Transition Behavior of Cellulose Nanocrystal Networks Induced by Nanoconfined Water

IF 6.2 Q2 ENERGY & FUELS
Siyuan Liu, Dan Xu, Chenyang Cai, Xizhou Cecily Zhang, Loren B. Andreas, Zengbin Wang, Qun Song, Jiaxiu Wang, Catalin R. Picu, Kai Zhang
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Abstract

Hydrogen bonding (HB) is essential for the mechanical properties of cellulose-based materials. However, the plastification of cellulose nanocrystals (CNC) caused by the transition of HB in the presence of water is still insufficiently understood. In this work, the rigid–soft transition of nanoconfined chains in non-ordered regions of CNC surfaces is quantitively described by comparing their strain behaviors with amorphous cellulose. Moreover, this softening (referred to as the “hydro-glass transition”) with increasing relative humidity (RH) is explored, and a threshold RH value (RHt) is identified to characterize the transition. The phenomenon is attributed to the monolayer to multilayer adsorption and eventually capillary condensation of water molecules in wedged mesopores of the CNC films. This triggers a rapid transition of HB from cellulose–cellulose to cellulose–water type in the vicinity of RHt. The hydro-glass transition is promoted by higher temperatures, for example, RHt at 65 °C decreases to 50%. In addition, the presence of surface groups with lower acid dissociation constant (comparing SO3 and OH/COO moieties) also accelerates this hydro-glass transition process. Thus, a detailed understanding of the thermodynamic changes in hydrogen-bonded nanoconfined polymer chains in the presence of humidity, with implications for developing nanomaterials with RH-controlled properties, is provided.

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CiteScore
8.20
自引率
3.40%
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0
期刊介绍: Advanced Energy and Sustainability Research is an open access academic journal that focuses on publishing high-quality peer-reviewed research articles in the areas of energy harvesting, conversion, storage, distribution, applications, ecology, climate change, water and environmental sciences, and related societal impacts. The journal provides readers with free access to influential scientific research that has undergone rigorous peer review, a common feature of all journals in the Advanced series. In addition to original research articles, the journal publishes opinion, editorial and review articles designed to meet the needs of a broad readership interested in energy and sustainability science and related fields. In addition, Advanced Energy and Sustainability Research is indexed in several abstracting and indexing services, including: CAS: Chemical Abstracts Service (ACS) Directory of Open Access Journals (DOAJ) Emerging Sources Citation Index (Clarivate Analytics) INSPEC (IET) Web of Science (Clarivate Analytics).
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