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A flexible and scalable scheme for mixing computed formation energies from different levels of theory

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npj Computational Materials 2022年第1期8卷 1857-1867页

作者： Ryan S.kingsbury Andrew S.Rosen Ayush S.Gupta Jason M.Munro Shyue Ping Ong Anubhav Jain Shyam Dwaraknath matthew k.horton kristin A.Persson Department of Materials Science and Engineering University of California BerkeleyBerkeleyCA94720USA Energy Technologies Area Lawrence Berkeley National LaboratoryBerkeleyCA94720USA Materials Science Division Lawrence Berkeley National LaboratoryBerkeleyCA94720USA Miller Institute for Basic Research in Science University of CaliforniaBerkeleyCA94720USA University of California San Diego La JollaCA92093USA Molecular Foundry Lawrence Berkeley National LaboratoryBerkeleyCA94720USA

Computational materials discovery efforts are enabled by large databases of properties derived from high-throughput density functional theory(DFT),which now contain millions of calculations at the generalized gradient approximation(GGA)level of *** is now feasible to carry out high-throughput calculations using more accurate methods,such as meta-GGA DFT;however recomputing an entire database with a higher-fidelity method would not effectively leverage the enormous investment of computational resources embodied in existing(GGA)***,we propose here a general procedure by which higher-fidelity,low-coverage calculations(e.g.,meta-GGA calculations for selected chemical systems)can be combined with lower-fidelity,high-coverage calculations(e.g.,an existing database of GGA calculations)in a robust and scalable *** then use legacy PBE(+U)GGA calculations and new r2SCAN meta-GGA calculations from the Materials Project database to demonstrate that our scheme improves solid and aqueous phase stability predictions,and discuss practical considerations for its implementation.

关键词： theory scheme theory

High-throughput predictions of metal-organic framework electronic properties:theoretical challenges,graph neural networks,and data exploration

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npj Computational Materials 2022年第1期8卷 1053-1062页

作者： Andrew S.Rosen Victor Fung Patrick Huck Cody T.O’Donnell matthew k.horton Donald G.Truhlar kristin A.Persson Justin M.Notestein Randall Q.Snurr Department of Materials Science and Engineering University of CaliforniaBerkeleyCA94720USA Miller Institute for Basic Research in Science University of CaliforniaBerkeleyBerkeleyCA94720USA Materials Science Division Lawrence Berkeley National LaboratoryBerkeleyCA94720USA Department of Chemical and Biological Engineering Northwestern UniversityEvanstonIL60208USA Center for Nanophase Materials Sciences Oak Ridge National LaboratoryOak RidgeTN37831USA Energy Technologies Area Lawrence Berkeley National LaboratoryBerkeleyCA94720USA Department of Chemistry Chemical Theory Centerand Minnesota Supercomputing InstituteUniversity of MinnesotaMinneapolisMN55455USA Molecular Foundry Lawrence Berkeley National LaboratoryBerkeleyCA94720USA

With the goal of accelerating the design and discovery of metal–organic frameworks(MOFs)for electronic,optoelectronic,and energy storage applications,we present a dataset of predicted electronic structure properties for thousands of MOFs carried out using multiple density functional *** to more accurate hybrid functionals,we find that the widely used PBE generalized gradient approximation(GGA)functional severely underpredicts MOF band gaps in a largely systematic manner for semi-conductors and insulators without magnetic ***,an even larger and less predictable disparity in the band gap prediction is present for MOFs with open-shell 3d transition metal *** regards to partial atomic charges,we find that different density functional approximations predict similar charges overall,although hybrid functionals tend to shift electron density away from the metal centers and onto the ligand environments compared to the GGA point of *** more significant differences in partial atomic charges are observed when comparing different charge partitioning *** conclude by using the dataset of computed MOF properties to train machine-learning models that can rapidly predict MOF band gaps for all four density functional approximations considered in this work,paving the way for future high-throughput screening *** encourage exploration and reuse of the theoretical calculations presented in this work,the curated data is made publicly available via an interactive and user-friendly web application on the Materials Project.

