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Design of bifunctional single-atom catalysts NiSA/ZIF-300 for CO_(2) conversion by ligand regulation strategy

Nano Research 2024年第5期17卷 3827-3834页

作者： Wengang fu Yapei Yun Hongting Sheng Xiaokang Liu Tao ding Shuxian Hu Tao Yao Binghui Ge yuanxin Du Didier Astruc Manzhou Zhu Department of Chemistry and Centre for Atomic Engineering of Advanced Materials Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationCollege of Materials Science and EngineeringInstitutes of Physical Science and Information Technology and Anhui Province Key Laboratory of Chemistry for Inorganic/Organic Hybrid Functionalized MaterialsAnhui UniversityHefei 230601China Universitéde Bordeaux ISMUMR CNRS N°5255351 Cours de La Libération33405 Talence CedexFrance National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei 230026China Department of Physics University of Science and Technology BeijingBeijing 100083China Anhui Tongyuan Environment Energy Saving Co. LtdHefei 230041China

Carbon-supported noble-metal-free single-atom catalysts(SACs)have aroused widespread interest due to their green chemistry aspects and excellent ***,we propose a“ligand regulation strategy”and achieve the successful fabrication of bifunctional SAC/MOF(MOF=metal-organic framework)nanocomposite(abbreviated NiSA/ZIF-300;ZIF=ZIF-8)with exceptional catalytic performance and *** designed NiSA/ZIF-300 has a planar interfacial structure with the Ni atom,involving one S and three N atoms bonded to Ni(Ⅱ),fabricated by controllable pyrolysis of volatile Ni-S *** CO_(2) cycloaddition to styrene epoxide,NiSA/ZIF-300 exhibits ultrahigh activity(turnover number(TON)=1.18×105;turnover frequency(TOF)=9830 molSC·mol_(Ni)^(-1)·h^(-1);SC=styrene carbonate)and durability at 70℃ under 1 atm CO_(2) pressure,which is much superior to Ni complex/ZIF,NiNP/ZIF-300,and most reported *** study offers a simple method of bifunctional SAC/MOF nanocomposite fabrication and usage,and provides guidance for the precise design of additional original SACs with unique catalytic properties.

关键词： single atom catalyst bifunctional CO_(2)conversion cycloaddition

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Relative exchangeable copper, a high-quality biomarker for differentiation of Traditional Chinese Medicine syndrome in Wilson's disease

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Journal of Traditional Chinese Medicine 2024年第5期44卷 1017-1023页

作者： ding Yufeng YANG Wenming CHENG yuan YANG Yulong ZHU Jun LU Yachun FANG Xiang ZHANG Jing Department of Neurology the First Affiliated Hospital of Anhui University of Traditional Chinese Medicine Department of clinical laboratory the First Affiliated Hospital of Anhui University of Traditional Chinese Medicine

OBJECTIVE: To investigate the value of relative exchangeable copper(REC) in diagnosing Wilson's disease(WD) and to determine its significance in the differentiation of Traditional Chinese Medicine(TCM) ***: A total of 78 patients with WD were recruited on the same day of the medical visit, and among them,32 were suffering from non-WD(N-WD) and 37 were heterozygous ATP7B carriers(HC) enrolled as *** genetic testing was performed for diagnosing WD and HC. Additionally, REC levels in different TCM syndromes were investigated. The correlation between REC and serum ceruloplasmin(Cp), serum copper oxidase(CO), and 24-h urinary copper was analyzed using the Global Assessment Scale and Unified Wilson's Disease Rating Scale and the significance of REC in WD diagnosis was investigated. Resting-state functional magnetic resonance imaging was used to assess the clinical symptoms of WD and analyze its severity in different TCM ***: REC determination helped in significantly distinguishing patients with N-WD or HC from those with WD with a cut-off of 21.15%. furthermore, the comparative analysis of REC ratios among different TCM syndromes showed markedly high REC levels in the dampness-heat internal accumulation syndrome ***, the seed-based functional connectivity value from the putamen to the cerebellum was significantly correlated with TCM ***: REC level is a high-quality biomarker for diagnosing WD that effectively reflects disease severity and plays an essential role in deciding on treatment strategies and prognosis. furthermore, REC levels are closely related to TCM syndromes in WD; thus, it is a potential objective quantitative indicator for distinguishing TCM syndromes in WD.

