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ADVANCED MATERIALS · 2024 · IF 27.4

Spatiotemporal Programmability of 3D Chiral Color Units Driven by Ink Spontaneous Diffusion toward Customized Printing

Wenjie Yang,Chenglin Zheng,Li Sun,Zhiying Bie,Yuchen Yue,Xiuhong Li,Wentao Sun,Tomiki Ikeda,Jingxia Wang,Lei Jiang

Blue phase liquid crystals (BPLCs) have exhibited promising applications in 3D flexible displays due to their molecular-level self-assembled chiral structures, fast response, and tunable polarized colors. However, there remain challenges for spatiotemporal programming of 3D chiral color units for BPLC dynamic patterning. Herein, the programmable temporal evolution of micrometer-scale color units and spatial configuration switch of chiral modes are achieved by spontaneous ink diffusion-driven asymmetric lattice deformation in dual-chiral polymer-templated blue phases. Custom-printed colorful patterns are designed by machine learning-assisted parameter optimization, which displays programmable multidimensional encrypted information that incorporates temporal evolving colors (wavelength), spatial distribution (depth), chiral modes (L/R). The quantitative relationship between ink diffusion kinetics and blue-phase dynamic 3D structural optics is established by in situ characterization, finite element analysis, and mathematical geometry modeling. This work provides insights into the microgeometric manipulation of 3D chiral color of BPLCs in the application of information security and self-adaptive indicators.

CAS / MDL: 9002-89-5
研究领域: 材料科学 · 光学 · 信息加密 · 自适应显示
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Nature Communications · 2025 ·Vol. 16 ·期 1 ·1-10 · IF 15.7

Control of water for high-yield and low-cost sustainable electrochemical synthesis of uniform monolayer graphene oxide

Guo Jiaqi,Pei Songfeng,Huang Kun,Zhang Qing,Zhou Xizhong,Tong Jinmeng,Liu Zhibo,Cheng Hui-Ming,Ren Wencai

With the rapid development of graphene industry, low-cost sustainable synthesis of monolayer graphene oxide (GO) has become more and more important for many applications such as water desalination, thermal management, energy storage and functional composites. Compared to the conventional chemical oxidation methods, water electrolytic oxidation of graphite-intercalation-compound (GIC) shows significant advantages in environmental-friendliness, safety and efficiency, but suffers from non-uniform oxidation, typically ~50 wt.% yield with ~50% monolayers. Here, we show that water-induced deintercalation of GIC is responsible for the non-uniform oxidation of the water electrolytic oxidation method. Using in-situ experiments, the control principles of water diffusion governing electrochemical oxidation and deintercalation of GIC are revealed. Based on these principles, a liquid membrane electrolysis method was developed to precisely control the water diffusion to achieve a dynamic equilibrium between oxidation and deintercalation, enabling industrial sustainable synthesis of uniform monolayer GO with a high yield (~180 wt.%) and a very low cost (~1/7 of Hummers’ methods). Moreover, this method allows precise control on the structure of GO and the synthesis of GO by using pure water. This work provides new insights into the role of water in electrochemical reaction of graphite and paves the way for the industrial applications of GO.

研究领域: 材料科学 · 电化学 · 环境科学
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CELLULOSE · 2014 ·Vol. 21 ·期 6 ·4009-4017 · IF 3.033

Investigation of water diffusion process in ethyl cellulose-based films by attenuated total reflectance Fourier transform infrared spectroscopy and two-dimensional correlation analysis

Hou Lei,Feng Kai,Wu Peiyi,Gao Hao

Two-dimensional correlation spectroscopy (2Dcos) analysis on the time-resolved attenuated total reflectance Fourier transform infrared spectroscopy has been employed to investigate the diffusion behavior of water in ethyl cellulose/triethyl citrate (EC/TEC) films with varied TEC content. The diffusion coefficients of water in the EC-based films are calculated from the diffusion curves according to the Fickian Diffusion Model. And they are observed to increase with TEC content, possibly caused by the increased free volume in the film matrix. In the 2Dcos analysis, the broad O–H stretching vibration region is split into at least four bands, which can be assigned to four different states of water molecules, that is, bulk water, cluster water, relatively free water and free water. Moreover, it is found that as water molecules disperse into the EC-based films, cluster water with moderate hydrogen bonds diffuses faster than bulk water with strong hydrogen bonds. The relatively free water and free water are formed during the diffusion process due to their interactions with the films matrix, which makes water molecules confined and restricted in limited space.

