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Strong metal-support interactions between highly dispersed Cu^(+) species and ceria via mix-MOF pyrolysis toward promoted water-gas shift reaction

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Journal of Energy Chemistry 2024年第4期91卷 475-483页

作者： Xiao-Chen Sun Xing-Chi Li Ze-Wei Xie Chen-Yue Yuan De-Jiu Wang Qian Zhang Xiao-Yu Guo Hao Dong Hai-Chao Liu Ya-Wen Zhang Beijing National laboratory for Molecular Sciences(BNLMS) State Key Laboratory of Rare Earth Materials Chemistry and ApplicationsPKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic ChemistryCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China Beijing National laboratory for Molecular Sciences(BNLMS) College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China Beijing National laboratory for Molecular Sciences(BNLMS) State Key Laboratory for Structural Chemistry of Stable and Unstable SpeciesCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China

The modulation of metal-support interfacial interaction is significant but challenging in the design of high-efficiency and high-stability supported catalysts.Here,we report a synthetic strategy to upgrade Cu-CeO_(2)interfacial interaction by the pyrolysis of mixed metal-organic framework(MOF)structure.The obtained highly dispersed Cu/CeO_(2)-MOF catalyst via this strategy was used to catalyze water-gas shift reaction(WGSR),which exhibited high activity of 40.5μmolCOgcat^(-1).s^(-1)at 300℃and high stability of about 120 h.Based on comprehensive studies of electronic structure,pyrolysis strategy has significant effect on enhancing metal-support interaction and then stabilizing interfacial Cu^(+)species under reaction conditions.Abundant Cu^(+)species and generated oxygen vacancies over Cu/CeO_(2)-MOF catalyst played a key role in CO molecule activation and H2O molecule dissociation,respectively.Both collaborated closely and then promoted WGSR catalytic performance in comparison with traditio nal supported catalysts.This study shall offer a robust approach to harvest highly dispersed catalysts with finely-tuned metal-support interactions for stabilizing the most interfacial active metal species in diverse heterogeneous catalytic reactions.

关键词： Cu-based catalyst MOF derivative Water-gas shift reaction Metal-support interaction

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Potential transformation of organic matter by microbes in cryoconite,Tibetan Plateau

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Science China earth Sciences 2024年第6期67卷 1978-1989页

作者： Bixi GUO Yongqin LIU Kevin Xu ZHONG Quan SHI Chen HE Qiang ZHENG Ruanhong CAI State key laboratory of Tibetan Plateau earth System Environment and Resources(TPESER)Institute of Tibetan Plateau ResearchChinese Academy of SciencesBeijing 100101China Center for the Pan-Third Pole Environment Lanzhou UniversityLanzhou 730000China Department of earth Oceanand Atmospheric SciencesUniversity of British ColumbiaVancouverBC V6T 1Z4Canada State key laboratory of Heavy Oil Processing Petroleum Molecules Engineering Center(PMEC)China University of PetroleumBeijing 102249China State key laboratory for Marine Environmental Science Collage of Ocean and Earth SciencesXiamen UniversityXiamen 361102China Fujian key laboratory of Marine Carbon Sequestration Xiamen UniversityXiamen 361005China

Microorganisms play an essential role in the glacier carbon cycle;how they transform organic matter in mountain glacial cryoconite remains to be studied.Here,we applied ultra-high resolution Fourier transform ion cyclotron resonance mass spectrometry(FT-ICR MS)and deep sequencing of 16S rRNA gene,to investigate the temporal microbial transformation of dissolved organic matter(DOM)of the Tibetan Plateau cryoconite.During the 60-day incubation,we found that DOM in cryoconite underwent a three-stage transformation,with decreasing bioavailability over time.The microbial community did not change much in the first week while degrading DOM molecules that were associated with higher H/C_(wa)and lower O/C_(wa).During days 15-30,DOM composition remained stable while microbial diversity increased.By day 60,the DOM was microbially converted into a higher state of recalcitrance,with higher values of aromatic index,O/C_(wa),and lower H/C_(wa),which contained molecules containing more heteroatoms.Cooperation among various microbial taxa,like Cyanobacteria,Bacteroidota,Gammaproteobacteria,Firmicutes,and Actinobacteriota,drove the DOM transformation in cryoconite.This study sheds light on the in-situ transformation of DOM composition meditated by microbial populations in cryoconite at a temporal scale,providing new insights into understanding the microbial roles in the glacier organic carbon transformation.

