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Tailored heterostructured ni_(3)n-niO nano-frameworks for boosting electrocatalytic oxygen evolution via surface-modulated plasma strategy

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nano Research 2024年第9期17卷 7909-7917页

作者： Bo Ouyang haonan Qin chao Sun Yilin Deng ang Li Jipeng Zhu Erjun Kan Rajdeep Singh Rawat MIIT Key Laboratory of Semiconductor Microstructure and Quantum Sensing School of ScienceNanjing University of Science&TechnologyNanjing 210094China The Laboratory of Road and Bridge Civil EngineeringSchool of ScienceNanjing University of Science&TechnologyNanjing 210094China Institute for Energy Research Jiangsu UniversityZhenjiang 212013China natural Sciences and Science Education National Institute of EducationNanyang Technological University637616Singapore

The facile reconfiguration of phases plays a pivotal role in enhancing the electrocatalytic production of h2 through heterostructure *** chemical methods have been explored extensively for this purpose,plasma-based techniques offer a promising avenue for achieving heterostructured ***,the conventional plasma approach introduces complexities,leading to a multi-step fabrication process and challenges in precisely controlling partial surface structure modulation due to the intricate interaction *** our pursuit of heterostructures with optimized oxygen evolution reaction(OER)behavior,we have designed a facile auxiliary insulator-confined plasma system to directly attain a ni_(3)n-niO heterostructure(hninO).By meticulously controlling the surface heating process during plasma processing,such approach allows for the streamlined fabrication of hninO *** resulting nano-framework exhibits outstanding catalytic performance,as evidenced by its overpotential of 320 mV at a current density of 10 mA·cm^(-2),in an alkaline *** stands in stark contrast to the performance of niO-covered ni_(3)n fabricated using the conventional plasma method(sninO).Operando plasma diagnostics,coupled with numerical simulations,further substantiates the influence of surface heating due to auxiliary insulator confinement of the substrate on typical plasma parameters and the formation of the ni_(3)n-niO nanostructure,highlighting the pivotal role of controlled surface temperature in creating a high-performance heterostructured electrocatalyst.

关键词： structural modulation auxiliary insulator-confined plasma surface heating control heterostructure electrocatalytic O2 evolution

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Direct observation of oxygen vacancy formation and migration over ceria surface by in situ environmental transmission electron microscopy

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Journal of Rare Earths 2024年第4期42卷 676-682页

作者： Dawei Pang Wei Li ningqiang Zhang hong he shengcheng Mao Yanhui chen Liwei Cao chong Li ang Li Xiaodong han Beijing Key Laboratory of Solid Microstructure and Properties Department of Materials and ManufacturingBeijing University of TechnologyBeijing 100124China Beijing Key Laboratory for Green Catalysis and Separation The Faculty of Environment and LifeBeijing University of TechnologyBeijing10124China International Joint Research Laboratory for Quantum Functional Materials of henan School of Physics and MicroelectronicsZhengzhou UniversityZhengzhou450001China

The extremely high structural tolerance of ceria to oxygen vacancies(Ov)has made it a desirable catalytic material for the hydrocarbon oxidation to chemicals and pharmaceuticals and the reduction of gaseous *** is proposed that the formation and diffusion of Ov originate from its outstanding reduction ***,the formation and diffusion process of Ov over the surface of ceria at the atomic level is still ***,the structural and valence evolution of CeO_(2)(111)surfaces in reductive,oxidative and vacuum environments from room temperature up to 700℃was studied with in situ aberration-corrected environmental transmission electron microscopy(ETEM)*** is found to form under a high vacuum at elevated temperatures;however,the surface can recover to the initial state through the adsorption of oxygen atoms in an oxygen-contained ***,in hydrogen environment,the step-CeO_(2)(111)surface is not stable at elevated temperatures;thus,the steps tend to be eliminated with increasing *** with first-principles density function calculations(DFT),it is proposed that O-terminated surfaces would develop in a hypoxic environment due to the dynamic diffusion of Ov from the outer surface to the ***,in a reductive environment,h2 facilitates the formation and diffusion of Ov while Ce-terminated surfaces *** results reveal dynamic atomic-scale interplay between the nanoceria surface and gas,thereby providing fundamental insights into the Ov-dependent reaction of nano-CeO_(2) during catalytic processes.

