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Fe-N-C core-shell catalysts with single low-spin Fe(Ⅱ)-N_(4)species for oxygen reduction reaction and high-performance proton exchange membrane fuel cells

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Journal of Energy Chemistry 2024年第6期93卷 538-546,I0013页

作者： Yan Wan Linhui Yu Bingxin Yang Caihong Li Chen Fang Wei Guo Fang-Xing Xiao Yangming Lin xiamen Key Laboratory of rare earth Photoelectric Functional materials Xiamen Institute of Rare Earth MaterialsHaixi InstituteChinese Academy of SciencesXiamen 361021FujianChina CAS Key Laboratory of Urban Pollutant Conversion Institute of Urban EnvironmentChinese Academy of SciencesXiamen 361021FujianChina Fujian institute of Research on the Structure of Matter Chinese Academy of SciencesFuzhou 350002FujianChina College of materials Science and Engineering Fuzhou UniversityNew CampusMinhou 350108FujianChina College of Chemistry and materials Science Fujian Normal UniversityFuzhou 350117FujianChina

Fe-N-doped carbon materials(Fe-N-C)are promising candidates for oxygen reduction reaction(ORR)relative to Pt-based catalysts in proton exchange membrane fuel cells(PEMFCs).However,the intrinsic contributions of Fe-N_(4)moiety with different chemical/spin states(e.g.D1,D2,D3)to ORR are unclear since various states coexist *** the present work,Fe-N-C core-shell nanocatalyst with single lowspin Fe(Ⅱ)-N_(4)species(D1)is synthesized and identified with ex-situ ultralow temperature Mossbauer spectroscopy(T=1.6 K)that could essentially differentiate various Fe-N_(4)states and invisible Fe-O *** quantifying with CO-pulse chemisorption,site density and turnover frequency of Fe-N-C catalysts reach 2.4×10^(-9)site g^(-1)and 23 e site~(-1)s^(-1)during the ORR,***-wave potential(0.915V_(RHE))of the Fe-N-C catalyst is more positive(approximately 54 mV)than that of Pt/***,we observe that the performance of PEMFCs on Fe-N-C almost achieves the 2025 target of the US Department of Energy by demonstrating a current density of 1.037 A cm^(-2)combined with the peak power density of 0,685 W cm^(-2),suggesting the critical role of Fe(Ⅱ)-N_(4)site(D1).After 500 h of running,PEMFCs still deliver a power density of 1.26 W cm^(-2)at 1.0 bar H_(2)-O_(2),An unexpected rate-determining step is figured out by isotopic labelling experiment and theoretical *** work not only offers valuable insights regarding the intrinsic contribution of Fe-N_(4)with a single spin state to alkaline/acidic ORR,but also provides great opportunities for developing high-performance stable PEMFCs.

关键词： Fuel cells Oxygen reduction reaction Non-platinum group metals(PGMs) Isotopic labelling Active site TOF

发射峰为875 nm的高热稳定性立方相Sc(PO_(3))_(3):Cr^(3+)荧光粉

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Science China materials 2024年第3期67卷 931-938页

作者：刘乐聂文东吴会杰张景荣梁思思朱浩淼 CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian 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 Research Center of Rare Earth MaterialsHaixi InstituteChinese Academy of SciencesXiamen 361021China

近红外(NIR)荧光粉转换型发光二极管(pc-LED)具有尺寸小、效率高以及光谱易于调节的特点,在特种照明、传感、微型近红外光谱仪等各领域有很好的应用前景.目前,已报道的发射波长超过850 nm的近红外荧光粉的荧光热稳定性较差.在本项研究中... 详细信息