研究领域: 材料科学 · 光谱学
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Nature Communications · 2022 ·Vol. 13 ·期 1 ·1-8 · IF 17.694

Spontaneous water-on-water spreading of polyelectrolyte membranes inspired by skin formation

Tang Sihan,Gong Jiang,Shi Yunsong,Wen Shifeng,Zhao Qiang

Stable interfaces between immiscible solvents are crucial for chemical synthesis and assembly, but interfaces between miscible solvents have been less explored. Here the authors report the spontaneous water-on-water spreading and self-assembly of polyelectrolyte membranes. An aqueous mixture solution containing poly(ethyleneimine) and poly(sodium 4-styrenesulfonate) spreads efficiently on acidic water, leading to the formation of hierarchically porous membranes. The reduced surface tension of the polyelectrolyte mixture solution drives the surface spreading, while the interfacial polyelectrolytes complexation triggered by the low pH of water mitigates water-in-water mixing. The synergy of surface tension and pH-dependent complexation represents a generic mechanism governing interfaces between miscible solvents for materials engineering, without the need for surfactants or sophisticated equipment. As a proof-of-concept, porous polyelectrolyte hybrid membranes are prepared by surface spreading, exhibiting exceptional solar thermal evaporation performance (2.8 kg/m 2 h) under 1-sun irradiation.

CAS / MDL: 9002-98-6
研究领域: 材料科学 · 化学工程 · 表面化学
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CHEMISTRY OF MATERIALS · 2022 · IF 10.508

Facile Guest-Mediated Method for Gram-Scale Synthesis of Superhydrophilic Metal–Organic Frameworks

Yang Xu,Yuxin Liu,Hongliang Han,Zhanfang Ma

Superhydrophilic metal–organic frameworks (MOFs) are ideal materials for many applications in an aqueous environment, such as catalysis, drug delivery, and pollute absorption. However, current approaches fail to provide either an efficient way to enhance inside aqueous diffusion or a facile method for mass production. Here, aiming at the above issues, we presented a guest-mediated strategy to rapidly produce superhydrophilic MOFs in gram scale, based on the interaction between polarized polyoxometalate guests and hydrophobic channels. Experimental observation and theoretical simulation show that the assembled guests induced aqueous diffusion into channels, promoting water transportation. The confirmatory biocatalytic application indicated enhanced water filtration and mass transfer in MOFs, which was manifested by efficient substrate conversion in biological buffers. Because this strategy was generally valid to a variety of MOFs, it would unleash the potential of MOFs in an aqueous environment and bring many possibilities to this field.

研究领域: 材料科学 · 化学工程 · 催化 · 环境科学
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JOURNAL OF POWER SOURCES · 2022 · IF 9.794

Interfacial water distribution behaviors in high performance bipolar membrane fuel cell

Zhengjian Li,Sian Chen,Liting Cui,Haining Wang,Shanfu Lu,Yan Xiang

The acidic-alkaline interface of a bipolar membrane fuel cell (BPMFC) is the place to generate water, which significantly affect the output performance of BPMFC by regulating the water distribution due to the ion conductivity and oxygen reduction reaction (ORR) kinetics in cathode. To investigate the influence of water diffusivity ( D w ) on the water distribution, four alkaline polymer electrolytes with different D w is selected as anion exchange membrane or alkaline electrolyte ionomer to assemble BPMFCs. A combined experimental and simulated study reveals the positive correlation relationship of D w to the water distribution and performance of BPMFC. By increasing the D w of the alkaline polymer electrolytes, the interfacial-generated water amount can be increased and promptly transport to the cathode, thereby satisfying the ion conductivity and increasing the ORR kinetics, and breakthrough the peak power density of the BPMFC with 1.06 W cm −2 without humidification .

研究领域: 电化学 · 能源材料 · 燃料电池 · 高分子科学 · 界面科学
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ACS Applied Polymer Materials · 2024 · IF 4.4

PVA–PNIPAM Hydrogel-Based Moisture-Electric Generators with Tunable Pore Structures for Enhanced Power Generation

Guangxin Ma,Weiman Li,Xin Zhou,Xiaoze Wang,Mengjie Cao,Wenjun Ma,Jingjing Wang,Hang Yu,Shigang Li,Yunfa Chen

