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JOURNAL OF MASS SPECTROMETRY · 2015 ·Vol. 50 ·期 1 ·212-219 · IF 2.379

Structure and further fragmentation of significant [a3 + Na − H]+ ions from sodium-cationized peptides

Huixin Wang,Bing Wang,Zhonglin Wei,Hao Zhang,Xinhua Guo

A good understanding of gas-phase fragmentation chemistry of peptides is important for accurate protein identification. Additional product ions obtained by sodiated peptides can provide useful sequence information supplementary to protonated peptides and improve protein identification. In this work, we first demonstrate that the sodiated a 3 ions are abundant in the tandem mass spectra of sodium-cationized peptides although observations of a 3 ions have rarely been reported in protonated peptides. Quantum chemical calculations combined with tandem mass spectrometry are used to investigate this phenomenon by using a model tetrapeptide GGAG. Our results reveal that the most stable [a 3 + Na − H] + ion is present as a bidentate linear structure in which the sodium cation coordinates to the two backbone carbonyl oxygen atoms. Due to structural inflexibility, further fragmentation of the [a 3 + Na − H] + ion needs to overcome several relatively high energetic barriers to form [b 2 + Na − H] + ion with a diketopiperazine structure. As a result, low abundance of [b 2 + Na − H] + ion is detected at relatively high collision energy. In addition, our computational data also indicate that the common oxazolone pathway to generate [b 2 + Na − H] + from the [a 3 + Na − H] + ion is unlikely. The present work provides a mechanistic insight into how a sodium ion affects the fragmentation behaviors of peptides. Copyright © 2015 John Wiley & Sons, Ltd.

研究领域: 生物化学 · 质谱分析 · 理论化学
✓ 已验证 DOI PubMed 高影响因子
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ACS Nano · 2023 · IF 17.1

Strong Replaces Weak: Design of H-Bond Interactions Enables Cryogenic Aqueous Zn Metal Batteries

Changhao Zhu,Xuye He,Yun Shi,Zhenkang Wang,Baojiu Hao,Wanhao Chen,Hao Yang,Lifang Zhang,Haoqing Ji,Jie Liu,Chenglin Yan,Jinqiu Zhou,Tao Qian

Despite the numerous advantages of aqueous Zn batteries, their practical application under cryogenic conditions is hindered by the freezing of the electrolyte because the abundance of hydrogen bonds (H-bonds) between H2O molecules drives the aqueous system to transform to an orderly frozen structure. Here, a design of H-bond interactions based on the guiding ideology of “strong replaces weak” is proposed. The strong H-bonds formed between introduced eutectic components and water molecules break down the weak H-bonds in the original water molecule network, which contributes to an ultralow freezing point and a high ionic conductivity of 1.7 mS cm–1 at −40 °C. Based on multiperspective theoretical simulations and tailor-made in situ cooling Raman characterizations, it has been demonstrated that substituting weak H-bonds with strong H-bonds facilitates the structural reshaping of Zn2+ solvation and remodeling of the H-bond network in the electrolyte. Endowed with this advantage, reversible and stable Zn plating/stripping behaviors could be realized at −40 °C, and the full cells display a high discharge capacity (200 mA h g–1) at −40 °C with ∼75% capacity retention after 1000 cycles. This study will expand the design philosophy of antifreezing aqueous electrolytes and provide a perspective to promote the adoption of Zn metal batteries for cryogenic environment large-scale energy storage.

研究领域: 材料科学 · 电化学 · 能源存储
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JOURNAL OF HAZARDOUS MATERIALS · 2024 · IF 12.2

Mechanism for airborne ozone decomposition on X-MIL-53(Fe) (X = H, NH2, NO2)

Jiami Ma,Zhixin Hu,Weihong Guo,Cheng Ni,Pan Li,Bosheng Chen,Songhua Chen,Jinlong Wang,Yanbing Guo

Ground−level ozone (O 3 ) pollution poses a significant threat to both ecosystem sustainability and human health. The catalytic decomposition of O 3 presents as a promising technology to address the issues of O 3 pollution. This study undertook the synthesis of various functionalized metal−organic framework (MOF) catalysts ( i.e., X-MIL-53(Fe) (X = H, NH 2 , NO 3 )) to delve into the influence of ligand functional groups on skeletal structure and catalytic efficacy, particularly focusing on unraveling the mechanism of O 3 catalytic decomposition under humid conditions. NH 2 -MIL-53(Fe) catalyst achieved complete O 3 decomposition under ambient temperature and high humidity conditions (RH=75 %), exhibiting a reaction rates (mol·m −2 ·s −1 ) 129 and 10.5 times greater than that of MIL-53(Fe) and NO 2 -MIL-53(Fe). The NH 2 group promotes electron flow within the backbone towards the hydroxyl group (OH) linked to Fe atom. In humid O 3 , H 2 O molecules augment the interaction between O 3 and NH 2 -MIL-53(Fe), and OH is converted to·O 2 − after deprotonation, promoting O 3 decomposition. Additionally, leveraging three−dimensional (3D) printing technology, a monolithic catalyst for O 3 decomposition was prepared for application. This study not only advances understanding of the mechanisms underlying O 3 decomposition but also offers practical solutions for addressing O 3 pollution at humid conditions.