关键词： Ceria Direct observation In situ ETEM Oxygen vacancy Density function calculations Rareearths

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Multifunctional properties of a polar spin chain compound[n(C_(3)h_(7))_(4)][Cu(C_(8)h_(4)nO_(4))]·h_(2)O exhibiting both one-dimensional magnetism and nonlinear optical activity

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chinese chemical Letters 2024年第2期35卷 622-625页

作者： ang Li Yanhong Wang haotian Tian Alimujiang Yalikun Yves Journaux Min Luo hongcheng Lu Key Laboratory of Material chemistry for Energy Conversion and Storage School of Chemistry and Chemical EngineeringHubei Key Laboratory of Bioinorganic Chemistry & Materia MedicaHuazhong University of Science and TechnologyWuhan 430074China Key Laboratory of optoelectronic Materials chemistry and Physics Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 35002China Institut Parisien de chimie Moléculaire IPCMSorbonne UniversitéCNRSParis F-75252France

Functional materials with multiple properties are urgent to be explored to reach high requirements for applications *** this work,a new multifunctional one-dimensional(1D)chain compound[n(C_(3)h_(7))_(4)][Cu(ohpma)]·h_(2)O 1(ohpma=deprotonated n-(2-hydoxyphenyl)oxamic acid)exhibiting both 1D antiferromagnetic and nonlinear optical properties,which are both originated from the same polar[Cu(C_(8)h_(4)nO_(4))]magnetic units,has been successfully synthesized by evaporation at room ***-polydentate nature of the(ohpma)3−ligand with constrained tridentate and bidentate coordination sites conducts Cu^(2+)ions coordinating in different geometries and forms 1D chains along the c axis,which are further separated by the[n(C_(3)h_(7))_(4)]+*** the 1D magnetic chains further exhibit noncentrosymmetric polar *** optical study shows polar compound 1 exhibits a discernible second-harmonic generation(shG)efficiency and the calculation of the partial density of states indicates that the shG efficiency of 1 is mainly originated from the polar[Cu(C_(8)h_(4)nO_(4))]magnetic ***,magnetic susceptibility shows a broad maximum around 70 K with strong intrachain interaction of J/k B=−113.0 K but no long-range order is observed down to 2 K,suggesting that 1 shows a good 1D *** good 1D magnetism and shG activity suggest that 1 could be as a potential multifunctional material,particularly.

关键词： Multifunctional properties Magnetic property nonlinear optical property Evaporation One-dimensional chain

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Reconcile the contradictory wettability requirements for the reduction and oxidation half-reactions in overall CO_(2) photoreduction via alternately hydrophobic surfaces

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Journal of Energy chemistry 2024年第6期93卷 202-212,I0006页

作者： hailing huo Ting hu chengxi h.ang Fang Wu Tongyu Wang Xuan Liu Liang Zhang Qiang Ju Zhiqing Zhong hongbin Xing Erjun Kan ang Li MIIT Key Laboratory of Semiconductor Microstructure and Quantum Sensing Nanjing University of Science and TechnologyNanjing 210094JiangsuChina College of Information Science and Technology Nanjing Forestry UniversityNanjing 210037JiangsuChina

The overall photocatalytic CO_(2) reduction reaction(OPCRR)that can directly convert CO_(2) and h_(2)O into fuels represents a promising renewable energy conversion *** a typical redox reaction,the OPCRR involves two half-reactions:the CO_(2) reduction half-reaction(CRhR)and the water oxidation half-reaction(WOhR).Generally,both half-reactions can be promoted by adjusting the wettability of ***,there is a contradiction in wettability requirements for the two ***,CRhR prefers a hydrophobic surface that can accumulate more CO_(2) molecules on the active sites,ensuring the appropriate ratio of gas-phase(CO_(2))to liquid-phase(h_(2)O)***,the WOhR prefers a hydrophilic surface that can promote the departure of the gaseous product(O_(2))from the catalyst surface,preventing isolation between active sites and the reactant(h_(2)O).here,we successfully reconciled the contradictory wettability requirements for the CRhR and WOhR by creating an alternately hydrophobic *** was achieved through a selectively hydrophobic modification method and a charge-transfer-control ***,the collaboratively promoted CRhR and WOhR led to a significantly enhanced OPCRR with a solar-to-fuel conversion efficiency of 0.186%.notably,in ethanol production,the catalyst exhibited a 10.64-fold increase in generation rate(271.44μmol g^(-1)h~(-1))and a 4-fold increase in selectivity(55.77%)compared to the benchmark *** innovative approach holds great potential for application in universal overall reactions involving gas participation.

