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Zhang, Miao

Publications and source records attributed to Zhang, Miao.

6 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Unveiling Highly Sensitive Active Site in Atomically Dispersed Gold Catalysts for Enhanced Ethanol Dehydrogenation

Developing a desirable ethanol dehydrogenation process necessitates a highly efficient and selective catalyst with low cost. Herein, we show that the “complex active site” consisting of atomically dispersed Au atoms with the neighboring oxygen vacancies (Vo) and undercoordinated cation on oxide supports can be prepared and display unique catalytic properties for ethanol dehydrogenation. The “complex active site” Au–Vo–Zr 3+ on Au 1 /ZrO 2 exhibits the highest H 2 production rate, with above 37,964 mol H 2 per mol Au per hour (385 g H 2 $\text{g}^{-1}_{\text{Au}} \text{h}^{–1}$) at 350 °C, which is 3.32, 2.94 and 15.0 times higher than Au 1 /CeO 2 , Au 1 /TiO 2 , and Au 1 /Al 2 O 3 , respectively. Combining experimental and theoretical studies, we demonstrate the structural sensitivity of these complex sites by assessing their selectivity and activity in ethanol dehydrogenation. Our study sheds new light on the design and development of cost-effective and highly efficient catalysts for ethanol dehydrogenation. Fundamentally, atomic-level catalyst design by colocalizing catalytically active metal atoms forming a structure-sensitive “complex site”, is a crucial way to advance from heterogeneous catalysis to molecular catalysis. Finally, our study advanced the understanding of the structure sensitivity of the active site in atomically dispersed catalysts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Unveiling Highly Sensitive Active Site in Atomically Dispersed Gold Catalysts for Enhanced Ethanol Dehydrogenation

Developing a desirable ethanol dehydrogenation process necessitates a highly efficient and selective catalyst with low cost. Herein, we show that the “complex active site” consisting of atomically dispersed Au atoms with the neighboring oxygen vacancies (Vo) and undercoordinated cation on oxide supports can be prepared and display unique catalytic properties for ethanol dehydrogenation. The “complex active site” Au-Vo-Zr 3+ on Au 1 /ZrO 2 exhibits the highest H 2 production rate, with above 37,964 mol H 2 per mol Au per hour (385 g H 2 $g^{-1}_{Au}$ h -1 ) at 350 °C, which is 3.32, 2.94 and 15.0 times higher than Au 1 /CeO 2 , Au 1 /TiO 2 , and Au 1 /Al 2 O 3 , respectively. Combining experimental and theoretical studies, we demonstrate the structural sensitivity of these complex sites by assessing their selectivity and activity in ethanol dehydrogenation. Our study sheds new light on the design and development of cost-effective and highly efficient catalysts for ethanol dehydrogenation. Fundamentally, atomic-level catalyst design by colocalizing catalytically active metal atoms forming a structure-sensitive “complex site”, is a crucial way to advance from heterogeneous catalysis to molecular catalysis. In conclusion, our study advanced the understanding of the structure sensitivity of the active site in atomically dispersed catalysts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Structural evidence for intermediates during O 2 formation in photosystem II

In natural photosynthesis, the light-driven splitting of water into electrons, protons and molecular oxygen forms the first step of the solar-to-chemical energy conversion process. The reaction takes place in photosystem II, where the Mn 4 CaO 5 cluster first stores four oxidizing equivalents, the S 0 to S 4 intermediate states in the Kok cycle, sequentially generated by photochemical charge separations in the reaction center and then catalyzes the O–O bond formation chemistry. Here, we report room temperature snapshots by serial femtosecond X-ray crystallography to provide structural insights into the final reaction step of Kok’s photosynthetic water oxidation cycle, the S 3 →[S 4 ]→S 0 transition where O 2 is formed and Kok’s water oxidation clock is reset. Our data reveal a complex sequence of events, which occur over micro- to milliseconds, comprising changes at the Mn 4 CaO 5 cluster, its ligands and water pathways as well as controlled proton release through the hydrogen-bonding network of the Cl1 channel. Importantly, the extra O atom O x , which was introduced as a bridging ligand between Ca and Mn1 during the S 2 →S 3 transition disappears or relocates in parallel with Y z reduction starting at approximately 700 μs after the third flash. The onset of O 2 evolution, as indicated by the shortening of the Mn1–Mn4 distance, occurs at around 1,200 μs, signifying the presence of a reduced intermediate, possibly a bound peroxide.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2022

Spatiotemporal Graph Convolutional Networks for Earthquake Source Characterization

Abstract Accurate earthquake location and magnitude estimation play critical roles in seismology. Recent deep learning frameworks have produced encouraging results on various seismological tasks (e.g., earthquake detection, phase picking, seismic classification, and earthquake early warning). Many existing machine learning earthquake location methods utilize waveform information from a single station. However, multiple stations contain more complete information for earthquake source characterization. Inspired by recent successes in applying graph neural networks (GNNs) in graph‐structured data, we develop a Spatiotemporal Graph Neural Network (STGNN) for estimating earthquake locations and magnitudes. Our graph neural network leverages geographical and waveform information from multiple stations to construct graphs automatically and dynamically by adaptive message passing based on graphs' edges. Using a recent graph neural network and a fully convolutional neural network as baselines, we apply STGNN to earthquakes recorded by the Southern California Seismic Network from 2000 to 2019 and earthquakes collected in Oklahoma from 2014 to 2015. STGNN yields more accurate earthquake locations than those obtained by the baseline models and performs comparably in terms of depth and magnitude prediction, though the ability to predict depth and magnitude remains weak for all tested models. Our work demonstrates the potential of using GNNs and multiple stations for better automatic estimation of earthquake epicenters.

58 GEOSCIENCES↗
DOE OSTI2022

Capturing the sequence of events during the water oxidation reaction in photosynthesis using XFELs

Ever since the discovery that Mn was required for oxygen evolution in plants by Pirson in 1937 and the period-four oscillation in flash-induced oxygen evolution by Joliot and Kok in the 1970s, understanding of this process has advanced enormously using state-of-the-art methods. The most recent in this series of innovative techniques was the introduction of X-ray free-electron lasers (XFELs) a decade ago, which led to another quantum leap in the understanding in this field, by enabling operando X-ray structural and X-ray spectroscopy studies at room temperature. This review summarizes the current understanding of the structure of Photosystem II (PS II) and its catalytic centre, the Mn 4 CaO 5 complex, in the intermediate S i ( i = 0-4)-states of the Kok cycle, obtained using XFELs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