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“Capture-activation-recapture” mechanism-guided design of double-atom catalysts for electrocatalytic nitrogen reduction

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Journal of Energy Chemistry 2024年第9期96卷 437-447页

作者： Cheng He Shiqi yan Wenxue Zhang State Key Laboratory for Mechanical Behavior of Materials School of Materials Science1nd EngineeringXi’an Jiaotong UniversityXi’an 710049ShaanxiChina School of Materials Science1nd Engineering Chang’an UniversityXi’an 710064ShaanxiChina

Compared with the traditional industrial nitrogen fixation, electrocatalytic methods, especially those utilizing double-atom catalysts containing nonmetals, can give good consideration to the economy and environmental protection. However, the existing “acceptance-donation” mechanism is only applicable to bimetallic catalysts and nonmetallic double-atom catalysts containing boron atoms. Herein, a novel “capture-activation-recapture” mechanism for metal-nonmetal double-atom catalyst is proposed to solve the problem by adjusting the coordination environments of nonmetallic atoms and utilizing the activation effect of metal atoms on nitrogen. Based on this mechanism, the nitrogen reduction reaction (NRR) activity of 48 structures is calculated by density functional theory calculation, and four candidates are selected as outstanding electrocatalytic nitrogen reduction catalysts: Si-Fe@NG (U_(L) = –0.14 V), Si-Co@NG (U_(L)= –0.15 V), Si-Mo@BP1 (U_(L) = 0 V), and Si-Re@BP1 (U_(L) = –0.02 V). The analyses of electronic properties further confirm “capture-activation-recapture” mechanism and suggest that the difference in valence electron distribution between metal and Si atoms triggers the activation of N≡N bonds. In addition, a machine learning approach is utilized to generate an expression and an intrinsic descriptor that considers the coordination environment to predict the limiting potential. This study offers profound insight into the synergistic mechanism of TM and Si for NRR and guidance in the design of novel double-atom nitrogen fixation catalysts.

关键词： "Capture-activation-recapture"mechanism Double-atom catalyst Nitrogen reduction reaction Density functional theory

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Synthetic host-guest pairs as novel bioorthogonal tools for pre-targeting

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Chinese Chemical Letters 2024年第2期35卷 44-56页

作者： yan-Long Ma Shi yan Xiong-Jie Xu Hua Cao Ruibing Wang School of Chemistry and Chemical Engineering and Guangdong Cosmetics Engineering & Technology Research Center Guangdong Pharmaceutical UniversityZhongshan 528458China State Key Laboratory of Quality Research in Chinese Medicine and the Institute of Chinese Medical ScienceUniversity of MacaoMacao 999078China

Due to its simplicity, high efficiency, and chemo-selectivity, bioorthogonal chemistry has shown a great application potential in ***, four bioorthogonal pairs as targeting tools, including (strept)avidin/biotin, antibody/antigen, oligonucleotide hybridization and IEDDA tools, have been developed and applied in targeted ***, all of these tools still suffer from some limitations, such as difficult modification, biochemical fragility and larger molecular weight for biological association tools, as well as chemical instability for IEDDA *** host-guest pairs with relatively small molecular sizes not only possess strong chemical stability, but also have the features of fast conjugation rate, tunable binding affinity , easy modification, and high ***, they can be used as a novel non-covalent bioorthogonal tool for *** order to further promote the development of host-guest pairs as novel bioorthogonal tools for pre-targeted delivery, we firstly calculate their conversion rate to make researcher aware of their unique advantages;next, we summarize the recent research progress in this *** future perspectives and limitations of these unique tools will be *** review will provide a systemic overview of the development of synthetic host-guest pairs as novel bioorthogonal tools for pre-targeting, and may serve as a “go for” resort for researchers who are interested in searching for new synthetic tools to improve pre-targeting.

关键词： Bioorthogonal chemistry Synthetic host-guest pairs Pre-targeting Molecular recognition Biomedical applications

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Sea level rise along China coast from 1950 to 2020

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Science China Earth Sciences 2024年第3期67卷 802-810页

作者： Dapeng MU Tianhe XU Haoming yan Institute of Space Sciences Shandong UniversityWeihai 264209China Innovation Academy for Precision Measurement Science and Technology Chinese Academy of SciencesWuhan 430071China Institute of Marine and Antarctic Science University of TasmaniaHobartTasmania 7004Australia

Global mean sea level rise has been reconstructed using tide gauges. However, long-term sea level rise along the China coast is unclear. To address this issue, a data assimilation approach is developed to reconstruct sea level rise along the China coast from 1950 to 2020 using a global distribution of tide gauges(TGs). This approach combines climate models and sea level fingerprints. The climate models provide stereodynamic sea level changes. The sea level fingerprints include increases in ocean mass due to global ice melting and changes in water storage on land. The reconstructed global mean sea level rise agrees well with previous studies. We quantify sea level rise at 20 TGs along the China coast. The results suggest that sea level rise along the China coast(1.95±0.33 mm yr^(-1)) is greater than the global mean(1.71±0.17 mm yr^(-1)). We also find that China's coastal sea level rise is more than three times faster after 1980, increasing from 0.84±0.28 mm yr^(-1)for 1950–1980 to3.12±0.21 mm yr^(-1)for 1980–2020. This finding implies a significant sea level acceleration along the China coast. Our results advance the understanding of long-term sea level changes along the China coast.