关键词： hydrophobic hydrophilic Gas transport Overall CO_(2)photoreduction Z-scheme

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high-density triple-phase contact points for enhanced photocatalytic CO_(2) reduction to methanol

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chinese chemical Letters 2024年第2期35卷 252-256页

作者： hanwen Jian Kaiming Deng Tongyu Wang chengxi h.ang Fang Wu hailing huo Bo Ouyang Xuan Liu Jingjing Ma Erjun Kan ang Li MIIT Key Laboratory of Semiconductor Microstructure and Quantum Sensing School of ScienceNanjing University of Science and TechnologyNanjing 210094China College of Information Science and Technology Nanjing Forestry UniversityNanjing 210037China State Key Laboratory of high-efficiency Utilization of Coal and Green chemical Engineering Ningxia UniversityYinchuan 750021China

The efficiency of photocatalytic CO_(2) reduction reaction(PCRR)is restricted by the low solubility and mobility of CO_(2) in water,poor CO_(2) adsorption capacity of catalyst,and competition with hydrogen evolution reaction(hER).Recently,hydrophobic modification of the catalyst surface has been proposed as a potential solution to induce the formation of triple-phase contact points(TPCPs)of CO_(2)(gas phase),h_(2) O(liquid phase),and catalysts(solid phase)near the surface of the catalyst,enabling direct delivery of highly concentrated CO_(2) molecules to the active reaction sites,resulting in higher CO_(2) and lower h+surface *** TPCPs thus act as the ideal reaction points with enhanced PCRR and suppressed ***,the initial synthesis of triple-phase photocatalysts tends to possess a lower bulk density of TPCPs due to the simple structure leading to limited active points and CO_(2) adsorption ***,based on constructing a hydrophobic hierarchical porous TiO_(2)(o-hPT)with interconnected macropores and mesopores structure,we have significantly increased the density of TPCPs in a unit volume of the *** with hydrophobic macroporous TiO_(2)(o-MacPT)or mesoporous TiO_(2)(o-MesPT),the o-hPT with increased TPCP density leads to enhanced photoactivity,enabling a high methanol production rate with 1111.5μmol g^(−1) h^(−1) from *** results emphasize the significance of high-density TPCPs design and propose a potential path for developing efficient PCRR systems.

关键词： Photocatalysis CO_(2)reduction reaction Photocatalyst Triple-phase contact points Methanol

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Molecular properties of dissolved organic matter across Earth systems: A meta-analysis

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Journal of Earth Science 2024年

作者： Lei han ang hu hellen Lucas Mzuka Xingting chen Ji shen Jianjun Wang Key Laboratory of Lake and Watershed Science for Water Security nanjing Institute of Geography and Limnology chinese Academy of Sciences School of Geography and Ocean Science nanjing University

Dissolved organic matter （DOM） represents the largest pool of reactive carbon on the Earth and plays a crucial role in various biogeochemical processes and ecosystem functions. however， it is understudied for a global understanding of DOM molecular properties such as molecular weight， stoichiometry， and oxidation state， and the linkages among them across Earth systems. here， a meta-analysis of 2，707 sites in 204 literatures was conducted by synthesizing four representative molecular properties of DOM， i.e.， mass， double bond equivalent （DBE）， modified aromaticity index (AImod)， and nominal oxidation state of carbon （nOSC）. By exploring h/C and O/C ratios， we examined the relationships among these DOM properties across waters and land systems， and their geographical patterns and environmental drivers. We found that， compared to land system， the mass， DBE， and AImodwere all significantly higher in water systems， with river sediments exhibiting the highest values. DOM oxidation state indicated by nOSC was greater on average in wastewater （nOSC = 0.226 ± 0.06） and marine water （nOSC = 0.133 ± 0.06） than in other habitats. Compared to waters， the mass in land system showed more strongly positive correlations with oxidation states such as nOSC and O/C， and the nOSC showed stronger relations to bioavailability properties such as DBE， AImod， and h/C. Among all the properties， h/C and AImodcontributed to the most variations in global DOM properties. In waters， nOSC monotonically increased towards high latitudes， while DBE and AImodshowed significant hump-shaped patterns indicating peaked unsaturation and aromaticity at mid-latitudes of approximately absolute 30°-50°. The variations in DOM properties were significantly correlated with environmental factors such as annual mean temperature and ph. Collectively， we revealed the spatial distribution and environmental drivers of DOM molecular properties across Earth ecosystems， which could shed light on our comprehensive understan