关键词： Cryoconite Dissolved organic matter Biodegradation Microbial community Temporal variation

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Loading capacity and emulsification phenomena of HREE extraction by dialkylphosphinic acids with different β,γ,δ-substituents

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Journal of Rare earths 2024年第1期42卷 191-199,I0007页

作者： Junlian Wang Guodong Xu Wen Xu Jianguo Cui Yufu Chen Ziyong Chang School of Civil and Resource Engineering University of Science and Technology BeijingBeijing100083China key laboratory of Ministry of Education for Efficient Mining and Safety of Metal Mines Beijing100083China State key laboratory of Baiyunobo Rare earth Resource Researches and Comprehensive Utilization Baotou Research Institute of Rare EarthsBaotou014030China

The relationship between dialkylphosphinic acid structure and their loading capacity for HREEs and emulsification phenomena has rarely been studied.In this paper,we took Lu extraction as an example to study the effect of β,γ,δ-substituents of dialkylphosphinic acids on their loading capacity and anti-emulsification performance for HREEs.To discuss conveniently,the dialkylphosphinic acids were classified into two groups:β-substituent group(P208,INET-1,P218,USTB-1 and P227)and γ,δ-substituent group(P218,P2132 and Cyanex 272).For β-substituent group extractants,their loading capacities are in the order P208(299.7 mg/L)≈INET-1(299.5 mg/L)>P218(270.8 mg/L)>>USTB-1(163.1 mg/L)>P227(151.4 mg/L),while their anti-emulsification/gelation performances are just in the opposite order P227>USTB-1>P218>P208≈INET-1 under the studied conditions.For γ,δ-substituent group extractants,their loading capacities are in the order P218(270.8 mg/L)>P2132(192.3 mg/L)>Cyanex272(131.7 mg/L),while the anti-emulsification performance of P218 is better than those of P2132 and Cyanex 272.The loading capacity data given in the parentheses are obtained through repeatedly extracting Lu from ~4×10^(-4)mol/L of Lu aqueous feed solution with initial pH of 2.40 by 0.01 mol/L extractant at phase ratio A/O of 1:1.

关键词： Heavy rare earth element Dialkylphosphinic acid Extraction Loading capacity Emulsification

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Challenges and opportunities in Quaternary palynology

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Science China earth Sciences 2024年第7期67卷 2148-2161页

作者： Qinghai XU Houyuan LU Zhuo ZHENG College of Geographical Sciences Hebei Key Laboratory of Environmental Change and Ecological ConstructionHebei Normal UniversityShijiazhuang 050024China key laboratory of Cenozoic Geology and Environment Institute of Geology and GeophysicsChinese Academy of SciencesBeijing 100029China School of earth Sciences and Engineering Sun Yat-sen UniversityZhuhai 519082China

Quaternary palynology plays a pivotal role in investigating global climate change and various other research fields,serving as an essential tool for the quantitative analysis of paleoenvironment changes.However,due to the vast diversity of terrestrial ecosystems and intricate interactions between vegetation,climate,and human activities,further advancements are required in the following aspects within this discipline.(1)The accuracy of classification in pollen morphology and fossil pollen identification needs improvement,particularly at the species level.This represents a significant challenge in present Quaternary palynology.Computer-aided intelligent recognition holds promise as a solution for species identification based on more detail pollen morphology.(2)Most pollen-based vegetation and climate reconstructions overlook the significance of bare ground.Neglecting bare ground can lead to substantial inaccuracies when quantitatively reconstructing past vegetation and climate.(3)While pollen records provide reliable information on paleoclimate changes,current quantitative climate reconstruction models heavily rely on modern pollen datasets derived from present-day vegetation disturbed more or less by human activities.This introduces bias and uncertainties into paleoclimate reconstruction.(4)Although pollen can serve as an indicator of human activities,accurately quantifying the intensity of human influence remains challenging.Improving accurate identification of crop pollen,reconstructing reliable land cover/use data,and integrating multidisciplinary data may enhance the identification and quantification of signals related to human activity in pollen records.

