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Hu, Guoxiang

Publications and source records attributed to Hu, Guoxiang.

25 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Machine learned features from density of states for accurate adsorption energy prediction

Materials databases generated by high-throughput computational screening, typically using density functional theory (DFT), have become valuable resources for discovering new heterogeneous catalysts, though the computational cost associated with generating them presents a crucial roadblock. Hence there is a significant demand for developing descriptors or features, in lieu of DFT, to accurately predict catalytic properties, such as adsorption energies. Here, we demonstrate an approach to predict energies using a convolutional neural network-based machine learning model to automatically obtain key features from the electronic density of states (DOS). The model, DOSnet, is evaluated for a diverse set of adsorbates and surfaces, yielding a mean absolute error on the order of 0.1 eV. In addition, DOSnet can provide physically meaningful predictions and insights by predicting responses to external perturbations to the electronic structure without additional DFT calculations, paving the way for the accelerated discovery of materials and catalysts by exploration of the electronic space.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Metal–insulator transition tuned by oxygen vacancy migration across TiO2/VO2 interface

Abstract Oxygen defects are essential building blocks for designing functional oxides with remarkable properties, ranging from electrical and ionic conductivity to magnetism and ferroelectricity. Oxygen defects, despite being spatially localized, can profoundly alter global properties such as the crystal symmetry and electronic structure, thereby enabling emergent phenomena. In this work, we achieved tunable metal–insulator transitions (MIT) in oxide heterostructures by inducing interfacial oxygen vacancy migration. We chose the non-stoichiometric VO 2-δ as a model system due to its near room temperature MIT temperature. We found that depositing a TiO 2 capping layer on an epitaxial VO 2 thin film can effectively reduce the resistance of the insulating phase in VO 2 , yielding a significantly reduced R OFF /R ON ratio. We systematically studied the TiO 2 /VO 2 heterostructures by structural and transport measurements, X-ray photoelectron spectroscopy, and ab initio calculations and found that oxygen vacancy migration from TiO 2 to VO 2 is responsible for the suppression of the MIT. Our findings underscore the importance of the interfacial oxygen vacancy migration and redistribution in controlling the electronic structure and emergent functionality of the heterostructure, thereby providing a new approach to designing oxide heterostructures for novel ionotronics and neuromorphic-computing devices.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Descriptors for Hydrogen Evolution on Single Atom Catalysts in Nitrogen-Doped Graphene

Single-atom catalysts (SACs) are a new research frontier in electrocatalysis such as in the hydrogen evolution reaction (HER). Recent theoretical and experimental studies have demonstrated that certain M–N–C (metal–nitrogen–carbon) based SACs exhibit excellent performance for HER. Here we report a new approach to tune HER activity for SACs by changing the size and dimensionality of the carbon substrate while maintaining the same coordination environment. In this work, we screen the 3d, 4d, and 5d transition metal SACs in N-doped 2D graphene and nanographenes of several sizes for HER using first-principles density functional theory (DFT). Nanographenes containing V, Rh, and Ir are predicted to have significantly enhanced HER activity compared to their 2D graphene counterparts. We turn to machine learning to accurately predict the free energy of hydrogen adsorption (ΔGH) based on various descriptors and compressed sensing to identify key descriptors for activity, which can be used to further screen for additional candidates.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Hydrogen in Nanocatalysis

Hydrogen is ubiquitous in catalysis. It is involved in many important reactions such as water splitting, N 2 reduction, CO 2 reduction, and alkane activation. In this Perspective, we focus on the hydrogen atom and follow its electron as it interacts with a catalyst or behaves as part of a catalyst from a computational point of view. In this work, we present recent examples in both nanocluster and solid catalysts to elucidate the parameters governing the strength of the hydrogen–surface interactions based on site geometry and electronic structure. We further show the interesting behavior of hydride in nanometal and oxides for catalysis. Overall, the key take-home messages are: (1) the in-the-middle electronegativity and small size of hydrogen give it great versatility in interacting with active sites on nanoparticles and solid surfaces; (2) the strength of hydrogen binding to an active site on a surface is an important descriptor of the chemical and catalytic properties of the surface; (3) the energetics of the hydrogen binding is closely related to the electronic structure of the catalyst; (4) hydrides in nanoclusters and oxides and on surfaces offer unique reactivity for reduction reactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Integrated Evaporator for Efficient Solar-Driven Interfacial Steam Generation

Solar-driven interfacial steam generation is a promising technique for clean water production as it can minimize thermal loss by localizing solar-to-heat conversion at the air/liquid interface. Here we report an integrated solar-evaporator by partially growing two-dimensional polypyrrole microsheets within a melamine foam through chemical vapor polymerization. These microsheets can induce multiple light reflections within the foam, enable omnidirectional light absorption, provide abundant surfaces to promote heat transfer, and achieve spatially-defined hydrophobicity to facilitate vapor escape. Meanwhile, the inherent hydrophilicity of the bottom part of the foam promotes spontaneous upward water transport and suppresses heat loss. The composite foam exhibits an excellent apparent evaporation rate of ~2 kg/(m 2 ·h) and solar-to-vapor efficiency of ~91%. Here, the combined advantages of large surface area, high efficiency, low cost, all weather application, excellent durability, and scalable manufacturing make our integrated design promising for fabricating large-scale solar steam generation systems that are suitable for practical clean water production.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Electronic band contraction induced low temperature methane activation on metal alloys

The catalytic conversion of methane under mild conditions is an appealing approach to selectively produce value-added products from natural gas. Catalysts which can chemisorb methane can potentially overcome challenges associated with its high stability and achieve facile activation. Although transition metals can activate C–H bonds, chemisorption and low-temperature conversion remain elusive on these surfaces. The broad electronic bands of metals can only weakly interact with the methane orbitals, in contrast to specific transition metal oxide and supported metal cluster surfaces which are now recognized to form methane σ-complexes. Here, we report methane chemisorption can, remarkably, occur on metal surfaces via electronic band contraction and localization from metal alloying. From a broad screening including single atom and intermetallic alloys in various substrates, we find early transition metals as promising metal solutes for methane chemisorption and low-temperature activation. These findings demonstrate a combinatorial diversity of possible candidates in earth abundant metal alloys with this attractive catalytic behavior.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