研究领域: 环境科学 · 材料科学
✓ 已验证 DOI PubMed 高影响因子
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Materials · 2019 ·Vol. 12 ·期 24 ·4112 · IF 2.972

Temperature Effects on the Dielectric Properties and Breakdown Performance of h-BN/Epoxy Composites

Yongzhe Tang,Peng Zhang,Mingxiao Zhu,Jiacai Li,Yuxia Li,Ziguo Wang,Liangsong Huang

Epoxy–boron nitride composites are promising insulating materials, and it is highly important to understand their insulating performances at different temperatures with different nano-doping amounts. In this study, we investigated the effects of different mass fractions of epoxy–micron hexagonal boron nitride composites on their thermal conductivity, as well as the effects of temperature and mass fraction on their insulating performances. The results demonstrated that the thermal conductivity of epoxy–micron hexagonal boron nitride composites was superior to that of neat epoxy. The thermal conductivity of epoxy–micron hexagonal boron nitride composites increased with the mass fraction of hexagonal boron nitride, and their dielectric constant and dielectric loss increased with temperature. The dielectric constant of epoxy–micron hexagonal boron nitride composites decreased as the mass fraction of hexagonal boron nitride increased, while their dielectric losses decreased and then increased as the mass fraction of hexagonal boron nitride increased. Due to internal heat accumulation, the alternating current breakdown strength of epoxy–micron hexagonal boron nitride composites increased and then decreased as the mass fraction of hexagonal boron nitride increased. Additionally, as the temperature increased, the composites transitioned from the glassy state to the rubbery or viscous state, and the breakdown strength significantly degraded.

✓ 已验证 DOI 高影响因子
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TETRAHEDRON-ASYMMETRY · 2014 ·Vol. 25 ·期 23 ·1520-1526 · IF 2.165

Preparation of enantiomerically pure α-hydroxyl phosphinates via hydrophosphorylation of aldehydes with H-phosphinate

Yong-Ming Sun,Zhong-Yuan Xu,Li-Juan Liu,Fan-Jie Meng,He Zhang,Bao-Ci Fu,Li-Jun Sun,Mei-Ju Niu,Shu-Wen Gong,Chang-Qiu Zhao,Li-Biao Han

The hydrophosphorylation of aldehydes with a P -stereogenic H -phosphinate was realized by heating two compounds in a neat state or catalyzed by a base , to afford P -retention α-hydroxyl phosphinates. The ( S P , S C ) and other diastereomers were isolated, and their structures were confirmed by NMR spectroscopy and crystallography.

✓ 已验证 DOI 高影响因子
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RARE METALS · 2014 ·Vol. 33 ·期 1 ·86-90 · IF 0.806

Improving hydrogen storage performance of Li–Mg–N–H system by adding niobium hydride

Zhu Xi-Lin,Han Shu-Min,Zhao Xin,Li Yuan,Liu Bao-Zhong

Hydrogen storage properties of 2LiNH 2 –MgH 2 – x NbH ( x  = 0 and 0.05) composites and the catalysis of NbH on hydrogen sorption reaction of the Li–Mg–N–H system were investigated. Hydrogen sorption properties of 2LiNH 2 –MgH 2 system are effectively improved by adding NbH. Temperature programmed desorption results show the addition of NbH reduces the dehydriding onset temperature of 2LiNH 2 –MgH 2 system by 21 K. Approximate 3.62 wt% hydrogen in 2LiNH 2 –MgH 2 –0.05NbH composite is released following a 500 min at 433 K, whereas the amount of hydrogen desorption is only ~3.16 wt% for the pristine system under the same condition. The sample with NbH exhibits higher dehydriding rate compared with the pristine one. Moreover, hydrogen absorption rate increases by adding NbH into the 2LiNH 2 –MgH 2 system. Hydrogen absorption capacity of the samples with NbH is 3.23 wt% within 400 min, which is higher than that of pristine sample. Fine NbH particles homogeneously distribute in the 2LiNH 2 –MgH 2 –0.05NbH composite, and catalyze the hydrogen sorption reaction rather than reacts as a reactant into new compound.