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真核生物mRnA应激状态下的帽-非依赖性翻译

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中国生物化学与分子生物学报 2024年第1期40卷 1-9页

作者：刘子昂金焰吴楠中国遗传资源保护与疾病防控教育部重点实验室(哈尔滨医科大学) 哈尔滨150081 哈尔滨医科大学医学遗传学研究室哈尔滨150081

在真核生物中,mRnA翻译过程包括起始、延伸和终止。其中,翻译的起始阶段最为重要且复杂,它决定了mRnA能否被有效翻译成蛋白质。根据翻译起始机制的不同,真核生物mRnA翻译可以分为传统的帽-依赖性翻译和替代机制帽-非依赖性翻译。当外部... 详细信息

在真核生物中,mRnA翻译过程包括起始、延伸和终止。其中,翻译的起始阶段最为重要且复杂,它决定了mRnA能否被有效翻译成蛋白质。根据翻译起始机制的不同,真核生物mRnA翻译可以分为传统的帽-依赖性翻译和替代机制帽-非依赖性翻译。当外部环境的刺激或细胞自身的改变使细胞处于应激状态时,传统的帽-依赖性翻译被抑制或下调,替代机制帽-非依赖性翻译得以启动,以保证翻译的顺利进行。真核生物在应激状态下为了维持蛋白质合成的需求,采用多种翻译起始机制来实现帽-非依赖性翻译。其中较常见的是IRES(internal ribosome entry site)、m6A修饰和CITE(cap-independent translation enhancer)所启动的翻译。这些机制允许核糖体在mRnA的特殊区域内部进行启动,而不依赖于传统的m7G帽结构。通过这些机制,真核生物可以在应激状态下仍然进行蛋白质合成,以满足细胞的需要。本文在总结传统帽-依赖性翻译研究进展基础上,着重介绍IRES、m6A和CITE所启动的帽-非依赖性翻译,为更好地探索细胞应激状态下的翻译机制提供参考,为未来的翻译研究和应用提供更多的思路。

关键词：真核生物mRnA 帽-非依赖性翻译内部核糖体进入位点 n6-甲基腺苷帽-非依赖性翻译增强子

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基于响应面法的轻质尾翼均匀挤压成形数值模拟及模具结构优化

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兵工学报 2024年第6期45卷 1824-1839页

作者：贾晶晶张治民于建民薛勇吴昂中北大学机电工程学院山西太原030051 郑州轻工业大学机电工程学院河南郑州450000 中北大学材料科学与工程学院山西太原030051

针对轻质镁合金尾翼正挤压成形金属流动不均匀和力学性能各向异性大的问题,提出一种可调控金属均匀流动的金属蓄料池模具结构。基于Deform-3D有限元模拟分析,采用Box-Behnken响应曲面法以金属蓄料池结构参数:深度h、池壁距尾翼芯部型腔... 详细信息

针对轻质镁合金尾翼正挤压成形金属流动不均匀和力学性能各向异性大的问题,提出一种可调控金属均匀流动的金属蓄料池模具结构。基于Deform-3D有限元模拟分析,采用Box-Behnken响应曲面法以金属蓄料池结构参数:深度h、池壁距尾翼芯部型腔长度D 1、池壁距翼片型腔长度D 2和池壁与翼片型腔之间夹角α为变量,建立出模口金属流速均方差和成形载荷与金属蓄料池结构参数之间的响应关系。响应曲面分析结果表明:最佳的金属蓄料池结构参数为h=7 mm,D 1=13 mm,D 2=6 mm,α=11°。采用优化后的模具结构参数进行模拟验证和物理试验,金属流动不均匀和力学性能各向异性均得到改善,并成功试制出形状尺寸和力学性能指标满足要求的尾翼形零件。

