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ACS ES&T Water · 2024 · IF 4.8

Exploring Real-Time Monitoring of Adsorption Processes at Solid–Liquid Interfaces through Chemical Force Microscopy

Yuyao Zhang,Zhonghao Wan,Tingjie Zhan

Adsorption processes in aqueous environments are critical for understanding pollutant dynamics, assessing ecological risks, and safeguarding human health. Many techniques have been developed to study solid–liquid adsorption including spectroscopic methods. However, there is still a need for supplementary techniques that provide real-time, atomic-scale, and in situ monitoring to achieve a more comprehensive understanding of adsorption mechanisms. Herein, chemical force microscopy (CFM) was utilized to measure hydrophobic interactions to determine the pollutant adsorption at the solid–liquid interface. The hydrophobized probe was employed to ramp onto the adsorbent substrate of interest under aqueous conditions. The forces detected were dependent on the surface adsorption of pollutants on the adsorbent surfaces. From the CFM force–distance curves, adsorption kinetics was obtained for tetracycline and phenol on the graphite surface, which aligned with the results from batch experiments and the in situ streaming potential test. Our findings demonstrate a novel strategy for the real-time interpretation of adsorption processes utilizing CFM that holds the potential to revolutionize studies in environmental interfaces.

CAS / MDL: 3069-40-7
研究领域: 环境科学 · 表面化学
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JOURNAL OF POWER SOURCES · 2022 · IF 9.794

Ionic covalent organic frameworks triggered efficient synergy: Li+ de-solvation and the formation of LiF-rich interphase

Weifeng Zhang,Guoxing Jiang,Wenwu Zou,Longhai Zhang,Shulian Li,Shengguang Qi,Xiujun Wang,Zhiming Cui,Huiyu Song,Li Du,Zhenxing Liang

The parasitic side reaction between the electrolyte and the lithium metal (Li 0 ) forms an unstable heterogeneous interphase, causing the poor reversibility of Li plating/stripping. The rational design of protection layer on Li 0 anode is imperative to inhibit side reactions and achieve fast Li  +  transport on the Li 0 /electrolyte interface. Herein, by firstly coordinating the bis(fluorosulfonyl)imide anion (FSI − ) to the protection layer, a layer consisting of 2D ionic vinylene-linked covalent organic frameworks (ivCOF-FSI) is proposed to stabilize the Li 0 /electrolyte interface. As demonstrated theoretically and experimentally, the triazine group in the cationic framework is identified to promote Li + de-solvation process while partial FSI − prefers to form LiF-rich interphase. Attributed to these superiorities, the ivCOF-FSI layer endows the Li 0 /electrolyte interface with high reversibility in carbonate-based electrolytes by simultaneously suppressing the side effect and achieving rapid Li + transfer. Combined with the high stability of solid-liquid interface, the LiFePO 4 full cells with ivCOF-FSI/Li anode display enhanced cyclability under a high cathode loading of 9.4 mg cm −2 and a low negative/positive capacity ratio of 5. This work provides a novel route for stabilizing the interfacial chemistry of solid-liquid interface, aiming to pave the way for the next-generation high-energy-density batteries .

研究领域: 材料科学 · 电化学
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Nano Energy · 2024 · IF 16.8

A green approach to induce and steer chemical reactions using inert solid dielectrics

Shaoxin Li,Zhiwei Zhang,Puguang Peng,Xiang Li,Zhong Lin Wang,Di Wei

The solid-liquid interface plays pivotal role in chemical reactions, but the contact electrification (CE) at interface is usually overlooked. Recently the CE effect was reported to promote interfacial chemistry as well as catalysis for organic pollutants. However, the exact role of CE in various chemical reactions remained unclear, and understanding of its influences has been a long-lasting challenge. Here, we proposed a paradigm of contact-electro-chemistry (CE-Chemistry) via CE between solid dielectrics and liquids to show how their physical contact can induce and even guide reactions. CE-Chemistry was proved to exist ubiquitously in various reactions within both aqueous and non-aqueous systems, including redox reactions , organic polymerizations, pollutant degradations etc. The trade-off between electron transfer and ion migration at the solid dielectrics and liquids interface was elucidated to optimize reactions. Furthermore, a guidance that unified the concept of work functions, electronegativity in triboelectric series and standard electrode potentials was developed based on the electron transfer capabilities to steer reactions and assess their extent. This work not only reveals the physicochemical essence of CE, but also offers a new perspective to investigate the interface interaction across interdisciplinary subjects of physics, chemistry and material science.