关键词： Sea level rise China coast Tide gauges Data assimilation

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Effects of different concentrations of nicotinamide on hematopoietic stem cells cultured in vitro

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World Journal of Stem Cells 2024年第2期16卷 163-175页

作者： yan Ren yan-Ni Cui Hong-Wei Wang The Second Clinical Medical College Shanxi Medical UniversityTaiyuan 030001Shanxi ProvinceChina Department of Hematology The Second Hospital of Shanxi Medical UniversityTaiyuan 030001Shanxi ProvinceChina Department of Hematology Key Laboratory of Molecular Diagnosis and Treatment of Blood Diseases in Shanxi ProvinceTaiyuan 030001Shanxi ProvinceChina

BACKGROUND In vitro expansion to increase numbers of hematopoietic stem cells(HSCs)in cord blood could improve clinical efficacy of this vital ***(NAM)can promote HSC expansion ex vivo,but its effect on hematopoietic stem and progenitor cells(HSPCs,CD34^(+)CD38)and functional subtypes of HSCs-shortterm repopulating HSCs(ST-HSCs,CD34^(+)CD38CD45RACD49f^(+))and long-term repopulating HSCs(LT-HSCs,CD34^(+)CD38CD45RACD49f^(+)CD90^(+))is not yet *** a sirtuin 1(SIRT1)inhibitor,NAM participates in regulating cell adhesion,polarity,migration,proliferation,and ***,SIRT1 exhibits dual effects by promoting or inhibiting differentiation in different tissues or *** propose that the concentration of NAM may influence proliferation,differentiation,and SIRT1 signaling of *** To evaluate the effects and underlying mechanisms of action of different concentrations of NAM on HSC proliferation and *** CD34^(+)cells were purified from umbilical cord blood using MacsCD34 beads,and cultured for 10-12 d in a serum-free medium supplemented with cytokines,with different concentrations of NAM added according to experimental *** cytometry was used to detect phenotype,cell cycle distribution,and apoptosis of the cultured ***-time polymerase chain reaction was used to detect the transcription levels of target genes encoding stemness-related factors,che mokines,components of hypoxia pathways,and antioxidant ***-dihydro-fluorescein diacetate probes were used to evaluate intracellular production of reactive oxygen species(ROS).Determination of the effect of different culture conditions on the balance of cytokine by cytometric bead *** Compared with the control group,the proportion and expansion folds of HSPCs(CD34^(+)CD38)incubated with 5 mmol/L or 10 mmol/L NAM were significantly increased(all P<0.05).The ST-HSCs ratio and fold expansion of the 5 mmol/L NAM group were significantly

关键词： Hematopoietic stem cells Nicotinamide Concentration Proliferation Differentiation Sirtuin 1

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Distributed Minimum-Energy Containment Control of Continuous-Time Multi-Agent Systems by Inverse Optimal Control

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IEEE/CAA Journal of Automatica sinica 2024年第6期11卷 1533-1535页

作者： Fei yan Xiangbiao Liu Tao Feng School of Information Science and Technology Southwest Jiaotong UniversityChengdu 611756China National Engineering Laboratory of Integrated Transportation Big Data Application Technology Chengdu 611756China

Dear Editor,This letter focuses on the distributed optimal containment control of continuous-time multi-agent systems(CTMASs)with respect to the minimum-energy performance index over fixed *** achieve this,we firstly investigate the optimal containment control problem using the inverse optimal control method,where all states of followers asymptotically converge to the convex hull spanned by the leaders while some quadratic performance indexes get minimized.A sufficient condition for existence of the distributed optimal containment control protocol is *** introducing the parametric algebraic Riccati equation(PARE),it is strictly proved that the global performance index can be used to approximate the standard minimumenergy performance index as the parameters tends to *** consequence,the standard minimum-energy cooperative containment control can be solved by local steady state feedback protocols.

