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1.
Adv Mater ; : e2403876, 2024 May 13.
Article in English | MEDLINE | ID: mdl-38739951

ABSTRACT

Sorption-based atmospheric water harvesting is an attractive technology for exploiting unconventional water sources. A critical challenge is how to facilitate fast and continuous collection of potable water from air. Here, a bio-based gel (CAL gel), resulting from the integration of a whole biomass-derived polymer network with lithium chloride is reported. A fast adsorption/desorption kinetics, with a water capture rate of 1.74 kg kg-1 h-1 at 30% relative humidity and a desorption rate of 1.98 kg kg-1 h-1, was simultaneously realized in one piece of CAL gel, because of its strong hygroscopicity, hydrophilic network, abundant water transport channels, photothermal conversion ability, and ∼200-µm-thick self-supporting bulky structure caused by multicomponent synergy. A solar-driven, drum-type, tunable, and portable harvester is designed that can harvest atmospheric water within a brief time. Under outdoor conditions, the harvester with CAL gels operates 36 switches (180°) per day realizes a water yield of 8.96 kg kggel -1 (18.87 g kgdevice -1). This portable harvester highlights the potential for fast and scalable atmospheric water harvesting in extreme environments. This article is protected by copyright. All rights reserved.

2.
Langmuir ; 40(15): 7982-7991, 2024 Apr 16.
Article in English | MEDLINE | ID: mdl-38569012

ABSTRACT

In this study, we explored an innovative application of heat-assisted solution electrospinning, a technique that significantly advances the control of phase separation in polystyrene (PS) fibers. Our experimental approach involved the use of direct heating and a convection air sheath applied through a coaxial needle, focusing on solvents with varying vapor pressures. This method enabled a detailed investigation into how solvent evaporation rates affect the morphology of the electrospun fibers. SEM and AFM measurements revealed that the application of direct heating and a heated air sheath offered precise control over the fiber morphology, significantly influencing both the surface and internal structure of the fibers. Additionally, we observed notable changes in fiber diameter, indicating that heat-assisted electrospinning can be effectively utilized to tailor fiber dimensions according to specific application requirements. Moreover, our research demonstrated the critical role of solvent properties, particularly vapor pressure, in determining the final characteristics of the electrospun fibers. By comparing fibers produced with different solvents, we gained insights into the complex interplay between solvent dynamics and heat application in fiber formation. The implications of these findings are far-reaching, offering new possibilities for the fabrication of nanofibers with customized properties. Furthermore, this could have profound impacts on various applications, from biomedical to environmental, where specific fiber characteristics are crucial. This study not only contributes to the understanding of phase separation in electrospinning but also opens avenues for further research on the optimization of fiber properties for diverse industrial and scientific applications.

3.
Adv Mater ; 36(12): e2209479, 2024 Mar.
Article in English | MEDLINE | ID: mdl-36652538

ABSTRACT

The effective management of atmospheric water will create huge value for mankind. Diversified and sustainable biopolymers that are derived from organisms provide rich building blocks for various hygroscopic materials. Here, a comprehensive review of recent advances in developing biopolymers for hygroscopic materials is provided. It is begun with a brief introduction of species diversity and the processes of obtaining various biopolymer materials from organisms. The fabrication of hygroscopic materials is then illustrated, with a specific focus on the use of biopolymer-derived materials as substrates to produce composites and the use of biopolymers as building blocks to fabricate composite gels. Next, the representative applications of biopolymer-derived hygroscopic materials for dehumidification, atmospheric water harvesting, and power generation are systematically presented. An outlook on future challenges and key issues worthy of attention are finally provided.

4.
Adv Mater ; 36(1): e2306653, 2024 Jan.
Article in English | MEDLINE | ID: mdl-37696052

ABSTRACT

Hygroscopic salt-based composite sorbents are considered ideal candidates for solar-driven atmospheric water harvesting. The primary challenge for the sorbents lies in exposing more hygroscopically active sites to the surrounding air while preventing salt leakage. Herein, a hierarchically structured scaffold is constructed by integrating cellulose nanofiber and lithium chloride (LiCl) as building blocks through 3D printing combined with freeze-drying. The milli/micrometer multiscale pores can effectively confine LiCl and simultaneously provide a more exposed active area for water sorption and release, accelerating both water sorption and evaporation kinetics of the 3D printed structure. Compared to a conventional freeze-dried aerogel, the 3D printed scaffold exhibits a water sorption rate that is increased 1.6-fold, along with a more than 2.4-fold greater water release rate. An array of bilayer scaffolds is demonstrated, which can produce 0.63 g g-1 day-1 of water outdoors under natural sunlight. This article provides a sustainable strategy for collecting freshwater from the atmosphere.

