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Review: Tip-based vibrational spectroscopy for nanoscale analysis of emerging energy materials

Amun JARZEMBSKI, Cedric SHASKEY, Keunhan PARK

《能源前沿（英文）》 2018年 第12卷 第1期   页码 43-71 doi: 10.1007/s11708-018-0524-8

摘要： Vibrational spectroscopy is one of the key instrumentations that provide non-invasive investigation of structural and chemical composition for both organic and inorganic materials. However, diffraction of light fundamentally limits the spatial resolution of far-field vibrational spectroscopy to roughly half the wavelength. In this article, we thoroughly review the integration of atomic force microscopy (AFM) with vibrational spectroscopy to enable the nanoscale characterization of emerging energy materials, which has not been possible with far-field optical techniques. The discussed methods utilize the AFM tip as a nanoscopic tool to extract spatially resolved electronic or molecular vibrational resonance spectra of a sample illuminated by a visible or infrared (IR) light source. The absorption of light by electrons or individual functional groups within molecules leads to changes in the sample’s thermal response, optical scattering, and atomic force interactions, all of which can be readily probed by an AFM tip. For example, photothermal induced resonance (PTIR) spectroscopy methods measure a sample’s local thermal expansion or temperature rise. Therefore, they use the AFM tip as a thermal detector to directly relate absorbed IR light to the thermal response of a sample. Optical scattering methods based on scanning near-field optical microscopy (SNOM) correlate the spectrum of scattered near-field light with molecular vibrational modes. More recently, photo-induced force microscopy (PiFM) has been developed to measure the change of the optical force gradient due to the light absorption by molecular vibrational resonances using AFM’s superb sensitivity in detecting tip-sample force interactions. Such recent efforts successfully breech the diffraction limit of light to provide nanoscale spatial resolution of vibrational spectroscopy, which will become a critical technique for characterizing novel energy materials.

关键词： vibrational spectroscopy     atomic force microscopy     photo-thermal induced resonance     scanning near-field optical microscopy     tip-enhanced Raman spectroscopy     photo-induced force microscopy     molecular resonances     surface phonon polaritons     energy materials    

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Solar fuel from photo-thermal catalytic reactions with spectrum-selectivity: a review

Sanli TANG, Jie SUN, Hui HONG, Qibin LIU

《能源前沿（英文）》 2017年 第11卷 第4期   页码 437-451 doi: 10.1007/s11708-017-0509-z

摘要： Solar fuel is one of the ideal energy sources in the future. The synergy of photo and thermal effects leads to a new approach to higher solar fuel production under relatively mild conditions. This paper reviews different approaches for solar fuel production from spectrum-selective photo-thermal synergetic catalysis. The review begins with the meaning of synergetic effects, and the mechanisms of spectrum-selectivity and photo-thermal catalysis. Then, from a technical perspective, a number of experimental or theoretical works are sorted by the chemical reactions and the sacrificial reagents applied. In addition, these works are summarized and tabulated based on the operating conditions, spectrum-selectivity, materials, and productivity. A discussion is finally presented concerning future development of photo-thermal catalytic reactions with spectrum-selectivity.

关键词： photo-thermal catalysis     spectrum-selectivity     solar fuel     full-spectrum    

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Hypoxia-induced activity loss of a photo-responsive microtubule inhibitor azobenzene combretastatin A4

Yang An, Chao Chen, Jundong Zhu, Pankaj Dwivedi, Yanjun Zhao, Zheng Wang

《化学科学与工程前沿（英文）》 2020年 第14卷 第5期   页码 880-888 doi: 10.1007/s11705-019-1864-6

摘要： The conformation-dependent activity of azobenzene combretastatin A4 (Azo-CA4) provides a unique approach to reduce the side-effects of chemotherapy, due to the light-triggered conformation transition of its azobenzene moiety. Under hypoxic tumor microenvironment, however, the high expression of azoreductase can reduce azobenzene to aniline. It was postulated that the Azo-CA4 might be degraded under hypoxia, resulting in the decrease of its anti-tumor activity. The aim of this study was to verify such hypothesis in HeLa cells . The quantitative drug concentration analysis shows the ratiometric formation of degradation end-products, confirming the bioreduction of Azo-CA4. The tubulin staining study indicates that Azo-CA4 loses the potency of switching off microtubule dynamics under hypoxia. Furthermore, the cell cycle analysis shows that the ability of Azo-CA4 to induce mitotic arrest is lost at low oxygen content. Therefore, the cytotoxicity of Azo-CA4 is compromised under hypoxia. In contrast, combretastatin A4 as a positive control maintains the potency to inhibit tubulin polymerization and break down the nuclei irrespective of light irradiation and oxygen level. This work highlights the influence of hypoxic tumor microenvironment on the anti-tumor potency of Azo-CA4, which should be considered during the early stage of designing translational Azo-CA4 delivery systems.