研究领域: 材料科学 · 氢能 · 固态化学
✓ 已验证 DOI 高影响因子
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ACS Applied Polymer Materials · 2025 · IF 4.7

Phase Change Materials via H-Bonding Cross-Linking for Cold Energy Storage and Management

Yu Han,Qiang He,Yuqun Fang,Jingkai Nie,Weinan Qin,Hao Liu,Kai Zhu

Phase change materials (PCMs) offer great potential for realizing zero-energy thermal management due to superior cold storage and stable phase change temperatures. However, the widespread use of PCMs is consistently impeded by issues such as liquid leakage and solid rigidity. Here, we present a simple yet effective strategy for developing highly flexible polymer-based phase change materials. Our approach involves creating a dual three-dimensional (3D) cross-linked network of acrylamide (AM) and sodium alginate (SA) within a poly(vinyl alcohol) (PVA) matrix. The synergy between H-bonds and AM-SA networks significantly enhances the mechanical strength, thermal stability, and leakage resistance of PVA@AM-SA. Our research offers a promising approach to designing phase change materials with both high latent heat capacity and exceptional mechanical strength, making them ideal for use in wearable thermal management applications.

研究领域: 材料科学 · 能源工程 · 高分子化学
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APPLIED PHYSICS A-MATERIALS SCIENCE & PROCESSING · 2019 ·Vol. 125 ·期 2 ·1-10 · IF 1.784

Enhancement in photocatalytic performance of Ag–AgCl decorated with h-WO3 and mechanism insight

Chai Chen,Liu Jianxin,Wang Yawen,Zhang Xiaochao,Duan Donghong,Fan Caimei,Wang Yunfang

A h-WO 3 decorated Ag–AgCl composite was prepared through facile precipitation and photoreduction methods and demonstrated to be a highly efficient and stable photocatalyst for the degradation of Rhodamine B (RhB) under visible light. Ag–AgCl/h-WO 3 exhibited much improved photocatalytic performance was elucidated from the physical–chemical properties of AgCl and h-WO 3 and the surface plasmon resonance effect of the Ag particles. The techniques of X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM), X-ray photoelectron spectrometry (XPS) and photocurrent were used to characterize crystalline phases, morphology, composition and separation efficiency between electrons (e − ) and holes (h + ) of the synthesized composite photocatalyst. XPS results confirmed the existence of W 5+ and W 6+ on the surface of h-WO 3 sample, which favored electrons transfer between AgCl and Ag, and generated superoxide radical for the degradation of RhB. The active species trapping experiments results further demonstrated that the formation of superoxide radical during the system. Finally, the underlying photocatalytic mechanism for the removal of RhB by Ag–AgCl/h-WO 3 composite was examined.

CAS / MDL: 7783-03-1
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PROGRESS IN ORGANIC COATINGS · 2019 · IF 3.42

Fabrication of h-BN-rGO@PDA nanohybrids for composite coatings with enhanced anticorrosion performance

Haowei Huang,Xiaofeng Huang,Yuhui Xie,Yuqin Tian,Xiang Jiang,Xinya Zhang

Inspired by mussels’ universal adhesive ability to various substrates, polydopamine (PDA) was used to bind graphene oxide (GO) and hexagonal boron nitride (h-BN) together to fabricate h-BN-rGO@PDA nanohybrids. The as-prepared h-BN-rGO@PDA nanohybrids were served as anticorrosive nanofillers for polyvinylbutyral (PVB) coatings on mild steel. The structure of h-BN-rGO@PDA nanohybrids were characterized by SEM, XRD, FT-IR, UV–vis and Raman spectroscopies. Electrochemical corrosion tests were conducted to examine the anticorrosion properties of h-BN-rGO@PDA/PVB composite coatings. The results show that the stacked h-BN nanosheets are exfoliated by GO. And PDA is successfully grafted onto the surface of h-BN-rGO@PDA and simultaneously reduced GO into rGO. The h-BN-rGO@PDA nanohybrids are homogeneously distributed in the PVB matrix. When the mass ratio of GO to h-BN in h-BN-rGO@PDA is 1:1, the as-prepared h-BN-rGO@PDA possesses effective aspect ratio and thus its PVB composite coating obtains the optimal anticorrosion performance with 2 orders of magnitude higher than pure PVB.

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DYES AND PIGMENTS · 2019 · IF 4.018

Superior adsorption of methyl orange by h-MoS2 microspheres: Isotherm, kinetics, and thermodynamic studies

Yanhong Wu,Minhua Su,Jiawei Chen,Zuopeng Xu,Jiafeng Tang,Xiangyang Chang,Diyun Chen

