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Journal of Materiomics 2024年第3期10卷 601-614页

作者： huihui Gao Penghui zhang hongjie Qin Shouwei zhang Jinghua Guo School of Physics and Technology University of JinanJinan250022China

The purposeful construction of dual Z-scheme system to the formation of intimate interface contact and multi-channel charge flow through the system remains a huge ***,a tandem 2D/0D/2D g-C_(3)N_(4)nanosheets/FeOOh quantum dots/ZnIn_(2)S_(4)nanosheets(CNFeZn)dual Z-scheme system(DZSS)has been successfully constructed using electrostatic self-assembly *** to the band structure and elaborate morphology of 2D g-C_(3)N_(4),0D FeOOh and 2D ZnIn_(2)S_(4)in unique designed DZSS,plenty of spatial charge transfer channels are formed between the g-C_(3)N_(4)/FeOOh and FeOOh/ZnIn_(2)S_(4)interfaces,which greatly accelerate the charge separation and *** bifunctional catalysts,CNFeZn DZSS achieves the highest h_(2)evolution rate of~436.6 mmol/h with a great promotion of~10.6 folds and~6.9 folds compared to pristine g-C_(3)N_(4)and ZnIn_(2)S_(4),***,the h_(2)O_(2)production rate reached~301.19 mmol/L after 60 min irradiation,up to~5.1 times and~2.3 times that of pristine g-C_(3)N_(4)and ZnIn_(2)S_(4).Experiment and DFT calculation further confirmed that the stable double built-in electronic field can be formed owing to the electron configuration between double interfaces,and reveal that the ample atomic-level charge transfer channels were established in the strong interaction connected double interfaces,which can act as the charge migration pathway promote the separation of photogenerated charges.

关键词： Dual Z-scheme 2D/0D/2D tandem system h_(2)and h_(2)O_(2)production Multi-channel charge flow Intimate interface contact

The degradation pathways of contaminants by reactive oxygen species generated in the Fenton/Fenton-like systems

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Chinese Chemical Letters 2024年第10期35卷 158-169页

作者： Chi zhang Ning Ding yuwei Pan Lichun Fu ying zhang Tianjin Key Laboratory of Environmental Technology for Complex Trans-Media Pollution College of Environmental Science and EngineeringNankai UniversityTianjin300350China Key Laboratory of Cleaner Production and Integrated Resource Utilization of China National Light Industry Beijing Technology and Business University.Beijing100048China College of Biology and the Environment Nanjing Forestry UniversityNanjing 210037China School of Iron and Steel Soochow UniversitySuzhou 205000China Key Laboratory of Pollution Process and Environmental Criteria Ministry of EducationCollege of Environmental Science and EngineeringNankai UniversityTianjin300350China

Reactive oxygen species(ROSs)in Fenton process are of great importance in treating contaminants in *** is crucial to understand their chemical properties,formation,and reaction mechanisms with *** review summarizes the reactive oxygen species in Fenton process,including hydroxyl radical(·Oh),superoxide radical(O_(2)·-),singlet oxygen(1O_(2)),hydroperoxyl radical(hO_(2)·),and high-valent iron.·Oh shows a trend to react with chemistry groups with abundant electrons through h-atom abstraction,radical adduct formation and single electron *** transfer is discovered to be an important pathway when1O_(2)degrades organic ***-opening andβ-scission are proposed to be the possible ways of1O_(2)to certain *** abstraction,nucleophilic substitution,and single electron transfer are proposed to explain how O_(2)·-degrade *** the conjugated acid of O_(2)·-,radical adduct formation and h-atom abstraction are reported for the reaction mechanisms of hydroperoxyl ***-valent iron in Fenton,namely Fe(IV),reacts with certain pollutants via single-or two-electron *** review is important for researchers to understand the ROSs produced in Fenton and how th.y.react with pollutants.

