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Tuning Structural and Electronic Configuration of FeN_(4) via External S for Enhanced Oxygen Reduction Reaction

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energy & Environmental Materials 2024年第2期7卷 93-101页

作者： Shidong Li Lixue Xia Jiantao Li Zhuo Chen Wei Zhang Jiexin Zhu Ruohan Yu Fang Liu Sungsik Lee Yan Zhao Liang Zhou Liqiang Mai State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China Foshan Xianhu Laboratory of the Advanced energy Science and Technology Guangdong Laboratory Foshan 528200China Chemical Sciences and Engineering Division Argonne National Laboratory9700 South Cass AvenueLemontIL 60439USA NRC(Nanostructure Research Centre) Wuhan University of TechnologyWuhan 430070China X-ray Science Division Advanced Photon SourcesArgonne National Laboratory9700 South CassAvenueLemontIL 60439USA State Key Laboratory of Silicate Materials for Architectures International School of Materials Science and EngineeringWuhan University of TechnologyWuhan 430070China The Institute of Technological Sciences Wuhan UniversityWuhan 430072China Hubei Longzhong Laboratory Xiangyang 441000China

The Fe-N-C material represents an attractive oxygen reduction reaction electrocatalyst,and the FeN_(4)moiety has been identified as a very competitive catalytic active *** tuning of the coordination structure of FeN_(4)has an essential impact on the catalytic ***,we construct a sulfur-modified Fe-N-C catalyst with controllable local coordination environment,where the Fe is coordinated with four in-plane N and an axial external *** external S atom affects not only the electron distribution but also the spin state of Fe in the FeN_(4)active *** appearance of higher valence states and spin states for Fe demonstrates the increase in unpaired *** the above characteristics,the adsorption and desorption of the reactants at FeN_(4)active sites are optimized,thus promoting the oxygen reduction reaction *** work explores the key point in electronic configuration and coordination environment tuning of FeN_(4)through S doping and provides new insight into the construction of M-N-C-based oxygen reduction reaction catalysts.

关键词： coordination structure electronic configuration FeN_(4)moiety oxygen reduction reaction sulfur doping

Excellent reusability of FeBC amorphous ribbons induced by progressive formation of through-pore structure during acid orange 7 degradation

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Journal of Materials Science & Technology 2020年第3期38卷 107-118页

作者： Fang Miao Qianqian Wang Qiaoshi Zeng Long Hou Tao Liang Zhiqiang Cui Baolong Shen School of Materials Science and Engineering Jiangsu Key Laboratory for Advanced Metallic MaterialsSoutheast UniversityNanjing211189China Institute of Massive Amorphous Metal Science China University of Mining and TechnologyXuzhou221116China

The high-efficient degrading ability of Fe BC amorphous ribbons toward acid orange 7(AO7)via redox reactions is reported and compared with that of Fe PC amorphous *** time required for degrading50%of AO7 using Fe BC amorphous ribbons is only 1/3 of that using Fe PC amorphous *** the Fe BC amorphous matrix,galvanic cell structures are formed between the Fe-B and Fe-C bonds because of the large difference in their bonding strengths,which contributes to the low reaction activation energy and the high degrading efficiency of Fe BC amorphous *** extremely long service life of Fe BC amorphous ribbons comes from the progressive formation of 3 D porous nanosheet networks that allow more efficient mass transport and a larger specific surface *** Fe BC amorphous ribbons show a satisfying degrading ability in not only acidic but also neutral and weak alkaline AO7 *** work provides an effective and environmental-friendly material for degrading azo dyes.

