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Boosting hydrocarbon conversion via Cu-doping induced oxygen vacancies on CeO2 in CO2 electroreduction

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Journal of Energy Chemistry 2025年第1期100卷 66-76页

作者： Lei Xue Tong Shi Chenhui Han Heng Zhang Fenrong Liu Haorun Li Yan Wang Xiaojun Gu Shanghong Zeng Inner Mongolia Key Laboratory of Chemistry and Physics of rare earth Materials School of Chemistry and Chemical Engineering Inner Mongolia University State Key Laboratory of Coal Conversion Institute of Coal Chemistry Chinese Academy of Sciences Institute of Catalysis Department of Chemistry Zhejiang University National Key Laboratory of Baiyunobo rare earth Resource research and Comprehensive Utilization Baotou Research Institute of Rare Earths

Conversion of CO2back to hydrocarbons is the most direct way of closing the“carbon cycle”,and its significance is further enlarged if this process is driven by renewable energies such as ***,precisely controlling the product selectivity towards hydrocarbons against the competitive hydrogen evolution remains challenging,especially for Cu-based ***,we report a novel defect engineering strategy,by which Cu-doping-induced oxygen vacancies on CeO2nanorods were effectively created,with adjustable vacancy/Cu *** resulting optimum catalyst shows up to 79% catalytic current density to hydrocarbons （excluding CO）,with 49% faradaic efficiency to *** and density functional theory unveil that the ratio between oxygen vacancy and Cu affects significantly the formation of*CHO and activation of H2O,which leads to the following deep hydrogenation to *** findings may spur new insights for designing and developing more controllable chemical process relevant to CO2utilization.

关键词： Nanorods

Gradient maturation experiment on hairs implies taphonomic changes in fossil hairs

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Science China earth Sciences 2025年第1期68卷 62-73页

作者： Xin LI Yibo ZHOU Tao ZHAO Xingjian HE Yanhong PAN State Key Laboratory for Mineral Deposits research Center for Critical Earth Material Cycling Centre for Research and Education on Biological Evolution and Environment and Frontiers Science School of Earth Sciences and Engineering Nanjing University Institute of Palaeontology Yunnan Key Laboratory of Earth System Science Yunnan Key Laboratory for PalaeobiologyYunnan University

Mammalian hair, as a key feature related to endothermy, physical protection, and camouflage, has a long geohistorical record that dates back even to the Mesozoic. However, the limited information on the taphonomy of hair hinders the understanding of its evolutionary significance in deep time. To address this, we conducted taphonomic experiments to simulate the transformation process of black hair. The changes in the morphological structure, microscopic characteristics, and chemical composition of hair during the simulated fossilization process were documented by scanning electron microscopy, Fourier transform infrared(FTIR) spectroscopy, and Raman spectroscopy. Our results revealed that damage to the morphology of hair began at a mild temperature(150–175°C), and hair transformed into a fluid-like mass at a relatively high temperature(200°C). In addition, the morphological structure of melanosomes had relatively greater preservation potential than keratins did, and the microscopic features of melanosomes were persistently stable. The Raman and FTIR spectra indicated that the characteristic melanin and keratin peaks changed as the temperature increased. Although the chemical signals were not lost completely, the variations in the characteristic amide bands in the FTIR spectra indicate that the keratins severely degraded at high temperatures(>200°C), whereas the characteristic melanin bands in the Raman spectra suggested that melanin signals were still recognizable, even at high temperatures(>200°C). These results were confirmed by principal component analysis(PCA) and principal component analysis linear discriminant analysis(PCA–LDA). In addition, the Raman signals of all the samples in the simulated experiments were distinguished from the signals of common geological carbonaceous materials(humic acid), which suggested that Raman spectroscopy can be used to detect melanin in fossils.

关键词： Mammalian hair Melanin Keratin Fossilization Experimental taphonomy

Deciphering Water Oxidation Catalysts:The Dominant Role of Surface Chemistry over Reconstruction Degree in Activity Promotion

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Nano-Micro Letters 2025年第3期17卷 340-354页