关键词： Global Assessment Scale Traditional Chinese Medicine syndrome Wilson’s disease relative exchangeable copper the Unified Wilson’s Disease Rating Scale

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Ribosome-inspired electrocatalysts inducing preferential nucleation and growth of three-dimensional lithium sulfide for high-performance lithium-sulfur batteries

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Journal of Energy Chemistry 2024年第7期94卷 517-526页

作者： Zhen Wu Wenfeng He Jiahui Yang Yunuo Gu Ruiqi Yang Yiran Sun Jiajia yuan Xin Wang Junwu Zhu Yongsheng fu Key Laboratory for Soft Chemistry and functional Materials of Ministry of Education Nanjing University of Science and TechnologyNanjing 210094JiangsuChina School of Energy and Power Engineering Jiangsu UniversityZhenjiang 212013JiangsuChina FEB Res Inst Far East BatteryWuxi 214200JiangsuChina

Nucleation of lithium sulfide(Li_(2)S)induced by electrocatalysts plays a crucial role in mitigating the shut-tle ***,short-chain polysulfides on electrocatalysts surfaces tend to re-dissolve into elec-trolytes,delaying Li_(2)S supersaturation and its *** this study,we draw inspiration from the ribosome-driven protein synthesis process in cells to prepare ultrasmall nitrogen-doped MoS_(2) nanocrys-tals anchored on porous nitrogen-doped carbon networks(N-MoS_(2)-NC)***,the ex-situ SEM demonstrates that ribosome-inspired N-MoS_(2)-NC electrocatalysts induce early nucleation and rapid growth of three-dimensional Li_(2)s during *** calculations reveal that the Li-s bond length in N-MoS_(2)-Li_(2)S(100)is shorter,and the corresponding interfacial formation energy is lower than in MoS_(2)-Li_(2)S(100).This accelerated conversion of lithium polysulfides to Li_(2)S can enhance the utilization of active substances and inhibit the shuttle *** study highlights the potential of ribosome-inspired N-MoS_(2)-NC in improving the electrochemical stability of Li-S batteries,providing valuable insights for future electrocatalyst design.

关键词： Lithium-sulfur batteries Electrocatalysts Nanocrystals Ribosome-inspired Nucleation and growth

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Network Defense Decision-Making Based on Deep Reinforcement Learning and Dynamic Game Theory

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China Communications 2024年第9期21卷 262-275页

作者： Huang Wanwei yuan Bo Wang Sunan ding Yi Li Yuhua College of Software Engineering Zhengzhou University of Light IndustryZhengzhou 450001China The Third Construction Co. Ltd of China CREC Railway Electrification Engineering GroupZhengzhou 450052China Electronic and Communication Engineering Shenzhen Polytechnic UniversityShenzhen 518055China

Existing researches on cyber attackdefense analysis have typically adopted stochastic game theory to model the problem for solutions,but the assumption of complete rationality is used in modeling,ignoring the information opacity in practical attack and defense scenarios,and the model and method lack *** such problem,we investigate network defense policy methods under finite rationality constraints and propose network defense policy selection algorithm based on deep reinforcement *** on graph theoretical methods,we transform the decision-making problem into a path optimization problem,and use a compression method based on service node to map the network *** this basis,we improve the A3C algorithm and design the DefenseA3C defense policy selection algorithm with online learning *** experimental results show that the model and method proposed in this paper can stably converge to a better network state after training,which is faster and more stable than the original A3C *** with the existing typical approaches,Defense-A3C is verified its advancement.

