INTERNATIONAL JOURNAL OF MASS SPECTROMETRY
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2010
·
IF 2.117
Mingfeng Xie,Zhongyue Zhou,Zhandong Wang,Dongna Chen,Fei Qi
The near-threshold absolute photoionization cross-sections of 12 oxygenated hydrocarbons, including 1-butanol, 2-butanol, iso -butanol, tert -butanol, 1-pentanol, tert -pentanol, iso -pentanol, methyl tert -butyl ether (MTBE), ethyl tert -butyl ether (ETBE), furan, 2-methylfuran, 2,5-dimethylfuran, were measured in the photon energy range from respective ionization thresholds to 11.5 eV. The experiments were performed with photoionization mass spectrometry and tunable synchrotron vacuum ultraviolet (VUV) light. Binary-liquid-mixtures of the investigated sample and benzene were used in the measurements where benzene acts as a calibration standard, due to its well known photoionization cross-section at the photon energies from its ionization energy (9.24 eV) to 11.5 eV. Photodissociative fragments from the molecules were also observed, and their photodissociation cross-sections are also presented.
研究领域:
化学
·
物理化学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF MASS SPECTROMETRY
·
2014
·
IF 2.227
Y.Y. Wang,X. Kang,Y.W. Liu,W.Q. Xu,L. Wang,C.Z. Hu,J. Chen,F.Y. Liu,L.S. Sheng,X.L. Zhao,P.F. Zhang,L.F. Zhu
Using vacuum ultraviolet photons produced by synchrotron radiation and reflection time-of-flight mass spectrometer, dissociative photoionization of isooctane was measured in the photon energy region of 9.7–15.6 eV under ultrasonic molecular beam. Then the dissociative ionization products at different photon energies were obtained. By measuring the photoionization efficiency curves, the appearance potentials of the dominative ion fragments and the vertical ionization energy of isooctane were determined. In addition, combining with G3 calculations we obtained the structure and energy of the parent, neutral and ion fragments. By comparing the experimental measurements with the theoretical calculations, the dissociative photoionization channels of isooctane were elucidated, and formation enthalpies of the fragmented ions and the dissociation energy of the parent ion were obtained.
研究领域:
化学物理
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分子光谱学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Hanxiao Wang,Zhaotie Liu,Zhongwen Liu,Jinqiang Jiang,Guo Li
An extendable double network design for hydrogels with programmable external geometries and actuating trajectories is presented. Chemically cross-linked polyacrylamide as the first network penetrated with linear alginate chains is prepared for demonstration. The coordination of Fe3+ ions with carboxylate groups in alginate chains acts as the second network, and its dissociation through photoreduction is utilized to realize the photoresponsive shape memory property; the shape fixity ratio and shape recovery ratio both exceed 90%. The gradient dissociation of Fe3+-carboxylate coordination under UV facilitates 3D programming of hydrogel geometry. On another aspect, the resulted cross-linking gradient differentiates the extent and rate of solvent-induced volume change of the PAAm network, endowing the hydrogel with photo-programmable solvent-driven actuating behavior. Furthermore, by inducing the formation of Fe3+-carboxylate coordination within the entire network for shape programming and cross-linking gradients in specific regions as active joints, hydrogels with designed actuating behaviors based on specific 3D shapes are realized. The shape memory and active morphing functionalities enabled by photo-dissociable Fe3+-carboxylate coordination in PAAm hydrogel can be generally extended to other hydrogels.
研究领域:
材料科学
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化学工程
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生物医学工程
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产品关联
DOI
PubMed
高影响因子
Journal of the American Chemical Society
·
2022
·
IF 16.383
Lingqiang Zhou,Zheyi Liu,Yongjie Guo,Shiwen Liu,Heng Zhao,Shan Zhao,Chunlei Xiao,Shun Feng,Xueming Yang,Fangjun Wang
Maintaining the protein high-order structures and interactions during the transition from aqueous solution to gas phase is essential to the structural analysis of native mass spectrometry (nMS). Herein, we systematically interrogate the effects of charge state and crown ether (CE) complexation on the gas-phase native-like protein structure by integrating nMS with 193 nm ultraviolet photodissociation (UVPD). The alterations of photofragmentation yields of protein residues and the charge site distribution of fragment ions reveal the specific sites and sequence regions where charge and CE take effect. Our results exhibit the CE complexation on protonated residues can largely alleviate the structure disruption induced by the intramolecular solvation of charged side chains. The influences of CE complexation and positive charge on gas-phase protein structure exhibit generally opposite trends because the CE microsolvation avoids the hydrogen-bonding formation between the charged side chains with backbone carbonyls. Thus, CE complexation leads to a more stable and native-like protein structure in the gas phase.