关键词： charges electronic centers

An improved symmetry-based approach to reciprocal space path selection in band structure calculations

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npj Computational Materials 2020年第1期6卷 731-736页

作者： Jason M.Munro katherine Latimer matthew k.horton Shyam Dwaraknath kristin A.Persson Energy Technologies Area Lawrence Berkeley National LaboratoryBerkeleyCA 94720USA Department of Physics University of CaliforniaBerkeleyCA 94720USA Department of Materials Science University of CaliforniaBerkeleyCA 94720USA

Band structures for electrons,phonons,and other quasiparticles are often an important aspect of describing the physical properties of periodic *** commonly,energy bands are computed along a one-dimensional path of high-symmetry points and line segments in reciprocal space(the“k-path”),which are assumed to pass through important features of the dispersion ***,existing methods for choosing this path rely on tabulated lists of high-symmetry points and line segments in the first Brillouin zone,determined using different symmetry criteria and unit cell *** we present a new“on-the-fly”symmetry-based approach to obtaining paths in reciprocal space that attempts to address the previous limitations of these *** a unit cell of a magnetic or nonmagnetic periodic solid,the site symmetry groups of points and line segments in the irreducible Brillouin zone are obtained from the total space *** elements in these groups are used alongside general and maximally inclusive high-symmetry criteria to choose segments for the final k-path.A smooth path connecting each segment is obtained using graph *** new framework not only allows for increased flexibility and user convenience but also identifies notable overlooked features in certain electronic band *** addition,a more intelligent and efficient method for analyzing magnetic materials is also enabled through proper accommodation of magnetic symmetry.

关键词： symmetry reciprocal approach

Engineering the atomic interface of porous ceria nanorod with single palladium atoms for hydrodehalogenation reaction

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Nano Research 2022年第2期15卷 1338-1346页

作者： Zhijun Li Mingyang Zhang Lili Zhang Xiuli Dong Leipeng Leng JHugh horton Jun Wang Joint International Research Laboratory of Advanced Chemical Catalytic Materials&Surface Science College of Chemistry and Chemical EngineeringNortheast Petroleum UniversityDaqing 163318China Shenyang National Laboratory for Materials Science Institute of Metal ResearchChinese Academy of SciencesShenyang 110016China Department of Chemistry Queens UniversityKingstonK7L 3N6Canada

Tuning the electronic properties of single atom catalysts(SACs)between the central metal and the neighboring surface atoms has emerged as an efficient strategy to boost catalytic efficiency and metal *** we describe a simple and efficient approach to create atomically dispersed palladium atoms supported over defect-containing porous ceria nanorod containing palladium up to 0.26 wt.%.The existence of singly dispersed palladium atoms is confirmed by spherical aberration correction electron microscopy and extended X-ray absorption fine structure *** catalyst shows excellent efficiency in hydrodehalogenation reactions at low H2 pressure under mild conditions,along with satisfactory recyclability and *** functional theory(DFT)calculations reveal that the high activity stems from the spatial isolation of palladium atoms and the modified electronic structure of palladium confined in defect-containing ceria *** work may lay the foundation for the facile creation of single atom catalysts within the synthetic community and shed light on the possibility for scale-up production.

关键词： heterogeneous catalysis palladium single atom catalyst porous ceria nanorod hydrodehalogenation catalytic activity

Synthesis of cobalt single atom catalyst by a solid-state transformation strategy for direct C-C cross-coupling of primary and secondary alcohols

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Nano Research 2022年第5期15卷 4023-4031页

作者： Zhijun Li Yuying Chen Xiaowen Lu Honghong Li Leipeng Leng Tinglei zhang JHugh horton Joint International Research Laboratory of Advanced Chemical Catalytic Materials&Surface Science College of Chemistry and Chemical EngineeringNortheast Petroleum UniversityDaqing 163318China Department of Chemistry Queen’s UniversityKingston K7L 3N6Canada