关键词： A3C cyber attack-defense analysis deep reinforcement learning stochastic game theory

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Twisted Phosphors that Violate Kasha's Exciton Model in Organic Systems

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Chinese Journal of Chemistry 2024年第11期42卷 1237-1246页

作者： Boyi fu Guangming Wang Jiuyang Li Junbo Li Xun Li Xiaoya Zhao Shuhui ding Guoping Yan Qianqian Yan Kaka Zhang School of Materials Science and Engineering Wuhan Institute of TechnologyWuhanHubei430205 China Key Laboratory of Synthetic and Self-Assembly Chemistry for Organic functional Molecules Shanghai Institute of Organic ChemistryUniversity of Chinese Academy of SciencesChinese Academy of Sciences345 Lingling RoadShanghai200032 China

Kasha's exciton model proposes that T1 energy levels of organic compounds are insensitive to molecular aggregation and microenvironment change because of negligible small transition dipole moments of T1 *** model holds true in most organic systems till *** we report the fabrication of twisted organic phosphors with intramolecular charge transfer characters and flexible molecular *** doped into different organic matrices,the twisted phosphor adopts different conformation,exhibits distinct phosphorescence colors and T1 energy levels,which violates Kasha's exciton model in organic *** that the change of phosphorescence colors and maxima can be readily distinguished by human eyes and conventional instrument,the twisted phosphors would be exploited as a new type of molecular probe,which would exhibit potential application in optical sensing and stimuli-responsive systems.

关键词： Afterglow Twisted phosphor Triplet excited state Room-temperature phosphorescence Luminescence Spin-orbit coupling

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Single-neuron projectome-guided analysis reveals the neural circuit mechanism underlying endogenous opioid antinociception

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National Science Review 2024年第7期11卷 106-125页

作者： Yan-Nong Dou yuan Liu Wen-Qun ding Qing Li Hua Zhou Ling Li Meng-Ting Zhao Zheng-Yi-Qi Li Jing yuan Xiao-Fei Wang Wang-yuan Zou Anan Li Yan-Gang Sun Institute of Neuroscience Key Laboratory of Brain Cognition and Brain-Inspired Intelligence Technology CAS Center for Excellence in Brain Science&Intelligence Technology Chinese Academy of Sciences Department of Biology School of Life Science and TechnologyShanghaiTech University Lingang Laboratory University of Chinese Academy of Sciences Britton Chance Center for Biomedical Photonics Wuhan National Laboratory for OptoelectronicsMoE Key Laboratory for Biomedical Photonics Huazhong University of Science and Technology Department of Anesthesiology Xiangya HospitalCentral South University HUST-Suzhou Institute for Brainsmatics JITRI

Endogenous opioid antinociception is a self-regulatory mechanism that reduces chronic pain, but its underlying circuit mechanism remains largely unknown. Here, we showed that endogenous opioid antinociception required the activation of mu-opioid receptors（MORs） in GABAergic neurons of the central amygdala nucleus（CEA） in a persistent-hyperalgesia mouse model. Pharmacogenetic suppression of these CEAMORneurons, which mimics the effect of MOR activation, alleviated the persistent ***, single-neuron projection analysis revealed multiple projectome-based subtypes of CEAMORneurons, each innervating distinct target brain regions. We found that the suppression of axon branches projecting to the parabrachial nucleus（PB） of one subtype of CEAMORneurons alleviated persistent hyperalgesia, indicating a subtype-and axonal-branch-specific mechanism of action. further electrophysiological analysis revealed that suppression of a distinct CEA-PB disinhibitory circuit controlled endogenous opioid antinociception. Thus, this study identified the central neural circuit that underlies endogenous opioid antinociception, providing new insight into the endogenous pain modulatory mechanisms.