关键词： Quaternary palynology Paleoclimate Paleovegetation Human activity

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Automated screening of primary cell-based aptamers for targeting and therapy of pancreatic cancer

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Chinese Chemical Letters 2024年第2期35卷 300-304页

作者： Zhukang Guo Baijiang Jin Yile Fang Lian Jin Song Li Yan Deng Zhu Chen Hui Chen Yuanying Zhang Rabia Usman Nongyue He State key laboratory of digital Medical Engineering School of Biological Science and Medical EngineeringSoutheast UniversityNanjing 210096China Hunan key laboratory of Biomedical Nanomaterials and Devices Hunan University of TechnologyZhuzhou 412007China Department of Molecular Biology Jiangsu Cancer HospitalNanjing 210009China

Although it has been developed for many years, nucleic acid aptamer screening technology still fails to be widely used, a considerable part of it is due to the variability of tumor cell morphology, which leads to the use of immortalized cell lines in the laboratory to screen nucleic acid aptamers for recognition ability of tumor cells in the diseased body.To address this, primary cells that can be stably passaged were isolated and extracted from spontaneous tumors of genetically engineered pancreatic ductal adenocarcinoma model mice in this study.Next, an automated screening instrument for nucleic acid aptamers developed autonomously by our group was used to perform efficient aptamer screening using a limited number of cells, and the obtained nucleic acid aptamers were affinity verified at the cellular level.Finally, to answer the question of the cell growth environment difference on the recognition ability of nucleic acid aptamers, we verified its targeting ability to tumors in vivo on a nude mice xenograft tumor model, and further used a common antitumor drug doxorubicin combined with nucleic acid aptamers to verify the drug loading ability of this aptamer combined with the targeting therapeutic ability.

关键词： Aptamer Cell-SELEX Automatic instrument Combination therapy Pancreatic cancer

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Robust tantalum tuned perovskite oxygen electrode for reversible protonic ceramic electrochemical cells

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Rare Metals 2024年第7期43卷 3055-3065页

作者： Yu-Shi Feng Yu Shen Fang Wang Chuan Tian Qin-Yi Hu Qian Duan Jing-Wei Li Di Bao School of Materials Science and Engineering Changchun University of Science and Technology Zhongshan Institute of Changchun University of Science and Technology State key laboratory of Rare earth Resource Utilization Changchun Institute of Applied Chemistry Chinese Academy of Sciences key laboratory of Preparation and Applications of Environmental Friendly Materials Ministry of EducationJilin Normal University

Perovskite oxides with diverse composition and structure have exhibited grand advances in boosting the oxygen reduction and evolution reaction（ORR/OER）,which are essential for the reversible protonic ceramic electrochemical cell（R-PCEC） toward the sustainable hydrogen production and utilization.However,enhancement of their activity and stability remains challenging.Herein,we develop the Ta-regulated BaCo0.7Fe0.3O3-δperovskite oxygen electrode(Ba(Co0.7Fe0.3)1-xTaxO3-δ)with abundant oxygen defects and achieve the simultaneous enhancement in the electrocatalytic activity and stability toward ORR and OER.As-fabricated R-PCEC with(Ba(Co0.7Fe0.3)0.9Ta0.1O3-δ)（BCFT10） oxygen electrode performs high power density of 1.47 W·cm-2at 650℃ in fuel cell mode,and the current density is up to-2.11 A·cm-2at 1.4 V at 650℃ in electrolysis mode,as well as the good stability in both the fuel cell and electrolysis modes.Importantly,the cell also demonstrates a stable cycling operation between fuel cell and electrolysis mode,suggesting a great potential of BCFT10 as oxygen electrode material for R-PCECs.