5.
Nat Commun ; 14(1): 8336, 2023 Dec 14.
Article in English | MEDLINE | ID: mdl-38097587

ABSTRACT

Body-centered cubic refractory metallic materials exhibit excellent high-temperature strength, but often suffer from brittle intergranular fracture due to the recrystallization-induced enrichment of trace elements at grain boundaries (GBs). Here, we report a fully-recrystallized pure molybdenum (Mo) material with room temperature (RT) superplasticity, fabricated by a facile method of powder metallurgy, Y-type hot rolling and annealing. By engineering the ultralow concentration of O at GBs, the inherent GB brittleness of Mo can be largely eliminated, which, in conjunction with high fractions of soft texture and low angle GBs, enables a significant development of ordered dislocation networks and the effective dislocation transmission across low angle GBs. Synergy of these factors greatly suppress the brittle intergranular fracture of Mo, contributing to an enhanced deformability of 108.7% at RT. These findings should have general implication for fabricating a broad class of refractory metals and alloys toward harsh applications.

6.
J Phys Chem Lett ; 14(48): 10825-10831, 2023 Dec 07.
Article in English | MEDLINE | ID: mdl-38019766

ABSTRACT

Here, we demonstrate a concentrated light-induced band edge tuning effect in photocatalytic hydrogen production. This band movement along with Femi level pinning leads to two distinct catalytic behaviors upon irradiation flux increase. Specifically, the concentration of the light promotes more long-lived carriers bound to the surface electronic states, progressively boosting energy conversion efficiency to a maximum value. Afterward, efficiency diminishes gradually due to poor carrier transfer. This work offers critical insights into efficient and economical photocatalytic hydrogen production.

7.
ACS Sustain Chem Eng ; 11(31): 11570-11579, 2023 Aug 07.
Article in English | MEDLINE | ID: mdl-37564956

ABSTRACT

In this study, we present an ecofriendly technique for encapsulating lauric acid (LA), a natural phase change material, within polystyrene (PS) nanofibers through coaxial electrospinning. The resulting LAPS core-sheath nanofibers exhibited a melting enthalpy of up to 136.6 J/g, representing 75.8% of the heat storage capacity of pristine LA (180.2 J/g), a value surpassing all previously reported core-sheath fibers. Scanning electron microscopy revealed uniform LAPS nanofibers free of surface LA until the core LA feed rate reached 1.3 mL/h. As the core LA feed rate increased, the fiber diameter shrank from 2.24 ± 0.31 to 0.58 ± 0.45 µm. Infrared spectra demonstrated a proportional increase in the LA content with rising core LA injection rates. Thermogravimetric analysis found the maximum core LA content in core-sheath nanofibers to be 75.0%. Differential scanning calorimetry thermograms displayed a trend line shift upon LA leakage for LA1.3PS nanofibers. LAPS fibers containing 75.0% LA effectively maintained consistent cycling stability and reusability across 100 heating-cooling cycles (20-60 °C) without heat storage deterioration. The core LA remained securely within the PS sheath after 100 cycles, and the LAPS nanofibers retained an excellent structural integrity without rupture. The energy-dense and form-stable LAPS core-sheath nanofibers have great potential for various thermal energy storage applications, such as building insulation, smart textiles, and electronic cooling systems, providing efficient temperature regulation and energy conservation.

8.
Org Lett ; 25(31): 5762-5767, 2023 Aug 11.
Article in English | MEDLINE | ID: mdl-37500499

ABSTRACT

An efficient and chemoselective transformation of ß-amido ynones to 3-acyl-substituted quinolones 2 and 3-H-quinolones 4 has been developed. In this reaction, ß-cyclic amido ynones can be selectively transformed into quinolones 2 in anhydrous EG via a selective C═O bond cleavage, 1,5-O migration, and C═C bond recombination process. The practical approach of this reaction renders it a viable alternative for the construction of various quinolones.