关键词： endogenous opioid antinociception mu-opioid receptors central amygdala nucleus parabrachial nucleus single-neuron projectome

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Carbene-Catalyzed Asymmetric Ring-Opening Reaction of Biaryl Lactams to Access Axially Chiral Biaryls

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Chinese Journal of Chemistry 2024年第15期42卷 1734-1740页

作者： Guanjie Wang Guowei yuan Chenlong Wei Ye Zhang Haibin Zhu Weiqi Yang Dongping Shi Xiaoxiang Zhang Zhenqian fu Institute of Advanced Materials Nanjing Tech UniversityNanjingJiangsu 211816China Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources College of Chemical EngineeringNanjing Forestry UniversityNanjingJiangsu 210037China

Axially chiral biaryls represent the most important class of atropisomers,and they widely exist in natural products and biologically active *** also constitute a unique scaffold for chiral ligands and catalysts in organic *** development of synthetic methods to obtain such chiral compounds has received widespread attention,among which catalytically atroposelective ring-opening of configurationally labile compounds represents one of the most attractive *** substrates with strained cyclic structures,such as the renowned Bringmann's lactones,can undergo asymmetric transformation into stable *** advancement primarily relies on metal catalyst combined with well-designed chiral ligands,the approaches utilizing organocatalysis as a critical resolution strategy are notably *** this study,we disclosed a N-heterocyclic carbene(NHC)-catalyzed asymmetric ring-opening reaction of biaryl lactams via direct atroposelective nucleophilic *** optimized bulky carbene catalyst ensures that the reaction can proceed under mild conditions,affording the desired product with good to excellent yields and atroposelectivity.

关键词： N-Heterocyclic carbene Axially chiral biaryls Organocatalysis Ring-opening reactions Dibenzo cyclic lactams Axially chiral amino acids Amide C-N bond activation Atropisomerism Asymmetric catalysis Lactams

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Wettability and corrosion behavior between alkaline slag from sodium smelting of vanadium-titanium magnetite and refractory substrates

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Journal of Iron and Steel Research International 2024年第6期31卷 1399-1410页

作者： Fei Zhao Zhi-wei Bian Hong-xin Zhao De-sheng Chen Zhang-fu yuan Yu-lan Zhen Li-na Wang Tao Qi Collaborative Innovation Center of Steel Technology University of Science and Technology BeijingBeijing 100083China National Engineering Research Center of Green Recycling for Strategic Metal Resources Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China Hebei Zhongke Tongchuang Vanadium&Titanium Technology Co. Ltd.Hengshui 053000HeheiChina

The sodium smelting of vanadium-titanium magnetite can achieve the comprehensive utilization of Fe,V,and ***,the generation of alkaline slag during this process may cause damage to refractory *** wettability and corrosion behavior of alkaline slag on three types of refractory(MgO-C,SiC,and high alumina refractory)substrates were investigated at temperatures up to 1200℃.The effects of duration on the wettability of molten slag on SiC substrates were also *** showed that the high alumina refractory exhibited better wettability with the molten slag than the others,and thus,it is easier to be *** results of scanning electron microscopy coupled with energy dispersive spectroscopy showed that MgO-C and high alumina refractory substrates were severely *** was a visible and regular interfacial reaction layer between the slag and SiC refractory substrate,which was produced by the redox reaction between the metal oxides in the slag and the SiC refractory *** the increase in holding time,the interface layer expands and silico-ferrite phases are generated at the *** redox reaction between Fe_(2)O_(3) and SiC substrate is the main reason for the *** comparing the differences in wettability and corrosion behavior between the alkaline slag from sodium smelting of vanadium-titanium magnetite and MgO-C,SiC and high alumina refractories,it is concluded that SiC refractory has good corrosion resistance to the *** oxides in the slag accelerate the oxidation rate of SiC refractory.