关键词： Reversible protonic ceramic electrochemical cells Perovskite oxide Oxygen electrode Ta element doping Oxygen defects

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VMMAO-YOLO:an ultra-lightweight and scale-aware detector for real-time defect detection of avionics thermistor wire solder joints

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Frontiers of Mechanical Engineering 2024年第3期19卷 77-92页

作者： Xiaoqi YANG Xingyue LIU Qian WU Guojun WEN Shuang MEI Guanglan LIAO Tielin SHI School of Mechanical Engineering and Electronic Information China University of GeosciencesWuhan 430074China State key laboratory of digital Manufacturing Equipment and Technology Huazhong University of Science and TechnologyWuhan 430074China

The quality of the exposed avionics solder joints has a significant impact on the stable operation of the inorbit spacecrafts.Nevertheless,the previously reported inspection methods for multi-scale solder joint defects generally suffer low accuracy and slow detection speed.Herein,a novel real-time detector VMMAO-YOLO is demonstrated based on variable multi-scale concurrency and multi-depth aggregation network(VMMANet)backbone and“one-stop”global information gather-distribute(OS-GD)module.Combined with infrared thermography technology,it can achieve fast and high-precision detection of both internal and external solder joint defects.Specifically,VMMANet is designed for efficient multi-scale feature extraction,which mainly comprises variable multi-scale feature concurrency(VMC)and multi-depth feature aggregation-alignment(MAA)modules.VMC can extract multi-scale features via multiple fix-sized and deformable convolutions,while MAA can aggregate and align multi-depth features on the same order for feature inference.This allows the low-level features with more spatial details to be transmitted in depth-wise,enabling the deeper network to selectively utilize the preceding inference information.The VMMANet replaces inefficient highdensity deep convolution by increasing the width of intermediate feature levels,leading to a salient decline in parameters.The OS-GD is developed for efficacious feature extraction,aggregation and distribution,further enhancing the global information gather and deployment capability of the network.On a self-made solder joint image data set,the VMMAOYOLO achieves a mean average precision mAP@0.5 of 91.6%,surpassing all the mainstream YOLO-series models.Moreover,the VMMAO-YOLO has a body size of merely 19.3 MB and a detection speed up to 119 frame per second,far superior to the prevalent YOLO-series detectors.

关键词： defect detection of solder joints VMMAO-YOLO ultra-lightweight and high-performance multiscale feature extraction VMC and MAA modules OS-GD

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Mars exploration——In situ K-Ar dating of jarosite

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Science China earth Sciences 2024年第3期67卷 641-656页

作者： Jing YANG Dewen ZHENG Ying WU Hong CHEN Li YANG Bin ZHANG key laboratory of Active Tectonics and Geological Safety Ministry of Natural ResourcesInstitute of GeomechanicsChinese Academy of Geological SciencesBeijing 100081China State key laboratory of earthquake Dynamics Institute of GeologyChina Earthquake AdministrationBeijing 100029China Institute of earth Sciences China University of GeosciencesBeijing 100083China key laboratory of Cenozoic Geology and Environment Institute of Geology and GeophysicsChinese Academy of SciencesBeijing 100029Chin

To accurately determine the chronological framework of climatic variations recorded by various Martian terrains, the absolute ages of Martian events and cratering rate need to be constrained by either in situ dating or returned samples. In situ K-Ar dating is currently a more plausible dating technique as compared with sample return. Jarosite(KFe_(3)[SO_(4)]_(2)[OH]_(6)) is the only confirmed K sulfate mineral that is widely present on Mars, as indicated by in situ detection, orbital remote sensing, and meteorite studies. Jarosite can be used for precise K-Ar and (40)Ar/(39)Ar dating. The preservation of jarosite on Mars provides information about the nature and duration of aqueous processes on the Martian surface. Different ages of Martian jarosite represent the key to constraining the transition from Martian surface water activity to arid climatic conditions. This paper summarizes recent advances in our knowledge of the spatial distribution of Martian jarosite, its mineralogical properties and stability on Mars, the Ar diffusion kinetics of jarosite, and the current status of in situ K-Ar dating. Moreover, we examine the key scientific issues to be addressed for in situ K-Ar dating of jarosite and Martian sample return missions, and discuss future research directions.

