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The configuration of Au^(δ+)-ZrO_(2)^(δ−)species induced activation enhances electrocatalytic CO_(2)to formate conversion

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Nano Research 2024年第7期17卷 6006-6015页

作者： Yongjian jia Yadi Zhang Mengque lin Yangyang Cheng Yanjie Xu National Engineering Research Center for Technology and Equipment of Environmental Deposition Lanzhou Jiaotong UniversityLanzhou 730070China Key Lab of Opt-Electronic Technology and Intelligent Control of Ministry of Education Lanzhou Jiaotong UniversityLanzhou 730070China School of Environmental Engineering and Chemistry Luoyang Institute of Science and TechnologyLuoyang 471023China

Electrochemical CO_(2)conversion into value-added chemicals is a promising technology to solve the greenhouse effect and recycle chemical ***,the electrochemical CO_(2)reduction reaction(e-CO_(2)RR)is seriously compromised by weak CO_(2)adsorption and a rough CO_(2)activation process based on the chemical inertness of the CO_(2)molecule and the formed fragile metal–C/O *** this paper,we designed and fabricated Au particles embedded in ZrO_(2).The configuration of Au particles being of positive charge and ZrO_(2)with negative charge is induced and generated by metal–support interactions(MSIs).As a result,Au/ZrO_(2)@C presents a big difference in the CO_(2)conversion compared with the known work,affording a formate yield of 112.5μmol·cm^(−2)·h^(−1)at−1.1 V *** hydrogen electrode(RHE),and a max formate Faradaic efficiency of up to 94.1%at−0.9 V *** superior performance was attributed to the activated Au–ZrO_(2)interface to form the Au^(δ+)*** insitu Fourier transform infrared(FTIR)spectroscopy and theoretical calculations show that the MSIs configuration can be inclined to the*OCO intermediate generation on Au^(δ+)species activating CO_(2)molecules and then accelerate the formation of the*OCHO intermediate in e-CO_(2)RR,thereby favoring the CO_(2)conversion to formate.

关键词： electrochemical CO_(2)reduction reaction(e-CO_(2)RR) Au_(δ+)species formic acid *OCHO intermediate metal-support interactions

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Fabrication of virus-like particles with strip-pattern surface：A two-step self-assembly approach

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Chinese Chemical Letters 2017年第4期28卷 839-844页

作者： Shuo Zhang Chun-Hua Cai Zhou Guan jia-ping lin Xing-Yu Zhu Shanghai Key Laboratory of Advanced Polymeric Materials State Key Laboratory of Bioreactor Engineering Key Laboratory for Ultrafine Materials of Ministry of Education School of Materials Science and Engineering East China University of Science and Technology Shanghai 200237 China

Spherical nanostructures with striped patterns on the surfaces resembling the essential structures of natural virus particles were constructed through a two-step self-assembly approach of polystyrene-boligo（acrylic acid）（PS-b-oligo-AA） and poly（γ-benzyI L-glutamate）-b-poly（ethylene glycol）（PBLG-bPEG） copolymer mixtures in *** the basis of difference in hydrophilicity and self-assembly properties of the two copolymers,the two-step self-assembly process is *** was found that PS-boligo-AA copolymers formed spherical aggregates by adding a certain amount of water into polymer solutions in the first *** the second step,two polymer solutions were mixed and water was further added,inducing the self-assembly of PBLG-b-PEG on the surfaces of PS-b-oligo-AA spheres to form striped ***-depth study was conducted for the indispensable defects of striped patterns which are dislocations and ＋1/2 *** influencing factors such as the mixing ratio of two copolymers and the added water content in the first step on the morphology and defects of the striped patterns were *** work not only presents an idea to interpret mechanism of the cooperative self-assembly behavior,but also provides an effective approach to construct virus-like particles and other complex structures with controllable morphology.