CAS / MDL: 10101-89-0
研究领域: 化学 · 材料科学 · 物理学
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ACS Nano · 2024 · IF 15.8

Dual-Steric Hindrance Modulation of Interface Electrochemistry for Potassium-Ion Batteries

Ningning Chen,Yinshuang Pang,Zhi Liu,Nai-Lu Shen,Hong Chen,Wanying Zhang,Qingxue Lai,Xiaoping Yi,Yanyu Liang

Electrolyte chemistry regulation is a feasible and effective approach to achieving a stable electrode–electrolyte interface. How to realize such regulation and establish the relationship between the liquid-phase electrolyte environment and solid-phase electrode remains a significant challenge, especially in solid electrolyte interphase (SEI) for metal-ion batteries. In this work, solvent/anion steric hindrance is regarded as an essential factor in exploring the electrolyte chemistry regulation on forming ether-based K+-dominated SEI interface through the cross-combination strategy. Theoretical calculation and experimental evidence have successfully indicated a general principle that the combination of increasing solvent steric hindrance with decreasing anion steric hindrance indeed prompts the construction of an ideal anion-rich sheath solvation structure and guarantees the cycling stability of antimony-based alloy electrode (Sb@3DC, Sb nanoparticles anchored in three-dimensional carbon). These confirm the critical role of electrolyte modulation based on molecular design in the formation of stable solid–liquid interfaces, particularly in electrochemical energy storage systems.

CAS / MDL: 120-65-0 110-71-4
研究领域: 电化学 · 材料科学
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Nano Energy · 2024 · IF 16.8

Macroscopic liquid superlubric triboelectric nanogenerator: An in-depth understanding of solid-liquid interfacial charge behavior

Kaiqiang Wang,Xinyi Wang,Yilin Sun,Zhuolin Wu,Hanli Zhang,Ke Xiao,Jiayu Du,Jinjin Li,Jianbin Luo

Triboelectric nanogenerator (TENG) has been seen as one of the most promising energy harvesting technologies. However, there are an irreconcilable contradiction between low friction and high electrical output performance of the TENG. Here, we have devised a macroscale liquid superlubric triboelectric nanogenerator based on solid-liquid-solid structure, leveraging the concept of liquid superlubricity technology, resulting in a remarkable increase in both the open circuit voltage and short-circuit current by 53.0 % and 58.4 %, respectively. This huge increase in electrical output performance is accompanied by a 99.1 % reduction in friction coefficient (≈ 0.0025) and 99.993 % reduction in wear rate (≈ 0.76×10 −7 mm 3 /N·m), when compared to those of a lubricant-free triboelectric nanogenerator. This work delves into the lubrication and charge transfer mechanisms. The liquid superlubricity technology achieves friction reduction through a hybrid mechanism combining boundary and hydrodynamic lubrication. And the high outputs arise from the charges transfer at solid-liquid interface. The triboelectric charges generated by the friction pair are transferred from solid to the lubricating liquid. Meanwhile, the lubricating liquid promotes electron transfer and contributes additional electrons. Our work provides profound insights into the lubrication and charge transfer mechanisms at solid-liquid interfaces, and addresses the paradox of high output and low friction in TENGs.

CAS / MDL: 544-76-3
研究领域: 材料科学 · 能源技术 · 表面工程
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Nature Communications · 2025 ·Vol. 16 ·期 1 ·1-8 · IF 15.7

Solid-liquid interface charge transfer for generation of H2O2 and energy

Hu Yunhao,Yang Weifeng,Ma Yuji,Qiu Yong,Wei Wei,Wu Bo,Li Kerui,Li Yaogang,Zhang Qinghong,Xiao Ru,Hou Chengyi,Wang Hongzhi

Solid-liquid contact electrification is a widespread interface phenomenon in nature. Recent research and theory demonstrate that electron transfer during this process holds the potential to initiate interfacial chemical reactions. Here, we design a dual-functional device for generation of H 2 O 2 and energy. Interfacial chemical reactions and solid-liquid contact charging occur simultaneously during the liquid phase flow process. Specifically, electron transfer at the solid-liquid interface induces the formation of hydroxyl radicals (·OH) in the liquid phase, leading to spontaneous generation of H 2 O 2 . The transfer of charges at the solid-liquid interface is accompanied by energy transfer. By designing an external electrode structure, we can effectively harvest the energy from the flowing liquid phase, yielding an output power of up to 5.8 kW/m 3 for water.