近红外(NIR)荧光粉转换型发光二极管(pc-LED)具有尺寸小、效率高以及光谱易于调节的特点,在特种照明、传感、微型近红外光谱仪等各领域有很好的应用前景.目前,已报道的发射波长超过850 nm的近红外荧光粉的荧光热稳定性较差.在本项研究中,我们合成了一种立方相结构的Sc(PO_(3))_(3):xCr^(3+)(x=0,1,5,10,12,14,16,18 at%)荧光粉,其具有725–1150 nm的宽发射带,发射峰为875 nm,与之前报道的发射峰超过850 nm的荧光粉相比,其表现出优异的热稳定性,在423 K下,5 at%样品的积分发光强度保留了室温下的73.4%.通过对比研究立方相和单斜相Sc(PO_(3))_(3):Cr^(3+)荧光粉变温X射线衍射,发现立方相荧光粉优异的荧光热稳定性可能归因于高温下较小的键长和键角变化.利用该荧光粉制备的NIR pc-LED在150 mA电流驱动下,产生了26.62 mW的NIR辐射功率.驱动电流为10 mA时,最高电光转换效率为11.87%.这项工作为开发具有优异荧光热稳定性的Cr^(3+)离子掺杂近红外荧光粉提供了思路.

关键词： near infrared phosphor pc-LEDs broadband emission Sc(PO_(3))_(3) luminescent materials

Li-air batteries:air stability of lithium metal anodes

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Science China Chemistry 2024年第1期67卷 122-136页

作者： Renfei Cao Kai Chen Jianwei Liu Gang Huang Wanqiang Liu Xinbo Zhang School of materials Science and Engineering Changchun University of Science and TechnologyChangchun 130022China State Key Laboratory of rare earth Resource Utilization Changchun Institute of Applied ChemistryChangchun 130022China

Aprotic rechargeable lithium-air batteries(LABs)with an ultrahigh theoretical energy density(3,500 Wh kg^(-1))are known as the‘holy grail’of energy storage systems and could replace Li-ion batteries as the next-generation high-capacity batteries if a practical device could be ***,only a few researches focus on the battery performance and reactions in the ambient air environment,which is a major obstacle to promote the practical application of ***,we have summarized the recent research progress on LABs,especially with respect to the Li metal *** chemical and electrochemical deteriorations of the Li metal anode under the ambient air are discussed in detail,and the parasitic reactions involving the cathode and electrolyte during the charge-discharge processes are *** also provide stability perspectives on protecting the Li metal anodes and propose design principles for realizing high-performance LABs.

关键词： parasitic reaction lithium metal anode anode protection Li-air batteries

A novel long persistent luminescent material CaGeO_(3):Tb^(3+)with photo-stimulation properties

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Journal of rare earths 2024年第7期42卷 1233-1239,I0002页

作者： Wei Meng Xiaoyan Fu Tongyan Lin Zewen Liu Naihui Chen Jiaxu Zhang Runyao Liu Rujun Yang Long Chen Hongwu Zhang School of Chemistry and Material Sciences Ludong UniversityYantai264025China College of materials Science and Engineering Xiamen University of TechnologyXiamen361024China College of materials Xiamen UniversityXiamen361005China

A novel green long afterglow material CaGeO_(3):Tb^(3+)was synthesized by high temperature solid phase *** to the experimental results,CaGeO_(3):Tb^(3+)is a green long persistent luminescent(LPL)material with excellent ***_(3):Tb^(3+)shows LPL emission peak at 442,490.9,548.7,588.5 and 623.8 nm,corresponding to ^(5)D_(3) to^(7)F_(4)and^(5)D_(4)to^(7)F_(J)(J=6,5,4,3)transitions of Tb^(3+).Its CIE coordinates are(0.27,0.50),indicating that the afterglow emission is close to the light of green *** addition,after the excitation source is turned off,the afterglow time is longer than 90 *** an interval of 7 h,the photo-stimulation luminescence(PSL)can be observed by using 980 nm laser cyclic *** thermoluminescence(ThL)results show that there are three types of traps in the material and their depths are 0.666,0.774 and 0.892 eV respectively,which are caused by the doping of Tb^(3+).All the results show that CaGeO_(3):Tb^(3+)is an excellent long afterglow luminescent material.

