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Interfacial oxidized Pd species dominate catalytic hydrogenation of polar unsaturated bonds

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Nano Research 2024年第1期17卷 228-234页

作者： Pengyao you Shaoqi Zhan Pengpeng Ruan Ruixuan Qin Shiguang Mo Yazhou Zhang Kunlong Liu Lansun Zheng Nanfeng Zheng State Key Laboratory for Physical Chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy Materialsand Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Department of Chemistry BMCUppsala UniversityBMC Box 576Uppsala S-75123Sweden Department of Chemistry University of OxfordOxford OX13QZUK

The determination of catalytically active sites is crucial for the design of efficient and stable catalysts toward desired ***,the complexity of supported noble metal catalysts has led to controversy over the locations of catalytically active sites(e.g.,metal,support,and metal/support interface).Here we develop a structurally controllable catalyst system(Pd/SBA-15)to reveal the catalytic active sites for the selective hydrogenation of ketones to alcohol using acetophenone hydrogenation as model *** investigations demonstrated that unsupported Pd nanocrystals have no catalytic activity for acetophenone ***,oxidized Pd species were catalytically highly active for acetophenone *** catalytic activity decreased with the decreased oxidation state of *** work provides insights into the hydrogenation mechanism of ketones but also other unsaturated compounds containing polar bonds,e.g.,nitrobenzene,N-benzylidene-benzylamine,and carbon dioxide.

关键词： oxidized Pd metal/oxide interface constant particle size Pd/SBA-15 acetophenone hydrogenation

Growth and inhibition of zinc anode dendrites in Zn-air batteries:Model and experiment

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Chinese Journal of Chemical Engineering 2024年第3期67卷 268-281页

作者： Cuiping He Qingyi Gou Yanqing Hou Jianguo Wang Xiang you Ni Yang Lin Tian Gang Xie Yuanliang Chen Kunming University of Science and Technology State Key Laboratory of Complex Nonferrous Metal Resources Clean UtilizationKunming 650093China Kunming University of Science and Technology Faculty of Metallurgical and Energy EngineeringKunming 650093China China Copper Co.Ltd KunmingYunnan 650051China State Key Laboratory of Advanced Metallurgy for Non-ferrous Metals Kunming 650051China Sichuan Shunying Power Battery Materials Co.Ltd Sichuan 620076China

Zinc(Zn)-air batteries are widely used in secondary battery research owing to their high theoretical energy density,good electrochemical reversibility,stable discharge performance,and low cost of the anode active material ***,the Zn anode also leads to many challenges,including dendrite growth,deformation,and hydrogen precipitation *** this context,Zn dendrite growth has a greater impact on the cycle *** this dissertation,a dendrite growth model for a Zn-air battery was established based on electrochemical phase field theory,and the effects of the charging time,anisotropy strength,and electrolyte temperature on the morphology and growth height of Zn dendrites were studied.A series of experiments was designed with different gradient influencing factors in subsequent experiments to verify the theoretical simulations,including elevated electrolyte temperatures,flowing electrolytes,and pulsed *** simulation results show that the growth of Zn dendrites is controlled mainly by diffusion and mass transfer processes,whereas the electrolyte temperature,flow rate,and interfacial energy anisotropy intensity are the main *** experimental results show that an optimal electrolyte temperature of 343.15 K,an optimal electrolyte flow rate of 40 ml·min^(-1),and an effective pulse charging mode.

关键词： Zn-air battery Zinc anode Zinc dendrite Simulated dendrite growth Inhibit dendrite growth Phase-field model

Design study of charge-stripping scheme of heavy ion beams for HIAF-BRing

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Nuclear Science and Techniques 2024年第5期35卷 30-41页

作者： Jun-Jie Zhang Zhi-you Xu Jin-Quan Zhang Wen-Wen Ge Liang-Ting Sun Huan-Yu Zhao Institute of Modern Physics Chinese Academy of SciencesLanzhou 730000China School of Nuclear Science and Technology University of Chinese Academy of SciencesBeijing 100049China

