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APPLIED SURFACE SCIENCE · 2023 · IF 6.7

Direct observation of anomalous water at the solid-liquid boundary on silica surface

Wei-qing An,Xiang-an Yue,Ji-rui Zou,Li-juan Zhang,Rong-jie Yan

In this study, we investigate the properties and behavior of interfacial water on solid silica surfaces and its implications for various applications. We utilize a combination of transmission electron microscopy (TEM), nuclear magnetic resonance, mass spectrometry, infrared, and Raman spectroscopy to explore the presence and characteristics of anomalous water on silica surfaces. Our findings reveal a stable, nanoscale layer of wall-bound water on the inner surface of silica tubes that persists under high vacuum and room temperature conditions. This layer is rich in hydrated hydrogen ions and exhibits a thickness that correlates with the density of hydroxyl groups in silica. Through additional experimentation, we demonstrate that reducing the density of silica hydroxyl groups causes the wall-bound water to return to a liquid state, highlighting the pivotal role of hydroxyl groups in the formation of this unique water layer. Our study offers valuable insights into the properties and behavior of interfacial water on solid surfaces and lays the foundation for potential applications in a wide range of fields, such as energy storage, drug delivery, environmental remediation, biological sample preparation, microfluidics, and nanofluidics. Future research will further explore the properties and behavior of interfacial water on different material surfaces and under various environmental conditions, laying the groundwork for technological innovation in related fields. By utilizing advanced approaches and fostering interdisciplinary collaboration, this research contributes significantly to our understanding of interfacial water and paves the way for the development of cutting-edge technologies that capitalize on its distinctive properties.

CAS / MDL: 7664-39-3 1310-73-2
研究领域: 材料科学 · 表面化学 · 纳米技术
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ACS Applied Materials & Interfaces · 2024 · IF 8.3

Efficient Electron Transfer through Interfacial Water Molecules across Two-Dimensional MoO3 for Humidity Sensing

Wanlun Jiang,Meng Su,Yangong Zheng,Teng Fei

Resistive humidity sensors are required in flexible and integrated devices. Two-dimensional MoO3 offers a large interface area, enabling the modulation of its electrical properties over a wide range. In this study, 2D MoO3 was synthesized via liquid-phase exfoliation for humidity-sensing tests. In terms of high sensitivity, negligible hysteresis, linearity, and stability, the humidity-sensing performance of MoO3 is superior to those of other materials. The sensitivity reaches 9794 Ω/RH at 25 °C. The sensing mechanism of MoO3 was investigated by using impedance spectra and voltage–current scans under different humidity levels. The results indicate that the resistance change of MoO3 due to humidity originates from the interfacial conductance. Interfacial H2O adsorption induces efficient conducting paths via hydrogen bonding, decreases the potential barrier for electron transfer, and supplies additional electron states to the valence bands. In this study, electronic humidity sensing was investigated in depth, and a new perspective was proposed for electronic humidity sensing.

CAS / MDL: 1313-27-5
研究领域: 材料科学 · 传感器技术
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JOURNAL OF DENTAL RESEARCH · 2023 · IF 7.6

Release of Interface Confined Water Significantly Improves Dentin Bonding

M. Pan,Z. Li,J. Xu,Y. Lei,C. Shu,W. Lao,Y. Chen,X. Li,H. Liao,Q. Luo,X. Li

Water residue and replacement difficulty cause insufficient adhesive infiltration in demineralized dentin matrix (DDM), which produces a defective hybrid layer and thus a bonding durability problem, severely plaguing adhesive dentistry for decades. In this study, we propose that the unique properties of a highly hydrated interface of the porous DDM can give rise to 1 new type of interface, confined liquid water, which accounts for most of the residue water and may be the main cause of insufficient infiltration. To prove our hypothesis, 3 metal ions with increasing binding affinity and complex stability (Na+, Ca2+, and Cu2+) were introduced respectively to coordinate negatively charged groups such as -PO43−, -COO− abundant in the DDM interface. Strong chelation of Ca2+ and Cu2+ rapidly released the confined water, significantly improving penetration of hydrophobic adhesive monomers, while Na+ had little effect. A significant decrease of defects in the hybrid layer and a much decreased modulus gap between the hybrid layer and the adhesive layer greatly optimized the microstructure and micromechanical properties of the tooth–resin bonding interface, thus improving the effectiveness and durability of dentin bonding substantially. This study paves the way for a solution to the core scientific issue of contemporary adhesive dentistry: water residue and replacement in dentin bonding, both theoretically and practically.

