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Pd-based nanocatalysts for oxygen reduction reaction:Preparation,performance,and in-situ characterization

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Chinese Journal of Structural Chemistry 2023年第11期42卷 55-68页

作者： Guan-Nan Xing di-ye wei Hua Zhang Zhong-Qun Tian Jian-Feng Li College of Materials State Key Laboratory of Physical Chemistry of Solid SurfacesMOE Key Laboratory of Spectrochemical Analysis and InstrumentationCollege of Chemistry and Chemical EngineeringiChEMFujian Key Laboratory of Advanced MaterialsXiamen UniversityXiamen361005China Shenzhen Research Institute of Xiamen University Shenzhen518000China

Electrochemical energy devices such as fuel cells have received extensive concern in recent ***,the commercial applications of fuel cells have been restricted by the slow kinetics of oxygen reduction reaction(ORR).Pd-based fuel cell catalysts are strong candidates for enhanced ORR activities,especially under alkaline ***,extensive exploration has been made to improve the performance of Pd-based nano-catalysts for oxygen reduction *** paper reviews the research progress of preparation,electrocatalytic performance,and in-situ characterization of various Pd-based oxygen reduction catalysts,from zero-dimensional nanoparticles,to one-dimensional nanowires,to two-dimensional nanosheets,and to Pd single-atom *** may provide some help for improving the activity of Pd-based catalysts and understanding the reaction mecha-nisms and structure-activity relationships.

关键词： Pd-based nanocatalyst Oxygen reduction reaction Electrocatalysis In-situ characterization

In situ studies of energy-related electrochemical reactions using Raman and X-ray absorption spectroscopy

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Chinese Journal of Catalysis 2022年第1期43卷 33-46页

作者： Heng‐Quan Chen Lie Zou di‐ye wei Ling‐Ling Zheng Yuan‐Fei Wu Hua Zhang Jian‐Feng Li College of Energy State Key Laboratory of Physical Chemistry of Solid SurfacesiChEMCollege of Chemistry and Chemical EngineeringCollege of MaterialsFujian Key Laboratory of Advanced MaterialsXiamen UniversityXiamen 361005FujianChina

Electrochemical energy conversion technologies involving processes such as water splitting and O_(2)/CO_(2) reduction,provide promising solutions for addressing global energy scarcity and minimizing adverse environmental ***,due to a lack of an in-depth understanding of the reaction mechanisms and the nature of the active sites,further advancement of these techniques has been limited by the development of efficient and robust ***,in situ characterization of these electrocatalytic processes under working conditions is *** this review,recent applications of in situ Raman spectroscopy and X-ray absorption spectroscopy for various nano-and single-atom catalysts in energy-related reactions are *** cases are highlighted,including the capture of oxygen-containing intermediate species formed during the reduction of oxygen and oxidation of hydrogen,and the detection of catalyst structural transformations occurring with the change in potential during the evolution of oxygen and reduction of CO_(2).Finally,the challenges and outlook for advancing in situ spectroscopic technologies to gain a deeper fundamental understanding of these energy-related electrocatalytic processes are discussed.

关键词： Raman spectroscopy X-ray absorption spectroscopy In situ characterization Electrocatalysis Energy conversion and storage

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direct identification of the carbonate intermediate during water-gas shift reaction at Pt-NiO interfaces using surface-enhanced Raman spectroscopy

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Chinese Journal of Catalysis 2022年第8期43卷 2010-2016页

作者： Si-Na Qin di-ye wei Jie wei Jia-Sheng Lin Qing-Qi Chen Yuan-Fei Wu Huai-Zhou Jin Hua Zhang Jian-Feng Li College of Materials State Key Laboratory of Physical Chemistry of Solid SurfacesMOE Key Laboratory of Spectrochemical Analysis and InstrumentationCollege of Chemistry and Chemical EngineeringiChEMFujian Key Laboratory of Advanced MaterialsCollege of EnergyXiamen UniversityXiamen 361005FujianChina College of Optical and Electronic Technology China Jiliang UniversityHangzhou 310018ZhejiangChina

Noble metal-reducible oxide interfaces have been regarded as one of the most active sites for water-gas shift ***,the molecular reaction mechanism of water-gas shift reaction at these interfaces still remains ***,water-gas shift reaction at Pt-NiO interfaces has been in-situ explored using surface-enhanced Raman spectroscopy by construction of Au@Pt@NiO *** Raman spectroscopic evidence demonstrates that water-gas shift reaction at Pt-NiO interfaces proceeds via an associative mechanism with the carbonate species as a key *** carbonate species is generated through the reaction of adsorbed CO with gaseous water,and its decomposition is a slow step in water-gas shift ***,the Pt-NiO interfaces would promote the formation of this carbonate intermediate,thus leading to a higher activity compared with pure *** spectral information deepens the fundamental understanding of the reaction mechanism of water-gas shift reaction,which would promote the design of more efficient catalysts.