Charge strippers play an essential role in heavy-ion accelerators by stripping the projectile ions to higher charge states to enhance the acceleration efficiency downstream of the *** the high-energy mode of the booster ring(BRing)of the high-intensity heavy-ion accelerator facility,the pre-accelerated ions from the iLinac will be stripped by a carbon foil to higher charge states and then injected into the *** key parameters of the stripper and stripped ions were calculated,and the influence of stripping on the beam quality was *** get high stripping efficiencies,the foil thicknesses and resultant charge state distributions for the typical ions were determined by the code *** equilibrium thickness was obtained for the U beam,while the stripper thicknesses for the Xe and Kr beams were determined based on a compromise between the stripped charge states and the stripping *** energy loss,energy straggling,and emittance growth due to stripping have a non-negligible impact on the transport of the stripped beams and the injection of the ***,these parameters were simulated by *** addition,the foil’s temperature evolution,which greatly affects the foil lifetime,was simulated by *** maximum temperature of the foil bombarded by the U and Xe beams with the nominal parameters will exceed the safe value in terms of the impact of evaporation on the foil’s *** the foil temperature constraint,the highest tolerable beam intensity and the injected ion number into the ring were derived for different beam *** results of this paper will present important reference data for the optimization design and commissioning of the beamline and injection to the BRing for the stripped ions.

关键词： High-intensity heavy-ion accelerator facility Charge stripper Energy spread Thermal analysis Emittance growth Injection turns

Exploring the Cation Regulation Mechanism for Interfacial Water Involved in the Hydrogen Evolution Reaction by In Situ Raman Spectroscopy

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Nano-Micro Letters 2024年第3期16卷 303-312页

作者： Xueqiu you Dongao Zhang Xia‑Guang Zhang Xiangyu Li Jing‑Hua Tian Yao‑Hui Wang Jian‑Feng Li School of Ocean Information Engineering Fujian Provincial Key Laboratory of Oceanic Information Perception and Intelligent ProcessingJimei UniversityXiamen 361021People’s Republic of China State Key Laboratory of Physical Chemistry of Solid Surfaces MOE Key Laboratory of Spectrochemical Analysis and InstrumentationiChEMCollege of Chemistry and Chemical EngineeringCollege of MaterialsCollege of EnergyXiamen UniversityXiamen 361005People’s Republic of China Key Laboratory of Green Chemical Media and Reactions Ministry of EducationCollaborative Innovation Center of Henan Province for Green Manufacturing of Fine ChemicalsCollege of Chemistry and Chemical EngineeringHenan Normal UniversityXinxiang 453007People’s Republic of China Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM) Xiamen 361005People’s Republic of China

Interfacial water molecules are the most important participants in the hydrogen evolution reaction(HER).Hence,understanding the behavior and role that interfacial water plays will ultimately reveal the HER ***,investigating interfacial water is extremely challenging owing to the interference caused by bulk water molecules and complexity of the interfacial ***,the behaviors of interfacial water in different cationic electrolytes on Pd surfaces were investigated by the electrochemistry,in situ core-shell nanostructure enhanced Raman spectroscopy and theoretical simulation *** spectral evidence reveals a red shift in the frequency and a decrease in the intensity of interfacial water as the potential is shifted in the positively *** comparing the different cation electrolyte systems at a given potential,the frequency of the interfacial water peak increases in the specified order:Li+

关键词： In situ Raman Interfacial water Hydrogen evolution reaction Cations

Single thiolate replacement of metal nanoclusters

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Science China Chemistry 2024年第2期67卷 523-528页

作者： Ambreen Ambreen Yue Zhou Wanmiao Gu Qing you Liang Fang Guoqing Bian Nan Yan Nan Xia Zhikun Wu Key Laboratory of Materials Physics Anhui Key Laboratory of Nanomaterials and NanotechnologyInstitute of Solid State PhysicsHefei Institutes of Physical Science(HFIPS)Chinese Academy of SciencesHefei230031China University of Science and Technology of China Hefei230601China Institute of Physical Science and Information Technology Anhui UniversityHefei230601China

Surface thiolates play important roles in evincing the structures and properties of thiolated metal nanoclusters—one type of recently emerging inorganic-organic hybrids,and thus the thiolate substitution,especially single thiolate substitution,is highly desirable for subtly tailoring the structures and properties of metal ***,such a single-thiolate substituting is challenging,and its influence on the metal-metal and metal-sulfur bonds remains mysterious due to the absence of the singlethiolate-substituted ***,we developed a combined method,concurrently synthesized the single-thiolate-substituted nanocluster and its parent nanocluster,and successfully resolved their structures by single crystal X-ray crystallography,which reveals that the single thiolate substitute has an obvious influence on the metal-metal and metal-sulfur bond lengths although it has no effect on the absorption ***,the metal-metal and metal-sulfur bonds show various thermal extensibility and even the negative thermal expansion phenomena of the Au–S bond were observed in the single-thiolate-substituted *** bond length-related stability was also ***,this study highlights a novel synthesis method and offers novel structural insights and an in-depth structure-property correlation of thiolated metal nanoclusters.