关键词： hypoxia     microtubule inhibitor     drug delivery     azo-combretastatin A4     photo-responsive    

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Photo-induced surface frustrated Lewis pairs for promoted photocatalytic decomposition of perfluorooctanoic

《环境科学与工程前沿（英文）》 2023年 第17卷 第1期 doi: 10.1007/s11783-023-1603-6

摘要：

● Terminal carboxylate group activation is PFOA degradation’s rate-limiting step.

关键词： Heterogeneous photocatalysis     Surface frustrated Lewis pairs     Perfluorooctanoic acid     Defluorination efficiency     Environmental remediation    

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Experimental and computational assessment of 1,4-Dioxane degradation in a photo-Fenton reactive ceramic

《环境科学与工程前沿（英文）》 2021年 第15卷 第5期 doi: 10.1007/s11783-020-1341-y

摘要：

• 1,4-Dioxane was degraded via the photo-Fenton reactive membrane filtration.

关键词： Photo-Fenton     Ceramic membrane     1     4-Dioxane     Goethite    

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Selective reduction of NO by photo-SCR with ammonia in an annular fixed-film photoreactor

YiangChen CHOU, Young KU

《环境科学与工程前沿（英文）》 2012年 第6卷 第2期   页码 149-155 doi: 10.1007/s11783-010-0296-9

摘要： Gaseous NO was photocatalytically reduced at room temperature by photo-assisted selective catalytic reduction (photo-SCR) with ammonia over TiO in this study. NO reduction efficiency and N selectivity were determined from gases composition at the outlet stream of photoreactor. Effect of operating conditions, e.g. light intensity and inlet concentrations of ammonia and oxygen, on the NO reduction efficiency and N selectivity were discussed to determine the feasible operating condition for photocatalytic reduction of NO. Experimental results showed that selective catalytic reduction of NO with ammonia over TiO in the presence of oxygen was a spontaneous reaction in dark. The photoirradiation on the TiO surface caused remarkable photocatalytic reduction of NO to form N , NO , and N O under 254 nm UV illuminations, while almost 90% of N selectivity was achieved in this study. The ammonia and oxygen molecules played the roles of reductant and oxidant for NO reduction and active sites regeneration, respectively. The reduction of NO was found to be increased with the increase of inlet ammonia and oxygen concentrations until specific concentrations because of the limited active sites on the surface of TiO . The kinetic model proposed in this study can be used to reasonably describe the reaction mechanism of photo-SCR.

关键词： photo-SCR     photocatalysis     NO reduction     Eley-Rideal model    

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Lignin-based electrospun nanofiber membrane decorated with photo-Fenton Ag@MIF-100(Fe) heterojunctions

《化学科学与工程前沿（英文）》 2023年 第17卷 第7期   页码 930-941 doi: 10.1007/s11705-023-2309-9

摘要： Membrane technology for wastewater remediation has aroused wide interest owing to its unique properties and potential applications. However, it remains challenging to explore green, efficient and robust membrane material and technique for complex wastewater treatment. Herein, we proposed using a simple electrospinning and in situ seeding method to fabricate a lignin-based electrospun nanofiber membrane (LENM) decorated with photo-Fenton Ag@MIL-100(Fe) heterojunctions for efficient separation of oil/water emulsions and degradation of organic dye. Thanks to the embedded lignin in LENM, an ultrahigh MIL-100(Fe) loading (53 wt %) with good wettability and high porosity was obtained. As a result, the hybrid Ag@MIL-100(Fe)/LENM exhibited excellent oil/water emulsions separation efficiency (more than 97%) without a compromise of water flux. Moreover, the hybrid membrane showed an excellent dye removal with degradation of 99% methylene blue within 30 min under illumination, which is attributed to a synergy of dye adsorption/enrichment and photo-Fenton catalytic degradation from Ag@MIL-100(Fe). Therefore, the lignin-based photo-Fenton hybrid membrane can lay the foundation for the preparation and application of green, sustainable and versatile membrane materials and technologies for efficient complex wastewater remediation.