研究领域: 口腔医学 · 材料科学 · 生物化学
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ACS Applied Materials & Interfaces · 2024 · IF 8.3

Flexible Janus Black Silicon Photothermal Conversion Membranes for Highly Efficient Solar-Driven Interfacial Water Purification

Chuanling Zhou,Qiuyu Mei,Limingming Huang,Tingting Mao,Shuangfu Li,Zhian Wang,Hua Wan,Hui Gu,Kai Han

Photothermal conversion materials are critical in the development of solar-driven interfacial evaporation techniques; however, achieving a high energy conversion efficiency remains challenging owing to the high cost and instability of light-absorbing materials, in addition to the difficulties of simultaneously improving light absorption while suppressing heat loss. A black silicon (Si) powder with a porous structure was prepared by chemical etching of a low-cost commercial micron-sized Al–Si alloy, and a flexible Janus black Si photothermal conversion membrane was constructed. The partially broken spherical particles and porous structure obtained after etching enhanced the refraction of light from the Si powder, imparting the prepared membrane with an average light absorption rate of 95.95% over the solar spectrum. Evaporation from the membrane increased the intermediate water content and reduced the equivalent evaporation enthalpy. The thermal conduction loss was inhibited through a one-dimensional water transport structure, and the membrane achieved a water evaporation rate of 2.17 kg m–2 h–1 and a photothermal efficiency of 94.95% under 1 sun illumination. Benefiting from the broadband absorption and high photothermal efficiency of black Si powder, surface modification of hydrophobic polydimethylsiloxane, and directional salt-out structure design, the evaporation rate of the Janus black Si membrane-based system in a 10% NaCl solution was maintained >2.10 kg m–2 h–1 after 7 days of continuous evaporation cycles. The removal rate of metal ions from simulated seawater and from practical wastewater containing complex heavy metals reached >99.9%, indicating the promising potential of black Si membrane for application in solar-driven interfacial water purification.

研究领域: 材料科学 · 环境科学
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ADVANCED FUNCTIONAL MATERIALS · 2023 ·Vol. 33 ·期 37 ·2302293 · IF 19

Excluding the Trouble from Interfacial Water by Covalent Organic Polymer to Realize Extremely Reversible Zn Anode

Xuyan Ni,Jinqiu Zhou,Haoqing Ji,Yuejiao Chen,Huaming Yu,Yiwei Zheng,Tao Qian,Mengfan Wang,Libao Chen,Chenglin Yan

The side reactions related to water are the major issue hindering practical application of Zn metal batteries. To exclude the trouble from interfacial water, a covalent organic polymer (COP) layer with N, N′-Bis(salicylidene)ethylenediamine structure is designed, whose strong coordination ability with Zn 2+ enhances the de-solvation kinetics of solvated Zn 2+ which is conducive to interfacial water removal thus alleviating the side reactions related to water. This function has been certified by density functional theory along with molecular dynamics analysis. Moreover, measurements including in situ electrochemical gas chromatography, in situ optical microscopy, in situ X-ray diffraction and in situ Raman spectroscopy verify the weakened side reactions (including hydrogen evolution and corrosion) along with homogenous Zn deposition contributed from the covalent organic polymer layer. Benefiting from these merits, when assemble into cells based on common ZnSO 4 -based aqueous electrolyte, the COP layer-decorated anode exhibits excellent electrochemical performance of a high average Coulombic efficiency value 99.5% at a high capacity of 5.0 mA h cm −2 . What's more, the symmetric cells can operate at −20 °C and the full cell with N/P ratio as low as 1.2 can cycle stably for 100 cycles, which would carry forward the promising practical application of Zn metal batteries.