A hygroscopic layer plays an important role in improving the output abilities of energy generation from ubiquitous moisture, whose mechanism is unclear. Herein, three kinds of hydrogels with different pore structures/functional groups are designed as hygroscopic layers, and a universal strategy was proposed to assemble them into hydrogel-based moisture-electric generators (HMEGs). The hydrogels’ pore structure affects the moisture absorption rate, while the functional groups regulate the diffusion path of water. HMEG’s power generation is a synergistic effect of ionic diffusion and streaming potential, which is closely related to the water diffusion within the material and is not directly related to the amount of moisture absorption. HMEG, which absorbs moisture quickly, stores water efficiently, and releases moisture slowly, has an excellent performance and stable voltage output. Based on this mechanism, HMEG employed the calcium chloride-poly(vinyl alcohol)-poly(N-isopropylacrylamide) (CPVPN), semi-interpenetrating network (semi-IPN) hydrogel as the hygroscopic layer showed an open-circuit voltage as high as 0.34 V and a power density of 33.23 μA cm–3. This study opens a perspective on hydrogel HMEG and provides insights into high-performance HMEG design.

CAS / MDL: 7727-54-0
研究领域: 材料科学 · 能源工程 · 化学工程 · 环境科学
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COMPOSITES PART B-ENGINEERING · 2025 · IF 14.2

Cross-Scale Simulation-Driven Design of rGO-PFAN/Epoxy Coatings: Synergistic Physical Barrier-Chemical Repulsion for Superior Moisture Resistance

Xiang Li,Yanji Zhu,Yue Sun,Dan Lin,Huaiyuan Wang

In harsh humid environments, conventional epoxy coatings suffer from inadequate corrosion resistance due to microporous defects formed during curing, while the trial-and-error optimization of fillers faces challenges such as unclear mechanisms and low design efficiency. This study proposes a novel "computation-driven material design" paradigm, elucidating the synergistic moisture-resistant mechanisms of fillers through cross-scale simulations. Molecular dynamics (MD) simulations show that adding 3 wt% graphene oxide (GO) reduces the free volume of epoxy by 15% and decreases the water diffusion coefficient by 10%. Density functional theory (DFT) calculations identify a high adsorption energy barrier (21.831 eV) generated by fluorine groups in polyfluoroaniline (PFAN) through electron cloud redistribution, effectively suppressing water penetration. Monte Carlo (MC) simulations further bridge microscopic energy barriers with macroscopic penetration flux. Guided by these insights, reduced graphene oxide-polyfluoroaniline (rGO-PFAN) composite fillers are synthesized via covalent grafting, experimentally demonstrating synergistic barrier-hydrophobic effects. Epoxy coatings containing 1.5 wt% rGO-PFAN retain an impedance modulus of 4.44×10 11 Ω·cm 2 after 90-day immersion, while 2 wt% filler reduces long-term water absorption by 73.63%. Salt spray tests confirm superior corrosion suppression at defect regions. Mechanical property tests show that the coating exhibits significantly reduced wear loss, enhanced adhesion strength, and perfect adhesion after thermal cycling. This work pioneers the multiscale correlation from electron-cloud interactions to macroscopic anticorrosion performance, establishing a theoretical framework for the rational design of intelligent coatings in extreme environments.

研究领域: 材料科学 · 高分子化学 · 表面工程 · 腐蚀防护 · 计算材料学 · 纳米复合材料
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Materials · 2019 ·Vol. 12 ·期 21 ·3515 · IF 2.972

Molecular Dynamics Simulation on the Diffusion of Flavor, O2 and H2O Molecules in LDPE Film

Binqing Sun,Lixin Lu,Yong Zhu

The diffusion of five flavor organic molecules, including D-limonene, myrcene, ethyl hexanoate, 2-nonanone, and linalool in low density polyethylene (LDPE) film were investigated by combined experimental and molecular dynamics (MD) simulation studies. The diffusion coefficients derived from the prediction model, experimental determination, and MD simulation were compared, and the related microscopic diffusion mechanism was investigated. The effects of the presence of the flavor organic molecules on the diffusion of O2and H2O in polyethylene (PE) were also studied by MD simulation. Results show that: The diffusion of five flavor molecules in LDPE is well followed to Fick’s second law by the immersion experiment; MD simulation indicates the dual mode diffusion mechanism of the flavor molecules is in LDPE; the diffusion coefficients from MD simulation are close to those from the experimental determination, but are slightly larger than those values; the presence of the flavor organic molecules hinders the diffusion of O2and H2O, which can be well explained from the fraction of free volume (FFV) and interaction energy calculation results derived from MD simulation.Keywords:flavor organic molecules;LDPE film;molecular dynamics simulation;diffusion

CAS / MDL: 123-35-3
研究领域: 材料科学 · 化学工程 · 高分子科学 · 食品科学
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