关键词： Water-gas shift reaction Surface-enhanced Raman spectroscopy Core-shell nanostructure In-situ characterization Carbonate intermediate

Soft coarse-grained particle model for particle-fluid systems

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Particuology 2024年第1期84卷 178-193页

作者： Yanhao ye Ji Xu wei Ge State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing100190China School of Chemical Engineering University of Chinese Academy of SciencesBeijing100049China Innovation Academy for Green Manufacture Chinese Academy of SciencesBeijing100190China

By modeling a group of neighboring real particles as a single coarse-grained particle(CGP),discrete particle method(DPM)is now capable of simulating industrial-scale particle-fluid ***,a systematic approach to determine the CGP properties and develop their interaction models is still lacking,which casts uncertainty on the predictivity of the *** this study,collisions between predefined particle groups are analyzed to construct kernel functions for modeling the CGPs and then the model parameters are determined by equating the statistical properties of the CGPs and the real particles in the physical process *** approach is implemented for homogeneous cooling of granular gas,then demonstrated effective in simulating experimental fluidized beds.

关键词： Coarse-grain(CG) discrete particle method(DPM) Fluidized bed Multi-scale simulation

Simplified liver imaging reporting and data system for the diagnosis of hepatocellular carcinoma on gadoxetic acid-enhanced magnetic resonance imaging

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World Journal of Gastrointestinal Oncology 2024年第6期16卷 2439-2448页

作者： Rong Lyu wei-Juan Hu di Wang Jiao Wang Yu-Bing ye Ke-Feng Jia Department of Radiology Tianjin Third Central HospitalTianjin Key Laboratory of Extracorporeal Life Support for Critical DiseasesArtificial Cell Engineering Technology Research CenterTianjin 300170China

BACKGROUND The liver imaging reporting and data system(LI-RADS)diagnostic table has 15 cells and is too *** diagnostic performance of LI-RADS for hepatocellular carcinoma(HCC)is not satisfactory on gadoxetic acid-enhanced magnetic resonance imaging(EOB-MRI).AIM To evaluate the ability of the simplified LI-RADS(sLI-RADS)to diagnose HCC on *** A total of 331 patients with 356 hepatic observations were retrospectively *** diagnostic performance of sLI-RADS A-D using a single threshold was evaluated and compared with LI-RADS v2018 to determine the optimal *** algorithms of sLI-RADS A-D are as follows:The single threshold for sLI-RADS A and B was 10 mm,that is,classified observations≥10mm using an algorithm of 10-19 mm observations(sLI-RADS A)and≥20 mm observations(sLI-RADS B)in the diagnosis table of LI-RADS v2018,respectively,while the classification algorithm remained unchanged for observationsding to the optimal sLI-RADS,and its diagnostic performance was *** times needed to classify the observations according to F-sLIRADS and LI-RADS v2018 were *** The optimal sLI-RADS was sLI-RADS D(with a single threshold of 20 mm),because its sensitivity was greater than that of LI-RADS v2018(89.8%vs 87.0%,P=0.031),and its specificity was not lower(89.4%vs 90.1%,P>0.999).With HBP hypointensity as an MF,the sensitivity of F-sLI-RADS was greater than that of LI-RADS v2018(93.0%vs 87.0%,P<0.001)and sLI-RADS D(93.0%vs 89.8%,P=0.016),without a lower specificity(86.5%vs 90.1%,P=0.062;86.5%vs 89.4%,P=0.125).Compared with that of LI-RADS v2018,the time to classif

关键词： Hepatocellular carcinoma Magnetic resonance imaging Liver diagnosis Contrast agent

3D coarse-grained DPM simulation of the MIP reaction-regeneration loop

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Particuology 2024年第6期89卷 57-66页

作者： Yanhao ye Shuai Zhang Ji Xu wei Ge State Key Laboratory of Mesoscience and Engineering(formerly State Key Laboratory of Multiphase Complex Systems) Institute of Process EngineeringChinese Academy of SciencesBeijing100190China School of Chemical Engineering University of Chinese Academy of SciencesBeijing100049China

The reactor-regenerator loop is the core facility of the maximizing iso-paraffin(MIP)*** the discrete particle method(DPM)simulation can provide detailed information at the particle scale,it has been unable to simulate such a complex loop system due to limitations of coarse-grained(CG)models,computing software,and *** this study,a newly proposed soft-shell CG-DPM model with a CG ratio of up to 800 is used to simulate a 3.5 Mt/a industrial-scale MIP reactor-regenerator *** solid fraction distribution obtained is found to agree well with in-situ *** properties including the distribution of solid fraction,gas and solid velocity,standard derivation of solid fraction with time,temporal distribution of the flow field,and particle residence time distribution are measured in the simulation,which are meaningful to better design and operate such systems in the future.