研究领域: 材料科学 · 电化学
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ACS Catalysis · 2024 · IF 11.3

In Situ Investigation of Interfacial Water in the Hydrogen Evolution Reaction: A Comparative Study Unraveling the Impact of Oxide Impurity

Lingjiao Li,Xiaoyi Jiang,Le Ke,Kai Zhao,Zhiyuan Mei,Haiyu Wang,Ning Yan

Understanding the sluggish kinetics of the hydrogen evolution reaction (HER) in neutral media is a grand challenge. The correlation between the interfacial water structure and HER activity has yet to be determined, particularly for catalysts with complex chemical compositions. Herein, we used in situ electrochemical and spectroscopic methods (e.g., surface-enhanced infrared absorption and shell-isolated nanoparticle-enhanced Raman spectroscopy) to investigate the evolution of the hydrogen bonding network of interfacial water molecules of typical HER catalysts (e.g., Pt/C and NiCo-phosphide, -sulfide, and -hybrid with/without oxide impurity) under potential bias in neutral media. The cathodic potentials always influenced the composition of interfacial water, rendering the records of distinct nominal tuning rates among different catalysts. Interestingly, we found that a suitable amount of surface oxide impurity, a HER inert phase, can drastically alter the dynamic behaviors of interfacial water, promoting the transition from ice-like and liquid-like water to free water while leading to an improved HER performance (j0 > 0.7 mA cm–2; η = 101.7 mV@10 mA cm–2). Such an effect was presumably correlated with the hydrophilic moieties, as evidenced by the in situ studies of pure oxide and hydroxide controls. This work provides insights of understanding the activity of the HER in neutral media, paving the way to the rational design of electrocatalysts.

CAS / MDL: 10026-22-9 13478-00-7
研究领域: 电化学 · 材料科学
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ACS Applied Materials & Interfaces · 2024 · IF 8.3

Highly Concentrated Electrolyte Superlubricants Enhanced by Interfacial Water Competition Around Chemically Active MgO Additives

Hongyu Liang,Shijing Zou,Manqiang Liu,Tianqiang Yin,Xiaojie Xia,Xijun Hua,Yonghong Fu,Yongfeng Bu

The low concentration of water-based lubricants and the high chemical inertness of the additives involved are often regarded as basic norms in the design of liquid lubricants. Herein, a novel liquid superlubricant of an aqueous solution containing a relatively high concentration of salt, lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), is reported for the first time, and the superlubricity stability and load-bearing capacity of the optimized system (MgO0.10/LiTFSI10) are effectively strengthened by the addition of only trace (0.10 wt %) water–chemically active MgO additives. It demonstrates higher applicable loads, lower COF (∼0.004), and stability relative to the base solution. Only a trace amount of MgO additive is needed for the superlubricity, which makes up for the cost and environmental deficiencies of LiTFSI10. The weak interaction region between free water and the outer-layer water of Li+ hydration shells becomes a possible ultralow shear resistance sliding interface; the Mg(OH)2 layer, generated by the reaction of MgO with water, further creates additional weakly interacting interfaces, leading to the formation of an asymmetric contact between the clusters/particles within the hydrodynamic film by moderating the competition between interfacial water and free water, thus achieving high load-bearing macroscopic superlubricity. This study deepens the contribution of electrolyte concentration to ionic hydration and superlubricity due to the low shear slip layer formed by interfacial water competition with water-activated solid additives, providing new insights into the next generation of high load-bearing water-based liquid superlubricity systems.

