Contribution of different state of adsorbed water to the sub-Tg dynamics of cellulose

Zhao, Hao; Chen, Zhe; Du, Xianfeng; Lin, Cheng

doi:10.1016/j.carbpol.2019.01.087

Cited by 37 publications

(51 citation statements)

References 30 publications

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“…The evolution of dielectric relaxation with drying time at this stage is demonstrated in Figure 4a, where it can be noticed that the magnitude of the relaxations is strikingly smaller than that at the first drying stage. The dielectric relaxation behaviors at four randomly selected drying moments are demonstrated in Figure 4b, which look similar to those of native cellulose with different MC at 20 °C [15]. Typical β-relaxation is observed in the frequency range of 10 6 –10 7 Hz, which is consistent with that found in native celluloses of different origins [11,15,34].…”

Section: Resultssupporting

confidence: 73%

“…The film in its initial state thus can be considered as a network of rearranged cellulose molecules immersing in water, where water is the continuous phase consisting of free water and bound water. The bound water could present in three states, including freezable loosely bound water, non-freezable loosely bound water, and tightly bound water, according to our previous study [15]. On the other hand, the film has been fully soaked in and washed with water, ionic species rather than H + ions should be negligible.…”

Section: Resultsmentioning

confidence: 94%

“…It is always puzzling to perform accurate fit on entangled dielectric relaxation spectra with superposition of many relaxations. The logarithmic derivative (LD) method based on the following equation, however, is effective in resolving overlapping relaxation peaks due to peak sharpening [15,23,24,25]. εʺLDfalse(ωfalse)=−π2∂ε∂lnω≈εʺRelfalse(ωfalse) where εʺLD and εʺRel denote the derivative dielectric loss and the measured dielectric loss, respectively.…”

Section: Methodsmentioning

confidence: 99%

“…Dielectric spectroscopy is a versatile method in the characterization of cellulosic materials, which inspects microscopic dynamics (either diffusional or orientational) of a material and is able to provide unique information regarding the structure and composition on molecular level [10,11,12,13,14,15]. Due to the non-invasion nature as well as other merits like rapidness in measurement, easy instrumentation, and simple sampling requirement [16,17], dielectric spectroscopy is also an effective tool in in-situ and real-time monitoring of kinetic processes, such as annealing of ultrastable glass [18], isothermal crystallization [19,20], and cell division [21].…”

Section: Introductionmentioning

confidence: 99%

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Evolution of Dielectric Behavior of Regenerated Cellulose Film during Isothermal Dehydration Monitored in Real Time via Dielectric Spectroscopy

Zhao

Chen

2019

Polymers

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The dielectric relaxation behavior of a regenerated cellulose (RC) film during isothermal dehydration was monitored in real time via dielectric spectroscopy, in order to investigate on one hand the influence of water on its dynamics and the variation of microstructure and phase composition during dehydration on the other. The progression of water loss is clearly revealed by the evolution of the dielectric relaxation behavior with drying time, which suggests two distinctly different drying stages separated by a striking transition period. The dielectric relaxation behavior at the first drying stage is found overwhelmingly dominated by ionic motion, and that at the second stage is basically a result of molecular dynamics. The mechanisms of these relaxations are proposed, through which the influence of water on the dynamics of the RC film and the variation of the microstructure and phase composition of the film at different hydration state are discussed in detail. An interesting finding is that highly ordered but noncrystalline arrangement of cellulose molecules exists, but it can be formed only when the film is in specific hydration state. This study demonstrates that dielectric spectroscopy is an effective tool in real-time monitoring kinetic process.

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Section: Resultssupporting

confidence: 73%

Section: Resultsmentioning

confidence: 94%

Section: Methodsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Evolution of Dielectric Behavior of Regenerated Cellulose Film during Isothermal Dehydration Monitored in Real Time via Dielectric Spectroscopy

Zhao

Chen

2019

Polymers

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“…As the 1st and 2nd water layers are located at a different distance from the polymer chain, their interactions with the polymer are also different. This induces different dynamics and mobility for these two populations (Li et al 1998;Zhao et al 2019). The crossover from one to two layers of water is likely to influence the properties of the hydrated polymer and to induce a transition, i.e.…”

Section: Double Layer Adsorptionmentioning

confidence: 99%

Moisture-induced crossover in the thermodynamic and mechanical response of hydrophilic biopolymer

et al. 2019

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The use of natural sustainable resources such as wood in green industrial processes is currently limited by our poor understanding of the impact of moisture on their thermodynamic and mechanical behaviors. Here, a molecular dynamics approach is used to investigate the physical response of a typical hydrophilic biopolymer in softwood hemicellulosexylan-when subjected to moisture adsorption. A unique moisture-induced crossover is found in the thermodynamic and mechanical properties of this prototypical biopolymer with many quantities such as the heat of adsorption, heat capacity, thermal expansion and elastic moduli exhibiting a marked evolution change for a moisture content about 30 wt%. By investigating the microscopic structure of the confined water molecules and the polymer-water interfacial area, the molecular mechanism responsible for this crossover is shown to correspond to the formation of a double-layer adsorbed film along the amorphous polymeric chains. In addition to this moisture-induced crossover, many properties of the hydrated biopolymer are found to obey simple material models.

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Methods for Characterization of Dielectric and Thermal Properties of Biomaterials

Ioniță¹,

Asăndulesa²,

Cristea³

2023

Functional Biomaterials

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Contribution of different state of adsorbed water to the sub-Tg dynamics of cellulose

Cited by 37 publications

References 30 publications

Evolution of Dielectric Behavior of Regenerated Cellulose Film during Isothermal Dehydration Monitored in Real Time via Dielectric Spectroscopy

Evolution of Dielectric Behavior of Regenerated Cellulose Film during Isothermal Dehydration Monitored in Real Time via Dielectric Spectroscopy

Moisture-induced crossover in the thermodynamic and mechanical response of hydrophilic biopolymer

Methods for Characterization of Dielectric and Thermal Properties of Biomaterials

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