关键词： Long persistent luminescence Photo-stimulation Trap CaGeO_(3):Tb^(3+) rare earths

Bioinspired nanofluidic iontronics for brain-like computing

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Nano Research 2024年第2期17卷 503-514页

作者： Lejian Yu Xipeng Li Chunyi Luo Zhenkang Lei Yilan Wang Yaqi Hou Miao Wang Xu Hou State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China institute of Artificial Intelligence Xiamen UniversityXiamen 361005China Department of Physics Research Institute for Biomimetics and Soft MatterFujian Provincial Key Laboratory for Soft Functional Materials ResearchJiujiang Research InstituteCollege of Physical Science and TechnologyXiamen UniversityXiamen 361005China The Higher Educational Key Laboratory for Biomedical Engineering of Fujian Province Department of BiomaterialsResearch Center of Biomedical Engineering of XiamenCollege of MaterialsXiamen UniversityXiamen 361005China The institute of Flexible Electronics(IFE Future Technologies)Xiamen UniversityXiamen 361005China Binzhou institute of Technology Binzhou 256600China Innovation Laboratory for Sciences and Technologies of Energy materials of Fujian Province(IKKEM) Xiamen 361102China Engineering Research Center of Electrochemical Technologies of Ministry of Education Xiamen UniversityXiamen 361005China

The human brain performs computations via a highly interconnected network of *** inspiration from the information delivery and processing mechanism of the human brain in central nervous systems,bioinspired nanofluidic iontronics has been proposed and gradually engineered to overcome the limitations of the conventional electron-based von Neumann architecture,which shows the promising potential to enable efficient brain-like *** and tunable nanofluidic ion transport behaviors and spatial confinement show promising controllability of charge carriers,and a wide range of structural and chemical modification paves new ways for realizing brain-like ***,a comprehensive framework of mechanisms and design strategy is summarized to enable the rational design of nanofluidic systems and facilitate the further development of bioinspired nanofluidic *** review provides recent advances and prospects of the bioinspired nanofluidic iontronics,including ion-based brain computing,comprehension of intrinsic mechanisms,design of artificial nanochannels,and the latest artificial neuromorphic functions ***,the challenges and opportunities of bioinspired nanofluidic iontronics in the pioneering and interdisciplinary research fields are proposed,including brain–computer interfaces and artificial neurons.

关键词： human brain ion transport nanofluidics brain-like computing memristive effect

Antitumor efficacy and potential mechanism of FAP-targeted radioligand therapy combined with immune checkpoint blockade

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Signal Transduction and Targeted Therapy 2024年第7期9卷 2936-2952页

作者： Liang Zhao Yizhen Pang Yangfan Zhou Jianhao Chen Hao Fu Wei Guo Weizhi Xu Xin Xue Guoqiang Su Long Sun Hua Wu Jingjing Zhang Zhanxiang Wang Qin Lin Xiaoyuan Chen Haojun Chen Department of Nuclear Medicine and Minnan PET Center Xiamen Key Laboratory of RadiopharmaceuticalsThe First Affiliated Hospital of Xiamen UniversitySchool of MedicineXiamen UniversityXiamenChina Departments of Diagnostic Radiology SurgeryChemical and Biomolecular Engineeringand Biomedical EngineeringYong Loo Lin School of Medicine and College of Design and EngineeringNational University of SingaporeSingaporeSingapore Clinical Imaging Research Centre Centre for Translational MedicineYong Loo Lin School of MedicineNational University of SingaporeSingaporeSingapore Department of Radiation Oncology Xiamen Cancer CenterXiamen Key Laboratory of Radiation OncologyThe First Affiliated Hospital of Xiamen UniversitySchool of MedicineXiamen UniversityXiamenChina Department of Colorectal Tumor Surgery Xiamen Cancer CenterXiamen Key Laboratory of Radiation OncologyThe First Affiliated Hospital of Xiamen UniversitySchool of MedicineXiamen UniversityXiamenChina Department of Cardiothoracic Surgery Zhongda HospitalSchool of MedicineSoutheast UniversityNanjingChina Nanomedicine Translational Research Program NUS Center for NanomedicineYong Loo Lin School of MedicineNational University of SingaporeSingaporeSingapore Department of Neurosurgery and Department of Neuroscience Fujian Key Laboratory of Brain Tumors Diagnosis and Precision TreatmentXiamen Key Laboratory of Brain Centerthe First Affiliated Hospital of Xiamen UniversitySchool of MedicineXiamen UniversityXiamenChina institute of Molecular and Cell Biology Agency for ScienceTechnology and Research(A*STAR)SingaporeSingapore xiamen Key Laboratory of rare earth Photoelectric Functional materials Xiamen Institute of Rare Earth MaterialsHaixi InstituteChinese Academy of SciencesXiamenChina