A batch equilibrium system was used in this study to investigate the adsorption of methyl orange (MO) on hollow molybdenum disulfide (h-MoS 2 ) microspheres . The effects of experimental conditions, such as the initial concentration, agitation time, solution pH and temperature, on the adsorption were examined. The adsorption of MO on h-MoS 2 microspheres was unexpectedly ultrafast. Adsorption equilibrium was rapidly achieved in 10 seconds, and the maximum adsorption capacity for MO was 41.52 mg/g. The Langmuir and Freundlich models were used for determining the adsorption parameters. The results reveal that the Freundlich model fits well with the experimental adsorption data. Pseudo-first-order, pseudo-second-order, and intraparticle diffusion models were applied to determine the kinetics of MO ultrafast adsorption. The obtained results indicate that the experimental kinetics data of h-MoS 2 microspheres are well explained by the second-order model. The obtained values of the thermodynamic parameters (Δ H 0 , Δ S 0 , and Δ G 0 ) indicated that MO adsorption on h-MoS 2 microspheres was an exothermic and spontaneous process. The thermodynamic parameters also confirmed that the MO adsorption is a chemical and physical adsorption process on the surfaces of h-MoS 2 microspheres. The adsorption mechanism was further advanced by FT-IR. The findings of this study open an avenue for applying h-MoS 2 microspheres for organic dyes removal from industrial wastewater streams.

CAS / MDL: 79917-90-1
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Journal of Physical Chemistry C · 2022 · IF 4.177

Low-Temperature C–H Bond Activation: Ethylbenzene-to-Styrene Conversion on Rutile TiO2(110)

Yuemiao Lai,Zhengtian Pu,Peng Liu,Fangliang Li,Jie Zeng,Xueming Yang,Qing Guo

The low-temperature C–H bond activation of alkanes remains a big challenge in alkane dehydrogenation. In this work, ethylbenzene (EB) oxidative dehydrogenation has been investigated on rutile(R)-TiO2(110) under both ultrahigh vacuum (UHV) and ambient conditions. Under UHV conditions, styrene is produced with nearly 100% selectivity in a stepwise manner, in which the first C–H bond dissociation of EB occurs at <285 K with the help of surface O22– species, followed by the second C–H bond dissociation at about 400 K. However, styrene, acetophenone, and 2,3-diphenylbutane products are produced from EB oxidative dehydrogenation under ambient conditions, suggesting that α-H dissociation is the initial step of EB oxidative dehydrogenation. This may be also possible for EB oxidative dehydrogenation on R-TiO2(110) under UHV conditions. The different pathways of EB oxidative dehydrogenation under UHV and ambient conditions may originate from different intermediates and O2 concentrations. This work provides new insight into the fundamental understandings of the low-temperature C–H bond activation of alkyl chains of aromatic hydrocarbons, which may promote the development of new catalysts for efficient styrene production from EB oxidative dehydrogenation under mild conditions.

✓ 已验证 产品关联 DOI 高影响因子
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JOURNAL OF DRUG DELIVERY SCIENCE AND TECHNOLOGY · 2021 · IF 3.981

Reduced In vivo burst release of ginkgolide B microcrystals achieved by polymeric H+ depot

Jingxin Gou,Silin Wang,Xu Li,Tian Yin,Haibing He,Yu Zhang,Xing Tang,Wei Xiao,Zhenzhong Wang

Drug microcrystal (MC) is an important category of long acting injections (LAIs), whose release profile is controlled mainly by particle size, crystal form, drug solubility , and other parameters. In this study, a polymeric H + depot composed of alginate was combined with drug MC using ginkgolide B (GB) as model drug to reduce the initial burst release of the drugs with elevated solubility in body fluid. The parameters of GB MC preparation by precipitation, including stabilizer type and amount, phase volume ratio, and stirring rate were investigated. And the particle size/distribution, particle morphology, crystallinity, in vitro release of optimized GB MC were characterized. The in vivo dissolution retardation effect of acidified alginate (SAA) was first confirmed by live imaging using fluorescein as probe. And the pharmacokinetic profiles of different GB MC-polymer blends were investigated by UPLC-MS/MS. The prepared GB MC was spherical-like particles with a mean particle size of 5.863 μm and a span value of 1.634. The crystallinity of GB MC was lowered by the precipitation process compared with that of the crude drug , which resulted in a faster in vitro dissolution with more than 90% of drugs dissolved in 20 min. When administered with SAA, an alginate amount-dependent reduction in C max (1243.5 ± 281.4 ng/mL of GB-SAA, 1:5, 820.9 ± 84.0 ng/mL of GB-SAA, 1:10, 2850.9 ± 1059.3 ng/mL of GB alone and 2476.9 ± 396.4 ng/mL of GB-HPMC E5, 1:10) and prolongation in T max (3.2 ± 1.1 h of GB-SAA, 1:5, 6.4 ± 2.2 h of GB-SAA, 1:10, 1.2 ± 0.45 h of GB alone and 1.4 ± 0.55 h of GB-HPMC E5, 1:10) was noticed, indicating the capability of polymeric H + depot in controlling GB release in vivo . In conclusion, the polymeric H + depot strategy influenced drug dissolution and outward drug diffusion sequentially to retard the initial burst release of drugs with elevated solubility in body fluid.

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