CAS / MDL: 90076-65-6 7782-42-5
研究领域: 材料科学 · 化学工程
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Efficient antibiotic wastewater treatment via interfacial water evaporation based soot-coated conjugated microporous polymer hollow microspheres

Wenwen Luo,Meichen Liu,Rui Jiao,Yunjia Wang,Jiyan Li,Zhaoqi Zhu,Weidong Liang,Hanxue Sun,An Li

Solar-driven interfacial evaporation (SDIE) technology holds the promise of purification and removal of organic pollutants from water samples. In this work, an efficient SDIE composed of multifunctional self-floating photothermal materials based on candle soot-coated conjugated microporous polymer hollow spheres (CS-CMPsHM) for treatment of tetracycline (TC) wastewater is reported. By depositing candle soot nanoparticles, CS-CMPsHM achieved excellent interfacial evaporation performance by extending the light absorption. Additionally, the π-π interaction between CMP's unique conjugated network and TC molecules and the well-developed porosity facilitates the capture of target contaminants. The synthesized CS-CMPsHM evaporator demonstrated remarkable properties, i.e., excellent photothermal performance (with superior photothermal conversion efficiency up to 94 % and evaporation rate of 1.55 kg m − 2 h − 1 under one sun irradiation), extremely low wet thermal conductivity (0.075 W m -1 K − 1 ), reusability, superior salt resistance, stability, adsorption of pollutants and renewable performance. Furthermore, CS-CMPsHM remains its excellent purification performance from real water samples (the Yellow River) measured by a three-dimensional fluorescence spectrometer. The results of biological toxicity show that the purified water recovered by the SDIE method effectively reduced the phytotoxicity of TC. With its straightforward and scalable manufacturing process, our CS-CMPsHM demonstrates promising potential as advanced photothermal materials for the treatment of various pollutants using SDIE.

研究领域: 环境科学 · 材料科学 · 化学工程
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2022 · IF 24.319

Boosting 2 e- water oxidation reaction on WO3 by F modification and revealing the mechanism by probing interfacial water structure

Zhen Chen,Shipeng Geng,Yawen Wang,Yi Wang,Shuqin Song

H 2 O 2 production by 2 electron water oxidation reaction (2e - WOR) is a promising approach, but still lacks mechanistic studies especially from a dynamic point of view. The interfacial water behavior on the solid/liquid interface is believed to play a crucial role in WOR activity. Here, F modification was used to accommodate the structure and dynamic process of interfacial water on WO 3 surface and boost the 2e- WOR activity. Electrochemical measurement, Raman spectra and computational techniques were used to investigate the mechanism. F modification was proved to guide the dipole moments of interfacial water molecules towards WO 3 surface, meaning more difficult to flip interfacial water molecules to perform the first step of WOR, in turn resulting in easy desorption of HO* and O-O*, thus benefiting for 2 e - WOR. This work paves a novel insight to understand mechanism of 2 e - WOR and rationally design the electrocatalysts for H 2 O 2 production from water.

研究领域: 电化学 · 催化材料科学 · 理论计算化学
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Nature Communications · 2024 ·Vol. 15 ·期 1 ·1-12 · IF 14.7

Bimetallic nanoalloys planted on super-hydrophilic carbon nanocages featuring tip-intensified hydrogen evolution electrocatalysis

Zhang Linjie,Hu Haihui,Sun Chen,Xiao Dongdong,Wang Hsiao-Tsu,Xiao Yi,Zhao Shuwen,Chen Kuan Hung,Lin Wei-Xuan,Shao Yu-Cheng,Wang Xiuyun,Pao Chih-Wen,Han Lili

The insufficient availability and activity of interfacial water remain a major challenge for alkaline hydrogen evolution reaction (HER). Here, we propose an “on-site disruption and near-site compensation” strategy to reform the interfacial water hydrogen bonding network via deliberate cation penetration and catalyst support engineering. This concept is validated using tip-like bimetallic RuNi nanoalloys planted on super-hydrophilic and high-curvature carbon nanocages (RuNi/NC). Theoretical simulations suggest that tip-induced localized concentration of hydrated K + facilitates optimization of interfacial water dynamics and intermediate adsorption. In situ synchrotron X-ray spectroscopy endorses an H* spillover-bridged Volmer‒Tafel mechanism synergistically relayed between Ru and Ni. Consequently, RuNi/NC exhibits low overpotential of 12 mV and high durability of 1600 h at 10 mA cm ‒2 for alkaline HER, and demonstrates high performance in both water electrolysis and chlor-alkali electrolysis. This strategy offers a microscopic perspective on catalyst design for manipulation of the local interfacial water structure toward enhanced HER kinetics.