Radiotherapy combined with immune checkpoint blockade holds great promise for synergistic antitumor *** radionuclide therapy delivers radiation directly to tumor ***1004 is a fibroblast activation protein(FAP)-targeting radiopharmaceutical,conjugated with the albumin binder Evans Blue,which has demonstrated enhanced tumor uptake and retention in previous preclinical and clinical ***,we demonstrate that^(68)Ga/^(177)Lu-labeled LNC1004 exhibits increased uptake and prolonged retention in MC38/NIH3T3-FAP and CT26/NIH3T3-FAP tumor *** therapy with^(177)Lu-LNC1004 induced a transient upregulation of PD-L1 expression in tumor *** combination of^(177)Lu-LNC1004 and anti-PD-L1 immunotherapy led to complete eradication of all tumors in MC38/NIH3T3-FAP tumor-bearing mice,with mice showing 100%tumor rejection upon ***,single-cell RNA sequencing(scRNA-seq),and TCR sequencing revealed that combination therapy reprogrammed the tumor microenvironment in mice to foster antitumor immunity by suppressing malignant progression and increasing cell-to-cell communication,CD8^(+)T-cell activation and expansion,M1 macrophage counts,antitumor activity of neutrophils,and T-cell receptor diversity.A preliminary clinical study demonstrated that^(177)Lu-LNC1004 was well-tolerated and effective in patients with refractory ***,scRNA-seq of peripheral blood mononuclear cells underscored the importance of addressing immune evasion through immune checkpoint blockade *** was emphasized by the observed increase in antigen processing and presentation juxtaposed with T cell *** conclusion,our data supported the efficacy of immunotherapy combined with^(177)Lu-LNC1004 for cancer patients with FAP-positive tumors.

关键词： immunity retention holds

Boosting ammonia production in electrocatalytic NO_(x)reduction on a robust Fe/FeMoO_(4)catalyst

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Nano Research 2024年第7期17卷 5801-5806页

作者： Dong-Xue Liu Xin Deng Yong-Fu Zhu Zhe Meng Xue-Feng Sun Miao-Miao Shi Hai-Xia Zhong Jun-Min Yan Key Laboratory of Automobile materials Ministry of EducationSchool of Materials Science and EngineeringJilin UniversityChangchun 130022China State Key Laboratory of rare earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

Electrocatalytic reduction of nitrate(NO_(3)^(−))and nitride(NO_(2)^(−))to ammonia(NH3)is of wide interest as a promising alternative to the energy-intensive Haber-Bosch route for mitigating the vast energy consumption and the accompanied carbon dioxide emission,as well as benefiting for the relevant sewage ***,exploring an efficient and low-cost catalyst with high atomic utilization that can effectively facilitate the slow multi-electron transfer process remains a grand ***,we present an efficient hydrogenation of NO_(3)^(−)/NO_(2)^(−)species to NH3 in both alkaline and neutral environments over the Fe_(2)(MoO_(4))_(3)derived hybrid electrocatalyst with the metallic Fe site on FeMoO_(4)(Fe/FeMoO_(4)).The Mo ingredient can play a synergistically positive role in further promoting the NH_(3) production on *** a result,Fe/FeMoO_(4)behaves well in the electrochemical NH_(3) generation from NO_(2)^(−)with a maximum NH_(3) Faradaic efficiency(FE)of 96.53%and 87.68%in alkaline and neutral electrolyte,corresponding to the NH_(3) yield rate of 640.68 and 302.56 mg·h^(−1)·mg_(cat.)^(−1),respectively,which outperforms the Fe and Mo counterpart and other similar catalyst,showing the robust catalytic capacity of each active site.