关键词： lignin     electrospinning     heterojunctions     photo-Fenton catalysis     wastewater remediation    

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Synthesis, spectroscopic, and electrochemical properties of two dyads consisted of tetrathiafulvalene and carbazole

Guoqiao LAI, Yibo LIU, Meijiang LI, Yongjia SHEN

《化学科学与工程前沿（英文）》 2009年 第3卷 第2期   页码 192-195 doi: 10.1007/s11705-009-0015-x

摘要： Two donor-σ-acceptor molecules containing tetrathiafulvalene (TTF) and carbazole moieties were synthesized by the reaction of 9-(4-bromo-butyl)-carbazole ( ) with 2,6-bis(hexylthio)-3-(2-cyanoethylthio)-7-(methylthio)-tetrathiafulvalene ( ) or 2,6-bis(2-cyanoethylthio)-3,7-bis(methylthio)tetrathiafulvalene ( ) in the presence of CsOH·H O, respectively. The structures of the molecules were characterized by H NMR, C NMR, MS, and elemental analyses. They showed negligible intramolecular charge-transfer interaction in their ground states as indicated by their UV-Vis spectroscopics and cyclic voltammetry results. Compared with carbazole, their fluorescence was strongly quenched, which implied that a photo induced electron transfer (PET) interaction between TTF and carbazole moieties occurred.

关键词： donor-σ-acceptor molecule     intramolecular charge transfer interaction     photo induced electron transfer     tetrathiafulvalene     carbazole    

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Highly selective detection of copper(II) by a “ligand-free” conjugated copolymer in nucleophilic solvents

Weixing Deng, Pengfei Sun, Quli Fan, Lei Zhang, Tsuyoshi Minami

《化学科学与工程前沿（英文）》 2020年 第14卷 第1期   页码 105-111 doi: 10.1007/s11705-019-1791-6

摘要： The synthesis of -cyclohexyl carbamate-attached fluorene- -phenylene copolymer (PFPNCC) and the use of PFPNCC as a “ligand-free” fluorescent chemosensor for Cu(II) are described. Addition of Cu(II) can efficiently quench the fluorescence of PFPNCC in nucleophilic solvents such as DMF and DMSO, but not in low nucleophilic solvents such as 1,4-dioxane and THF. Ultraviolet-visible spectra of the mixture of the conjugated polymer and Cu(II) indicate the presence of a reduced Cu(I) ion in the solution. Furthermore, fluorescence recovery of PFPNCC observed at low temperature suggests that the quenching and reducing mechanism is most probably due to a photo-induced electron transfer from excited PFPNCC to Cu(II). Our findings provide a novel strategy for highly selective conjugated polymer-based chemosensors for various target analytes, albeit “ligand-free”.

关键词： ligand-free     fluorescent chemosensor     copper     photo-induced electron transfer    

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Multi-harmonic forced vibration and resonance of simple beams to moving vehicles

《结构与土木工程前沿（英文）》   页码 981-993 doi: 10.1007/s11709-023-0979-5

摘要： This study modeled the moving-vehicle-induced forcing excitation on a single-span prismatic bridge as a multiple frequency-multiplication harmonic load on the modal coordinates of a linear elastic simple Euler–Bernoulli beam, and investigated the forced modal oscillation and resonance behavior of this type of dynamic system. The forced modal responses consist of multiple frequency-multiplication steady-state harmonics and one damped mono-frequency complementary harmonic. The analysis revealed that a moving load induces high-harmonic forced resonance amplification when the moving speed is low. To verify the occurrence of high-harmonic forced resonance, numerical tests were conducted on single-span simple beams based on structural modeling using the finite element method (FEM) and a moving sprung-mass oscillator vehicle model. The forced resonance amplification characteristics of the fundamental mode for beam response estimation are presented with consideration to different end restraint conditions. The results reveal that the high-harmonic forced resonance may be significant for the investigated beams subjected to vehicle loads moving at specific low speeds. For the investigated single-span simple beams, the moving vehicle carriage heaving oscillation modulates the beam modal frequency, but does not induce notable variation of the modal oscillation harmonic structure for the cases that vehicle of small mass moves in low speed.

关键词： forced vibration     linear Euler beam     moving load     harmonic structure     frequency modulation     end restraints    

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Sectional model test study on vortex-excited resonance of vehicle-bridge system of Shanghai Bridge over