关键词： Fenton hydroxyl radical Superoxide radical Singlet oxygen hydroperoxyl radical high-valent iron

Evolution hydrothermal aging resistance mechanism study of zirconium and manganese doped CeO_(2)catalysts in soot catalytic combustion based on low Miller indices crystal surface effect

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Journal of Rare Earths 2024年第7期42卷 1272-1281,I0003页

作者： Zonglin Li Pan Wang hong Ni Chengcheng Ao Lidong zhang hefeng zhang Kai Li School of Automotive and Traffic Engineering Jiangsu UniversityZhenjiang212013China State Environmental Protection Key Laboratory of Vehicle Emission Control and Simulation Chinese Research Academy of Environmental ScienceBeijing100012China National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei230026China

The thermogravimetric analysis(TGA)experiments were carried out to reveal the mechanism of Zr and Mn doping on catalytic activity of CeO_(2)catalyst both fresh and after hydrothermal aging,and the lattice morphology and valence changes were characterized by means of Brunauer-Emmett-Teller(BET)method,X-ray diffraction(XRD),X-ray photoelectron spectroscopy(XPS),and h_(2)-temperature programmed reduction(h_(2)-TPR).Density functional theory(DFT)and molecular thermodynamics calculations were applied to investigate the change in catalytic activity,crystal surface energy and crystal morphology caused by hydrothermal *** maximum reaction rate temperature of fresh Mn/CeO_(2)(389℃)is similar to that of CeO_(2)(371℃)and lower than that of Zr/CeO_(2)(447℃),but the catalytic performance of CeO_(2)decreases more severely after hydrothermal *** catalyst crystals show different degrees of crystal surface migration after hydrothermal aging,which leads to the reduction of Ce^(3+)/Ce^(4+) ratio and the active sites *** calculations indicate that the doping of Zr and Mn reduces the surface energy of the low Miller indices surface and increases the oxygen vacancy formation energy,leading to better thermal stability and lower catalytic *** Zr and Mn doping also changes the adsorption energy and Gibbs free energy of h_(2)O,which dominates the migration of(111)to(110)and(100)in the vapor *** crystal surface migration mechanism of CeO_(2)catalysts doped with Zr and Mn induced by h_(2)O molecules at high temperature obtained in this study can provide a valuable addition to the regeneration of CeO_(2)catalysts in the after-treatment systems of diesel engines.

关键词： Soot CeO_(2)-based catalyst CDPF Rare earth metal oxides DFT calculations

hydrogen evolution reaction activity enhancement from active site turnover mechanism

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Journal of Energy Chemistry 2024年第5期92卷 629-638页

作者： Jiacheng Wang Tongqing yang Xiyue Li haiqin zhang yixue zhang yan he hongyao Xue College of Electromechanical Engineering Qingdao University of Science and TechnologyQingdao 266061ShandongChina

Although heteroatom doping is an effective way to improve the catalytic activity of transition metal phosphides(TMPs),the mechanism of activity enhancement needs to be further *** this end,we synthesized a Co-doped Ni_(2)P catalyst as a research model and found that the introduction of heterogeneous Co reconstructed the charge distribution around the P site,which effectively enhanced the hydrogen evolution reaction(hER)activity of the pure Ni_(2)*** on in-situ Raman real-time monitoring technology,we monitored for the first time that Co doping triggered a switch of the active site(from the original Co-active site to the P-active site),which promoted the adsorption of h_(2)O to enhance the hER *** density functional theory(DFT)calculations indicated that the P site of Co-Ni_(2)P expressed the highest activity and the Ni site of pure Ni_(2)P expressed the highest activity,which further confirms the in-situ Raman monitoring *** active site turnover mechanism discovered in this study will undoubtedly provide more rational and targeted ideas for future catalyst design.

关键词： In-situ Raman observation heteroatom doping Activesites turnover hydrogen production

Unlock the full potential of carbon cloth-based scaffolds towards magnesium metal storage via regulation on magnesiophilicity and surface geometric structure

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Journal of Energy Chemistry 2024年第3期90卷 423-434,I0010页

作者： Jing Liu Min Wang Zhonghua zhang Jinlei zhang yitao he Zhenfang Zhou Guicun Li College of Materials Science and Engineering Qingdao University of Science and TechnologyQingdao 266042ShandongChina Department of Pharmacy Jining Medical UniversityRizhao 276826ShandongChina Department of Energy and Power Engineering School of Energy and EnvironmentAnhui University of TechnologyMa’anshan 243000AnhuiChina