CAS / MDL: 7447-39-4
研究领域: 材料科学 · 电化学 · 催化作用
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Journal of Water Process Engineering · 2024 · IF 6.3

Enhanced waste water purification performance of solar-driven interfacial water evaporation through the integration of electrocatalysis

Chaorui Xue,Chi Zhang,Yu Zhang,Lei Liu,Wenjing Zheng,Ying Li,Huinian Zhang,Suping Jia,Ning Li,Qing Chang,Shengliang Hu

Solar-driven interfacial water evaporation (SDIWE) has been proven to be an effective method for purifying polluted water. However, the challenging issue of removing volatile organic compounds (VOCs) from wastewater is frequently encountered. In this study, the SDIWE-electrocatalysis coupling system is established by employing defective TiO 2 as both photothermal and electrode materials, and significant enhancements are achieved in terms of water evaporation rate and distilled water quality. The application of voltage not only generates joule heat but also reduces water evaporation enthalpy, contributing to the improved water evaporation rate. Under solar irradiation of 1.0 kW·m −2 , the water evaporation rate increases from 1.43 kg·m −2 ·h −1 at 0 V to 1.63 kg·m −2 ·h −1 at 2.0 V. With the utilization of Ti@R-TiO 2 foam as the anode and Ti@TiO 2 foam as the cathode, it becomes feasible to directly oxidize VOCs at the anode and electrocatalytically reduce O 2 at the cathode. Consequently, the VOCs can be effectively eliminated from distilled water. Applying 2.0 V under 1.0 kW·m −2 with oxygen inlet, approximately 25 % removal efficiency was achieved through electrolysis-SDIWE coupling system. This study's approach combining electrolysis with SDIWE presents a promising avenue for advancing SDIWE technology in order to achieve efficient wastewater treatment.

研究领域: 环境科学 · 材料科学
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LANGMUIR · 2020 · IF 3.557

Revealing Molecular-Level Interaction between a Polymeric Drug and Model Membrane Via Sum Frequency Generation and Microfluidics

Chu Wang,Yongsheng Luo,Xu Li,Furong Zhang,Feng Wang,Xiaofeng Han,Ting Wang,Tamás Beke-Somfai,Xiaolin Lu

Body fluids flow all over the body and affect the biological processes at biointerfaces. To simulate such a case, sum frequency generation (SFG) vibrational spectroscopy and a self-designed microfluidic chip were combined together to investigate the interaction between a pH-responsive polymeric drug, poly(α-propylacrylic acid) (PPAAc), and the model cell membranes in different liquid environments. By examining the SFG spectra under the static and flowing conditions, the drug–membrane interaction was revealed comprehensively. The interfacial water layer was screened as the key factor affecting the drug–membrane interaction. The interfacial water layer can prevent the side propyl groups on PPAAc from inserting into the model cell membrane but would be disrupted by numerous ions in buffer solutions. Without flowing, at pH 6.6, the interaction between PPAAc and the model cell membrane was strongest; with flowing, at pH 5.8, the interaction was strongest. Flowing was proven to substantially affect the interaction between PPAAc and the model cell membranes, suggesting that the fluid environment was of key significance for biointerfaces. This work demonstrated that, by combining SFG and microfluidics, new information about the molecular-level interaction between macromolecules and the model cell membranes can be acquired, which cannot be obtained by collecting the normal static SFG spectra.

研究领域: 生物物理学 · 药学
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