关键词： Virus-like particles Two-step self-assembly Striped patterns Defects Polypeptide Ordered structure

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Simultaneous Bulk-and Surface-initiated Living Polymerization Studied with a Heterogeneous Stochastic Reaction Model

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Chinese Journal of Polymer Science 2024年第3期42卷 364-372,I0008页

作者： jia-Shu Ma Zhi-Ning Huang jia-Hao Li Bang-ping jiang Yan-Da Liao Shi-Chen Ji Xing-Can Shen State Key Laboratory for Chemistry and Molecular Engineering of Medicinal Resources Key Laboratory for Chemistry and Molecular Engineering of Medicinal Resources(Ministry of Education of China)School of Chemistry and Pharmaceutical SciencesGuangxi Normal UniversityGuilin 541004China School of Computer Science and Engineering&School of Software Guangxi Normal UniversityGuilin 541004China

To better characterize the properties of surface-initiated polymers, simultaneous bulk-and surface-initiated polymerizations are usually carried out by assuming that the properties of the surface-initiated polymers resemble those of the bulk-initiated polymers. Through a Monte Carlo simulation using a heterogeneous stochastic reaction model, it was discovered that the bulk-initiated polymers exhibit a higher molecular weight and a lower dispersity than the corresponding surface-initiated polymers, which indicates that the equivalent assumption is invalid. Furthermore, the molecular weight distributions of the two types of polymers are also different, suggesting different polymerization mechanisms. The results can be simply explained by the heterogeneous distributions of reactants in the system. This study is helpful to better understand surface-initiated polymerization.

关键词： Surface-initiated polymerization Polymer brush Stochastic reaction model Heterogeneous polymerization Simultaneous polymerization

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Work-function-induced interfacial electron redistribution of MoO_(2)/WO_(2) heterostructures for high-efficiency electrocatalytic hydrogen evolution reaction

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Rare Metals 2024年第2期43卷 489-499页

作者： Tong-Fei Li Jing Li Lu-ping Zhang jia-Wei Ke Meng-Xing Fan Li-Fang Zhang Cheng-Wei Deng Yi Sun Tao Qian Cheng-lin Yan School of Chemistry and Chemical Engineering Nantong UniversityNantong226019China jiangsu Key Laboratory of New Power Batteries Jiangsu Collaborative Innovation Centre of Biomedical Functional MaterialsSchool of Chemistry and Materials ScienceNanjing Normal UniversityNanjing210023China Aerospace Hydrogen Energy Technology(Shanghai)Co.Ltd. Shanghai201800China Key Laboratory of Core Technology of High Specific Energy Battery and Key Materials for Petroleum and Chemical Industry College of EnergySoochow UniversitySuzhou215006China Light Industry Institute of Electrochemical Power Sources Suzhou215006China

The engineering of the electronic configurations of active sites,together with the production of more accessible active sites through heterostructure design,has been established as a forceful methodology for boosting water electrolysis ***,a facile approach is developed to fabricate well-dispersed MoO_(2) and WO_(2) nanoparticles with abundant heterointerfaces entrapped in N,P-doped carbon nanofibers(referred to as MoO_(2)/WO_(2)@N,P-CNFs hereafter)as hydrogen evolution reaction(HER)electrocatalysts in alkaline and acidic *** spectroscopic analyses and theoretical findings manifest that the heterointerface formed by the work function modulation of MoO_(2)/WO_(2) triggers the spontaneous electron redistribution from MoO_(2)to WO_(2) and a built-in electric field,which is essential to promote water adsorption,optimize the H-intermediate adsorption energy,result in the enhanced charge transfer efficiency,and ultimately increase the intrinsic HER ***,the intimate confinement of MoO_(2)/WO_(2) heterostructures in the porous carbon substrate can restrain the active sites from unfavorable coarsening and detachment,thus ensuring facilitated HER kinetics and outstanding structural *** a result,MoO_(2)/WO_(2)@N,P-CNFs exhibit superior catalytic HER performance in acidic and basic solutions,requiring 118 and 95 mV overpotentials to achieve 10 mA·cm^(−2),respectively,surpassing a number of reported non-noble metal-based *** work provides guidelines for the rational design and construction of special metallic heterocomponents with optimized interfacial electronic structure for various electrochemical technologies.