关键词： metal nanoclusters single thiolate replacement thermal expansion stability intercluster interaction

Optimizing 2D-metal contact in layered Tin-selenide via native oxide modulation

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Nano Research 2024年第4期17卷 3014-3020页

作者： Yue Zheng Qi you Zhentian Yin Jian Tang Ke Jiang Zihao Xie Henan Li Cheng Han Yumeng Shi International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education Institute of Microscale OptoelectronicsShenzhen UniversityShenzhen 518060China College of Electronics and Information Engineering Shenzhen UniversityShenzhen 518060China

The discovery of two-dimensional(2D)semiconductor has opened up new avenues for the development of short-channel field-effect transistors(FETs)with desired electrical *** them,orthorhombic tin-selenide(SnSe)has garnered increasing attention due to its potential applications in a variety of electronic,optoelectronic,and thermoelectric ***,the realization of high-performance SnSe FETs with low contact resistance(Rc)remains a ***,we systematically investigate the contact of few-layer SnSe FETs through the modulation of native oxide on SnSe by using different *** is found that chromium(Cr)-contacted devices possess the best FET performance,such as electron mobility up to 606 cm^(2)/(V·s)at 78 K,current on/off ratio exceeding 1010,and saturation current of~550μA/μm,where a negligible Schottky barrier(SB)of~30 meV and a low contact resistance of~425Ωμm are achieved.X-ray photoelectron spectroscopy(XPS)and cross-sectional electron dispersive X-ray spectroscopy(EDX)results further reveal that the improved contact arises from the Cr-induced reduction of native oxide(SnOx)to Sn,which thins the tunneling barrier for efficient electron *** findings provide a deep insight into the 2D-metal contact of SnSe and pave the way for its applications in future nanoelectronics.

关键词： few-layer SnSe field-effect transistors(FETs) Cr contact native oxide contact resistance(Rc) Schottky barrier(SB)

MdbHLH162 connects the gibberellin and jasmonic acid signals to regulate anthocyanin biosynthesis in apple

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Journal of Integrative Plant Biology 2024年第2期66卷 265-284页

作者： Jian-Ping An Rui-Rui Xu Xiao-Na Wang Xiao-Wei Zhang Chun-Xiang you Yuepeng Han Apple technology innovation center of Shandong Province College of Horticulture Science and EngineeringShandong Agricultural UniversityTai-An 271018China CAS Key Laboratory of Plant Germplasm Enhancement and Specialty Agriculture Wuhan Botanical GardenHubei Hongshan LaboratoryThe Innovative Academy of Seed Design of Chinese Academy of SciencesWuhan 430074China College of Biology and Oceanography Weifang UniversityWeifang 261061China

Anthocyanins are secondary metabolites induced by environmental stimuli and developmental *** positive regulators of anthocyanin biosynthesis have been reported,whereas the anthocyanin repressors have been *** the signal transduction pathways of gibberellin(GA)and jasmonic acid(JA)and their regulation of anthocyanin biosynthesis have been investigated,the cross-talk between GA and JA and the antagonistic mechanism of regulating anthocyanin biosynthesis remain to be *** this study,we identified the anthocyanin repressor MdbHLH162 in apple and revealed its molecular mechanism of regulating anthocyanin biosynthesis by integrating the GA and JA ***162 exerted passive repression by interacting with MdbHLH3 and MdbHLH33,which are two recognized positive regulators of anthocyanin ***162 negatively regulated anthocyanin biosynthesis by disrupting the formation of the anthocyanin-activated MdMYB1-MdbHLH3/33complexes and weakening transcriptional activation of the anthocyanin biosynthetic genes MdDFR and MdUF3GT by MdbHLH3 and *** GA repressor MdRGL2a antagonized MdbHLH162-mediated inhibition of anthocyanins by sequestering MdbHLH162 from the MdbHLH162-MdbHLH3/33 *** JA repressors MdJAZ1 and MdJAZ2 interfered with the antagonistic regulation of MdbHLH162 by MdRGL2a by titrating the formation of the MdRGL2a-MdbHLH162 *** findings reveal that MdbHLH162 integrates the GA and JA signals to negatively regulate anthocyanin *** study provides new information for discovering more anthocyanin biosynthesis repressors and explores the cross-talk between hormone signals.