9.
Nat Commun ; 14(1): 3245, 2023 Jun 05.
Article in English | MEDLINE | ID: mdl-37277342

ABSTRACT

Producing functional soft fibers via existing spinning methods is environmentally and economically costly due to the complexity of spinning equipment, involvement of copious solvents, intensive consumption of energy, and multi-step pre-/post-spinning treatments. We report a nonsolvent vapor-induced phase separation spinning approach under ambient conditions, which resembles the native spider silk fibrillation. It is enabled by the optimal rheological properties of dopes via engineering silver-coordinated molecular chain interactions and autonomous phase transition due to the nonsolvent vapor-induced phase separation effect. Fiber fibrillation under ambient conditions using a polyacrylonitrile-silver ion dope is demonstrated, along with detailed elucidations on tuning dope spinnability through rheological analysis. The obtained fibers are mechanically soft, stretchable, and electrically conductive, benefiting from elastic molecular chain networks via silver-based coordination complexes and in-situ reduced silver nanoparticles. Particularly, these fibers can be configured as wearable electronics for self-sensing and self-powering applications. Our ambient-conditions spinning approach provides a platform to create functional soft fibers with unified mechanical and electrical properties at a two-to-three order of magnitude less energy cost under ambient conditions.

10.
Langmuir ; 39(31): 10881-10891, 2023 Aug 08.
Article in English | MEDLINE | ID: mdl-37390484

ABSTRACT

In this study, we explored the influence of molecular interactions and solvent evaporation kinetics on the formation of porous structures in electrospun nanofibers, utilizing polyacrylonitrile (PAN) and polystyrene (PS) as model polymers. The coaxial electrospinning technique was employed to control the injection of water and ethylene glycol (EG) as nonsolvents into polymer jets, demonstrating its potential as a powerful tool for manipulating phase separation processes and fabricating nanofibers with tailored properties. Our findings highlighted the critical role of intermolecular interactions between nonsolvents and polymers in governing phase separation and porous structure formation. Additionally, we observed that the size and polarity of nonsolvent molecules affected the phase separation process. Furthermore, solvent evaporation kinetics were found to significantly impact phase separation, as evidenced by less distinct porous structures when using a rapidly evaporating solvent like tetrahydrofuran (THF) instead of dimethylformamide (DMF). This work offers valuable insights into the intricate relationship between molecular interactions and solvent evaporation kinetics during electrospinning, providing guidance for researchers developing porous nanofibers with specific characteristics for various applications, including filtration, drug delivery, and tissue engineering.

11.
ACS Sens ; 8(7): 2731-2739, 2023 07 28.
Article in English | MEDLINE | ID: mdl-37231654

ABSTRACT

Water seepage-induced geological hazards (SIGHs), including landslides, collapse, debris flow, and ground fissures, often cause substantial human mortality, economic losses, and environmental damage. However, an early warning of geological water seepage remains a significant challenge. A self-powered, cost-effective, reliable, and susceptible SIGH early warning system (SIGH-EWS) is reported herein. This system designed the all-solid, sustainable, fire retardant, and safe-to-use bio-ionotronic batteries to provide a stable power supply for Internet of Things chipsets. Furthermore, the batteries' outstanding humidity and water sensitivity allow sensing of the water seepage emergence. Integrating energy management and wireless communication systems, the SIGH-EWS realizes timely alerts for early water seepage in different water and soil environments with a time resolution in seconds. Based on these merits, the SIGH-EWS demonstrates promising application prospects for early warning of geological disasters and corresponding design strategies that can potentially guide the designs of next-generation geological hazard alarm systems.


Subject(s)
Soil , Water Movements , Humans , Water Supply , Electric Power Supplies , Water
12.
Adv Mater ; 35(22): e2211437, 2023 Jun.
Article in English | MEDLINE | ID: mdl-36843238

ABSTRACT

Stimulus-responsive actuators play a vital role in the new generation of intelligent systems. However, poor mechanical performance, complicated fabrication processes, and the inability to complex deformation limit their practical applications. Herein, these challenges are overcome via designing a strong hygrothermic wood actuator with asymmetric water affinity. The actuator is readily constructed by sandwiching polypyrrole-coated wood with a Ni complex hygroscopic gel top layer for moisture absorption and a polyimide bottom layer as the water barrier. The resulting hygrothermic wood spontaneously stretches and bends itself in response to moisture and thermal/light stimulation. A robotic hand and a series of grippers made of hygrothermic wood demonstrate dexterous object-hand interactions during grasping and holding, while the reversible hygrothermic property allows the actuator to be potentially applied in fire rescue scenarios to rescue trapped objects. A combination of good mechanical properties, multi-stimulus-response, complex deformation, wide working temperature range, low manufacturing cost, and biocompatibility are simultaneously realized by one device. It is thus believed that such a strong wood actuator will open up a new avenue for building intelligent robotic hand systems.