The development of rechargeable magnesium(Mg) batteries is of practical significance to upgrade the electric energy storage devices due to exceptional capacity and abundant resources of Mg-metal ***,the reversible Mg electrochemistry suffers from unsatisfied rate capability and lifespan,mainly caused by non-uniform distribution of *** this work,a fresh design concept of threedimensional carbon cloths scaffolds is proposed to overcome the uncontrollable Mg growth via homogenizing electric field and improving magnesiophilicity.A microscopic smooth and nitrogen-containing defective carbonaceous layer is constructed through a facile pyrolysis of ZIF8 on carbon *** revealed by finite element simulation and DFT calculation results,the smooth surface endows with uniform electric field distribution and simultaneously the nitrogen-doping species enable good magnesiophilicity of *** fine and uniform Mg nucleus as well as the inner electrodeposit behavior are also *** a result,an exceptional cycle life of 500 cycles at 4.0 mA cm^(-2) and 4.0 mA h cm^(-2) is firstly realized to our best ***,the functional scaffolds can be cycled for over 2200 h at 2.0 mA cm^(-2) under a normalized capacity of 5.0 mA h cm^(-2),far exceeding previous *** work offers an effective approach to enable the full potential of carbon cloths-based scaffolds towards metal storage for next generation battery applications.

关键词： Magnesium metal anodes Electrodeposition heterogeneous nucleation

12.6μm-Thick Asymmetric Composite Electrolyte with Superior Interfacial Stability for Solid-State Lithium-Metal Batteries

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Nano-Micro Letters 2024年第9期16卷 397-409页

作者： Zheng zhang Jingren Gou Kaixuan Cui Xin zhang yujian yao Suqing Wang haihui Wang Beijing Key Laboratory for Membrane Materials and Engineering Department of Chemical EngineeringTsinghua UniversityBeijing 100084People’s Republic of China School of Chemistry and Chemical Engineering South China University of TechnologyGuangzhou 510000People’s Republic of China

Solid-state lithium metal batteries(SSLMBs)show great promise in terms of high-energy-density and high-safety ***,there is an urgent need to address the compatibility of electrolytes with high-voltage cathodes/Li anodes,and to minimize the electrolyte thickness to achieve highenergy-density of ***,we develop an ultrathin(12.6μm)asymmetric composite solid-state electrolyte with ultralight areal density(1.69 mg cm^(−2))for *** electrolyte combining a garnet(LLZO)layer and a metal organic framework(MOF)layer,which are fabricated on both sides of the polyethylene(PE)separator separately by tape *** PE separator endows the electrolyte with flexibility and excellent mechanical *** LLZO layer on the cathode side ensures high chemical stability at high *** MOF layer on the anode side achieves a stable electric field and uniform Li flux,thus promoting uniform Li^(+)*** to the well-designed structure,the Li symmetric battery exhibits an ultralong cycle life(5000 h),and high-voltage SSLMBs achieve stable cycle *** assembled pouch cells provided a gravimetric/volume energy density of 344.0 Wh kg^(−1)/773.1 Wh L^(−1).This simple operation allows for large-scale preparation,and the design concept of ultrathin asymmetric structure also reveals the future development direction of SSLMBs.

关键词： Solid-state lithium metal batteries Composite solid-state electrolyte Ultrathin asymmetric structure Pouch cells

Effect of Bogie Cavity End Wall Inclination on Flow Field and Aerodynamic Noise in the Bogie Region of high-Speed Trains

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Computer Modeling in Engineering & Sciences 2024年第5期139卷 2175-2195页

作者： Jiawei Shi Jiye zhang State Key Laboratory of Rail Transit Vehicle System Southwest Jiaotong UniversityChengdu610031China

