A5063093801- Catalytic Processes in Materials Science
- Electrocatalysts for Energy Conversion
- Machine Learning in Materials Science
- Catalysis and Oxidation Reactions
- Nanomaterials for catalytic reactions
- Catalysis and Hydrodesulfurization Studies
- Silicon and Solar Cell Technologies
- Thin-Film Transistor Technologies
- Catalysis for Biomass Conversion
- Catalysts for Methane Reforming
- Advanced Chemical Physics Studies
- Ammonia Synthesis and Nitrogen Reduction
- Polyoxometalates: Synthesis and Applications
- Diamond and Carbon-based Materials Research
- Silicon Nanostructures and Photoluminescence
- Advanced Photocatalysis Techniques
- Advanced Battery Materials and Technologies
- Electron and X-Ray Spectroscopy Techniques
- Biochemical and Molecular Research
- Asymmetric Hydrogenation and Catalysis
- Mesoporous Materials and Catalysis
- Semiconductor materials and interfaces
- Nanocluster Synthesis and Applications
- Enzyme Structure and Function
- HIV/AIDS drug development and treatment
University of California, Los Angeles
2000-2025
University of California System
1999-2025
Chongqing University
2022-2025
Beijing National Laboratory for Molecular Sciences
2013-2016
Peking University
2011-2016
State Key Laboratory of Rare Earth Materials Chemistry and Application
2015-2016
Ames National Laboratory
2014
Iowa State University
2014
We report an efficient, highly selective, and low temperature graphene-catalyzed reaction process for one-step oxidation of benzene to phenol with hydrogen peroxide as the oxidant. The chemically converted graphene (CCG) from small graphite was used catalyst. conversion reaches 18%, being sole product. catalyst reusable very stable. By XPS, C K-edge X-ray absorption spectra, benzene-TPD, kinetic measurements, it concluded that moderate H2O2 activation rate, good adsorption ability, balanced...
Unlike nanostructured metal catalysts, supported single-atom catalysts (SACs) contain only atomically dispersed atoms, hinting at much more pronounced metal–support effects. Herein, we take a series of polyoxometalate-supported Pt as examples to quantitatively investigate the stability atoms on oxide supports and how Pt–support interaction influences catalytic performance. For this entire series, show that prefer stay 4-fold hollow site one polyoxometalate molecule least adsorption energy...
Abstract The sluggish electrochemical kinetics of sulfur species has impeded the wide adoption lithium-sulfur battery, which is one most promising candidates for next-generation energy storage system. Here, we present electronic and geometric structures all possible construct an diagram to unveil their reaction pathways in batteries, as well molecular origin kinetics. By decoupling contradictory requirements accelerating charging discharging processes, select two pseudocapacitive oxides...
Reactivity studies on catalytic transition metal clusters are usually performed a single global minimum structure. With the example of Pt13 cluster under pressure hydrogen, we show from first-principle calculations that low energy metastable structures can play major role for reactivity and hence consideration structure alone severely underestimate activity. The catalyst is fluxional with an ensemble energetically accessible at reaction conditions. A modified genetic algorithm proposed to...
In the context of arenes generated from bioresources, a hydrothermally stable catalyst Ru/HZSM-5 is reported for quantitative conversion lignin-derived phenol, anisole, guaiacols, and syringols into bioaromatic hydrocarbons in one-pot aqueous-phase process moderate conditions (240 °C, 2 bar H<sub>2</sub>), with high carbon balance 98.6%.
Fischer–Tropsch synthesis (FTS) is an important catalytic process for liquid fuel generation, which converts coal/shale gas/biomass-derived syngas (a mixture of CO and H2) to oil. While FTS thermodynamically favored at low temperature, it desirable develop a new system that could allow working relatively reaction temperature. In this article, we present one-step hydrogenation–reduction route the Pt–Co nanoparticles (NPs) were found be excellent catalysts aqueous-phase 433 K. Coupling with...
Abstract Heteronuclear Au–Pd nanoparticles were prepared and immobilized in the functionalized ionic liquid [C 2 OHmim][NTf ]. The structural electronic properties of characterized by a range techniques surface was found to be enriched Pd. Moreover, extent Pd enrichment is easily controlled varying ratio Au salts used synthesis. heteronuclear effective catalysts dehalogenation reactions with no activity observed for pure only limited nanoparticles. may attributed charge transfer from...
Sub-nanometer metal oxide clusters are very important materials that widely used, for example, in catalysis or electronic devices such as sensors. Hence, it is critical to understand the atomic structures and properties of sub-nanometer under a reactive gas environment, O2. We consider here experimentally accessible precise-size Cu (Cu4) supported on partially hydroxylated amorphous alumina show can access, catalytic conditions at high temperature pressure O2, large ensemble oxidized...
Heterogeneous thermocatalytic hydrogenation is widely believed to occur via co-adsorption of H2 and other reactants, but in aqueous phase an ionic or electrochemical mechanism was also proposed. Herein, we conduct 4-nitrophenol unbiased H-cell, where the substrate are separately supplied into two chambers connected by a proton exchange membrane, comparison with same reaction single cell which co-fed. Based on observation almost identical performance between H-cell cell, conclude that not...
Data-driven machine learning force fields (MLFs) are more and popular in atomistic simulations exploit methods to predict energies forces for unknown structures based on the knowledge learned from an existing reference database. The latter usually comes density functional theory calculations. One main drawback of MLFs is that physical laws not incorporated models, instead, designed be very flexible simulate complex quantum chemistry potential energy surface (PES). In general, have poor...