13.
Mater Horiz ; 10(1): 136-148, 2023 01 03.
Article in English | MEDLINE | ID: mdl-36317638

ABSTRACT

The emerging applications of hydrogel ionotronics (HIs) in devices and machines require them to maintain their robustness under complex mechanical environments. Nevertheless, existing HIs still suffer from various mechanical limitations, such as the lack of balance between softness, strength, toughness, and fatigue fracture under cyclic loads. Inspired by the structure of the cytoskeleton, this study develops a sustainable HI supported by a double filamentous network. This cytoskeleton-like structure can enhance the strength of the HI by 26 times and its toughness by 3 times. It also enables HI to tolerate extreme mechanical stimuli, such as severe deformation, long-term cyclic loading, and high-frequency shearing and shocking. The advantages of these structurally- and mechanically-optimized HI devices in tactile perception and electroluminescent display, i.e., two practical applications where complex mechanical stimuli need to be sustained, are demonstrated. The findings reported in this study can inspire the design of human skin-like robust and anti-fatigue-fracture HI devices for long-term stable use.


Subject(s)
Hydrogels , Touch Perception , Humans , Materials Testing , Cytoskeleton , Microtubules
14.
Small ; 18(20): e2201045, 2022 05.
Article in English | MEDLINE | ID: mdl-35429099

ABSTRACT

The interface plays a pivotal role in stabilizing metal anode. Extensive studies have been made but systematic research is lacking. In this study, preliminary studies are conducted to explore the prime conditions of interfacial modification to approach the practical requirements. Critical factors including reaction kinetics, transport rate, and modulus are identified to affect the Zn anode morphology significantly. The fundamental principle to enhance the Zn anode stability is systematically studied using the TEMPO-oxidized cellulose nanofiber (TOCNF) coating layer with thin a separator. Its advantageous mechanical properties buffer the huge volume variation. The existence of hydrophilic TOCNF in the Zn anode interface enhances the mass transfer process and alters the Zn2+ distribution with a record high double-layer capacitance (390 uF cm-2 ). With the synergetic effect, the modified Zn anode works stably under 5 mA cm-2 with a thin nonwoven paper as the separator (thickness 113 µm). At an ultra-high current density of 10 mA cm-2 , this coated anode cycles for more than 300 h. This strategy shows an immense potential to drive the Zn anode forward toward practical applications.


Subject(s)
Electric Power Supplies , Nanofibers , Electrodes , Zinc
15.
Adv Mater ; 34(17): e2200865, 2022 Apr.
Article in English | MEDLINE | ID: mdl-35179809

ABSTRACT

Dehumidification is significant for environmental sustainability and human health. Traditional dehumidification methods involve significant energy consumption and have negative impact on the environment. The core challenge is to expose hygroscopic surfaces to the air, and appropriately store the captured water and avoid surface inactivation. Here, a nanostructured moisture-absorbing gel (N-MAG) for passive dehumidification, which consists of a hydrophilic nanocellulose network functionalized by hygroscopic lithium chloride, is reported. The interconnected nanocellulose can transfer the captured water to the internal space of the bulky N-MAG, eliminating water accumulation near the surfaces and hence enabling high-rate moisture absorption. The N-MAG can reduce the relative humidity from 96.7% to 28.7% in 6 h, even if the space is over 2 × 104 times of its own volume. The condensed water can be completely confined in the N-MAG, overcoming the problem of environmental pollution. This research brings a new perspective for sustainable humidity management without energy consumption and with positive environmental footprint.

16.
PhytoKeys ; 214: 39-46, 2022.
Article in English | MEDLINE | ID: mdl-36760550

ABSTRACT

A new species of Orchidaceae, Phalaenopsismedogensis, from Motuo, Xizang, is described and illustrated based on morphological characters and molecular phylogenetics analysis. Molecular phylogenetic analysis and morphological characters indicate that P.medogensis is close to P.deliciosa, P.gibbosa and P.lobbii, but differs from them by having triangular wings on the column foot, rhombic lip mid-lobe with a fleshy-horned appendage at the base, and concave lip lateral lobes, the lower part white with a deep purplish-red spot and hairy, the upper part pale yellow with dense rust spots.

