INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Jie Chen,Chunlei Qin,Shengzheng Guo,Yuechao Cao,Songgu Wu,Junbo Gong
Probenecid (PB), as a pharmacotherapeutic agent for treating gout, confronts challenges associated with heterogeneous particle size distribution and irregular morphology, impacting postprocessing efficiency. Therefore, further investigation of the nucleation behavior of PB is necessary to address these issues. The nucleation behavior of PB in four solvents was investigated using metastable zone width (MSZW) experiments, the Nývlt model, and the modified Sangwal’s theory. The results revealed that the MSZW broadened, and the interfacial energy (γ) and pre-exponential factor (A) increased with higher cooling rates and lower saturation temperatures. As the chemical potential increases, the critical nucleus size (rcrit) and Gibbs free energy (ΔGcrit) decrease. Infrared (FTIR) spectral analysis suggested that the distinct nucleation behavior of PB in various solvents can be attributed to the competition between intermolecular interactions, predominantly hydrogen bonding and dimerization. Radial distribution function (RDF) analysis and solvation energy calculation suggested that the nucleation behavior becomes more difficult as the solute–solvent intermolecular interactions become stronger.
研究领域:
药学
·
物理化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Junhan Zhang,Chenyue Wang,Chenyang Shen,Muyang Chen,Bingchen He,Zhenhuang Su,Liang Cao,Xingyu Gao
Understanding the interfacial energetics between metal halide perovskites and organic charge transport layers is critical for optimizing charge transport and achieving high-performance optoelectronic devices. While significant progress has been made in improving device efficiency, the fundamental interfacial electronic structure, particularly the influence of fabrication methods on energy level alignments, remains insufficiently explored. In this study, we compare CsPbI 2 Br films fabricated via spin coating and vacuum co-evaporation, using rubrene as a model hole-transporting layer. Ultraviolet photoelectron spectroscopy (UPS) and X-ray photoelectron spectroscopy (XPS) reveal that spin-coated CsPbI 2 Br films contain surface iodine vacancies and dangling bonds, which facilitate chemical interactions with rubrene. This results in the emergence of a new state below the valence band maximum and a relatively large hole injection barrier of ∼ 0.6 eV. In contrast, vacuum-evaporated CsPbI 2 Br films exhibit smoother, defect-less surfaces that interact physically with rubrene. The resulting interfacial electron transfer induces a band bending like effect, along with a reduced hole injection barrier of ∼ 0.4 eV, favoring more efficient hole collection. These findings highlight the critical role of fabrication techniques in modulating interfacial energetics and charge injection barriers through structural and electronic modifications, offering essential insights into interface engineering strategies for optimizing the performance of perovskite-based optoelectronic devices.
研究领域:
材料科学
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物理化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 14
·6795-6803
·
IF 11.301
Lang Pei,Jiasong Zhong,Taozhu Li,Wangfeng Bai,Shiting Wu,Yongjun Yuan,Yifan Chen,Zhengtao Yu,Shicheng Yan,Zhigang Zou
Developing a highly efficient and low-cost oxygen-evolution-reaction (OER) electrocatalyst is an important route to overcome the rate-determining step of water splitting. Here, we directly grew a CoS2 nanoarray core with an N-doped graphitic carbon (NGC) shell on Ni foam (NF) to construct a core–shell nanorod array electrode, CoS2@NGC@NF. The CoS2 core with a high work function (∼5.5 eV) tends to capture electrons from the NGC layer (4.5–5.2 eV) to induce an electron-poor NGC shell with a significant downshift of the carbon Fermi level, facilitating the adsorption of O-containing intermediates and affording decreased activation energy during the OER process. As a result, the three-dimensional NGC encapsulated CoS2 array assembly exhibited excellent electrocatalytic OER activity with a low overpotential of 243 mV at a current density of 10 mA cm−2 and a small Tafel slope of 71 mV dec−1 in 1.0 M KOH. Our findings may suggest that manipulating the interface energetics by the work function difference is a potential route to the design of high-performance OER electrocatalysts.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Nanoscale
·
2021
·Vol. 13
·期 9
·4812-4820
·
IF 7.79
Rong Huang,Songbin Liu,Jinshu Huang,Huiming Liu,Zhiyong Hu,Lili Tao,Bo Zhou
Photon upconversion is a fascinating phenomenon that can convert low-energy photons to high-energy photons efficiently. However, most previous relevant research has been focused on upconversion systems with a sufficiently low lanthanide emitter concentration, such as 2 mol% for Er3+ in an Er–Yb coupled system. Realizing the upconversion from lanthanide heavily doped systems in particular, the emitter sublattice is still a challenge. Here, we report a mechanistic strategy to achieve the intense upconversion of the holmium sublattice in a core–shell-based nanostructure design through interfacial energy transfer channels. This design allowed a spatial separation of Ho3+ and sensitizers (e.g., Yb3+) into different regions and unwanted back energy transfers between them could then be minimized. By taking advantage of the dual roles of Yb3+ as both a migrator and energy trapper, a gradual color change from red to yellowish green was achievable upon 808 nm excitation, which could be further markedly enhanced by surface attaching indocyanine green dyes to facilitate the harvesting of the incident excitation energy. Moreover, emission colors could be tuned by applying non-steady state excitation. Such a fine-tunable color behavior holds great promise in anti-counterfeiting. Our results present a facile but effective conceptual model for the upconversion of the holmuim sublattice, which is helpful for the development of a new class of luminescent materials toward frontier applications.
