many photolabile chromophore groups that create a monotonic brownish color and make wood susceptible to photodegradation. Herein, a new strategy is reported for modifying lignin using an in situ, rapid, and scalable process that involves the photocatalytic oxidation of native lignin in wood by H2 O2 and UV light. The reaction selectively eliminates lignin's chromophores while leaving the aromatic skeleton intact, thus modulating the optical properties of wood. The resulting "photonic wood" retains ≈80% of its original lignin content, which continues to serve as a strong binder and water-proofing agent. As a result, photonic wood features a much higher mechanical strength in a wet environment (20-times higher tensile strength and 12-times greater compression resistance), significant scalability (≈2 m long sample), and largely reduced processing times (1-6.5 h vs 4-14 h) compared with delignification methods. Additionally, this in situ lignin-modified wood structure is easily patterned through a photocatalytic oxidation process. This photocatalytic production of photonic wood paves the way for the large-scale manufacturing of sustainable biosourced functional materials for a range of applications, including energy-efficient buildings, optical management, and fluidic, ionic, electronic, and optical devices.

19.
Adv Mater ; 32(46): e2002853, 2020 Nov.
Article En | MEDLINE | ID: mdl-33020998

Mixing multimetallic elements in hollow-structured nanoparticles is a promising strategy for the synthesis of highly efficient and cost-effective catalysts. However, the synthesis of multimetallic hollow nanoparticles is limited to two or three elements due to the difficulties in morphology control under the harsh alloying conditions. Herein, the rapid and continuous synthesis of hollow high-entropy-alloy (HEA) nanoparticles using a continuous "droplet-to-particle" method is reported. The formation of these hollow HEA nanoparticles is enabled through the decomposition of a gas-blowing agent in which a large amount of gas is produced in situ to "puff" the droplet during heating, followed by decomposition of the metal salt precursors and nucleation/growth of multimetallic particles. The high active sites per mass ratio of such hollow HEA nanoparticles makes them promising candidates for energy and electrocatalysis applications. As a proof-of-concept, it is demonstrated that these materials can be applied as the cathode catalyst for Li-O2 battery operations with a record-high current density per catalyst mass loading of 2000 mA gcat. -1 , as well as good stability and durable catalytic activity. This work offers a viable strategy for the continuous manufacturing of hollow HEA nanomaterials that can find broad applications in energy and catalysis.

20.
Adv Mater ; 32(46): e2005059, 2020 Nov.
Article En | MEDLINE | ID: mdl-33051910

The discovery of new solid-state electrolytes (SSEs) can be guided by computation for next-generation Li batteries toward higher energy density and better safety. However, conventional synthetic methods often suffer from severe loss of Li and poor material quality, therefore preventing the promise of the predicted SSE candidates to be realized. In this study, computationally predicted SSEs with desirable material quality are synthesized via an ultrafast sintering technique. Three new garnet-type Li+ conductors, including Li6.5 Nd3 Zr1.5 Ta0.5 O12 (LNZTO), Li6.5 Sm3 Zr1.5 Ta0.5 O12 (LSZTO), and Li6.5 (Sm0.5 La0.5 )3 Zr1.5 Ta0.5 O12 (L-LSZTO), are screened by density functional theory to exhibit good synthesizability and stability. The ultrafast sintering method by Joule heating effectively shorten the sintering time from several hours to <25 s, thereby reducing the Li loss and effectively merging the grains toward high material quality. In agreement with the computational prediction, LNZTO demonstrates the best synthesizability and phase stability, thereby achieving the highest conductivity of 2.3 × 10-4 S cm-1 among the three new SSE candidates. Using a current density of 0.2 mA cm-2 , the Li/LNZTO/Li symmetric cell can cycle for ≈90 h without obvious increase of overpotentials. This study showcases the successful realization of computational predictions by the ultrafast sintering technique for the rapid optimization and screening of high-performance SSEs.

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