关键词： Electrospinning MoO_(2)/WO_(2) heterostructure Work function Hydrogen evolution reaction

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Vulnerable brain regions in adolescent major depressive disorder:A resting-state functional magnetic resonance imaging activation likelihood estimation meta-analysis

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World Journal of Psychiatry 2024年第3期14卷 456-466页

作者： Hui Ding Qin Zhang Yan-ping Shu Bin Tian Ji Peng Yong-Zhe Hou Gang Wu Li-Yun lin jia-lin Li Department of Radiology The Second People’s Hospital of Guizhou ProvinceGuiyang 550000Guizhou ProvinceChina Department of Radiology Guizhou Provincial People’s HospitalGuiyang 550000Guizhou ProvinceChina Department of Psychiatry of Women and Children The Second People's Hospital of Guizhou ProvinceGuiyang 550000Guizhou ProvinceChina Department of Radiology Zhijin County People's HospitalBijie 552100Guizhou ProvinceChina Medical Humanities College Guizhou Medical UniversityGuiyang 550000Guizhou ProvinceChina

BACKGROUND Adolescent major depressive disorder(MDD)is a significant mental health concern that often leads to recurrent depression in ***-state functional magnetic resonance imaging(rs-fMRI)offers unique insights into the neural mechanisms underlying this ***,despite previous research,the specific vulnerable brain regions affected in adolescent MDD patients have not been fully *** To identify consistent vulnerable brain regions in adolescent MDD patients using rs-fMRI and activation likelihood estimation(ALE)*** We performed a comprehensive literature search through July 12,2023,for studies investigating brain functional changes in adolescent MDD *** utilized regional homogeneity(ReHo),amplitude of low-frequency fluctuations(ALFF)and fractional ALFF(fALFF)*** compared the regions of aberrant spontaneous neural activity in adolescents with MDD vs healthy controls(HCs)using *** Ten studies(369 adolescent MDD patients and 313 HCs)were *** the ReHo and ALFF/fALFF data,the results revealed that the activity in the right cuneus and left precuneus was lower in the adolescent MDD patients than in the HCs(voxel size:648 mm3,P<0.05),and no brain region exhibited increased *** on the ALFF data,we found decreased activity in the right cuneus and left precuneus in adolescent MDD patients(voxel size:736 mm3,P<0.05),with no regions exhibiting increased *** Through ALE meta-analysis,we consistently identified the right cuneus and left precuneus as vulnerable brain regions in adolescent MDD patients,increasing our understanding of the neuropathology of affected adolescents.

关键词： Major depressive disorder Resting-state functional magnetic resonance imaging Adolescent Activation likelihood estimation Meta-analysis

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Isocyanide-Based One-Pot Cascade Synthesis of 3-Acyl Isoindolinones

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Chinese Journal of Chemistry 2024年第3期42卷 259-263页

作者： jia Liu Yi-Ming Zhu Xiao-ping Xu Shun-Jun Ji Key Laboratory of Organic Synthesis of jiangsu Province College of ChemistryChemical Engineering and Materials Science & Collaborative Innovation Center of Suzhou Nano Science and TechnologySoochow UniversitySuzhouJiangsu215123 China Suzhou Baolidi Functional Materials Research Institute SuzhouJiangsu215144 China

A series of 3-acyl-substituted isoindolinone derivatives were synthesized in a one-pot manner via the reaction of o-bromobenzaldehydes,isocyanides,and carboxylic acids in the presence of palladium catalyst and base. The reaction employing easily available starting materials features simple operation and high efficiency. The mechanistic study showed that the reaction might undergo 1) Pd-catalyzed [3+2] cyclization of o-bromobenzaldehyde with isocyanide and the re-insertion of another molecule of isocyanide,2) addition of carboxylic acid to in situ formed ketenimine followed by a rearrangement relay to give 3,3-diacyl-substituted isoindolinone derivative. Further transformations of the obtained products through decarbonylation could also be realized.