作者： Li An Jianyi Li Yuanmiao Sun Jiamin Zhu Justin Zhu Yeow Seow Hong Zhang Nan Zhang Pinxian Xi * Zhichuan JXu Chun‑Hua Yan State Key Laboratory of Applied Organic Chemistry Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu ProvinceFrontiers Science Center for Rare IsotopesCollege of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou 730000People’s Republic of China School of Materials Science and engineering Nanyang Technological UniversitySingapore 639798Singapore Faculty of Materials Science and Energy engineering Institute of Technology for Carbon NeutralityShenzhen Institute of Advanced TechnologyChinese Academy of SciencesShenzhen 518055People’s Republic of China Key Laboratory of Electromagnetic Materials and Devices National Center for International Research On Photoelectric and Energy MaterialsSchool of Materials and EnergyElectron Microscopy CenterYunnan UniversityKunming 650091People’s Republic of China State Key Laboratory of Baiyunobo rare earth Resource researches and Comprehensive Utilization Baotou Research Institute of Rare EarthsBaotou 014030People’s Republic of China Beijing National Laboratory for Molecular Sciences State Key Laboratory of Rare Earth Materials Chemistry and ApplicationsPKU‑HKU Joint Laboratory in Rare Earth Materials and Bioinorganic ChemistryPeking UniversityBeijing 100871People’s Republic of China

Water splitting hinges crucially on the availability of electrocatalysts for the oxygen evolution *** surface reconstruction has been widely observed in perovskite catalysts,and the reconstruction degree has been often correlated with the activity ***,a systematic study on the roles of Fe substitution in activation of perovskite LaNiO_(3)is *** substituting Fe content influences both current change tendency and surface reconstruction ***_(0.9)Fe_(0.1)O_(3)is found exhibiting a volcano-peak intrinsic activity in both pristine and reconstructed among all substituted perovskites in the LaNi_(1-x)Fe_(x)O_(3)(x=0.00,0.10,0.25,0.50,0.75,1.00)*** reconstructed LaNi_(0.9)Fe_(0.1)O_(3)shows a higher intrinsic activity than most reported NiFe-based ***,density functional theory calculations reveal that Fe substitution can lower the O 2p level,which thus stabilize lattice oxygen in LaNi0.9Fe0.1O3 and ensure its long-term ***,it is vital interesting that activity of the reconstructed catalysts relied more on the surface chemistry rather than the reconstruction *** effect of Fe on the degree of surface reconstruction of the perovskite is decoupled from that on its activity enhancement after surface *** finding showcases the importance to customize the surface chemistry of reconstructed catalysts for water oxidation.

关键词： Oxygen evolution reaction Perovskite oxides Doping Activation and reconstruction

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Tuning the porosity of {Co12IICo8III（μ3-OH）24（X）}11+ supramolecular frameworks by reaction time for D2/H2 separation

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Science China Chemistry 2025年

作者： Zhuozhou Xie Zhu Zhuo Zi-Ang Nan Qing Li Xiufang Li Zi-Xiu Lu Linzhe Lü Jin Liu Luyao Liu Wenjing Wang Wei Wang Daqiang Yuan You-Gui Huang State Key Laboratory of Structure Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences University of Chinese Academy of Sciences Xiamen Key Laboratory of rare earth Photoelectric Functional Materials Xiamen Institute of Rare Earth Materials Haixi InstitutesChinese Academy of Sciences State Key Laboratory of Physical Chemistry of Solid Surfaces Department of Chemistry College of Chemistry and Chemical EngineeringXiamen University

Systematicly tuning the porosities of porous materials is crucial for targeted gas mixture separation,yet it remains a longstanding *** a common strategy,altering the phenylene ring count in the organic building units has been exploited to adjust pore apertures in metal organic frameworks （MOFs） and covalent organic frameworks （COFs）,resulting in only a stepwise pore size variation of approximately 2.8?.Unlike MOFs and COFs,the porosities for supramolecular assembly frameworks are highly dependent on the packings of the molecular building units in the *** above strategy cannot be applied to supramolecular assembly frameworks and other strategies are required to adjust pore apertures in supramolecular frameworks,especially to achieve porous materials with the optimal pore size for D2/H2separation （～3?）.Here,we successfully modulate the porosity of supramolecular frameworks of[CoII1+12CoIII8L12（μ3-OH）24（X）]1clusters （L=mono-deprotonated 1-iminoisoindole-3-amine,X=ClO?4or Cl?） by controlling the duration of self-assembly *** simply adjusting the reaction time,we obtain three[CoII12CoIII8L12（μ3-OH）24（X）]11+supramolecular frameworks:[CoII12CoIII8（μ3-OH）24（ClO4）L12)]·（Cl）4·（HCO2）7（1）,[CoII12CoIII8L12（μ3-OH）24（Cl）]·（ClOI4）4·（Cl）6·（HCO2）·（H2O）10（2）,and[CoI12CoIII8L12（μ3-OH）24（Cl）]·（Cl）11·（H2O）12（3）.The different stacking patterns of the[CoII12CoIII8L12（μ3-OH）24（X）]11+clusters in these frameworks lead to significantly varied stabilities and *** 1 exhibits permanent porosity with interconnected channels and maintains stability under harsh *** contrast,compound 2 is nearly nonporous,and compound 3 becomes unstable upon *** pores of compound 1 show higher affinity to D2than H2,and the pore aperture diameter of compound 1 （～3.06?） meets the optimal porosity for D2/***,compound 1 demonstrates moderate D2/H2separation at 77 K (retention time:～7 min/g for D2/H2/Ne （10/10/80 vol%） in a flow of 5 mL