Combining the detached eddy simulation(DES)method and Ffowcs Williams-hawkings(FW-h)equation,the effect of bogie cavity end wall inclination on the flow field and aerodynamic noise in the bogie region is numerically ***,the simulation is conducted based on a simplified cavity-bogie model,including five cases with different inclination angles of the front and rear walls of the *** comparing and analyzing the flow field and acoustic results of the five cases,the influence of the regularity and mechanism of the bogie cavity end wall inclination on the flow field and the aerodynamic noise of the bogie region are ***,the noise reduction strategy determined by the results of the simplified cavity-bogie model is applied to a three-car marshaling train model to verify its effectiveness when applied to the real *** results reveal that the forward inclination of the cavity front wall enlarges the influence area of shear vortex structures formed at the leading edge of the cavity and intensifies the interaction between the vortex structures and the front wheelset,frontmotor,and front gearbox,resulting in the increase of the aerodynamic noise generated by the bogie *** backward inclination of the cavity rear wall is conducive to guiding the vortex structures flow out of the cavity and weakening the interaction between the shear vortex structures and the cavity rear wall,leading to the reduction of the aerodynamic noise generated by the bogie *** the rear end wall of the foremost bogie cavity of the head car is a feasible aerodynamic noise reduction measure for high-speed trains.

关键词： Bogie cavity flow aerodynamic noise end wall inclination

西太平洋麦哲伦海山群hemler、Vlinder和Il’ichev海山熔岩的成因及其形成的深部动力学机制

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中国科学：地球科学 2024年第6期54卷 1883-1900页

作者：位荀张艳石学法张辉自然资源部第一海洋研究所海洋地质与成矿作用重点实验室青岛266061 青岛海洋科技中心海洋地质过程与环境功能实验室青岛266237 山东省深海矿产资源开发重点实验室(筹) 青岛266061

经典的“地幔柱假说”能够很好解释年龄随空间位置线性变化的大洋板内火山链的成因.而位于西太平洋的众多海山群,空间分布广、年龄-位置关系杂乱,很难用经典的“地幔柱假说”来解释,其成因存在争议.本研究选择西太平洋麦哲伦海山群hemle... 详细信息

经典的“地幔柱假说”能够很好解释年龄随空间位置线性变化的大洋板内火山链的成因.而位于西太平洋的众多海山群,空间分布广、年龄-位置关系杂乱,很难用经典的“地幔柱假说”来解释,其成因存在争议.本研究选择西太平洋麦哲伦海山群hemler、Vlinder和Il’ichev海山熔岩,对其进行40Ar-39Ar年代学、主量和微量元素以及Sr-Nd-Pb-hf同位素分析,来揭示其岩石成因和形成的深部动力学机制. hemler、Vlinder和Il’ichev海山熔岩属于碱性玄武岩、碧玄岩/霞石岩和粗面岩, MgO>8wt.%的熔岩具有较高的CaO、FeOT和TiO2含量,是碳酸盐化榴辉岩熔融的熔体与橄榄岩反应的产物.这些熔岩具有较高的Zr/hf比值(40.6~45.2)和Zr-hf负异常,指示它们的地幔源区存在碳酸盐组分. hemler、Vlinder和Il’ichev海山熔岩富集不相容元素,其Sr-Nd-Pb-hf同位素显示EM1(1型富集地幔)特征,与Rarotonga和Samoa热点相似.虽然产出于同一个海山, Il’ichev碱性玄武岩与Il’ichev碧玄岩的同位素组成明显不同:前者具有更为亏损的Sr-Nd-hf同位素特征.结合板块构造恢复结果, hemler(100.1Ma)、Vlinder造盾前(100.2Ma)和造盾期后((87.5±0.4)Ma)以及Il’ichev((56.4±1.2)Ma)海山熔岩的形成时间明显偏离了南太平洋Macdonald、Arago、Rarotonga和Samoa热点的运移轨迹,因此它们并非来源于深部地幔柱的直接熔融,更可能是浅部过程的产物.麦哲伦海山群所在的大洋板块的一个典型特征是:岩石圈断裂带在该区域广泛分布.我们提出,在中白垩世当麦哲伦海山群所在的太平洋板块经过Rarotonga地幔柱上方时, Rarotonga地幔柱直接熔融形成Vlinder(造盾期)、Pako和Ioah海山.随着地幔对流分散在周围软流圈中的Rarotonga和Samoa地幔柱物质,在岩石圈裂隙处发生减压熔融,形成hemler和Vlinder造盾前和造盾期后熔岩;Il’ichev海山碱性玄武岩和碧玄岩是岩石圈裂隙诱发的软流圈中不均一富集组分熔融的产物.这种不均一组分最可能是滞留在软流圈中的不同地幔柱的物质,也有可能是残留在软流圈中的再循环的地球表层物质.