关键词： ammonia synthesis NO_(x)reduction synergistic effect alkaline/neutral electrolyte

Investigation of Ce/BEA as a passive NO_(x)adsorber:*** occurrences of cerium and adsorption behavior

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Journal of rare earths 2024年第7期42卷 1265-1271,I0003页

作者： Minghui Yu Yiying Ding Xiaojie Yu Siwei Yan Meiqing Shen Jianqiang Wang Jun Wang Gurong Shen School of materials Science and Engineering Tianjin UniversityTianjin300350China School of Chemical Engineering and Technology Tianjin UniversityTianjin300350China National rare earth Catalysis Research institute Dongying257000China

Ce/BEA has great potential as a passive NO_(x)absorber(PNA)to reduce the NO_(x)emissions during the cold start phase especially in diesel engine for its high resistance to CO and suitable NO_(x)desorption temperature ***,as a novel material,its physical and chemical properties still remain *** this work,Ce/BEA was synthesized by ion-exchange method to identify the active species in NO_(x)adsorption,compared with aggregated Ce species in Ce/SiAlO_(x) prepared by impregnation method.X-ray diffraction(XRD),high resolution-transmission electron microscopy(HR-TEM)and aberration-corrected-scanning transmission electron microscopy(AC-STEM)were performed to confirm the isolated single atom formation of Ce species in Ce/***-vis diffraction reflection spectra(DRS)and X-ray photoelectron spectroscopy(XPS)were conducted to find the difference of chemical environment between the isolated Ce species and aggregated *** performance evaluation and temperature programmed reduction of hydrogen(H_(2)-TPR)results show the high NO_(x)storage capacity and active oxygen species quantity in Ce/*** is also found that the main NO_(x)adsorption species are Ce^(4+)-O^(∗)rather than Ce^(3+).NO_(x)-diffuse reflectance infrared Fourier transform spectroscopy(NO_(x)-DRIFTS)confirms that the bidentate nitrite species are the critical NO_(x)adsorption intermediates and the conception of NO_(x)adsorption and desorption processes is proposed.

关键词： Passive NO_(x)absorber Ce/BEA Isolated Ce species rare earths

Investigation of Ce/BEA as a passive NO_(x)adsorber:*** aging deactivation mechanism

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Journal of rare earths 2024年第8期42卷 1524-1530,I0004页

作者： Yiying Ding Minghui Yu Xiaojie Yu Meiqing Shen Jianqiang Wang Jun Wang Gurong Shen School of Chemical Engineering and Technology Tianjin UniversityTianjin300350China School of materials Science and Engineering Tianjin UniversityTianjin300350China National rare earth Catalysis Research institute Dongying257000China

Ce/BEA has the potential to be applied as a novel passive NO_(x)absorber(PNA)in the after-treatment of vehicles due to its considerable NO_(x)storage ***,as a vehicle exhaust after-treatment material,it must withstand the test of long-term hydrothermal *** work examined the deactivation mechanism of Ce/BEA during hydrothermal aging.3.0 wt%Ce/BEA was prepared using the ionexchange method,and then subjected to hydrothermal treatment at 650℃with 10%H_(2)O for 1-12 h to obtain samples with different aging *** comparison,the H-BEA support was aged under the same ***-Emmett-Teller(BET)method,X-ray diffraction(XRD),NH_(3)temperature programmed reduction(NH_(3)-TPD),^(27)Al MAS nuclear magnetic resonance(^(27)Al MAS NMR),H_(2)temperature programmed reduction(H_(2)-TPR),and high resolution-transmission electron microscopy(HR-TEM)were performed to characterize the changes in PNA performance,structure,Ce species,and *** HR-TEM and H_(2)-TPR results show that CeO_(x)particles appear after hydrothermal aging,which results from the detachment and aggregation of active Ce *** on the^(27)Al MAS NMR results,we conclude that BEA zeolite dealumination leads to the loss of acidic sites and the transformation of active Ce species on the acidic sites into the less active CeO_(x).This is the primary reason for the hydrothermal aging deactivation of Ce/BEA.

关键词： Passive NO_(x)adsorber Ce/BEA Hydrothermal aging CeO_(x) Dealumination rare earths