关键词： Mars Jarosite In situ K-Ar dating Ar diffusion Stability

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Recent progress in CdS-based S-scheme photocatalysts

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Journal of Materials Science & Technology 2024年第4期171卷 162-184页

作者： Yajing Ren Yunfeng Li Guixu Pan Ning Wang Yan Xing Zhenyi Zhang College of Environmental and Chemical Engineering Xi’an Polytechnic UniversityXi’an 710048China Jilin Provincial key laboratory of Advanced Energy Materials Department of ChemistryNortheast Normal UniversityChangchun 130024China key laboratory of New Energy and Rare earth Resource Utilization of State Ethnic Affairs Commission Key Laboratory of Photosensitive Materials and Devices of Liaoning ProvinceSchool of Physics and Materials EngineeringDalian Minzu UniversityDalian 116600China

Photocatalytic technology with sunlight as driving force can convert solar energy into other energy sources for storage and further use.Cadmium sulfide(CdS),as a typical reducing semiconductor of metal sulfides,represents an interesting research hotspot in photocatalysis due to its suitable bandgap(2.4 eV)for utilizing visible light and strong reducing ability for inducing surface catalytic reactions.Unfortunately,the photocatalytic performance of CdS is still limited by its fast carrier recombination and serious pho-tocorrosion.So far,CdS semiconductor has been widely developed as a typical reducing photocatalyst in constructing novel S-scheme heterojunction to overcome the above drawbacks.In this review,the de-sign concepts,basic principles,and charge transfer characteristics of CdS-based S-scheme heterojunction photocatalysts have been comprehensively introduced.Several advanced and effective characterization methods for studying the mechanism of CdS-based S-scheme heterojunction are analyzed in detail.Fur-thermore,we also summarize the typical applications of CdS-based S-scheme heterojunctions for water splitting,CO_(2) reduction,pollutant degradation,etc.Eventually,according to the current investigation sta-tus,some drawbacks in the current synthetic strategy,mechanism exploration,and application prospect of CdS-based S-scheme heterojunction are proposed,which need to be addressed by further expansion and innovative research.

关键词： Photocatalysis CdS semiconductor Heterojunction S-scheme Metal sulfide

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Glacial-interglacial cycles recorded in clay minerals from the eastern Tibetan Plateau over the last 800 ka and their indications

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Science China earth Sciences 2024年第7期67卷 2162-2177页

作者： Xiaoyan ZHANG Chunxia ZHANG Yan ZHAO Bin HU Zhengtang GUO key laboratory of Cenozoic Geology and Environment Institute of Geology and GeophysicsChinese Academy of SciencesBeijing 100029China College of earth and Planetary Sciences University of Chinese Academy of SciencesBeijing 100049China College of earth Science and Engineering Shandong University of Science and TechnologyQingdao 266590China key laboratory of Land Surface Pattern and Simulation Institute of Geographic Sciences and Natural Resources ResearchChinese Academy of SciencesBeijing 100101China

Clay mineral proxies have been widely used to reconstruct changes in provenance and the paleoclimate.However,high-altitude clay mineral indications and long-term and orbital variations have not been fully explored.Herein,we present an800-ka clay-mineral record from a lacustrine sediment core(ZB13-C2)from the Zoige Basin on the eastern Tibetan Plateau(TP).X-ray diffraction and scanning electron microscopy were used to identify the clay mineral assemblages and their micromorphological characteristics of core ZB13-C2.The results revealed that the clay minerals in core ZB13-C2 are mainly illite,with small amounts of chlorite,kaolinite,and smectite(including irregular mixed-layers of illite-smectite(I/S)and chloritesmectite(C/S)).The clay mineral assemblages and proxies exhibit three stages of change,which are mainly controlled by the Zoige watershed range under different climate conditions.The watershed was limited to the southeastern region with altitudes ranging from~3500 to~4200 meters above sea level(m a.s.l.),and glacial-interglacial hydraulic erosion controlled the input of bedrock debris during 800-621 ka BP.It expanded to higher altitudes(~4200 to~4700 m a.s.l.)due to stronger seasonal freezethaw weathering without significant glacial-interglacial variations under a cooling and drying climate during 621-100 ka BP.Finally,it expanded to its highest altitudes of~4700 to~5200 m a.***.l.northwest of the watershed after 100 ka BP,and hydraulic erosion increased obviously under a warm climate of the interstadial MIS 3 on the TP.The watershed underwent two major expansions under different climatic conditions at~621 ka and 100 ka BP,with the wet/dry alternation became strong at~621 ka BP.These results reveal that long-term temperature changes and the wet/dry alternation at high altitudes controlled the watershed range and degree of the physical erosion,and that the indications of clay minerals should be carefully clarified before they are used as climate indicators,especially on the TP.

关键词： Quaternary Zoige Basin Lacustrine sediments Paleoenvironment Weathering

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