研究领域:
生物化学
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质谱学
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蛋白质结构研究
✓ 已验证
DOI
PubMed
高影响因子
Research
·
2022
·
IF 11.036
Hai-Fang Li,Jing Zhao,Wenbo Cao,Wenpeng Zhang,Yu Xia,Zheng Ouyang
Unraveling the complexity of the lipidome requires the development of novel approaches to facilitate structural identification and characterization of lipid species with isomer-level discrimination. Ultraviolet photodissociation tandem mass spectrometry (UVPD MS/MS) is a promising tool for structure determination of lipids. The sensitivity of UVPD for lipid analysis however is limited mainly due to weak absorption of UV photons by a C=C. Herein, a C=C site-specific derivatization, the Paternò-Büchi (PB) reaction, was used to incorporate a chromophore to the C=C moiety in fatty acyls, leading to significantly improved UVPD efficiency and sensitivity for pinpointing C=C locations. The wavelength-dependent photodissociation of the PB products demonstrated 4-CF3-benzophenone as the best reagent for UVPD in terms of the efficiency of generating C=C diagnostic fragments and simplicity for C=C location assignments. We demonstrated the effectiveness of this approach for the shotgun profiling of C=C location isomers in different lipid classes from complex lipid extracts, highlighting its potential to advancing the identification of the C=C bond locations in unsaturated lipids.
研究领域:
生物化学
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分析化学
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质谱技术
✓ 已验证
DOI
高影响因子
COMBUSTION AND FLAME
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2020
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IF 4.57
Jin-Tao Chen,Dan Yu,Wang Li,Wen-Ye Chen,Shu-Bao Song,Cheng Xie,Jiu-Zhong Yang,Zhen-Yu Tian
The oxidation of benzaldehyde (A1CHO) at atmospheric pressure in a jet-stirred reactor at equivalence ratios of 0.4 and 2.0 within 475–900 K was studied. The intermediates and products were identified by synchrotron radiation photoionization and molecular beam mass spectrometry . Compared with previous studies, 29 species such as HCHO, CH 3 O, H 2 O 2 , ketene, furan, 2,4-cyclopentadiene-1-one (C 5 H 4 O), furfural , o-benzoquinone, 1,4-benzenediol and 1,4-cyclohex-2-enedione were newly detected. A kinetic model , involving 376 species and 2163 reactions was proposed, which reasonably predicted the experimental value. Rate-of-production analysis shows that H-abstractions reactions involving H atoms, OH, CH 3 , HO 2 and phenoxy radicals dominate the consumption of A1CHO. The decarbonylation reactions and ring opening reactions have a certain contribution to the promotion of oxidation process. Phenoxy radicals, phenol and C 5 H 4 O are one of the most significant intermediates for A1CHO oxidation. Sensitivity analysis shows that A1CHO+OH=A1CO+H 2 O and H 2 O 2 (+M) =OH+OH(+M) are among the most sensitive reactions to promote the consumption of A1CHO at both conditions while the reaction A1OH+O 2 =A1O+HO 2 has strong inhibiting effect. A1CHO is more difficult to produce benzene compared with benzyl alcohol oxidation while is easier to generate phenol at the same condition. These results will enrich the understanding the oxidation mechanism and soot formation of A1CHO as a potential aromatic fuel.
研究领域:
化学动力学
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燃烧科学
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燃料化学
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-10
·
IF 14.7
Xu Guangxian,Wang Hong,Zhang Jinyang,Gao Jiao,Guan Jiwen,Xu Qiang,Truhlar Donald G.,Wang Zhandong
Elucidating the formation mechanism of polycyclic aromatic hydrocarbons (PAHs) is crucial to understand processes in the contexts of combustion, environmental science, astrochemistry, and nanomaterials synthesis. An excited electronic-state pathway has been proposed to account for the formation of 14π aromatic anthracene in the benzyl ( b -C 7 H 7 ) self-reaction. Here, to improve our understanding of anthracene formation, we investigate C 7 H 7 bimolecular reactions in a tubular SiC microreactor through an isomer-resolved method that combines in situ synchrotron-radiation VUV photoionization mass spectrometry and ex-situ gas chromatography–mass spectrometry. We observe the formation of o -tolyl ( o -C 7 H 7 ) radical isomer, and identify several C 14 H 10 products (diphenylacetylene, phenanthrene and anthracene) and key C 14 H 14 and C 14 H 12 intermediates. These isomer-specific results support the occurrence of reactions on the electronic ground-state potential energy surface, with no evidence for key intermediates of the proposed excited-state pathway as the key pathway. Furthermore, theoretical calculations unveil new facile reaction pathways that may contribute to the enhanced production of anthracene, and these mechanistic findings are further substantiated by pyrolysis experiments. The results add insight into the molecular formation of PAHs in C 7 H 7 bimolecular reaction, and contribute to establishing accurate models to predict PAH chemistry in diverse laboratory, environmental, and extraterrestrial contexts.