Li ZHOU, Yaojun GE

《结构与土木工程前沿（英文）》 2009年 第3卷 第1期   页码 67-72 doi: 10.1007/s11709-009-0007-4

摘要： It is necessary to study how vehicles influence the vortex-excited resonance of vehicle-bridge systems, because lock-in wind speed is low and vortex-excited resonance is sensitive to any change in the main girder sections. Based on the Shanghai Bridge over the Yangtse River, the vortex-excited resonance of a 1∶60 scale sectional model was tested in a TJ-1wind tunnel, with or without vehicles at the attack angle of 0°, +3 and -3°, respectively. The conversion relationships between the resonant amplitudes of the sectional model and that of the prototype bridge were also established by mode shape correction. The result indicates that: 1) for the bridge with vehicles, the vertical vortex-excited resonance is accompanied by torsion vibration with the same frequency, and vice versa, 2) the amplitude of vortex-excited resonance of the bridge with vehicles is much larger than that of the bridge without vehicles, and 3) the lock-in wind speed of the vortex-excited resonance becomes smaller due to the disturbance of vehicles. It is obvious that vehicles bring about changes in the aerodynamic shape of the main girder. Therefore, the influence of vehicles on vortex-excited resonance performance of vehicle-bridge systems, in terms of both amplitude and mode, should not be ignored.

关键词： vehicle-bridge system     sectional mode     vortex-excited resonance     wind tunnel test     mode shape correction    

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A method of determining flame radiation fraction induced by interaction burning of tri-symmetric propane

Jie JI, Junrui DUAN, Huaxian WAN

《能源前沿（英文）》 2022年 第16卷 第6期   页码 1017-1026 doi: 10.1007/s11708-020-0716-x

摘要： The interaction of multiple fires may lead to a higher flame height and more intense radiation flux than a single fire, which increases the possibility of flame spread and risks to the surroundings. Experiments were conducted using three burners with identical heat release rates (HRRs) and propane as the fuel at various spacings. The results show that flames change from non-merging to merging as the spacing decreases, which result in a complex evolution of flame height and merging point height. To facilitate the analysis, a novel merging criterion based on the dimensionless spacing / was proposed. For non-merging flames ( / >0.368), the flame height is almost identical to a single fire; for merging flames ( / ≤0.368), based on the relationship between thermal buoyancy and thrust (the pressure difference between the inside and outside of the flame), a quantitative analysis of the flame height, merging point height, and air entrainment was formed, and the calculated merging flame heights show a good agreement with the measured experimental values. Moreover, the multi-point source model was further improved, and radiation fraction of propane was calculated. The data obtained in this study would play an important role in calculating the external radiation of propane fire.

关键词： flame interaction     air entrainment     flame height     multi-point source model     thermal radiation    

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Discovery of the mechanisms of acupuncture in the treatment of migraine based on functional magnetic resonance

《医学前沿（英文）》   页码 993-1005 doi: 10.1007/s11684-023-0989-7

摘要： Migraine is one of the most prevalent and disabling neurological disease, but the current pharmacotherapies show limited efficacy and often accompanied by adverse effects. Acupuncture is a promising complementary therapy, but further clinical evidence is needed. The influence of acupuncture on migraine is not an immediate effect, and its mechanism remains unclear. This study aims to provide further clinical evidence for the anti-migraine effects of acupuncture and explore the mechanism involved. A randomized controlled trial was performed among 10 normal controls and 38 migraineurs. The migraineurs were divided into blank control, sham acupuncture, and acupuncture groups. Patients were subjected to two courses of treatment, and each treatment lasted for 5 days, with an interval of 1 day between the two courses. The effectiveness of treatment was evaluated using pain questionnaire. The functional magnetic resonance imaging (fMRI) data were analyzed for investigating brain changes induced by treatments. Blood plasma was collected for metabolomics and proteomics studies. Correlation and mediation analyses were performed to investigate the interaction between clinical, fMRI and omics changes. Results showed that acupuncture effectively relieved migraine symptoms in a way different from sham acupuncture in terms of curative effect, affected brain regions, and signaling pathways. The anti-migraine mechanism involves a complex network related to the regulation of the response to hypoxic stress, reversal of brain energy imbalance, and regulation of inflammation. The brain regions of migraineurs affected by acupuncture include the lingual gyrus, default mode network, and cerebellum. The effect of acupuncture on patients’ metabolites/proteins may precede that of the brain.

关键词： acupuncture     migraine     fMRI     metabolome     proteome    

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Extended stochastic resonance (SR) and its applications in weak mechanical signal processing

Niaoqing HU, Min CHEN, Guojun QIN, Lurui XIA, Zhongyin PAN, Zhanhui FENG,

《机械工程前沿（英文）》 2009年 第4卷 第4期   页码 450-461 doi: 10.1007/s11465-009-0072-3

摘要： To catch symptoms of machine failure as early as possible, one of the most important strategies is to apply more progressive techniques during signal processing. This paper presents a method based on stochastic resonance (SR) to detect weak fault signal. First, a discrete model of a bistable system that can demonstrate SR is researched, and the stability condition for controlling the selection of model parameters of the discrete model and guarantee the solving convergence are established. Then, the frequency range of the weak signals that the SR model can detect is extended through a type of normalized scale transformation. Finally, the method is applied to extract the weak characteristic component from heavy noise to indicate the little crack fault in a bearing outer circle.