CAS / MDL: 68-12-2 64-18-6 67-64-1
研究领域: 材料科学 · 化学工程 · 能源科学
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Science Advances · 2021 ·Vol. 7 ·期 23 · IF 14.143

Renatured hydrogel painting

Zhaoxiang Yang,Yonglin He,Shenglong Liao,Yingchao Ma,Xinglei Tao,Yapei Wang

Hydrogel coatings pave an avenue for improving the lubricity, biocompatibility, and flexibility of solid surfaces. From the viewpoint of practical applications, this work establishes a scalable method to firmly adhere hydrogel layers to diverse solid surfaces. The strategy, termed as renatured hydrogel painting (RHP), refers to adhering dehydrated xerogel to a surface with appropriate glues, followed by the formation of a hydrogel layer after rehydration of the xerogel. With the benefits of simplicity and generality, this strategy can be readily applied to different hydrogel systems, no matter what the substrate is. Hydrogel adhesion is demonstrated by its tolerance against mechanical impact with hydrodynamic shearing at 14 m/s. This method affords powerful supplements to renew the surface chemistry and physical properties of solid substrates. In addition, we show that the RHP technique can be applied to living tissue, with potential for clinical applications such as the protection of bone tissue.

研究领域: 材料科学 · 生物医学工程 · 表面化学
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Materials · 2022 ·Vol. 16 ·期 1 ·9 · IF 3.748

A Form of Non-Volatile Solid-like Hexadecane Found in Micron-Scale Silica Microtubule

Weiqing An,Xiangan Yue,Jirui Zou,Lijuan Zhang,Yu-Chun Fu,Rongjie Yan

Anomalous solid-like liquids at the solid–liquid interface have been recently reported. The mechanistic factors contributing to these anomalous liquids and whether they can stably exist at high vacuum are interesting, yet unexplored, questions. In this paper, thin slices of silica tubes soaked in hexadecane were observed under a transmission electron microscope at room temperature. The H-spectrum of hexadecane in the microtubules was measured by nuclear magnetic resonance. On the interior surface of these silica tubes, 0.2–30 μm in inside diameter (ID), a layer (12–400 nm) of a type of non-volatile hexadecane was found with thickness inversely correlated with the tube ID. A sample of this anomalous hexadecane in microtubules 0.4 μm in ID was found to be formable by an ion beam. Compared with the nuclear magnetic resonance H-spectroscopy of conventional hexadecane, the characteristic peaks of this abnormal hexadecane were shifted to the high field with a broader characteristic peak, nuclear magnetic resonance hydrogen spectroscopy spectral features typical of that of solids. The surface density of these abnormal hexadecanes was found to be positively correlated with the silanol groups found on the interior silica microtubular surface. This positive correlation indicates that the high-density aggregation of silanol is an essential factor for forming the abnormal hexadecane reported in this paper.Keywords:solid-liquid interface;transmission electron microscope;silica;microtubules;hexadecane;surface-silanol

CAS / MDL: 7664-39-3
研究领域: 材料科学 · 化学
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CHEMICAL ENGINEERING JOURNAL · 2019 · IF 8.355

Adsorption and competition investigation of phenolic compounds on the solid-liquid interface of three-dimensional foam-like graphene oxide

Weixue Wang,Qiaobin Gong,Zhe Chen,Weidong Devin Wang,Qiang Huang,Shuang Song,Jianrong Chen,Xiangke Wang

Phenolic contaminants existed widely in ecological environment. Due to the various structure and functional groups, the interaction behavior of phenolic organic compounds with adsorbent was complex and changeable. Therefore, the exploration of adsorption and competition about phenolic compounds on solid-liquid interface in aqueous solution is of great significance. Herein, through a simple sugar-blowing route and post-oxidation modification, a free-standing, large-scale nanoporous three-dimensional graphene oxide (3D GO) was achieved. The synthesized 3D GO possessed hierarchical interconnected porous structure and abundant active sites, which showed excellent removal performance for many phenolic compounds. The maximum adsorption capacity ( q max ) was 135.6 mg/g, 191.3 mg/g, 237.7 mg/g, 398.6 mg/g, 420.9 mg/g and 585.8 mg/g for phenol, 2-chlorophenol (2-CP), 4-chlorophenol (4-CP), 2,4-dichlorophenol (DCP), bisphenol-A (BPA) and 2,4,6-trichlorophenol (TCP) at 25 °C respectively. The competitive adsorption between BPA and TCP on 3D GO was also explored. Batch adsorption experiments and characterization revealed that the outstanding performance benefited from various factors, including structural advantage, electrostatic interaction, π-π interaction, hydrophobic effect, hydrogen bond, the synergy of heteroatom and the new active sites of preferential adsorbed organics. The cost-effective and highly active 3D GO adsorbent showed great promising in environmental field, and supplied insight to understand the underlying behavior of phenolic compounds on the solid-liquid interface.

