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Chain Dynamics Heterogeneity in Plasticized Poly(vinyl butyral)(PVB) as Elucidated by Solid-State NMR

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Chinese Journal of Polymer Science 2024年第1期42卷 113-124,I0010页

作者： Jing Lv Xu chen Zi-Shuo Wu ya-Hui Li Wei chen National Synchrotron Radiation Laboratory Anhui Provincial Engineering Laboratory of Advanced Functional Polymer FilmCAS Key Laboratory of Soft Matter ChemistryUniversity of Scienceand Technology of ChinaHefei 230026China

The chain dynamics heterogeneity of the poly(vinyl butyral)(PVB) plasticized by triethylene glycol bis(2-ethylhexa noate)(TEG-EH) was investigated by various solid-state NMR *** plasticized PVB shows two domains in distinct molecular dynamics differences,namely,rigid and soft domains,where the latter is the plasticizer-rich *** time domain low field NMR was first used to investigate the dynamics heterogeneity of the plasticized PVB,and the results show the decreasing activated energy of components in the soft domain of plasticized PVB(E_a=20.2 kJ/mol) as compared with that of the pristine one(E_a=24.3 kJ/mol).Detailed dynamics heterogeneity was obtained by high-field NMR with site-specific *** quadrupole-echo ~2H-NMR was adopted to elucidate the dynamics heterogeneity of the vinyl alcohol(VA) units,where only the hydroxyl group of VA is *** ~1H-^(13)C WISE NMR spectra show that there is not much difference in the mobility of the VB unit in PVB with and without plasticizer,whereas the glass transition temperature differed by approximately 53℃.This is further supported by Torchia's T_1 relaxation *** origin of such an unusual phenomenon is attributed to the critical role of the remaining VA(~22%) in the soft domain,where the VA units locally aggregate through hydrogen ***,the existence of a mobility gradient in the VB unit has been ***,the mobility difference for VB with different stereo-geometry(meso or racemic conformation) is observed for the first *** indicates the importance of modulating the ratio of meso over racemic VB for controlling the macroscopic perfo rmance of PVB.

关键词： Poly(vinyl butyral) Dynamics heterogeneity Plasticizer Solid state NMR

Stability of the Phase Separation State for Compressible Navier-Stokes/Allen-Cahn System

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Acta Mathematicae Applicatae Sinica 2024年第1期40卷 45-74页

作者： ya-zhou chen hakho Hong Xiao-ding Shi Department of Mathematics College of Mathematics and PhysicsBeijing University of Chemical TechnologyBeijing100029China Institute of Mathematics State Academy of SciencesPyongyangKorea

This paper is concerned with the large time behavior of the Cauchy problem for Navier-Stokes/AllenCahn system describing the interface motion of immiscible two-phase flow in 3-D. The existence and uniqueness of global solutions and the stability of the phase separation state are proved under the small initial perturbations. Moreover, the optimal time decay rates are obtained for higher-order spatial derivatives of density,velocity and phase. Our results imply that if the immiscible two-phase flow is initially located near the phase separation state, then under small perturbation conditions, the solution exists globally and decays algebraically to the complete separation state of the two-phase flow, that is, there will be no interface fracture, vacuum, shock wave, mass concentration at any time, and the interface thickness tends to zero as the time t → +∞.

关键词： Navier-Stokes/Allen-Cahn system existence uniqueness large time behavior decay rate

Localization for mixed near-field and far-field sources under impulsive noise

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Journal of Systems Engineering and Electronics 2024年第2期35卷 302-315页

作者： GAO Hongyuan ZhaNG Yuze DU ya’nan chenG Jianhua chen Menghan College of Information and Communication Engineering Harbin Engineering UniversityHarbin 150001China College of Intelligent Systems Science and Engineering Harbin Engineering UniversityHarbin 150001China

In order to solve the problem that the performance of traditional localization methods for mixed near-field sources(NFSs)and far-field sources(FFSs)degrades under impulsive noise,a robust and novel localization method is *** eliminating the impacts of impulsive noise by the weighted out-lier filter,the direction of arrivals(DOAs)of FFSs can be estimated by multiple signal classification(MUSIC)spectral peaks *** on the DOAs information of FFSs,the separation of mixed sources can be ***,the estimation of localizing parameters of NFSs can avoid two-dimension spectral peaks search by decomposing steering *** Cramer-Rao bounds(CRB)for the unbiased estimations of DOA and range under impulsive noise have been *** experiments verify that the proposed method has advantages in probability of successful estimation(PSE)and root mean square error(RMSE)compared with existing localization *** can be concluded that the proposed method is effective and reliable in the environment with low generalized signal to noise ratio(GSNR),few snapshots,and strong impulse.