关键词： One-pot reaction Isocyanide Pd catalysis Rearrangement reaction Isoindolinone

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Multimodal abnormalities of brain structures in adolescents and young adults with major depressive disorder:An activation likelihood estimation meta-analysis

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World Journal of Psychiatry 2024年第7期14卷 1106-1117页

作者： Yan-ping Shu Qin Zhang Yong-Zhe Hou Shuang Liang Zu-Li Zheng jia-lin Li Gang Wu Department of Psychiatry of Women and Children The Second People’s Hospital of Guizhou ProvinceGuiyang 550000Guizhou ProvinceChina Department of Radiology The Second People’s Hospital of Guizhou ProvinceGuiyang 550000Guizhou ProvinceChina Department of Radiology Guizhou Provincial People’s HospitalGuiyang 550000Guizhou ProvinceChina Medical Humanities College Guizhou Medical UniversityGuiyang 550000Guizhou ProvinceChina

BACKGROUND Major depressive disorder(MDD)in adolescents and young adults contributes significantly to global morbidity,with inconsistent findings on brain structural changes from structural magnetic resonance imaging *** likeli-hood estimation(ALE)offers a method to synthesize these diverse findings and identify consistent brain *** We performed a comprehensive literature search in PubMed,Web of Science,Embase,and Chinese National Knowledge Infrastructure databases for neuroi-maging studies on MDD among adolescents and young adults published up to November 19,*** independent researchers performed the study selection,quality assessment,and data *** ALE technique was employed to synthesize findings on localized brain function anomalies in MDD patients,which was supplemented by sensitivity *** Twenty-two studies comprising fourteen diffusion tensor imaging(DTI)studies and eight voxel-based morphome-try(VBM)studies,and involving 451 MDD patients and 465 healthy controls(HCs)for DTI and 664 MDD patients and 946 HCs for VBM,were ***-based ALE demonstrated significant reductions in fractional anisotropy(FA)values in the right caudate head,right insula,and right lentiform nucleus putamen in adolescents and young adults with MDD compared to HCs,with no regions exhibiting increased FA ***-based ALE did not demonstrate significant alterations in gray matter *** analyses highlighted consistent findings in the right caudate head(11 of 14 analyses),right insula(10 of 14 analyses),and right lentiform nucleus putamen(11 of 14 analyses).CONCLUSION Structural alterations in the right caudate head,right insula,and right lentiform nucleus putamen in young MDD patients may contribute to its recurrent nature,offering insights for targeted therapies.

关键词： Major depressive disorder Adolescent Young adults Neuroimaging Diffusion tensor imaging Voxel-based morphometry Activation likelihood estimation Meta-analysis

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The dual-action mechanism of Arabidopsis cryptochromes

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Journal of Integrative Plant Biology 2024年第5期66卷 883-896页

作者： Gao-ping Qu Bochen jiang Chentao lin Basic Forestry and Plant Proteomics Research Center Fujian Agriculture and Forestry UniversityFuzhou 350002China Department of Chemistry Department of Biochemistry and Molecular BiologyInstitute for Biophysical DynamicsThe University of ChicagoChicagoIL 60637USA

Photoreceptor cryptochromes (CRYs) mediate blue-light regulation of plant growth and development. It has been reported that Arabidopsis CRY1and CRY2 function by physically interacting with at least 84 proteins, including transcription factors or co-factors, chromatin regulators, splicing factors, messenger RNA methyltransferases, DNA repair proteins, E3 ubiquitin ligases, protein kinases and so on. Of these 84 proteins, 47 have been reported to exhibit altered binding affinity to CRYs in response to blue light, and 41 have been shown to exhibit condensation to CRY photobodies. The blue light-regulated composition or condensation of CRY complexes results in changes of gene expression and developmental programs. In this mini-review, we analyzed recent studies of the photoregulatory mechanisms of Arabidopsis CRY complexes and proposed the dual mechanisms of action, including the “Lock-and-Key” and the “Liquid-Liquid Phase Separation (LLPS)” mechanisms. The dual CRY action mechanisms explain, at least partially, the structural diversity of CRY-interacting proteins and the functional diversity of the CRY photoreceptors.