研究领域: 环境科学 · 材料科学
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY · 2022 · IF 4.598

The electrochemical reduction process of converting solid sulfides to liquid metals in molten salt: A case study of ZnS

Yanyang Guo,Xianyang Li,Zhuqing Zhao,Jiakang Qu,Qiang Ma,Dihua Wang,Huayi Yin

The electrochemical desulfurization in the molten salt is a promising green route to extract metals directly from sulfide ores. However, less attention has been paid to the process of converting solid sulfides to liquid metals, especially the evolution of the solid sulfide/liquid metal interface. Herein, the electrochemical desulfurization process of converting solid ZnS to liquid Zn in NaCl-KCl was studied through electrochemical measurements, wettability test, and postmortem analysis of the electrolytic product. The continuous solid-to-liquid reaction in the molten salt is ascribed to the poor wettability of liquid Zn on the solid ZnS which prevents the liquid Zn from fully covering the sulfide surface and allows S 2- ions transfer. The desulfurization process consisted of three stages: two-step reduction of zinc sulfide and the reduction of Na + on the liquid Zn to form Na-Zn alloys. The understanding of the solid-to-liquid conversion process is helpful to understand various solid-to-liquid reactions so as to design efficient electrolyzers.

研究领域: 电化学 · 冶金工程 · 材料科学 · 无机化学 · 能源材料
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Nano Energy · 2023 · IF 17.6

The process of free radical generation in contact electrification at solid-liquid interface

Yi Zhao,Yang Liu,Yuying Wang,Shulan Li,Yi Liu,Zhong Lin Wang,Peng Jiang

Solid-liquid interfaces are ubiquitous in nature and widely used in various applications such as catalysis, sensing, batteries , etc. Recently, we found the existence of electron transfer at the interface in solid-liquid contacting, and proposed a “two-step” theory for the formation of solid-liquid electric double layer (EDL). In this work, we found that hydroxyl radical (·OH) was generated when the droplet contact with the tube inner wall without external interference, and the concentration of·OH was increased with increasing pH, demonstrating that the·OH was generated from hydroxide ions (OH - ) by electron transfer during contact electrification. This can be further supported by the fact that capillaries made of materials with stronger electron-withdrawing ability could generate more·OH. Interestingly, superoxide anion radical (·O 2 - ) was not generated at the solid-liquid interface if no external energy is provided. However, if ultrasonic was applied,·O 2 - could be generated at the solid-liquid interface, because ultrasonication provides transition energy for the electron to transfer from the solid to O 2 at the interface. Based on the generation of reactive oxygen species (·OH and·O 2 - ), we demonstrated a proof-of-concept for degradation of tetracycline pollution. This work provides an excellent strategy to study the solid-liquid interface and also provides a new insight into the free radical generation at the interface in solid-liquid contacting.

研究领域: 化学 · 环境科学 · 材料科学
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Nature Communications · 2025 ·Vol. 16 ·期 1 ·1-11 · IF 15.7

Proton-coupled electron transfer controls peroxide activation initiated by a solid-water interface

Chen Jian-Hua,Li Wan-Ting,Cai Kun-Yu,Tu Hui-Jie,Long Zi-Tong,Akhtar Shoaib,Liu Lin-Dong

Decentralized water treatment technologies, designed to align with the specific characteristics of the water source and the requirements of the user, are gaining prominence due to their cost and energy-saving advantages over traditional centralized systems. The application of chemical water treatment via heterogeneous advanced oxidation processes using peroxide (O–O) represents a potentially attractive treatment option. These processes serve to initiate redox processes at the solid-water interface. Nevertheless, the oxidation mechanism exemplified by the typical Fenton-like persulfate-based heterogeneous oxidation, in which electron transfer dominates, is almost universally accepted. Here, we present experimental results that challenge this view. At the solid-liquid interface, it is demonstrated that protons are thermodynamically coupled to electrons. In situ quantitative titration provides direct experimental evidence that the coupling ratio of protons to transferred electrons is almost 1:1. Comprehensive thermodynamic analyses further demonstrate that a net proton-coupled electron transfer occurs, with both protons and electrons entering the redox cycle. These findings will inform future developments in O–O activation technologies, enabling more efficient redox activity via the tight coupling of protons and electrons.

研究领域: 环境科学 · 化学工程 · 材料科学
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