研究领域:
材料科学
·
光学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Advanced Science
·
2024
·
IF 14.3
Jiaqi Miao,Alan C. H. Tsang
Manipulating small-volume liquids is crucial in natural processes and industrial applications. However, most liquid manipulation technologies involve complex energy inputs or non-adjustable wetting gradient surfaces. Here, a simple and adjustable 3D liquid manipulation paradigm is reported to control liquid behaviors by coupling liquid–air–solid interfacial energy with programmable magnetic fields. This paradigm centers around a hierarchical rectifier with magnetized microratchets, using Laplace pressure asymmetry to enable multimodal directional steering of various surface tension liquids (23–72 mN m −1 ). The scale-dependent effect in microratchet design shows its superiority in handling small-volume liquids across three orders of magnitude (10 0 –10 3 µL). Under programmed magnetic fields, the rectifier can reconfigure its morphology to harness interfacial energy to exhibit richer liquid behaviors without dynamic real-time control. Reconfigured rectifiers show improved rectification performance in the inertia-dominant fluid regime, i.e., a remarkable 2000-fold increase in the critical Weber number for pure ethanol. Moreover, the rectifier's switchable reconfigurations offer flexible control over liquid transport directions and spatiotemporally controllable 3D liquid manipulation reminiscent of inchworm motions. This scalable liquid manipulation paradigm promotes versatile engineering and biochemistry applications, e.g., portable liquid purity testing (screening resolution <1 mN m −1 ), logical open-channel microfluidics, and automated chemical reaction platforms.
研究领域:
材料科学
·
生物工程
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Nano
·
2025
·
IF 16
Jiaqi Miao,Alan C. H. Tsang
Structured surfaces leverage interfacial energy for directional liquid manipulation without external power, showing tremendous potential in microfluidics, green energy and biomedical applications. While the interplay of interfacial energy between solid surfaces and liquids is crucial for liquid manipulation, a systematic understanding of how the balance in liquid–solid interfacial energy affects liquid behaviors remains lacking. Here, using the curvature-ratchet surface as a generic example, we reveal the complex directional liquid dynamics inherent in the subtle regulation of liquid–solid interfacial energy. We show that curvature and tilt features regulate Laplace pressure asymmetry to enable directional, bidirectional and reverse liquid manipulation. These processes can be modulated by surface free energy and liquid surface tension, and we define their ratio as a new dimensionless number ζ to characterize the liquid–solid interfacial energy relationship. The balanced liquid control happens when ζ ∼ 1, which facilitates versatile liquid behaviors, e.g., fan-shaped spreading, gradient-induced redirection, and back-and-forth transport on various surface array arrangements, all resulting from matching structural designs with the proper ζ. Inspired by this, we showcase an innovative liquid-based information encryption technique, where the liquid displays correct information on preprogrammed surfaces only at designated ζ values. This study lays the groundwork for smart directional liquid manipulation and broadens its application domains.