关键词： source localization far-field source(NFS) near-field source(FFS) impulsive noise Cramer-Rao bound(CRB)

Quantitative prediction model for the depth limit of oil accumulation in the deep carbonate rocks:A case study of Lower Ordovician in Tazhong area of Tarim Basin

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Petroleum Science 2024年第1期21卷 115-124页

作者： Wen-yang Wang Xiong-Qi Pang ya-Ping Wang Zhang-Xin chen Fu-Jie Jiang Ying chen State Key Laboratory of Lithospheric Evolution Institute of Geology and GeophysicsChinese Academy of SciencesBeijing100029China State Key Laboratory of Petroleum Resources and Prospecting China University of Petroleum(Beijing)Beijing102249China College of Geosciences China University of Petroleum(Beijing)Beijing102249China Research Institute of Exploration and Development PetroChina Southwest Oil&Gas Field CompanyChengdu610041SichuanChina Chemical and Petroleum Engineering Schulich School of EngineeringUniversity of CalgaryCalgaryT2N 1N4Canada

With continuous hydrocarbon exploration extending to deeper basins,the deepest industrial oil accumulation was discovered below 8,200 m,revealing a new exploration ***,the extent to which oil exploration can be extended,and the prediction of the depth limit of oil accumulation(DLOA),are issues that have attracted significant attention in petroleum *** it is difficult to characterize the evolution of the physical properties of the marine carbonate reservoir with burial depth,and the deepest drilling still cannot reach the ***,the DLOA cannot be predicted by directly establishing the relationship between the ratio of drilling to the dry layer and the *** this study,by establishing the relationships between the porosity and the depth and dry layer ratio of the carbonate reservoir,the relationships between the depth and dry layer ratio were obtained *** depth corresponding to a dry layer ratio of 100%is the *** on this,a quantitative prediction model for the DLOA was finally *** results indicate that the porosity of the carbonate reservoir,Lower Ordovician in Tazhong area of Tarim Basin,tends to decrease with burial depth,and manifests as an overall low porosity reservoir in deep *** critical porosity of the DLOA was 1.8%,which is the critical geological condition corresponding to a 100%dry layer ratio encountered in the *** depth of the DLOA was 9,000 *** study provides a new method for DLOA prediction that is beneficial for a deeper understanding of oil accumulation,and is of great importance for scientific guidance on deep oil drilling.

关键词： Deep layer Tarim Basin Hydrocarbon accumulation Depth limit of oil accumulation Prediction model

Dynamic lithium-compensation mechanism for densification of garnet-type Li_(7)La_(3)Zr_(2)O_(12)electrolyte by Li_(2)O atmosphere buffer pair

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Nano Research 2024年第7期17卷 6184-6191页

作者： Chujun Zheng ya chen haoxin Dong yan Lu Jun Jin Zhaoyin Wen CAS Key Laboratory of Materials for Energy Conversion Shanghai Institute of CeramicsChinese Academy of ScienceShanghai 200050China State Key Lab High Performance Ceram and Superfine Shanghai Institute of CeramicsChinese Academy of SciencesShanghai 200050China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China

Solid-state lithium metal batteries are one of the most promising options for next-generation batteries pursuing high-energy density and ***,the inevitable volatilization of lithium compounds during sintering leads to low relative density and low ionic conductivity of solid-state ***,the dynamic lithium-compensation mechanism is proposed to facilitate the densification of Ta-substituted garnet-type electrolyte(Li_(6.5)La_(3)Zr_(1.5)Ta_(0.5)O_(12)(LLZT))through the reversible manipulating of Li_(2)O ***_(2)ZrO_(3)is used as mother powder additive,which reacts with Li_(2)O in sintering atmosphere and forms Li_(6)Zr_(2)O_(7).Li_(2)ZrO_(3)/Li_(6)Zr_(2)O_(7)buffer pair manipulates the sintering Li_(2)O atmosphere,which is vital for LLZT,within the Li_(2)O partial pressure range corresponding to Li_(2)ZrO_(3)and Li_(6)Zr_(2)O_(7).Furthermore,the reversibility mechanism of buffer pair for Li_(2)O absorption and release is *** obtained LLZT exhibits a relative density of over 96%and an ionic conductivity exceeding 7×10^(−4)S·cm^(−1)with no abnormal grain *** symmetric cell demonstrates an excellent lithium dendrite suppressing ability(stable cycling at a current density of 0.3 mA·cm^(−2)for over 1000 h).Such dynamic lithium-compensation strategy has been successfully applied in atmosphere manipulation of LLZT sintering process,which reduces the dependence of LLZT on the Li_(2)O atmosphere,making it conducive to large-scale preparation of electrolyte ceramics.