关键词： discrete particle method Coarse-grain Maximizing iso-paraffins Full-loop Reaction-regeneration system

Structural phase transition in a new organic-inorganic hybrid post-perovskite:(N,N-dimethylpyrrolidinium)[Mn(N(CN)2)3]

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结构化学 2024年第6期43卷 40-44页

作者： Le ye wei-Xiong Zhang MOE Key Laboratory of Bioinorganic and Synthetic Chemistry School of ChemistryIGCMESun Yat-Sen UniversityGuangzhou510275China

In the realm of molecular phase transition research,particularly for applications in sensors,data storage and switching technologies,the role of organic-inorganic hybrid perovskite materials has been increasingly recog-nized for their significant ***,hybrid post-perovskites,as a critical subclass of perovskites,have not been thoroughly studied and mainly limit in the instances based on polyatomic bridging agents like dicyanamide(dca-)and non-cyclic organic ***,a polar cyclic quaternary ammonium cation,N,N-dimethylpyrrolidinium(DMP+),was used to assemble a new hybrid post-perovskite,(DMP)[Mn(dca)3](1),which undergoes a phase transition from orthorhombic Bmmb to monoclinic P21/n space group at 249 *** employing multiple techniques such as differential scanning calorimetry,variable-temperature single-crystal X-ray analysis,dielectric measurements,and Hirshfeld surface analysis,we disclosed the role of polar cyclic quaternary ammonium DMP+in elevating the phase-transition temperature by 48 K,generating significant dielectric switching effect and facilitating interlayer sliding of inorganic framework.

关键词： Structural phase transitions dielectric switching Organic-inorganic hybrid crystals Post-perovskites

Multiscale Characteristics and Connection Mechanisms of Attraction Networks:A Trajectory Data Mining Approach Leveraging Geotagged Data

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Chinese Geographical Science 2024年第3期34卷 533-547页

作者： JIANG Hongqiang wei ye MEI Lin WANG Zhaobo School of Resource and Environment Engineering Ludong UniversityYantai 264025China School of Geographical Sciences Northeast Normal UniversityChangchun 130024China Changchun University of Finance and Economics Changchun 130122China Jilin Jizhi City Architectural Design Co. LTDChangchun 130012China

Urban tourism is considered a complex system,and multiscale exploration of the organizational patterns of attraction networks has become a topical issue in urban tourism,so exploring the multiscale characteristics and connection mechanisms of attraction networks is important for understanding the linkages between attractions and even the future destination *** paper uses geotagging data to compare the links between attractions in Beijing,China during four different periods:the pre-Olympic period(2004–2007),the Olympic Games and subsequent‘heat period’(2008–2013),the post-Olympic period(2014–2019),and the COVID-19(Corona Virus disease 2019)pandemic period(2020–2021).The aim is to better understand the evolution and patterns of attraction networks at different scales in Beijing and to provide insights for tourism planning in the *** results show that the macro,meso-,and microscales network characteristics of attraction networks have inherent logical relationships that can explain the commonalities and differences in the development process of tourism *** macroscale attraction network degree Matthew effect is significant in the four different periods and exhibits a morphological monocentric structure,suggesting that new entrants are more likely to be associated with attractions that already have high *** mesoscale links attractions according to the common purpose of tourists,and the results of the community segmentation of the attraction networks in the four different periods suggest that the functional polycentric structure describes their clustering effect,and the weak links between clusters result from attractions bound by incomplete information and distance,and the functional polycentric structure with a generally more efficient network of *** pattern structure at the microscale reveals the topological transformation relationship of the regional collaboration pattern,and the attraction network structure in the four diff

关键词： attraction network travel mobility polycentric structure network motif connectivity mechanism destination management organization(DMO) destination planning Beijing,China

Tuning the surface electronic structure of noble metal aerogels to promote the electrocatalytic oxygen reduction

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Journal of Energy Chemistry 2024年第2期89卷 557-564,I0013页

作者： Hongxing Yuan wei Gao Xinhao Wan Jianqi ye Dan Wen State Key Laboratory of Solidification Processing School of Materials Science and EngineeringNorthwestern Polytechnical UniversityXi’an 710072ShaanxiChina

The sluggish kinetics of the oxygen reduction reaction(ORR)is the bottleneck for various electrochemical energy conversion *** the electronic structure of electrocatalysts by ligands has received particular attention in deriving valid ORR ***,the surface electronic structure of Ptbased noble metal aerogels(NMAs)was modulated by various organic ligands,among which the electron-withdrawing ligand of 4-methylphenylene effectively boosted the ORR *** calculations suggested the smaller energy barrier for the transformation of O^(*) to OH^(*) and downshift the d-band center of Pt due to the interaction between 4-methylphenylene and the surface metals,thus enhancing the ORR intrinsic *** Pt3Ni and Pt Pd aerogels with 4-methylphenylene decoration performed significant enhancement in ORR activity and durability in different ***,the 4-methylphenylene modified Pt Pd aerogel exhibited the higher halfwave potential of 0.952 V and the mass activity of 10.2 times of commercial Pt/*** work explained the effect of electronic structure on ORR electrocatalytic properties and would promote functionalized NMAs as efficient ORR electrocatalysts.

关键词： Noble metal aerogels Surface electronic structure ORR Electrocatalyst Organic ligands