研究领域:
燃烧科学
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环境科学
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天体化学
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纳米材料合成
✓ 已验证
DOI
高影响因子
JOURNAL OF CHEMICAL PHYSICS
·
2017
·Vol. 146
·期 13
·
IF 2.965
Zhan Huaqi,Hu Yongjun,Wang Pengchao,Chen Jiaxin
Tetrahydropyran-2-methanol (THPM) is a typical alcohol containing a six-member cyclic ether, which can be considered as the model molecule of cyclic sugar. Herein, vacuum ultraviolet (VUV) photodissociation spectroscopy is employed to study fragmentation pathways and infrared (IR) plus VUV photoionization spectroscopy to investigate the structures of neutral THPM and its clusters with the size up to the trimer. Qualitative structural assignments are confirmed for the neutral species and ions based on MP2/aug-cc-pVTZ and ωB97X-D/cc-pVTZ calculations. The fragment cations at m/z = 84, 85, and 98 arise by the losing of CH 2 OH, CH 3 OH, and H 2 O from the monomer, respectively, as a result of C–C bond and C–O bond dissociation under the VUV (118 nm) radiation. It is found that the loss of CH 3 OH and H 2 O involves hydrogen transfer from the CH 2 group to the dissociating CH 2 and OH groups. Comparing the observed and calculated spectra of the monomer THPM, it suggests that the conformer containing a chair tetrahydropyran ring and an intramolecular hydrogen bond would be dominantly survived in a supersonic beam. Moreover, the IR spectra of larger clusters n > 1 (n = 2, 3) show only the broad hydrogen bonded OH stretch mode, and thus these larger clusters would form a closed-cyclic structure, where all OH groups are participating in hydrogen bonding. Partially the CH stretch positions of THPM clusters do not change significantly with the increasing of cluster size, thus the CH and CH 2 groups are not involved in H-bonding interactions.
研究领域:
物理化学
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分子光谱学
✓ 已验证
DOI
PubMed
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-13
·
IF 14.7
Zhang Lei,Chen Lu,Wang Siheng,Wang Shanshan,Wang Dan,Yu Le,Xu Xu,Liu He,Chen Chaoji
Self-powered skin attachable and detachable electronics are under intense development to enable the internet of everything and everyone in new and useful ways. Existing on-demand separation strategies rely on complicated pretreatments and physical properties of the adherends, achieving detachable-on-demand in a facile, rapid, and universal way remains challenging. To overcome this challenge, an ingenious cellulose nanofiber-mediated manifold dynamic synergy strategy is developed to construct a supramolecular hydrogel with both reversible tough adhesion and easy photodetachment. The cellulose nanofiber-reinforced network and the coordination between Fe ions and polymer chains endow the dynamic reconfiguration of supramolecular networks and the adhesion behavior of the hydrogel. This strategy enables the simple and rapid fabrication of strong yet reversible hydrogels with tunable toughness ((Value max -Value min )/Value max of up to 86%), on-demand adhesion energy ((Value max -Value min )/Value max of up to 93%), and stable conductivity up to 12 mS cm −1 . We further extend this strategy to fabricate different cellulose nanofiber/Fe 3+ -based hydrogels from various biomacromolecules and petroleum polymers, and shed light on exploration of fundamental dynamic supramolecular network reconfiguration. Simultaneously, we prepare an adhesive-detachable triboelectric nanogenerator as a human-machine interface for a self-powered wireless monitoring system based on this strategy, which can acquire the real-time, self-powered monitoring, and wireless whole-body movement signal, opening up possibilities for diversifying potential applications in electronic skins and intelligent devices.