关键词： solid-state batteries garnet-type electrolyte high-density electrolyte dynamic lithium-compensation buffer pair

Cone-beam computed tomography noise reduction method based on U-Net with convolutional block attention module in proton therapy

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Nuclear Science and Techniques 2024年第7期35卷 89-100页

作者： Xing-Yue Ruan Xiu-Fang Li Meng-ya Guo Mei chen Ming Lv Rui Li Zhi-Ling chen Shanghai Institute of Applied Physics Chinese Academy of SciencesShanghai201800China University of Chinese Academy of Sciences Beijing100049China Shanghai Advanced Research Institute Chinese Academy of SciencesShanghai201210China Department of Radiation Oncology Ruijin HospitalShanghai Jiao Tong University School of MedicineShanghai200025China Shanghai Key Laboratory of Proton therapy Shanghai201801China

Cone-beam computed tomography(CBCT) is mostly used for position verification during the treatment process. However,severe image artifacts in CBCT hinder its direct use in dose calculation and adaptive radiation therapy re-planning for proton therapy. In this study, an improved U-Net neural network named CBAM-U-Net was proposed for CBCT noise reduction in proton therapy, which is a CBCT denoised U-Net network with convolutional block attention modules. The datasets contained 20 groups of head and neck images. The CT images were registered to CBCT images as ground truth. The original CBCT denoised U-Net network, sCTU-Net, was trained for model performance comparison. The synthetic CT(SCT) images generated by CBAM-U-Net and the original sCTU-Net are called CBAM-SCT and U-Net-SCT images, respectively. The HU accuracies of the CT, CBCT, and SCT images were compared using four metrics: mean absolute error(MAE), root mean square error(RMSE), peak signal-to-noise ratio(PSNR), and structure similarity index measure(SSIM). The mean values of the MAE, RMSE, PSNR, and SSIM of CBAM-SCT images were 23.80 HU, 64.63 HU, 52.27 dB, and 0.9919, respectively,which were superior to those of the U-Net-SCT images. To evaluate dosimetric accuracy, the range accuracy was compared for a single-energy proton beam. The γ-index pass rates of a 4 cm × 4 cm scanned field and simple plan were calculated to compare the effects of the noise reduction capabilities of the original U-Net and CBAM-U-Net on the dose calculation results. CBAM-U-Net reduced noise more effectively than sCTU-Net, particularly in high-density tissues. We proposed a CBAM-U-Net model for CBCT noise reduction in proton therapy. Owing to the excellent noise reduction capabilities of CBAM-U-Net, the proposed model provided relatively explicit information regarding patient tissues. Moreover, it maybe be used in dose calculation and adaptive treatment planning in the future.

关键词： Proton therapy Cone-beam CT CBAM-U-Net γ-index

Enhancing reversible hydrogen storage performance of 2LiBH_(4)–MgH_(2)via in-situ building heterogeneous nucleation sites

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Rare Metals 2024年第9期43卷 4367-4376页

作者： Wei chen ya-Hui Sun Tian Xu Xue-Bin Yu Guang-Lin Xia Department of Materials Science Fudan UniversityShanghai 200433China

2LiBH_(4)-MgH_(2)composite is one of the most attractive reactive hydride composites with a theoretic hydrogen capacity of 10.8 wt%.However,the large nucleation restriction of MgB_(2)during the second step of dehydrogenation results in sluggish hydrogen storage kinetics and high operating temperature,which hinders its practical application as on-board hydrogen storage ***,Al3Ti doped Al nanoparticles(AT NPs)are prepared by a facile chemical reduction reaction to improve the hydrogen storage performance of 2LiBH_(4)-MgH_(2)*** the initial H_(2)desorption process,MgAlB_(4)and TiB_(2)that have identical crystal structure and low d-value mismatch with MgB_(2)resulting from the reaction between AT NPs and 2LiBH_(4)-MgH_(2)composite serve as effective nucleation sites for the formation of MgB_(2).As a result,the apparent activation energy of the two-step H_(2)desorption of AT NPs doped 2LiBH_(4)-MgH_(2)composite are notably decreased to(110.0±5.9)and(119.6±1.4)kJ·mol^(-1),which is 55.5 and 33.5 kJ·mol^(-1)lower than that of the undoped *** importantly,a reversible hydrogen storage capacity of 9.2 wt%after 10cycles of H_(2)desorption and adsorption could be achieved,corresponding to a capacity retention rate of 99%.The building of reactive bimetallic catalyst towards in situ formation of heterogeneous nucleation sites provides a new strategy for improving the hydrogen storage performance of reactive hydride composites.