17.
Polymers (Basel) ; 13(24)2021 Dec 19.
Article in English | MEDLINE | ID: mdl-34961004

ABSTRACT

The Hummers method is the most commonly used method to prepare graphene oxide (GO). However, many waste acids remain in the raw reaction mixture after the completion of this reaction. The aim of this study was to reuse these waste acids efficiently. In this study, microcrystalline cellulose (MCC) was directly dissolved in the mixture after the high-temperature reaction of the Hummers method. The residual acid was used to hydrolyze MCC, and the graphene oxide/microcrystalline cellulose (GO/MCC) composites were prepared, while the acid was reused. The effects of MCC addition (0.5 g, 1.0 g, and 1.5 g in 20 mL) on the properties of the composites were discussed. The structure, composition, thermal stability, and hydrophobicity of GO/MCC composites were characterized and tested by SEM, XRD, FTIR, TG, and contact angle tests. The results showed that MCC could be acid hydrolyzed into micron and nano-scale cellulose by using the strong acidity of waste liquid after GO preparation, and it interacted with the prepared GO to form GO/MCC composites. When the addition amount of MCC was 1 g, the thermal stability of the composite was the highest due to the interaction between acid-hydrolyzed MCC and GO sheets. At the same time, the hydrophobic property of the GO/MCC composite is better than that of the GO film. The freeze-dried GO/MCC composites are more easily dispersed in water and have stronger stability.

18.
Small Methods ; 5(12): e2100964, 2021 Dec.
Article in English | MEDLINE | ID: mdl-34928025

ABSTRACT

Phosphorus-doped carbon materials are promising alternatives to noble metal-based catalysts for the highly selective oxidation of benzyl alcohol to benzaldehyde, but it is challenging to achieve high loadings of high-activity P dopants in metal-free catalysts. Here, the preparation of high-loading and well-dispersed P atoms confined to the surfaces of cellulose-derived carbon via a dissolving-doping strategy is reported. In this method, cellulose is dissolved in phosphoric acid to generate a cellulose-phosphoric supramolecular collosol, which is then directly carbonized. The as-prepared carbon possesses a high specific surface area of 1491 cm3 g-1 and a high P content of 8.8 wt%. The P-doped nanoporous carbon shows a superior catalytic activity and cyclic stability toward benzyl alcohol oxidation, with a high turnover frequency of 3.5 × 10-3 mol g-1 h-1 and a low activation energy of 35.6 kJ mol-1 . Experimental results and theoretical calculations demonstrate that the graphitic C3 PO species is the leading catalytic active center in this material. This study provides a novel strategy to prepare P dopants in nanoporous carbon materials with excellent catalytic performance.

19.
ACS Appl Mater Interfaces ; 13(49): 59174-59184, 2021 Dec 15.
Article in English | MEDLINE | ID: mdl-34870409

ABSTRACT

Lithium-sulfur batteries are afflicted with capacity fading on account of polysulfide shuttling. A novel cost-effective electrode that can hinder the polysulfide shuttling and realize high active material utilization is highly required. Here, we demonstrate a flexible, electrically conductive, nanostructured, and asymmetric hybrid cathode by integrating a high-aspect-ratio wood nanocellulose and a low-cost commercial carbon nanotube (∼$ 0.2 g-1) into an entangled aerogel film. The vacuum filtration combined with lyophilization enables the aerogel film with quite different nanofiber/nanotube packing densities and pore structures at its two sides. The cooperative effects of the entangled building blocks and the asymmetric porous structure of the aerogel film stimulate the simultaneous increase of active sulfur loading, enhancing the electrolyte penetration, alleviating dissolution and shuttling of polysulfide ions, and promoting the fast electron transportation. The as-generated cathode exhibited a capacity fading of 0.01% per cycle over 1000 discharge/charge cycles at a 0.5 C rate (1 C = 1675 mA g-1). The average Coulombic efficiency reached ∼99.7%.

20.
Org Lett ; 23(22): 8873-8877, 2021 11 19.
Article in English | MEDLINE | ID: mdl-34748358

ABSTRACT

A novel P,N-bidentate ligand-assisted gold-catalyzed oxidative amination of ß-amino-ynones has been developed, allowing the simple and efficient construction of various quaternary ammonium-olate salts in good to excellent yields. These unprecedented quaternary ammonium-olate salts can be isolated and purified via simple suction filtration. The broad substrate scope, easy purification, easy further transformation, and mild conditions make it a viable alternative for the synthesis of various quaternary ammonium-olate salts.

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