研究领域:
材料科学
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生物医学工程
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智能设备
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ANALYTICAL CHEMISTRY
·
2024
·
IF 6.7
Yinlong Zhu,Zheyi Liu,Jialiang Liu,Heng Zhao,Rui Feng,Kunxian Shu,Fangjun Wang,Cheng Chang
Ultraviolet photodissociation (UVPD) mass spectrometry unlocks insights into the protein structure and sequence through fragmentation patterns. While N- and C-terminal fragments are traditionally relied upon, this work highlights the critical role of internal fragments in achieving near-complete sequencing of protein. Previous limitations of internal fragment utilization, owing to their abundance and potential for random matching, are addressed here with the development of Panda-UV, a novel software tool combining spectral calibration, and Pearson correlation coefficient scoring for confident fragment assignment. Panda-UV showcases its power through comprehensive benchmarks on three model proteins. The inclusion of internal fragments boosts identified fragment numbers by 26% and enhances average protein sequence coverage to a remarkable 93% for intact proteins, unlocking the hidden region of the largest protein carbonic anhydrase II in model proteins. Notably, an average of 65% of internal fragments can be identified in multiple replicates, demonstrating the high confidence of the fragments Panda-UV provided. Finally, the sequence coverages of mAb subunits can be increased up to 86% and the complementary determining regions (CDRs) are nearly completely sequenced in a single experiment. The source codes of Panda-UV are available at https://github.com/PHOENIXcenter/Panda-UV.
研究领域:
分析化学
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蛋白质组学
·
质谱学
·
生物信息学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
PARTICLE & PARTICLE SYSTEMS CHARACTERIZATION
·
2021
·Vol. 38
·期 11
·2100193
·
IF 3.31
Shuang Qi,Zhihui Jin,Yuanjun Hou,Chao Li,Xuesong Wang,Qianxiong Zhou
Ru(II) complexes with weak ligand fields may undergo light-induced ligand dissociation, and the resulted Ru(II) aqua complexes may bind with biomolecules such as DNA, showing potential as photoactivated chemotherapy (PACT) agents. However, Ru(II) complexes with efficient PACT activity are still rare. Some Ru(II) complexes exhibit efficient photoinduced ligand dissociation but poor cytotoxicity. It is speculated that the low nuclear accumulation levels may account for their low PACT efficacy. In order to confirm this hypothesis, the almost noncytotoxic [Ru(7-OCH 3 -dppz)(4-OCH 3 -py) 4 ](PF 6 ) 2 (Ru1) is loaded on nucleus-targeted C 5 N 2 nanoparticles (NPs). Compared with the free Ru1, Ru1–C 5 N 2 NPs exhibit significantly increased cellular uptake and nuclear accumulation. Therefore, Ru1–C 5 N 2 NPs show efficient PACT activity toward various cancer cell lines (including cisplatin-resistant one) with half maximal inhibitory concentration (IC 50 ) values of 0.18 × 10 −6 –0.29 × 10 −6 m and phototoxicity index (IC 50 dark /IC 50 light ) values above 137 under both normoxic and hypoxic conditions. Moreover, Ru1–C 5 N 2 NPs also exhibit efficient PACT activity toward cisplatin-resistant 3D multicellular tumor spheroids upon two-photon irradiation (800 nm). The same strategy is also feasible to greatly improve the PACT activity of [Ru(7-OCH 3 -dppz)(py) 4 ] 2+ , which itself only has a medium effect. The results may provide new sights for developing efficient Ru(II) PACT agents.
研究领域:
化学
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药学
·
肿瘤学
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材料科学
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生物医学工程
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2024
·
IF 7.7
Ke Deng,Qin Huang,Xiaotong Yan,Yan Dai,Juan Zhao,Xia Xiong,Hailan Wang,Xianggui Chen,Pengfei Chen,Li Liu
Achieving the controllable detachment of polysaccharide-based wound dressings is challenging. In this study, a novel, photodetachable salecan-based hydrogel dressing with injectable, self-healing, antibacterial, and wound healing properties was developed using a green and facile approach. A salecan hydrogel with a uniform porous structure and water content of 90.4 % was prepared by simply mixing salecan and an Fe 3+ –citric acid complexing solution in an acidic D-(+)-glucono-1,5-lactone environment. Metal coordinate interactions were formed between the released Fe 3+ ions and carboxyl groups on the salecan polysaccharide, inducing homogeneous gelation. Benefiting from this dynamic and reversible crosslinking, the salecan hydrogel exhibited self-healing and injectable behavior, facilitating the formation of the desired shapes in situ. The exposure of Fe 3+ –citric acid to UV light (365 nm) resulted in the reduction of Fe 3+ to Fe 2+ through photochemical reactions, enabling phototriggered detachment. Moreover, the hydrogel exhibited excellent biocompatibility and satisfactory antibacterial efficacy against Escherichia coli and Staphylococcus aureus of 72.5 % and 85.3 %, respectively. The adhesive strength of the salecan hydrogel to porcine skin was 1.06 ± 0.12 kPa. In vivo wound healing experiments further highlighted the advantages of the prepared hydrogel in alleviating the degree of wound inflammation and promoting tissue regeneration within 12 days.
研究领域:
材料科学
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生物材料
·
伤口愈合
·
药学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）