研究领域:
材料科学
·
微流体技术
·
生物医学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
·
2020
·
IF 5.065
Jing Yang,Shijie Xu,Jingkang Wang,Junbo Gong
The experimental metastable zone widths (MSZWs) of ethyl vanillin (EVA) in ethanol, n-propanol, and n-butanol were measured by the polythermal method to describe the nucleation behavior of its unseeded cooling crystallization. In the framework of the classical nucleation theory (CNT), the effects of saturation temperature T 0 and cooling rate R on MSZWs were mainly investigated by employing the modified Sangwal's theory to derive the pre-exponential factor A and the interfacial energy γ . It was found that when T 0 decreases or R increases (resulting in a lower nucleation temperature), the value of γ increases proportionally, whereas the value of A changes slightly, which is largely determined by the type of solvent . Thus, the MSZWs in the given solvents are dominated by the change in the thermodynamic term γ . At lower T 0 , a large chemical driving force ∆ μ is required to induce the nucleation event owing to the higher value of γ , which means that the solute molecules should pay more of a penalty to create the crystallite surface. Thus, the results indicate that the occurrence of nucleation depends on the balance between the chemical driving force ∆ μ for nucleation and the initial saturation temperature T 0 .
研究领域:
化学工程
·
物理化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Wenwu Liu,Yixiao Lei,Caixia Li,Shiji Da,Yawen Zheng,Youzhi Wu
In ambient air, a long-chain dodecafluorosuberic acid (DFSA) with lower Young’s modulus was introduced to improve the mechanical compatibility of perovskite/carbon interface. Firstly, the carbonyl groups C O and F – in DFSA can passivate the intrinsic defects of perovskite, the DFSA effectively reduces the Young’s modulus of the perovskite and mitigates residual stress generated during perovskite annealing procedure. Most importantly, DFSA significantly enhances the Young’s modulus compatible degree between DFSA-CH 3 NH 3 PbI 3 (DFSA-MAPbI 3 , 35.8 GPa) and carbon (6.3 GPa), alleviating the interfacial stress concentration. Based on quantitatively analysis, interfical crack driving energy ( G d ) is reduced from 0.63 to 0.43 J m −2 , while the adhesive fracture energy ( G a ) is increased from 0.47 to 0.54 J m −2 , which reduces the probability of crack propagation and ductile delamination, and is conducive to the extraction and transmission of photogenerated carrior. This was also verified in finite element simulations. Finally, the photoelectric conversion efficiency (PCE) of the organic-inorganic hybrid perovskite (MAPbI 3 ) PSC device is improved from 10.27 % to optimal 14.12 %. After service at room temperature with relative humidity (RH) of 50–55 % and high temperature of 85 °C for 720 h, the original efficiency is maintained at 72 % and 89 %, respectively.
研究领域:
材料科学
·
能源技术
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED MATERIALS
·
2024
·Vol. 36
·期 25
·2400451
·
IF 27.4
Zhen Tang,Dan Yang,Hengyu Guo,Shiquan Lin,Zhong Lin Wang
Wettability significantly influences various surface interactions and applications at the liquid–solid interface. However, the understanding is complicated by the intricate charge exchange occurring through contact electrification (CE) during this process. The understanding of the influence of triboelectric charge on wettability remains challenging, especially due to the complexities involved in concurrently measuring contact angles and interfacial electrical signals. Here, the relationship is investigated between surface charge density and change of contact angle of dielectric films after contact with water droplets. It is observed that the charge exchange when water spared lead to a spontaneous wetting phenomenon, which is termed as the contact electrification induced wetting (CEW). Notably, these results demonstrate a linear dependence between the change of contact angle (CA) of the materials and the density of surface charge on the solid surface. Continuous CEW tests show that not only the static CA but also the dynamics of wetting are influenced by the accumulation charges at the interface. The mechanism behind CEW involves the redistribution of surface charges on a solid surface and polar water molecules within liquid. This interaction results in a decrease in interface energy, leading to a reduction in the CA. Ab initio calculations suggest that the reduction in interface energy may stem from the enhanced surface charge on the substrate, which strengthens the hydrogen bond interaction between water and the substrate. These findings have the potential to advance the understanding of CE and wetting phenomena, with applications in energy harvesting, catalysis, and droplet manipulation at liquid–solid interfaces.