关键词： extended stochastic resonance (SR)     stability analysis of SR     scale transform     weak signal detection     incipient fault detection     envelope analysis    

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Cyanobacterial photo-driven mixotrophic metabolism and its advantages for biosynthesis

Ni Wan,Mary Abernathy,Joseph Kuo-Hsiang Tang,Yinjie J. Tang,Le You

《化学科学与工程前沿（英文）》 2015年 第9卷 第3期   页码 308-316 doi: 10.1007/s11705-015-1521-7

摘要： Cyanobacterium offers a promising chassis for phototrophic production of renewable chemicals. Although engineered cyanobacteria can achieve similar product carbon yields as heterotrophic microbial hosts, their production rate and titer under photoautotrophic conditions are 10 to 100 folds lower than those in fast growing Cyanobacterial factories face three indomitable bottlenecks. First, photosynthesis has limited ATP and NADPH generation rates. Second, CO fixation by ribulose-1,5-bisphosphate carboxylase/oxygenase (RuBisCO) has poor efficiency. Third, CO mass transfer and light supply are deficient within large photobioreactors. On the other hand, cyanobacteria may employ organic substrates to promote phototrophic cell growth, N fixation, and metabolite synthesis. The photo-fermentations show enhanced photosynthesis, while CO loss from organic substrate degradation can be reused by the Calvin cycle. In addition, the plasticity of cyanobacterial pathways (e.g., oxidative pentose phosphate pathway and the TCA cycle) has been recently revealed to facilitate the catabolism. The use of cyanobacteria as “green ” could be a promising route to develop robust photo-biorefineries.

关键词： CO2 mass transfer     N2 fixation     photosystem     RuBisCO     the TCA cycle    

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标题 作者 时间 类型 操作

Review: Tip-based vibrational spectroscopy for nanoscale analysis of emerging energy materials

Amun JARZEMBSKI, Cedric SHASKEY, Keunhan PARK

期刊论文

Solar fuel from photo-thermal catalytic reactions with spectrum-selectivity: a review

Sanli TANG, Jie SUN, Hui HONG, Qibin LIU

期刊论文

Hypoxia-induced activity loss of a photo-responsive microtubule inhibitor azobenzene combretastatin A4

Yang An, Chao Chen, Jundong Zhu, Pankaj Dwivedi, Yanjun Zhao, Zheng Wang

期刊论文

Photo-induced surface frustrated Lewis pairs for promoted photocatalytic decomposition of perfluorooctanoic

期刊论文

Experimental and computational assessment of 1,4-Dioxane degradation in a photo-Fenton reactive ceramic

期刊论文

Selective reduction of NO by photo-SCR with ammonia in an annular fixed-film photoreactor

YiangChen CHOU, Young KU

期刊论文

Lignin-based electrospun nanofiber membrane decorated with photo-Fenton Ag@MIF-100(Fe) heterojunctions

期刊论文

Synthesis, spectroscopic, and electrochemical properties of two dyads consisted of tetrathiafulvalene and carbazole

Guoqiao LAI, Yibo LIU, Meijiang LI, Yongjia SHEN

期刊论文

Highly selective detection of copper(II) by a “ligand-free” conjugated copolymer in nucleophilic solvents

Weixing Deng, Pengfei Sun, Quli Fan, Lei Zhang, Tsuyoshi Minami

期刊论文

Multi-harmonic forced vibration and resonance of simple beams to moving vehicles

期刊论文

Sectional model test study on vortex-excited resonance of vehicle-bridge system of Shanghai Bridge over

Li ZHOU, Yaojun GE

期刊论文

A method of determining flame radiation fraction induced by interaction burning of tri-symmetric propane

Jie JI, Junrui DUAN, Huaxian WAN

期刊论文

Discovery of the mechanisms of acupuncture in the treatment of migraine based on functional magnetic resonance

期刊论文

Extended stochastic resonance (SR) and its applications in weak mechanical signal processing

Niaoqing HU, Min CHEN, Guojun QIN, Lurui XIA, Zhongyin PAN, Zhanhui FENG,

期刊论文

Cyanobacterial photo-driven mixotrophic metabolism and its advantages for biosynthesis

Ni Wan,Mary Abernathy,Joseph Kuo-Hsiang Tang,Yinjie J. Tang,Le You

期刊论文