Atomic engineering of single atom catalysts(SACs)with high-density available active sites and optimized electronic properties can substantially boost catalytic ***,we report a solid-state transformation strategy to access Co SACs by introducing Co species from commercial CO_(2)O3 powders into nitrogen-doped carbon *** catalyst exhibited excellent catalytic activity,with a turnover frequency(TOF)of 2,307 h^(-1)and yield of 95%,in the direct C-C cross-coupling of benzyl alcohol and 1-phenylethanol(1 atm O2@80℃)to yield *** functional theory(DFT)calculations demonstrate the coordination environment and electronic metal-support interaction impact the catalytic *** particular,a wide substrate scope and a broad functional-group tolerance of this SAC were validated,and the employment of this strategy for large-scale synthesis was also shown to be *** work might shed light on the facile and scalable synthesis of highly active,selective,and stable SACs for heterogeneous catalysis.

关键词： single atom catalysis solid-state transformation C-C cross-coupling a,β-unsaturated ketones catalytic activity

Single palladium atoms stabilized byβ-FeOOH nanorod with superior performance for selective hydrogenation of cinnamaldehyde

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Nano Research 2022年第4期15卷 3114-3121页

作者： Zhijun Li Leipeng Leng Xiaowen Lu Mingyang Zhang Qian Xu J.Hugh horton Junfa Zhu Joint International Research Laboratory of Advanced Chemical Catalytic Materials&Surface Science College of Chemistry and Chemical EngineeringNortheast Petroleum UniversityDaqing 163318China National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei 230029China Department of Chemistry Queen′s UniversityKingstonK7L 3N6Canada

Atomically dispersed single atom catalysts represent an ideal means of converting less valuable organics into value-added chemicals of interest with high ***,we describe a facile synthetic approach to create defect-containingβ-FeOOH doped with isolated palladium atoms that bond covalently to the nearby oxygen and iron *** presence of singly dispersed palladium atoms is confirmed by spherical aberration correction electron microscopy and extended X-ray absorption fine structure *** single palladium atom catalyst manifests outstanding catalytic efficiency(conversion:99%;selectivity 99%;turnover frequency:2,440 h^(-1))in the selective hydrogenation of cinnamaldehyde to afford *** measurements and density functional theory(DFT)calculations elucidate the high catalytic activity and the strong metal-support interaction stem from the unique coordination environment of the isolated palladium *** findings may pave the way for the facile construction of single atom catalysts in a defect-mediated strategy for efficient organic transformations in heterogeneous catalysis.

关键词： heterogeneous catalysis palladium single atom catalyst β-FeOOH nanorod coordination environment hydrogenation of cinnamaldehyde

Consistent plate rotation patterns in the Qaidam Basin during the Miocene

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Consistent plate rotation patterns in the Qaidam Basin durin...

Engineering the morphology and electronic structure of atomic cobalt-nitrogen-carbon catalyst with highly accessible active sites for enhanced oxygen reduction

作者： Zhongbao Zhang Junsheng Nie Joel Saylor Brian k.horton Wenjiao Xiao

Uplift and deformation timing and processes of the NE Tibetan Plateau figures importantly in testing models for uplift of the Tibetan Plateau as well as understanding forcing mechanisms for Cenozoic central-east Asian environmental variations and Asian monsoon evolution. Past studies focus mostly on upward and outward growth processes of the NE Tibetan Plateau, but its rotation history is in debate. Here we calculated paleomagnetic declination data of several sections from the Qaidam Basin.

关键词： Consistent plate rotation patterns in the Qaidam Basin during the Miocene

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Journal of Energy Chemistry 2022年第10期31卷 469-477,I0012页

作者： Zhijun Li Leipeng Leng Siqi Ji Mingyang Zhang Hongxue Liu Jincheng Gao Jiangwei Zhang J.Hugh horton Qian Xu Junfa Zhu Joint International Research Laboratory of Advanced Chemical Catalytic Materials&Surface Science College of Chemistry and Chemical EngineeringNortheast Petroleum UniversityDaqing 163318HeilongjiangChina Dalian National Laboratory for Clean Energy&State key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina Department of Chemistry Queen0s UniversityKingstonOntario K7L 3N6Canada National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei 230029AnhuiChina