研究领域:
材料科学
·
物理化学
·
表面科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Research
·
2023
·
IF 11
Siyang Li,Panpan Zhu,Yaoting Xue,Lei Wang,Tuck-Whye Wong,Xuxu Yang,Haofei Zhou,Tiefeng Li,Wei Yang
Heterogeneous nucleation plays a critical role in the phase transition of water, which can cause damage in various systems. Here, we report that heterogeneous nucleation can be inhibited by utilizing hydrogel coatings to isolate solid surfaces and water. Hydrogels, which contain over 90% water when fully swelled, exhibit a high degree of similarity to water. Due to this similarity, there is a great energy barrier for heterogeneous nucleation along the water–hydrogel interface. Additionally, hydrogel coatings, which possess polymer networks, exhibit higher fracture energy and more robust adhesion to solid surfaces compared to water. This high fracture and adhesion energy acts as a deterrent for fracture nucleation within the hydrogel or along the hydrogel–solid interface. With a hydrogel layer approximately 100 μm thick, the boiling temperature of water under atmospheric pressure can be raised from 100 to 108 °C. Notably, hydrogel coatings also result in remarkable reductions in cavitation pressure on multiple solid surfaces. We have demonstrated the efficacy of hydrogel coatings in preventing damages resulting from acceleration-induced cavitation. Hydrogel coatings have the potential to alter the energy landscape of heterogeneous nucleation on the water–solid interface, making them an exciting avenue for innovation in heat transfer and fluidic systems.
研究领域:
材料科学
·
热力学
·
流体力学
✓ 已验证
DOI
高影响因子
CONSTRUCTION AND BUILDING MATERIALS
·
2022
·
IF 7.693
Lingyun Kong,Songxiang Zhu,Xiujie Quan,Yi Peng
The demulsification of emulsified asphalt is required to form the adhesion of the asphalt. Using conductivity experiments and validated molecular dynamics simulations, this paper investigated the micro-mechanism of the demulsification process of emulsified asphalt. The results show that the phenyl functional group causes a decrease in the diffusion coefficient of the SiO 2 aggregate system and an increase in its interfacial energy, whereas an inverse tendency occurs in the CaCO 3 aggregate system, which significantly affects the demulsification rate and adhesion between the emulsified asphalt and aggregates. The electrostatic force between Na + and CaCO 3 allows the emulsifiers to adsorb well to the aggregates, and the demulsification time can be controlled by adjusting the relative content of phenyl functional groups and Na + . The adsorption rate and the adsorption amount of dodecyl anion emulsified asphalt on the aggregate surface grow with increasing phenyl functional group content, leading to a faster demulsification rate of the system and enabling the demulsification rate of the SiO 2 emulsified asphalt system to be greater than that of the CaCO 3 system. This research demonstrates that the demulsification process of emulsified asphalt can potentially be adjusted by managing the relative content of Na + and phenyl functional groups in the emulsifier, which gives critical insight into improving the design and construction of asphalt pavements.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
WATER RESEARCH
·
2018
·
IF 7.051
Kai-Ge Lu,Haiou Huang
Silica scaling of reverse osmosis membranes in brackish water desalination is less understood than hardness scaling due to the complex silica behaviors at the membrane/water interface. In this study, -COOH, -SO 3 H, -NH 2 and -OH functional groups were introduced onto polyamide membranes to create distinct surface physicochemical properties . The resulting membranes were further studied under similar scaling conditions to yield temporal flux loss data that were empirically interpreted by a logistic growth model. The scaled membranes were also characterized by complementary analytical techniques. It was found that permeate flux loss was strongly correlated to the initial silica layer formed by direct interaction between reactive silanol (Si-OH) and reciprocal groups on the membrane surface, rather than the entire scaling layer. Importantly, membrane surface properties dictated the initial silica layer formation through three possible mechanisms, i.e., electrostatic repulsion, competitive adsorption, and interfacial energy change. Of these, electrostatic repulsion was identified as the primary one. Therefore, by modifying the membrane surface properties, the three aforementioned mechanisms may be enhanced to favor the formation of a loose, disordered initial silica scaling layer. Accordingly, membrane flux loss may be mitigated. This finding provided important insights into the design heuristics of scaling-resistant reverse osmosis membrane for brackish water desalination.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
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