关键词： Arabidopsis blue light cryptochrome CRY1 CRY2 phaseseparation

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Combined effects of massive reclamation and dredging on the variations in hydrodynamic and sediment transport in lingdingyang Estuary,China

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Frontiers of Earth Science 2024年第1期18卷 127-147页

作者： Kanglin CHEN Yitong lin Jing LIU Zixiao HE Liangwen jia School of Geography and Remote Sensing Guangzhou UniversityGuangzhou 510006China School of Marine Science Sun Yat-Sen UniversityGuangzhou 510275China School of Marine Engineering and Technology Sun Yat-Sen UniversityGuangzhou 510275China Southern Marine Science and Engineering Guangdong Laboratory(Zhuhai)Zhuhai 519080China Guangdong Province Engineering Research Center of Coasts Islands and ReefsGuangzhou 510275China

Anthropogenic disturbances associated with the rapid development of coastal cities have drastically influenced the hydrodynamics and sediment transport processes in many large estuaries *** Estuary(LE),located in the central and southern part of the Pearl River Delta,southern China with a long history of high-intensity anthropogenic disturbances,was studied to explore the contribution rate and mechanism underlying the alteration in hydrodynamics and sediment transport under each phase of human activity.A state-of-the-art modeling tool(TELEMAC-2D),was used to study the variations in the hydrodynamics and sediment transport,accounting for reclamation-induced shoreline and dredging-induced topography *** results indicated that:i)under the influence of successive land reclamation,the general distribution of the Confluence Hydrodynamic Zone(CHZ)in LE varied from scattered to concentrated,and these zones moved 3–5 km ***)Large-scale channel dredging weakened the residual flow in LE,decreasing the residual flow in the Inner-lingding Estuary(ILE)by 62.45%.This was initiated by the enhancement of tidal dynamics through changes in the bottom friction caused by dredging in the *** contrast,massive reclamation decreased the residual flow in the ILE by 17.55%and increased that in the Outer-lingding Estuary(OLE).iii)Despite disturbances related to land reclamation and dredging,the estuarine jet flow in LE remained a turbulent jet system,and the estuarine jet flow became more *** addition,the position of the estuarine jet source moved 6–13 km ***)Both reclamation and dredging decreased the SSC in the ILE and increased the SSC in the *** weakened the SSC in the ILE by 62.19%,whereas dredging enhanced the SSC in the OLE by 49%.Spatially,reclamation resulted in an increase in the SSC near the outlets and a decrease in the SSC in the northern portion of the Western *** mainly increased the SSC in the north

关键词： reclamation and dredging estuarine jet flow dynamics and sediment transport mechanism lingdingyang Estuary

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Digital signal acquisition system for complex nuclear reaction experiments

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Nuclear Science and Techniques 2024年第1期35卷 124-133页

作者： Wei-Liang Pu Yan-lin Ye jian-ling Lou jia-Hao Chen School of Physics and State Key Laboratory of Nuclear Physics and Technology Peking UniversityBeijing 100871China Institute of Applied Physics and Computational Mathematics Beijing 100094China

A digital data-acquisition system based on XIA LLC products was used in a complex nuclear reaction experiment using radioactive ion beams.A flexible trigger system based on a field-programmable gate array(FPGA)parametrization was developed to adapt to different experimental sizes.A user-friendly interface was implemented,which allows converting script language expressions into FPGA internal control *** proposed digital system can be combined with a conventional analog data acquisition system to provide more *** performance of the combined system was veri-fied using experimental data.

关键词： Digital signal acquisition system Trigger Programmable logic Timestamp

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