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Formation mechanism of deep natural hydrogen in the Sichuan Basin

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Science China earth Sciences 2025年

作者： Xiaomei WANG Kun HE Chunlong YANG Hao XIE Xiaobo WANG Yitong LYU Linfeng XIE Shuichang ZHANG research Institute of Petroleum Exploration & Development PetroChina Key Laboratory of Petroleum Geochemistry China National Petroleum Corporation International center for Isotope Effects research School of Earth Science and Engineering Nanjing University

As a potential renewable and clean energy source,the distribution and exploration prospects of natural hydrogen have garnered widespread ***,the limitations in understanding the formation mechanisms and accumulation patterns of underground natural hydrogen have significantly constrained its efficient exploration and *** study reports H2content and isotopes in natural gas from deep formations in sedimentary basins through geochemical analysis of 58 conventional gas samples from the Sinian to Triassic strata in the central Sichuan *** discovered that H2content in deep natural gas in central Sichuan generally exceeds 0.1%,with a maximum of 1.6%,and hydrogen isotopes (δ2HH2) range from-850‰to-586‰.Analysis of the geological conditions,hydrogen generation mechanisms,and isotope fractionation characteristics in the study area confirms that microbial fermentation or in-situ organic matter cracking are not effective pathways for deep *** with helium content and isotope analysis of the natural gas,it is inferred that the volcanic basement in the central Sichuan area is the potential source rock for natural H2in the Sinian to Triassic ***,H2originates from the radiolysis of water and hydrothermal reactions of Fe（II） in the basement ***,a diffusion fractionation model reveals significant isotope fractionation during the migration and accumulation of deep H2into sedimentary reservoirs,which lead to anomalously light δ2HH2in deep natural gas in central *** indicates that the underground natural hydrogen accumulation is in a long-term dynamic process,with simultaneous H2accumulation and dissipation in the gas *** research not only elucidates the formation mechanism of deep H2but also provides insights for the resource potential of natural hydrogen in sedimentary basins.

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The composition of magmatic-hydrothermal fluids and their related metal mineralization

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Science China earth Sciences 2025年第1期68卷 208-225页

作者： Qihai SHU Jun DENG State Key Laboratory of Geological Processes and Mineral Resources School of Earth Sciences and Resources China University of Geosciences Frontiers Science center for Deep-time Digital earth China University of Geosciences

Magmatic hydrothermal deposits are important sources of many bulk, precious, and rare metals, and have attracted interest from both academic and industrial communities. However, it is still unclear if the major enrichment of the ore-forming metals occurs in the parental magma source region, during the magma evolution, or after the fluid exsolution. Fluid inclusions trapped in hydrothermal minerals crystallized in the early, high-temperature stage before metal precipitation record information close to that of the initially exsolved magmatic fluids, which are helpful in revealing whether the metals have been already significantly enriched prior to the hydrothermal stage. In this study, available compositional data of such early-stage fluid inclusions from magmatic hydrothermal systems globally have been compiled. The results indicate that the concentrations of Cu,Sn, and W respectively from the Cu-, Sn-, and W-mineralized fluids are significantly higher than the hydrothermal systems that do not produce ores with the corresponding metals. This suggests that Cu, Sn, and W could have already been enriched in the magma source and/or magma evolution stage. The Mo concentrations show no difference between Mo-mineralized and Mobarren fluid systems, indicating no significant pre-enrichment in the source region or during the magma evolution. This also implies that an efficient collection of Mo from a large volume of magmas is required to account for the formation of a large Mo deposit. Almost all the hydrothermal fluids contain high concentrations of Fe and Zn-Pb, but only a few of them eventually form Fe or Zn-Pb deposits, reflecting an important role of the hydrothermal evolution process on the selective metal *** above results indicate that different metals are enriched in different stages of a magmatic hydrothermal system, and that the major roles played in the formation of a deposit vary with the metal types. In addition to the metal concentrations in the o

关键词： Magmatic hydrothermal deposits Fluid inclusions LA-ICP-MS Metal enrichment Mineralization mechanism

An investigation on the wind profiles and gravity wave dynamics in MLT region based on the meteor radars from the Meridian Project

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earth and Planetary Physics 2025年第1期9卷 29-38页