关键词：地幔柱麦哲伦海山链碳酸盐化地幔热点岩石圈伸展

Minimizing the ratio of ionizable lipid in lipid nanoparticles for in vivo base editing

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National Science Review 2024年第6期11卷 285-293页

作者： Qiubing Chen Xuebin Wang yizhou zhang Ming Tian Junyi Duan ying zhang hao yin Departments of Urology and Laboratory Medicine Frontier Science Center for Immunology and Metabolism Medical Research InstituteZhongnan Hospital of Wuhan UniversityWuhan University State Key Laboratory of Virology Tai Kang Center for Life and Medical Sciences Tai Kang Medical SchoolWuhan University Department of Rheumatology and Immunology Zhongnan Hospital of Wuhan UniversityWuhan University Wuhan Research Center for Infectious Diseases and Cancer Chinese Academy of Medical Sciences RNA Institute Wuhan University

Lipid nanoparticles(LNPs) have gained clinical approval as carriers for both siRNA and mRNA. Among the crucial components of LNPs, ionizable lipids play a pivotal role in determining the efficiency of RNA delivery. In this study, we synthesized a series of ionizable lipids, denoted as hTO, with a higher count of hydroxyl groups compared to SM-102. Remarkably, LNPs based on hTO12 lipid demonstrated comparable mRNA delivery efficiency and biosafety to those based on SM-102. however, the former reduced the ratio of ionizable lipid/total lipids to mRNA in LNPs by 2.5 times compared to SM-102. The hTO12 LNP efficiently encapsulated adenine base editor mRNA and sgRNA targeting Pcsk9, leading to substantial gene editing within the liver of mice and effective reduction of the target protein. Our study underscores that ionizable lipids with multiple hydroxyl groups may facilitate an improved lipid-to-mRNA ratio to minimize the dosage of ionizable lipids for in vivo delivery.

关键词： ionizable lipid lipid nanoparticle mRNA delivery base editor delivery Pcsk9

Optimizing Electrocatalytic hydrogen Evolution Stability via Minimal Bubble Adhesion at Electrodeposited Crack-Structured NiPx Catalysts

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Energy & Environmental Materials 2024年第5期7卷 248-258页

作者： Qian Sun Xiaoyu hao Dina zhang Tianyi zhang yuanfang Zhao Xiaolei huang Xuqing Liu State Key Laboratory of Solidification Processing Center of Advanced Lubrication and Seal Materials Northwestern Polytechnical University College of Art and Design Shenzhen University Institute of Material and Chemistry Ganjiang Innovation Academy Chinese Academy of Sciences Shandong Laboratory of yantai Advanced Materials and Green Manufacture

In response to the ongoing energy crisis, advancing the field of electrocatalytic water splitting is of utmost significance, necessitating the urgent development of high-performance, cost-effective, and durable hydrogen evolution reaction catalysts. But the generated gas bubble adherence to the electrode surface and sluggish separation contribute to significant energy loss, primarily due to the insufficient exposure of active sites, thus substantially hindering electrochemical performance. here, we successfully developed a superaerophobic catalytic electrode by loading phosphorus-doped nickel metal （NiPx） onto various conductive substrates via an electrodeposition method. The electrode exhibits a unique surface structure, characterized by prominent surface fissures, which not only exposes additional active sites but also endows the electrode with superaerophobic properties. The NiPx/Ti electrode demonstrates superior electrocatalytic activity for hydrogen evolution reaction, significantly outperforming a platinum plate, displaying an overpotential of mere 216 mV to achieve a current density of-500 mA cm-2in 1 M KOh. Furthermore,the NiPx/Ti electrode manifests outstanding durability and robustness during continuous electrolysis, maintaining stability at a current density of-10 mA cm-2over a duration of 2000 h. Owing to the straightforward and scalable preparation methods, this high.y.efficient and stable NiPx/Ti electrocatalyst offers a novel strategy for the development of industrial water electrolysis.

关键词： electrocatalyst gas bubble adhesion hydrogen evolution reaction long-term durability superaerophobic surface