关键词：尾翼构件均匀流动有限元模拟模具优化 Box-Behnken响应曲面

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基于多位移光谱遥感图像的空间引力模型亚像元定位

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哈尔滨工程大学学报 2024年第6期45卷 1179-1186页

作者：王鹏严昂陈永康赵春雷石立新中国测绘科学研究院测绘科学与地球空间信息技术自然资源部重点实验室北京100039 湖南省国土资源规划院自然资源部南方丘陵区自然资源监测监管重点实验室湖南长沙410114 南京航空航天大学电子信息工程学院江苏南京211106 河北省气象科学研究所河北省气象与生态环境重点实验室河北石家庄050022

目前基于多位移光谱遥感图像的亚像元定位方法通常很少考虑点扩散函数效应影响,本文提出了一种基于多位移光谱遥感图像的空间引力模型亚像元定位方法。为了生成粗糙丰度图像,首先对多个多位移光谱遥感图像进行解混;在点扩散函数效应被... 详细信息

目前基于多位移光谱遥感图像的亚像元定位方法通常很少考虑点扩散函数效应影响,本文提出了一种基于多位移光谱遥感图像的空间引力模型亚像元定位方法。为了生成粗糙丰度图像,首先对多个多位移光谱遥感图像进行解混;在点扩散函数效应被考虑的前提下,对粗糙丰度图像实施面积到点的克里插值处理,然后通过理想方波滤波进行滤波,最终获得改进后的粗糙丰度图像;利用空间引力模型对改进后的粗糙丰度图像进行上采样,从而得到上采样丰度图像,再对上采样丰度图像执行整合处理,以生成精细丰度图像;在完成上述所有图像处理步骤后,最终通过应用类别分配方法,将类别标签分发给各个亚像元,以此获得精确的定位结果。在2组实验数据集上的实验结果表明:本文提出的方法比现有的亚像元定位方法获得了更好的定位效果。

关键词：遥感图像高光谱图像亚像元定位点扩散函数空间引力模型多位移光谱遥感图像

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Fe-金属有机框架玻璃的形成过程与机理

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硅酸盐学报 2024年第8期52卷 2553-2558页

作者：刘鑫宇郭超慧陶海征乔昂武汉理工大学硅酸盐建筑材料国家重点实验室武汉430070 中山市武汉理工大学先进工程技术研究院广东中山528400

不同的中心金属离子能够赋予金属有机框架材料(MOFs)不同的性能,众多Fe基MOF材料具有优异的电、磁性能。但由于Fe元素存在变价,且Fe—n配位键难以形成,可熔融成玻Fe-MOF材料鲜有报道。使用无溶剂法成功制备Fe_(3)(C_(3)h_(2)n_(2))_6(C_... 详细信息

不同的中心金属离子能够赋予金属有机框架材料(MOFs)不同的性能,众多Fe基MOF材料具有优异的电、磁性能。但由于Fe元素存在变价,且Fe—n配位键难以形成,可熔融成玻Fe-MOF材料鲜有报道。使用无溶剂法成功制备Fe_(3)(C_(3)h_(2)n_(2))_6(C_(3)h_(4)n_(2))_(2)晶体,命名为FCIR,即Fe-MOF晶体,并且利用熔融淬冷法制成了Fe-MOF玻璃,并探究该Fe-MOF晶体在加热过程中的形态和结构演变,以及其玻璃态形成的机理。结果表明:相较于以Zn为中心离子的可熔融MOF材料,Fe离子对晶体加热过程中的熔融过程和结构演变会产生较大影响;FCIR晶体熔融淬冷后发生近程序结构变化,即由晶态时Fe离子与咪唑的6配位八面体脱去2个单配位咪唑转变为玻璃态的4配位四面体。

关键词：金属有机框架玻璃形成熔融结构变化

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