Alumina supported Pt nanoclusters under a hydrogen environment play crucial role in many heterogeneous catalysis applications. We conducted grand canonical genetic algorithm simulations for Pt8 clusters gas to study the intracluster, cluster-support, and cluster-adsorbate interactions. Two alumina surfaces, α-Al2O3(0001) γ-Al2O3(100), two conditions, T = 600 °C, pH2 0.1 bar 25 1.0 bar, were considered corresponding low high chemical potential μH, respectively. The free energy ensemble of is...
Abstract Single‐atom catalysts (SACs) have become a prominent theme in heterogeneous catalysis, not least because of the potential fundamental insight into active sites. The desired level understanding, however, is prohibited due to inhomogeneity most supported SACs and lack suitable tools for structure–activity correlation studies with atomic resolution. Herein, we describe potency electrospray ionization mass spectrometry (ESI‐MS) study molecularly defined on polyoxometalates catalytic...
Although there is evidence that catalytic active sites can restructure under reaction conditions, their optimal reconstruction to provide the lowest activation barrier still unclear. Here, we show with methane on supported Pt clusters and by an explicit sampling of cluster configurations at transition state important restructuring required reach most state. The capability reconstruct, simultaneously C–H dissociation, a key aspect for activity. We underline two types reconstructions,...
ConspectusThe rationale of the catalytic activity observed in experiments is a crucial task fundamental catalysis studies. Efficient catalyst design relies on an accurate understanding origin at atomic level. Theoretical studies have been widely developed to reach such scale activity. Current theories ascribe geometric and electronic structure active site, which geometrical effects are derived from equilibrium geometry sites characterizing static property catalyst; however catalysts,...
X-ray absorption near edge structure (XANES) spectroscopy is widely used for operando catalyst characterization. We show that, highly fluxional supported nanoclusters, the customary extraction of oxidation state metal from XANES data by fitting to bulk standards questionable. The signatures as well apparent such clusters arise a complex combination many factors, and not only chemical composition in reaction conditions (e.g., oxygen content oxidizing atmosphere). thermally accessible...
Abstract One key goal of heterogeneous catalysis study is to understand the correlation between catalyst structure and its corresponding catalytic activity. In this review, we focus on recent strategies synthesize well-defined Fischer-Tropsch synthesis (FTS) nanostructured catalysts their performance in FTS. The development those promising highlights potentials materials unravel complex dynamic reaction mechanism, particularly under situ conditions. crucial factors associated with...
In traditional hydrogenation, where H2 and substrates with unsaturated bonds are activated on the same catalyst (contact mode), competitive hydrogenation of multiple reducible groups often occurs. We employ an unbiased H-cell for selective nitro group when present. The setup spatially separates nitroarenes into two chambers connected by a proton-exchange membrane, thus adding barriers Langmuir–Hinshelwood-type mechanism that is common in thermocatalytic hydrogenation. Through unique...
Propylene oxide, a key commodity of the chemical industry for wide range consumer products, is synthesized through sequential propane dehydrogenation and epoxidation reactions. However, lack direct catalytic route from to propylene oxide reduces efficiency represents major challenge catalysis science. Herein, we report discovery highly active selective catalyst, made alumina-supported subnanometer copper clusters, which can directly convert at temperatures as low 150 °C. Moreover, higher...
Aside from activity and selectivity, catalyst stability is a key focus in heterogeneous catalysis research. While sintering of metal species has been considered the primary cause for deactivation catalysts, our study reveals that loss at low reaction temperatures CeO2‐supported Pt (Pt/CeO2) catalysts propane oxidation due to dispersion ensemble sites (nanoclusters) their subsequent operando conversion into single atoms under conditions. These single‐atom exhibit reactivity act as spectators...
Aside from activity and selectivity, catalyst stability is a key focus in heterogeneous catalysis research. While sintering of metal species has been considered the primary cause for deactivation catalysts, our study reveals that loss at low reaction temperatures CeO2‐supported Pt (Pt/CeO2) catalysts propane oxidation due to dispersion ensemble sites (nanoclusters) their subsequent operando conversion into single atoms under conditions. These single‐atom exhibit reactivity act as spectators...
Achieving a precisely understanding of the active site structure has long been an ultimate goal in fundamental heterogeneous catalysis research, yet it remains exceptionally challenging nanocluster catalysis. In Pt‐catalyzed dehydrogenation reactions, such as cyclohexane for liquid organic carriers (LOHC), previous efforts have provided valuable insights into size effects nanoclusters. However, optimal geometry sites remained elusive and, at times, contradictory. this study, we investigate...
Achieving a precisely understanding of the active site structure has long been an ultimate goal in fundamental heterogeneous catalysis research, yet it remains exceptionally challenging nanocluster catalysis. In Pt‐catalyzed dehydrogenation reactions, such as cyclohexane for liquid organic carriers (LOHC), previous efforts have provided valuable insights into size effects nanoclusters. However, optimal geometry sites remained elusive and, at times, contradictory. this study, we investigate...
Semihydrogenation of acetylene is an essential process in the ethylene industry for removing impurities and ensuring production polymer-grade ethylene. Atomically dispersed Cu catalysts have attracted significant attention due to their cost-effectiveness catalytic potential. However, inherently weak hydrogen dissociation ability results low activity, necessitating elevated reaction temperatures, which limit its practical applicability. To overcome this limitation, we design a Ru...