关键词： 3D nanosheet arrays Through-pore Wastewater treatment FeBC amorphous alloys Synchrotron XRD

Iron-Imprinted Single-Atomic Site Catalyst-Based Nanoprobe for Detection of Hydrogen Peroxide in Living Cells

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Nano-Micro Letters 2021年第9期13卷 364-376页

作者： Zhaoyuan Lyu Shichao Ding Maoyu Wang Xiaoqing Pan Zhenxing Feng Hangyu Tian Chengzhou Zhu Dan Du Yuehe Lin School of Mechanical and Materials Engineering Washington State UniversityPullmanWA 99164USA School of Chemical Biologicaland Environmental EngineeringOregon State UniversityCorvallisOR 97331USA Irvine Materials Research Institute(IMRI) University of CaliforniaIrvineCA 92697USA

Fe-based single-atomic site catalysts(SASCs),with the natural metalloproteases-like active site structure,have attracted widespread attention in biocatalysis and ***,controlling the isolated single-atom Fe-N-C active site structure is crucial to improve the SASCs’*** this work,we use a facile ion-imprinting method(IIM)to synthesize isolated Fe-N-C single-atomic site catalysts(IIM-Fe-SASC).With this method,the ion-imprinting process can precisely control ion at the atomic level and form numerous well-defined single-atomic Fe-N-C *** IIM-Fe-SASC shows better peroxidase-like activities than that of non-imprinted *** to its excellent properties,IIM-Fe-SASC is an ideal nanoprobe used in the colorimetric biosensing of hydrogen peroxide(H_(2)O_(2)).Using IIM-Fe-SASC as the nanoprobe,in situ detection of H_(2)O_(2)generated from MDA-MB-231 cells has been successfully demonstrated with satisfactory sensitivity and *** work opens a novel and easy route in designing advanced SASC and provides a sensitive tool for intracellular H_(2)O_(2)detection.

关键词： Single-atomic site catalysts Nanoprobe Peroxidase-like activities Biosensing Living cell

Three-dimensional coherent X-ray diffraction imaging via deep convolutional neural networks

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npj Computational Materials 2021年第1期7卷 1592-1599页

作者： Longlong Wu Shinjae Yoo Ana F.Suzana Tadesse A.Assefa Jiecheng Diao Ross J.Harder Wonsuk Cha Ian K.Robinson Computational Science Initiative Brookhaven National LaboratoryUptonNYUSA Condensed Matter Physics and Materials Science department Brookhaven National LaboratoryUptonNYUSA Stanford Institute for Materials and energy Sciences SLAC National Accelerator LaboratoryCaliforniaUSA London Centre for Nanotechnology University College LondonLondonUK Advanced Photon Source ArgonneILUSA

As a critical component of coherent X-ray diffraction imaging(CDI),phase retrieval has been extensively applied in X-ray structural science to recover the 3D morphological information inside measured *** meeting all the oversampling requirements of Sayre and Shannon,current phase retrieval approaches still have trouble achieving a unique inversion of experimental data in the presence of ***,we propose to overcome this limitation by incorporating a 3D Machine Learning(ML)model combining(optional)supervised learning with transfer *** trained ML model can rapidly provide an immediate result with high accuracy which could benefit real-time experiments,and the predicted result can be further refined with transfer *** significantly,the proposed ML model can be used without any prior training to learn the missing phases of an image based on minimization of an appropriate‘loss function’*** demonstrate significantly improved performance with experimental Bragg CDI data over traditional iterative phase retrieval algorithms.

关键词： coherent convolution overcome

Novel in-capsule synthesis of metal-organic framework for innovative carbon dioxide capture system

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Green energy & Environment 2023年第3期8卷 767-774页

作者： Wei Yu Ming Gao Guanhe Rim Tony G.Feric Mark L.Rivers Ammar Alahmed Aqil Jamal Ah-Hyung Alissa Park State Key Laboratory of Clean energy Utilization Zhejiang UniversityHangzhou310027China Lenfest Center for Sustainable energy The Earth InstituteColumbia University918 S.W.Mudd HallMail Code 4711500 W 120th St.New YorkNY10027USA department of Earth and Environmental Engineering 918 S.W.Mudd HallMail Code 4711500 W 120th St.New YorkNY10027USA department of Chemical Engineering Columbia UniversityNew YorkNY10027USA University of Chicago ChicagoIL60637USA Research and Development Center Saudi AramcoDhahran31311Saudi Arabia