关键词： Wettability Corrosion Alkaline slag-Contact angle Vanadium-titanium magnetite Refractory

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Rotating tank experiments for the study of geophysical fluid dynamics

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Journal of Oceanology and Limnology 2024年第5期42卷 1385-1398页

作者： Changming DONG Xiaojie LU Yuli LIU Guoqing HAN Minghan fu Qian CAO Yang ZHANG Xu CHEN Yeping yuan International Geophysical Fluid Dynamics Laboratory Nanjing University of Information Science and TechnologyNanjing 210044China Department of Atmospheric and Oceanic Sciences University of CaliforniaLos Angeles CA 90095USA State Key Laboratory of Satellite Ocean Environment Dynamics Second Institute of OceanographyMinistry of Natural ResourcesHangzhou 310012China Southern Marine Science and Engineering Guangdong Laboratory(Zhuhai) Zhuhai 519000China Zhejiang Ocean University Zhoushan 316022China Guangdong Ocean University Zhanjiang 524088China Ocean University of China Qingdao 266100China Zhejiang University Hangzhou 310058China

Geophysical fluid dynamics(GFD)is an interdisciplinary field that studies the large-scale motion of fluids in the natural *** a wide range of applications such as weather forecasts and climate prediction,GFD employs various research approaches including in-situ observations,satellite measurements,numerical simulations,theoretical analysis,artificial intelligence,and physical model experiments in *** these approaches,rotating tank experiments provide a valuable tool for simulating naturally-occurring fluid motions in *** proportional scaling and proper techniques,scientists can reproduce multi-scale physical processes of stratified fluids in the rotation system,which allows for the simulation of essential characteristics of fluid motions in the atmosphere and *** this review,rotating tanks of various scales in the world are introduced,as these tanks have been actively used to explore fundamental scientific questions in ocean and atmosphere *** illustrate the GFD experiments,three representative cases are presented to demonstrate the frontier achievements in the the GFD study by using rotating tank experiments:mesoscale eddies in the ocean,convection processes,and plume *** references for the experimental procedures are *** studies are encouraged to further explore the utilization of rotating tanks with improvements in experimental design and integration of other research *** is a promising direction of GFD to help enhance our understanding of the complex nature of fluid motions in the natural world and to address the challenges posed by global environmental changes.

关键词： laboratory experiment rotating tank geophysical fluid dynamics(GFD)

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Highly selective photocatalytic reduction of CO_(2) to CH_(4) on electron-rich Fe species cocatalyst under visible light irradiation

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Carbon Energy 2024年第1期6卷 255-266页

作者： Qianying Lin Jiwu Zhao Pu Zhang Shuo Wang Ying Wang Zizhong Zhang Na Wen Zhengxin ding Rusheng yuan Xuxu Wang Jinlin Long State Key Laboratory of Photocatalysis on Energy and Environment College of ChemistryFuzhou UniversityFuzhouChina

Efficient photocatalytic reduction of CO_(2) to high-calorific-value CH4,an ideal target product,is a blueprint for C_(1)industry relevance and carbon neutrality,but it also faces great ***,we demonstrate unprecedented hybrid SiC photocatalysts modified by Fe-based cocatalyst,which are prepared via a facile impregnation-reduction method,featuring an optimized local electronic *** exhibits a superior photocatalytic carbon-based products yield of 30.0μmol g^(−1) h^(−1) and achieves a record CH_(4) selectivity of up to 94.3%,which highlights the effectiveness of electron-rich Fe cocatalyst for boosting photocatalytic performance and ***,the synergistic effects of directional migration of photogenerated electrons and strongπ-back bonding on low-valence Fe effectively strengthen the adsorption and activation of reactants and intermediates in the CO_(2)→CH_(4) *** study inspires an effective strategy for enhancing the multielectron reduction capacity of semiconductor photocatalysts with low-cost Fe instead of noble metals as cocatalysts.

关键词： artificial synthesis of CH_(4) electronic structure optimization Fe species cocatalyst photocatalytic CO_(2) reduction SiC

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