关键词： anthocyanin biosynthesis bHLH transcription factor gibberellin jasmonic acid regulatory network transcriptional regulation

Shedding light on the reversible deactivation of carbon-supported single-atom catalysts in hydrogenation reaction

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Nano Research 2024年第6期17卷 4807-4814页

作者： Runze Chen Xiaoying Wang Jianfei Dang Songjie Yun Liqiang Wang Fangong Kong you-Nian Liu State Key Laboratory of Biobased Material and Green Papermaking Qilu University of TechnologyJinan 250353China School of Material Science and Engineering Zhengzhou UniversityZhengzhou 450001China School of Chemical Engineering Zhengzhou UniversityZhengzhou 450001China Hunan Provincial Key Laboratory of Micro&Nano Materials Interface Science College of Chemistry and Chemical EngineeringCentral South UniversityChangsha 410083China

Carbon-supported single-atom catalysts were found to suffer reversible deactivation in catalytic hydrogenation,but the mechanism is still ***,nitro compounds hydrogenation catalyzed by N-doped carbon-supported Co single atom(Co1/NC)was taken as a model to uncover the mechanism of the reversible deactivation ***1/NC exhibited moderate adsorption towards the substrate molecules(i.e.,nitro compounds or related intermediates),which could be strengthened by the confinement effect from the porous ***,substrate molecules tend to accumulate within the pore channel,especially micropores that host Co1,making it difficult for the reactants to access the active sites and finally leading to their *** situation could be even worse when the substrate molecules possess a large ***,the catalytic activity of Co1/NC could be restored via a simple thermal treatment,which could remove the adsorbates within the pore channel,hence releasing active sites that were originally inaccessible to reactants.

关键词： single-atom catalysts porous carbon support reversible deactivation mechanistic study hydrogenation reaction

Forebrain excitatory neuron-specific loss of Brpf1 attenuates excitatory synaptic transmission and impairs spatial and fear memory

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Neural Regeneration Research 2024年第5期19卷 1133-1141页

作者： Baicheng Zhao Hang Zhang Ying Liu Gaoyu Zu Yuxiao Zhang Jiayi Hu Shuai Liu Linya you Department of Human Anatomy&Histoembryology School of Basic Medical SciencesFudan UniversityShanghaiChina Shanghai Key Laboratory of Brain Functional Genomics(Ministry of Education) Affiliated Mental Health Center(ECNU)School of Psychology and Cognitive ScienceEast China Normal UniversityShanghaiChina Shanghai Changning Mental Health Center ShanghaiChina NYU-ECNU Institute of Brain and Cognitive Science at NYU Shanghai ShanghaiChina Key Laboratory of Medical Imaging Computing and Computer Assisted Intervention of Shanghai ShanghaiChina

Bromodomain and plant homeodomain(PHD)finger containing protein 1(Brpf1)is an activator and scaffold protein of a multiunit complex that includes other components involving lysine acetyltransferase(KAT)6A/6B/***1,KAT6A,and KAT6B mutations were identified as the causal genes of neurodevelopmental disorders leading to intellectual *** previous work revealed strong and specific expression of Brpf1 in both the postnatal and adult forebrain,especially the hippocampus,which has essential roles in learning and ***,we hypothesized that Brpf1 plays critical roles in the function of forebrain excitatory neurons,and that its deficiency leads to learning and memory *** test this,we knocked out Brpf1 in forebrain excitatory neurons using *** found that Brpf1 deficiency reduced the frequency of miniature excitatory postsynaptic currents and downregulated the expression of genes Pcdhgb1,Slc16a7,Robo3,and Rho,which are related to neural development,synapse function,and memory,thereby damaging spatial and fear memory in *** findings help explain the mechanisms of intellectual impairment in patients with BRPF1 mutation.

关键词： behavioral test Brpf1 CAMKIIa-Cre intellectual disability miniature excitatory postsynaptic current mRNA-Seq