关键词： optimal infinity algebraic

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Metal-organic framework-derived CoSe_(2)@N-doped carbon nanocubes for high-performance lithium-ion capacitors

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Rare Metals 2024年第5期43卷 2150-2160页

作者： Lei Wang Xiong Zhang yan-yan Kong Chen Li Ya-Bin An Xian-Zhong Sun Kai Wang yan-Wei Ma Institute of Electrical Engineering Chinese Academy of SciencesBeijing 100190China School of Engineering Sciences University of Chinese Academy of SciencesBeijing 100190China Institute of Electrical Engineering and Advanced Electromagnetic Drive Technology Qilu ZhongkeJinan 250013China School of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450001China

Cobalt selenide(CoSe_(2))has garnered considerable attention as a prospective anode candidate for advanced lithium-ion storage,prompting comprehensive ***,CoSe_(2)-based anodes usually suffer from significant volume variation upon lithiation leading to unsatisfactory cycling ***,a versatile synthesis route is proposed for the in-situ fabrication of CoSe2nanoparticles embedded in N-dope carbon skeleton(CoSe_(2)@NC)through annealing treatment and selenization of a metal–organic framework-derived(MOF)*** N-doped carbon derived from the MOF serves not only as an excellent conductive substrate but also as a confined reactor,effectively inhibiting the structural instability and alleviating the inevitable volume change of CoSe_(2).Owing to their unique nanostructure,the as-prepared CoSe_(2)@NC exhibits a high capacity of 745.9mAh·g^(-1)at 0.1 A·g^(-1),while maintaining excellent rate capability and an impressive ***,the assembled lithium-ion capacitor(LIC)based on CoSe_(2)@NC demonstrates an energy density of 130Wh·kg^(-1),a power density of 24.6 kW·kg^(-1),and remarkable capacity retention of 90.8%after 8000 *** results highlight the great potential of CoSe_(2)@NC for practical applications.

关键词： Lithium capacitors Cobalt selenide Metal-organic frameworks N-doped carbon

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Corrosion behavior of Gd_(2)Zr_(2)O_(7)thermal barrier coatings under Fe-containing environmental sediment attack

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Journal of Advanced Ceramics 2024年第4期13卷 447-462页

作者： Lei Guo yanyan Li Kai yan School of Materials Science and Engineering Tianjin UniversityTianjin 300072China Tianjin Key Laboratory of Advanced Joining Technology Key Lab of Advanced Ceramics and Machining Technology of Ministry of EducationTianjin 300072China Key Laboratory of Special Equipment Safety and Energy-saving for State Market Regulation China Special Equipment Inspection&Research InstituteBeijing 100029China

Environmental sediments mainly consisting of CaO–MgO–Al_(2)O_(3)–SiO_(2)(CMAS)corrosion are a serious threat to thermal barrier coatings(TBCs),in which Fe element is usually ***_(2)Zr_(2)O_(7)TBCs are famous for their excellent CMAS *** this study,the characteristics of Fe-containing environmental sediments(CMAS-Fe)and their corrosiveness to Gd_(2)Zr_(2)O_(7)coatings were *** types of CMAS-Fe glass with different Fe contents were *** melting points were measured to be 1322–1344℃,and the high-temperature viscosity showed a decreasing trend with increasing Fe *** corrosion behavior of four types of CMAS-Fe to Gd_(2)Zr_(2)O_(7)coatings at 1350℃was *** the initial corrosion stage(0.1 h),anorthite was precipitated in CMAS-Fe with a high Ca:Si ratio,while Fe-garnet was formed in the melt with the highest Fe *** the corrosion time resulted in the formation of a reaction layer,which exhibited an interpenetrating network composed of Gd-oxyapatite,ZrO_(2),and residual *** spinel was precipitated within the reaction *** 1 h or even longer time,the reaction layers tended to be stable and compact,which had comparable hardness and fracture toughness to those of Gd_(2)Zr_(2)O_(7)*** the cyclic CMAS-Fe attack,the residual CMAS-Fe in the interpenetrating network provided a pathway for the redeposited CMAS-Fe infiltration,resulting in the continuous growth of the reaction *** a result,the Gd_(2)Zr_(2)O_(7)coatings had a large consumption in the thickness,degrading the coating ***,the Gd_(2)Zr_(2)O_(7)coatings exhibit unsatisfactory corrosion resistance to CMAS-Fe attack.