作者： Tai Liu Zhe Wang MengXi Shi Willie Soon ShiCan Qiu Department of Geophysics College of the Geology Engineering and GeomaticsChang’an UniversityXi’an 710054China center for Environmental research and earth Sciences(CERES) SalemMA 01970USA Institute of earth Physics and Space Science(ELKH EPSS) 9400SopronHungary

The meteor radar can detect the zenith angle,azimuth,radial velocity,and altitude of meteor trails so that one can invert the wind profiles in the mesosphere and low thermosphere(MLT)region,based on the Interferometric and Doppler *** this paper,the horizontal wind field,gravity wave(GW)disturbance variance,and GW fluxes are analyzed through the meteor radar observation from 2012−2022,at Mohe(53.5°N,122.4°E)and Zuoling(30.5°N,114.6°E)stations of the(Chinese)Meridian *** Lomb−Scargle periodogram method has been utilized to analyze the periodic variations for time series with observational data *** results show that the zonal winds at both stations are eastward dominated,while the meridional winds are southward *** variance of GW disturbances in the zonal and meridional directions increases gradually with height,and there is a strong pattern of annual *** zonal momentum flux of GW changes little with height,showing weak annual *** meridional GW flux varies gradually from northward to southward with height,and the annual periodicity is *** both stations,the maximum values of zonal and meridional wind occur close to the peak heights of GW flux,with opposite *** observational evidence is consistent with the filtering *** horizontal wind velocity,GW flux,and disturbance variance of the GW at Mohe are overall smaller than those at Zuoling,indicating weaker activities in the MLT at *** power spectral density(PSD)calculated by the Lomb−Scargle periodogram shows that there are 12-month period and 6-month period in horizontal wind field,GW disturbance variance and GW flux at both stations,and especially there is also a 4-month cycle in the disturbance *** PSD of the 12-month and 6-month cycles exhibits maximum values below 88 km and above 94 km.

关键词： meteor radar wind field gravity wave Lomb−Scargle method

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Potential dependence in electrocatalysis: a theoretical perspective

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Science China Chemistry 2025年第1期68卷 21-25页

作者： Leyu Liu Zhaoming Xia Zeyu Wang Yinjuan Chen Hai Xiao Department of Chemistry Tsinghua University Fundamental Science center of rare earths Ganjiang Innovation Academy Chinese Academy of Sciences Key Laboratory of Advanced Catalytic Materials and Technology Advanced Catalysis and Green Manufacturing Collaborative Innovation Center Changzhou University

Electrocatalysis is a key technology for the new energy era and sustainable development, serving as the interface for interconversion of electrical and chemical energies, which spans a wide spectrum of applications in sustainable energy and environmental engineering. Electrocatalytic reactions including electrochemical CO2reduction reaction （eCO2RR）, hydrogen evolution reaction （HER）, and oxygen evolution/reduction reactions （OER/ORR）, hold essential promise for renewable energy technologies as well as complement the biogeochemical carbon and oxygen cycles.

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提高锌离子电池低温性能和抑制阴极溶解:V2O5的局部结构和电化学串扰控制（英文）

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Science China Materials 2025年

作者：王俊鹏刘佳玉富达阙兰芳李明春卢灿忠谢奕明 engineering research center of Environment-Friendly Functional Materials Ministry of Education Institute of Materials Physical Chemistry Huaqiao University Xiamen Key Laboratory of rare earth Photoelectric Functional Materials Xiamen Institute of Rare Earth Materials Haixi Institutes Chinese Academy of Sciences CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Key Laboratory of Nanomaterials Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences

深入了解温度和相变之间的关系对于提高锌离子电池的电化学效率至关重要.然而,电化学相互作用的复杂性,特别是与长时间结构演变有关的相互作用,仍然是一个谜.在本研究中,我们利用V2O5作为晶体的初始结构模型,通过施加不同的机械研磨强...

深入了解温度和相变之间的关系对于提高锌离子电池的电化学效率至关重要.然而,电化学相互作用的复杂性,特别是与长时间结构演变有关的相互作用,仍然是一个谜.在本研究中,我们利用V2O5作为晶体的初始结构模型,通过施加不同的机械研磨强度来细致地控制晶体缺陷,从而揭开电极反应动力学和整体电化学降解的衰变机制.研究表明,经过研磨的V2O5（GVO）具有稳定的晶体结构,可以抑制钒的溶解/穿梭,减轻电化学过程引起的锌阳极副产物.因此,GVO作为正极材料,在室温和低温下均具有优异的Zn存储容量,在室温和-20℃下分别为380和246 mA h g-1.值得注意的是,GVO阴极在-20℃和1 A g-1条件下,经过1500次循环后,容量保持率为99%,保持比容量为160 mA h g-1这项工作为水锌离子电池（AZIBs）在宽温度范围内的电化学串扰行为提供了新的见解.

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