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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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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 O_(2) evolution

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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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microRNA-2184 orchestrates Mauthner-cell axon regeneration in zebrafish via syt3 modulation

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Journal of Genetics and Genomics 2024年第9期51卷 911-921页

作者： Xinghan chen Yueru Shen Zheng Song Xinliang Wang huaitong Yao Yuan Cai Zi-ang Zhao Bing hu hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of ChinaHefeiAnhui 230026China The First Affiliated hospital of USTC Division of Life Sciences and MedicineUniversity of Science and Technology of ChinaHefeiAnhui 230026China Center for Advanced Interdisciplinary Science and Biomedicine of IhM Division of Life Sciences and MedicineUniversity of Science and Technology of ChinaHefeiAnhui 230026China

MicroRNAs(miRNAs)play a significant role in axon regeneration following spinal cord ***,the functions of numerous miRNAs in axon regeneration within the central nervous system(CNS)remain largely ***,we elucidate the positive role of microRNA-2184(miR-2184)in axon regeneration within zebrafish Mauthner cells(M-cells).The upregulation of miR-2184 in a single M-cell can facilitate axon regeneration,while the specific sponge-induced silencing of miR-2184 leads to impeded *** show that syt3,a downstream target of miR-2184,negatively regulates axon regeneration,and the regeneration suppression modulated by syt3 depends on its binding to Ca2+.Furthermore,pharmacological stimulation of the cAMP/PKA pathway suggests that changes in the readily releasable pool may affect axon *** data indicate that miR-2184 promotes axon regeneration of M-cells within the CNS by modulating the downstream target syt3,providing valuable insights into potential therapeutic strategies.

关键词： Axon regeneration Axon ablation miR-2184 syt3 Readily releasable pool

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A new class of crystalline X-ray induced photochromic materials assembled from anion-directed folding of a flexible cation

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chinese chemical Letters 2024年第8期35卷 554-557页

作者： hong-Jin Liao Zhu Zhuo Qing Li Yoshihito Shiota Jonathan P.hill Katsuhiko Ariga Zi-Xiu Lu Lu-Yao Liu Zi-ang Nan wei Wang You-Gui h.ang CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key Laboratory of NanomaterialsFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China College of chemistry and Materials Science Fujian Normal UniversityFuzhou 350007China Xiamen Key Laboratory of Rare Earth Photoelectric Functional Materials Xiamen Institute of Rare Earth MaterialsHaixi InstitutesChinese Academy of SciencesXiamen 361021China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of china Fuzhou 350108China Institute for Materials chemistry and Engineering Kyushu UniversityFukuoka 819-0395Japan World Premier International(WPI)Center for Materials Nanoarchitectonics(MANA) National Institute for Materials Science(NIMS)Ibaraki 305-0044Japan

Electron-deficient viologens are widely used as ligands or structure-directing agents(SDAs)to synthesize crystalline X-ray induced photochromic ***,a new rational strategy of anion-directed fold-ing a flexible cation(h_(2)imb)^(2+)((h_(2)imb)^(2+)=di-protonated 2,3-bis(imidazolin-2-yl)-2,3-dimethylbutane)has been ***-donating Cl−and(ZnCl4)2−are used to direct folding a flexible electron-deficient(h_(2)imb)^(2+)*** complexes(h_(2)imb)(NO_(3))2(1),(h_(2)imb)Cl2·h_(2)O(2),and(h_(2)imb)ZnCl4(3)have been synthesized in which(h_(2)imb)^(2+)crystallize in an anti-conformation,88.8°-gauche,and 51.8°-gauche,*** contrary to X-ray silent complex 1,X-ray induced photochromism has been achieved in both complex 2 and *** intermolecular charge-transfer mechanism has been elucidated and the anion directed folding of(h_(2)imb)^(2+)has been validated to be critical to yield colored long-lived charge-separated states.

关键词： Supramolecular Photochromic X-ray induced Anion-directed folding Electron-deficient viologens

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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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Engineering hydrophobic protective layers on zinc anodes for enhanced performance in aqueous zinc-ion batteries

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Journal of Energy chemistry 2024年第10期97卷 1-11页

作者： Taofeng Li Suxia Yan hongyu Dong Yang Zheng Kun Ming Ying chen haitao Li Guochun Li Zhixia he weimin Li Quan Wang Xiaohui Song Junfeng Liu Edison huixiang ang Yong Wang Institute for Energy Research Jiangsu University School of Mechanical Engineering Jiangsu University Shenzhen College of Advanced Technology University of Chinese Academy of Sciences Shandong Zhongke Advanced Technology Co. Ltd School of Materials Science and Engineering Hefei University of Technology Natural Sciences and Science Education National Institute of Education Nanyang Technological University

Aqueous zinc-ion batteries possess substantial potential for energy storage applications;however,they are hampered by challenges such as dendrite formation and uncontrolled side reactions occurring at the zinc *** our investigation,we sought to mitigate these issues through the utilization of in situ zinc complex formation reactions to engineer hydrophobic protective layers on the zinc anode *** robust interfacial layers serve as effective barriers,isolating the zinc anode from the electrolyte and active water molecules and thereby preventing hydrogen evolution and the generation of undesirable ***,the presence of numerous zincophilic sites within these protective layers facilitates uniform zinc deposition while concurrently inhibiting dendrite *** comprehensive evaluation of functional anodes featuring diverse functional groups and alkyl chain lengths,we meticulously scrutinized the underlying mechanisms influencing performance *** analysis involved precise modulation of interfacial hydrophobicity,rapid Zn2+ion transport,and ordered deposition of Zn2+***,the optimized anode,fabricated with octadecylphosphate（OPA）,demonstrated exceptional performance *** Zn//Zn symmetric cell exhibited remarkable longevity,exceeding 4000 h under a current density of 2 mA cm-2and a capacity density of 2 mA h cm-2,Furthermore,when integrated with a VOh cathode,the complete cell exhibited superior capacity retention compared to anodes modified with alternative organic molecules.

关键词： Aqueous zinc-ion batteries Dendrite growth inhibition Energy storage hydrophobic protective layers Zinc anode stability

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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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