关键词： thermal barrier coatings(TBCs) Gd_(2)Zr_(2)O_(7) Fe-containing CaO-MgO-Al2O3-SiO_(2)(CMAS) corrosion resistance reaction layer

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High-throughput screening of single-atom catalysts confined in monolayer black phosphorus for efficient nitrogen reduction reaction

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Nano Research 2024年第4期17卷 2360-2367页

作者： Xiao-yan Li Manyi Duan Pengfei Ou Department of Electrical and Computer Engineering University of TorontoTorontoOntario M5S 1A4Canada School of Physics and Electronic Engineering Sichuan Normal UniversityChengdu 610101China Department of Chemistry Northwestern UniversityEvanstonIL 60208USA

The discovery of metal-nitrogen centers as the active sites for electrolysis has aroused significant interest in utilizing single-atom catalysts for nitrogen reduction reaction(NRR).Properly designed nanostructured catalysts that strongly interact with nitrogen molecules(N_(2))can promote adsorption and activation,thereby resulting in efficient catalysts with high stability,activity,and *** this study,using density functional theory calculations,we selected monolayer black phosphorus(BP)as the substrate and screened a series of single-atom transition metals confined in tri-coordinated and tetra-coordinated active centers(without and with N dopants)to electro-catalyze *** a result,we have identified two promising candidates(Hf_(1)-N_(1)P_(2)-1 and Tc_(1)-N_(4)),which exhibit not only low overpotentials of 0.56 and 0.49 V but also high thermodynamic and electrochemical stability,as well as good selectivity towards NRR over the competing hydrogen evolution *** also demonstrate the ability of Hf_(1)-N_(1)P_(2)-1 and Tc_(1)-N_(4) to activate and hydrogenate N_(2) by donating electrons and regulating charge *** study not only predicts new BP-based promising catalysts but also provides guidance for the rational design of high-performance NRR electrocatalysts under ambient conditions.

关键词： N_(2) electroreduction reaction single-atom catalysts black phosphorus density functional theory high-throughput calculations

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Model-driven path planning for robotic plasma cutting of branch pipe with single Y-groove based on pipe-rotating scheme

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Advances in Manufacturing 2024年第1期12卷 94-107页

作者： yan Liu Qiu Tang Xin-Cheng Tian School of Control Science and Engineering Shandong UniversityJinan250061People’s Republic of China Engineering Research Center of Intelligent Unmanned System Ministry of EducationJinan250061People’s Republic of China School of Mechanical and Electronic Engineering Shandong Jianzhu UniversityJinan250101People’s Republic of China

The automatic cutting of intersecting pipes is a challenging task in *** improved automation and accuracy,this paper proposes a model-driven path planning approach for the robotic plasma cutting of a branch pipe with a single ***,it summarizes the intersection forms and introduces a dual-pipe intersection *** on this model,the moving three-plane structure(a description unit of the geometric characteristics of the intersecting curve)is constructed,and a geometric model of the branch pipe with a single Y-groove is ***,a novel mathematical model for plasma radius and taper compensation is ***,the compensation model and groove model are integrated by establishing movable ***,to prevent collisions between the plasma torch and workpiece,the torch height is planned and a branch pipe-rotating scheme is *** the established models and moving frames,the planned path description of cutting robot is provided in this novel *** accuracy of the proposed method is verified by simulations and robotic cutting experiments.

关键词： Automatic groove cutting of intersecting pipes Model-driven robot path planning Plasma beam radius and taper compensation

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Integrated separation-electrochemical detection device based on wood column for online identification of enantiomer

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Nano Research 2024年第3期17卷 1893-1901页

作者： Junli Guo Yuanfei Xue Chenxi Zhao Junjian Zhao Zhida Gao Ye Mei yan-yan Song College of Sciences Northeastern UniversityShenyang 110004China State Key Laboratory of Precision Spectroscopy School of Physics and Electronic ScienceEast China Normal UniversityShanghai 200062China NYU-ECNU Center for Computational Chemistry at NYU Shanghai Shanghai 200062China Collaborative Innovation Center of Extreme Optics Shanxi UniversityTaiyuan 030006China

Chiral chemicals have attracted significant interest in the pharmaceutical industry,yet the separation methods to get pure enantiomers from racemic mixture are still *** date,the separation of enantiomers still mainly depends on chromatography using high-cost chiral stationary ***,wood channels were used as the handheld integrated device,and enantiomer separation was simultaneously detected using an electrochemical *** this method,a chiral UIO-66(L-UIO-66)modified enantiomer separation zone and carbonized wood based online detection zone are integrated along a single wood *** on the in situ separation results from the chronoamperometry data,the wood device shows excellent separation ability for a wide range of electrochemically active enantiomers,including 3,4-dihydroxyphenylalanine,amino acids,ascorbic acid,carnitine,and penicillamine with high chirality *** unbiased molecular dynamic simulations indicate that the excellent chiral recognition and separation are attributed to the different barriers from the bound states to the dissociated state of the enantiomers in the homochiral microenvironment of the *** integrated enantiomer separation-electrochemical detection device provides a novel,easy,and low-cost platform for the separation of pure enantiomer from racemic mixture.

关键词： wood column integrated separation-detection device enantioselectivity online sensing free energy barrier

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