The stabilization of non-precious metals as isolated active sites with high loading density over nitrogendoped carbon materials is essential for realizing the industrial application of single atom ***,achieving high loading of single cobalt active sites with greatly enhanced oxygen reduction reaction(ORR)activity and stability remains ***,an efficient approach was described to create a single atom cobalt electrocatalyst(Co SAs/NC)which possesses enhanced mesoporosity and specific surface area that greatly favor the mass transportation and exposure of accessible active *** electronic structure of the catalyst by the strong metal-support interaction has been elucidated through experimental characterizations and theoretical *** to dramatically enhanced mass transport and electron transfer endowed by morphology and electronic structure engineering,Co SAs/NC exhibits remarkable ORR performance with excellent activity(onset and half-wave potentials of 1.04 V(RHE)and 0.90 V(RHE),Tafel slope of 69.8 mV dec^(-1)and J_(k) of 18.8 mA cm^(-2)at 0.85 V)and stability(7 mV activity decay after 10,000 cycles).In additio n,the catalyst demonstrates great promise as an alternative to traditional Pt/C catalyst in zinc-air batteries while maintaining high performance in terms of high specific capacity of(796.1 mAh/g_(Zn)),power density(175.4 mW/cm^(2)),and long-term cycling stability(140 h).This study presents a facile approach to design SACs with highly accessible active sites for electrochemical transformations.

关键词： Single atom electrocatalyst Non-precious metal Coordination environment Oxygen reduction reaction Catalytic activity Zn-air battery

Alkali ion-promoted palladium subnanoclusters stabilized on porous alumina nanosheets with enhanced catalytic activity for benzene oxidation

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Nano Research 2022年第7期15卷 5912-5921页

作者： Zhijun Li Minghui Di Wei Wei Leipeng Leng Zhijun Li Cheng He Qiang Tan Qian Xu J.Hugh horton Li Li Junfa Zhu Joint International Research Laboratory of Advanced Chemical Catalytic Materials&Surface Science College of Chemistry and Chemical EngineeringNortheast Petroleum UniversityDaqing 163318China key Laboratory of Functional Inorganic Materials Chemistry(Ministry of Education) School of Chemistry and Materials ScienceHeilongjiang UniversityHarbin 150080China State key Laboratory for Mechanical Behavior of Materials School of Material Science and EngineeringXi’an Jiaotong UniversityXi’an 710049China National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei 230029China Department of Chemistry Queen’s UniversityKingston K7L 3N6Canada College of Chemistry and Chemical Engineering Qiqihar UniversityQiqihar 161006China

Catalytic C−H bond activation is one of the backbones of the chemical *** metal subnanoclusters consisting of a few atoms have shown attractive properties for heterogeneous ***,the creation of such catalyst systems with high activity and excellent anti-sintering ability remains a grand ***,we report on alkali ion-promoted Pd subnanoclusters supported over defectiveγ-Al_(2)O_(3) nanosheets,which display exceptional catalytic activity for C−H bond activation in the benzene oxidation *** presence of Pd subnanoclusters is verified by aberration-corrected high-angle annular dark-field scanning transmission electron microscopy,X-ray absorption spectroscopy,and X-ray photoelectron *** catalyst shows excellent catalytic activity,with a turnover frequency of 280 h^(−1) and yield of 98%,in benzene oxidation reaction to give phenol under mild ***,the introduction of alkali ion greatly retards the diffusion and migration of metal atoms when tested under high-temperature sintering *** functional theory(DFT)calculations reveal that the addition of alkali ion to Pd nanoclusters can significantly impact the catalyst’s structure and electronic properties,and eventually promote its activity and *** work sheds light on the facile and scalable synthesis of highly active and stable catalyst systems with alkali additives for industrially important reactions.

关键词： Pd subnanoclusters γ-Al_(2)O_(3)nanosheets heterogeneous catalysis benzene oxidation catalytic activity