Metal-Organic Frameworks(MOFs)have been developed as solid sorbents for CO_(2) capture applications and their properties can be controlled by tuning the chemical blocks of their crystalline units.A number of MOFs(e.g.,HKUST-1)have been developed but the question remains how to deploy them for gas-solid ***,the direct use of MOFs as nanocrystals would lead to serious problems and ***,for the first time,we report a novel MOF-based hybrid sorbent that is produced via an innovative in-situ microencapsulated *** a custom-made double capillary microfluidic assembly,double emulsions of the MOF precursor solutions and UV-curable silicone shell fluid are ***,HKUST-1 MOF is successfully synthesized within the droplets enclosed in the gas permeable *** developed MOF-bearing microcapsules uniquely allow the deployment of functional nanocrystals without the challenge of handling ultrafine particles,and further,can selectively reject undesired compounds to protect encapsulated MOFs.

关键词： Encapsulation Metal-Organic Frameworks(MOFs) Carbon capture In-situ microencapsulated synthesis

Elucidating the impact of the ionomer equivalent weight on a platinum group metal-free PEMFC cathode via oxygen limiting current

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SusMat 2023年第1期3卷 72-90页

作者： HaoWang Luigi Osmieri Haoran Yu Michael J.Zachman Jae Hyung Park Nancy N.Kariuki Firat C.Cetinbas Sunilkumar Khandavalli Scott Mauger Deborah J.Myers David A.Cullen Kenneth C.Neyerlin Chemistry and Nanoscience Center National Renewable Energy LaboratoryGoldenColoradoUSA Center for Nanophase Materials Sciences Oak Ridge National LaboratoryOak RidgeTennesseeUSA Chemical Sciences and Engineering Division Argonne National LaboratoryLemontIllinoisUSA Nuclear Science and Engineering Division Argonne National LaboratoryLemontIllinoisUSA

Leveraging the interactions between ionomer and catalyst can increase the performance of proton exchangemembrane fuel *** impacts of the equivalent weight(EW)of perfluorosulfonic acid-based ionomers on the platinum group metal-free electrode structure and fuel cell performance have not been fully *** membrane electrode assemblies(MEAs)were prepared by using a commercial Fe-N-C catalyst,two perfluorosulfonic acid ionomers with different EWs,that is,Aquivion 720(A720)and Nafion 1100(N1100),and two ionomer-tocatalyst(I/C)*** four MEAswere characterized to understand the impact of the ionomer EW and content on the capacitance,proton conductivity,and mass transport on the *** mass transport resistance was measured for the first time using a new oxygen reduction reaction limiting current method enabling to couple the effects of oxygen diffusion with liquid water *** EW ionomer combined with a moderate I/C results in improved performance due to its enhanced proton ***,when used at high I/C,it can cause severewater flooding at high current density due to the enhanced liquid water uptake,especially at high relative humidity,resulting in lower catalyst utilization and higher mass transport resistance.

关键词： ionomer equivalent weight limiting current mass transport oxygen reduction reaction PGMfree catalyst proton exchange membrane fuel cell

Deep mantle hydrogen in the pyrite-type FeO_(2)–FeO_(2)H system

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Geoscience Frontiers 2021年第2期12卷 975-981页

作者： Qingyang Hu Jin Liu Center for High Pressure Science and Technology Advanced Research(HPSTAR) Beijing100094China

The pyrite-type FeO_(2)and FeO_(2)H were synthesized at the pressure-temperature conditions relevant to Earth’s deep lower *** the water-iron reaction,the pyrite-phase is a good candidate to explain the chemical heterogeneities and seismological anomalies at the bottom of the *** solid solution of pyrite-type FeO_(2)and FeO_(2)H,namely the FeO_(2)Hx(0≤x≤1),is particularly interesting and introduces puzzling chemical states for both the O and H atoms in the deep *** the role of H in the FeO_(2)–FeO_(2)H system has been primarily investigated,discrepancies *** this work,we summarize recent progress on the pyrite-phase,including FeO_(2),FeO_(2)H,and FeO_(2)Hx,which is critical for understanding the water cycling,redox equilibria,and compositional heterogenicities in the deep lower mantle.