关键词： Reversible hydrogen storage Reactive hydride composites Catalytic effects Heterogeneous nucleation

Introducing urea into tirapazamine derivatives to enhance anticancer therapy

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National Science Review 2024年第4期11卷 245-253页

作者： yajun Xu Jianlin Lv Chaoying Kong ya Liu Kun Wang Zhaohui Tang Xuesi chen Key Laboratory of Polymer Ecomaterials Changchun Institute of Applied ChemistryChinese Academy of Sciences School of Applied Chemistry and Engineering University of Science and Technology of China

Tirapazamine（TPZ） has been approved for multiple clinical trials relying on its excellent anticancer ***,as a typical hypoxia-activated prodrug（haP）,TPZ did not exhibit survival advantages in Phase Ⅲ clinical trials when used in combination therapy due to the insufficient hypoxia levels in patients' *** this study,to improve the therapeutic effects of TPZ,we first introduced urea to synthesize a series of urea-containing derivatives of *** urea-containing TPZ derivatives showed increased hypoxic cytotoxicity（9.51-30.85-fold） compared with TPZ,while maintaining hypoxic ***,one of these derivatives,showed 20-fold higher cytotoxicity than TPZ while maintaining a similar hypoxic cytotoxicity *** highly efficiently deliver TPZP to the tumors and reduce its side effects on healthy tissues,we further prepared TPZP into a nanodrug with fibrin-targeting ability:***4-NPs,a vascular disrupting agent,was used to increase the fibrin level within tumors and exacerbate tumor *** being combined with CA4-NPs,FT11-TPZP-NPs can accumulate in the hypoxia-aggravated tumors and activate sufficiently to kill tumor *** a single-dose treatment,FT11-TPZP-NPs+CA4-NPs showed a high inhibition rate of 98.1% against CT26 tumor models with an initial volume of ～480 mm3and four out of six tumors were completely eliminated;it thereby exerted a significant antitumor *** study provides a new strategy for improving the therapeutic effect of TPZ and other haPs in anticancer therapy.

关键词： tirapazamine vascular disrupting agent hypoxia-activated prodrug combretastatin A4 urea

Boosting solar hydrogen production via electrostatic interaction mediated ***-TiO_(2−x)biohybrid system

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Nano Research 2024年第6期17卷 5390-5398页

作者： Xingxing Lv Weicheng Huang ya Gao Rui chen Xiaowei chen Danqing Liu Ling Weng Liangcan He Shaoqin Liu School of Material Science and Chemical Engineering Harbin University of Science and TechnologyHarbin 150040China School of Medicine and Health and Key Laboratory of Micro-systems and Micro-structures Manufacturing of Ministry of EducationHarbin Institute of TechnologyHarbin 150001China Department of Physics School of ScienceJimei UniversityXiamen 361021China Zhengzhou Research Institute Harbin Institute of TechnologyZhengzhou 450046China

Hydrogen is garnering growing attention as a green energy source with zero carbon ***,most hydrogen production technologies still rely on the consumption of fossil fuels and are therefore *** has driven the search for more environmentally friendly methods of hydrogen *** this work,we present an innovative approach to enhance hydrogen generation via electrostatic interaction in the Escherichia coli and defective titanium dioxide(TiO_(2−x))*** method involves narrowing the forbidden bandwidth of TiO2 while introducing defect bands into its conduction band to facilitate visible light absorption and efficient charge *** biohybrid system,consisting of *** and TiO_(2−x),demonstrates a remarkable capability to produce 1.25 mmol of hydrogen within a 3-h timeframe under visible light *** accomplishment signifies a 3.31-fold rise in hydrogen production in comparison to ***,signifying a substantial enhancement in hydrogen production ***,we delve into the alterations in biological metabolites associated with hydrogen production and the changes in electron transfer in different biohybrid *** provides valuable insights into the understanding of the intrinsic mechanisms that drive the *** work introduces a novel and promising avenue for achieving this exciting goal.

关键词： Escherichia coli TiO_(2−x)nanoparticles biohybrid system hydrogen production