关键词： Deep lower mantle Core-mantle boundary Pyrite-type phase Hydrogen-bearing phase

Structural stability of methane hydrate at high pressures

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Geoscience Frontiers 2011年第1期2卷 93-100页

作者： I.-Ming Chou Russell J.Hemley Ho-kwang Mao 954 National Center U.S.Geological SurveyRestonVA 20192USA Geophysical Laboratory Carnegie Institution of WashingtonWashingtonDC 20015USA

The structural stability of methane hydrate under pressure at room temperature was examined by both in-situ single-crystal and powder X-ray diffraction techniques on samples with structure types I, II, and H in diamond-anvil ceils. The diffraction data for types II （slI） and H （sH） were refined to the known structures with space groups Fd3m and P63/mmc, respectively. Upon compression, sl methane hydrate transforms to the sll phase at 120 MPa, and then to the sH phase at 600 MPa. The slI methane hydrate was found to coexist locally with sI phase up to 500 MPa and with sH phase up to 600 MPa. The pure sH structure was found to be stable between 600 and 900 MPa. Methane hydrate decomposes at pressures above 3 GPa to form methane with the orientationally disordered Fm3m structure and ice VII （Pn3m）. The results highlight the role of guest （CH4）-host （H2O） interactions in the stabilization of the hydrate structures under pressure.

关键词： Methane hydrate Structural stability High pressure

New yellow Ba_(0.93)Eu_(0.07)Al_(2)O_(4) phosphor for warm-white light-emitting diodes through single-emitting-center conversion

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Light(Science & Applications) 2013年第1期2卷 226-233页

作者： Xufan Li John D Budai Feng Liu Jane Y Howe Jiahua Zhang Xiao-Jun Wang Zhanjun Gu Chengjun Sun Richard S Meltzer Zhengwei Pan College of Engineering University of GeorgiaAthensGA 30602USA department of Physics and Astronomy University of GeorgiaAthensGA 30602USA Materials Science and Technology Division Oak Ridge National LaboratoryOak RidgeTN 37831USA State Key Laboratory of Luminescence and Applications Changchun Institute of OpticsFine Mechanics and PhysicsChinese Academy of SciencesChangchun 130033China department of Physics Georgia Southern UniversityStatesboroGA 30460USA Key Laboratory for Biomedical Effects of Nanomaterials and Nanosafety Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China X-ray Science Division Argonne National LaboratoryArgonneIL 60439USA

Phosphor-converted white light-emitting diodes for indoor illumination need to be warm-white(i.e.,correlated color temperature,4000 K)with good color rendition(i.e.,color rendering index.80).However,no single-phosphor,single-emitting-center-converted white light-emitting diodes can simultaneously satisfy the color temperature and rendition requirements due to the lack of sufficient red spectral component in the phosphors’emission ***,we report a new yellow Ba_(0.93)Eu_(0.07)Al_(2)O_(4) phosphor that has a new orthorhombic lattice structure and exhibits a broad yellow photoluminescence band with sufficient red spectral ***-white emissions with correlated color temperature,4000 K and color rendering index.80 were readily achieved when combining the Ba_(0.93)Eu_(0.07)Al_(2)O_(4) phosphor with a blue light-emitting diode(440–470 nm).This study demonstrates that warm-white light-emitting diodes with high color rendition(i.e.,color rendering index.80)can be achieved based on single-phosphor,single-emitting-center conversion.

关键词： luminescence single-phosphor-conversion warm-white light-emitting diode yellow phosphor