Research

●    Industrial Catalysis

●    Photocatalysis

●    Electrocatalysis

●    Interfacial & Surface Catalysis

●    Batteries

Industrial Catalysis

We are interested in designing nanostructured materials to produce hydrogen from green and renewable resources. Hydrogen is the most abundant element on the planet making up three-quarters of matter, with most of this available hydrogen tied up in molecules such as oxygenates and water. Hydrogen has a high energy content per unit weight (120.7 kJ/g). The widespread use of H2 as an energy carrier requires the development of efficient and renewable methods for its production.

1. Hydrogen production via steam reforming 

Reforming is a chemical process where hydrogen-containing compounds react with steam, oxygen, or both into hydrogen-rich gas stream. Steam reforming is one of the most widely used technologies for hydrogen production, and achieved by reaction over a catalyst at elevated temperatures. The steam reforming of biomass-derived oxygenates draws much attention as a sustainable and potentially carbon-neutral process. 
CxHyOz + H2O --> nCO + mCO2 + pH2

The initial step in steam reforming is dissociative adsorption of oxygenates on the metal sites of the catalysts; the formed surface species subsequently reacts with water\hydroxyls that are, in most cases, activated on oxide supports. 
Our approach to understand this process consists of (1) design and fabrication of nanostructured catalysts that can efficiently convert oxygenates (e.g., bio-derived alcohols) to hydrogen; (2) understanding the roles of different surface active sites in the catalytic reforming processes; (3) figuring out the reactivity-structure correlations in reforming reactions; (4) fundamental mechanistic insights into the origin of deactivation on metal-based catalysts; (5) understanding of differences and similarities of the reforming process of mono- and poly-alcohols; and (6) exploration and manipulation of reaction pathways (e.g., the water-gas shift reaction and methanation) involved in the system. Current projects include:
●Steam reforming of bio-derived alcohols (e.g., ethanol, ethylene glycerol, and glycerin) on
  supported metal clusters
●Promoting the resistance to sintering and coke deposition by rational catalyst design
●Studying reforming reactions on surface by ultra-high vacuum surface techniques
●Mechanistic investigations of steam reforming of methanol/ethanol on metal surfaces via DFT calculations
●Process intensification and optimization

2. Propane dehydrogenation to propylene

Ethylene Propylene is an important feedstock employed in the production of a vast array of chemicals (e.g., polypropylene, acrylonitrile). Owing to the extensive demand of propylene, propane dehydrogenation (PDH) has acquired considerable attention and massive commercial applications in recent years. Pt is the only noble metal utilized in commercial PDH processes because of its superior activation of paraffinic C-H bonds and low activity to C-C cleavage. However, catalyst deactivation due to coke formation and generation of lighter hydrocarbons caused by C-C cleavage remain challenging. We aim to develop a range of efficient Pt-based catalysts possessing high desired-product selectivity and eminent anti-coking capability. A set of research has been conducted to achieve our goal:
●Rational design and fabrication of effective Pt-based catalysts (e.g., PtCu/Al2O3, Pt/TiO2-Al2O3) and alternative non-noble metal oxide based catalysts
●Exploration of the nanostructure of designed catalysts and understanding the reaction pathways and functional mechanism of Pt-based catalysts
●Mechanistic studies of PDH and/or catalyst deactivation via DFT calculations

3. Selective oxidation of alcohols over solid acid catalysts 

The selective oxidation of alcohols is an important step in synthesizing many valuable intermediates for the food, fragrance and pharmaceutical industries. This chemistry traditionally uses stoichiometric amounts of hazardous and toxic oxidants such as peroxides and chromates and generates large quantities of harmful waste. We aimed to develop a range of supported transition metals and oxides which are effective for the aerobic selective oxidation of alcohols to the corresponding aldehydes, ketenes, and esters under mild conditions. We have employed a number of advanced characterization tools to look at surface reaction and pathways of the reaction and the role that metal, oxide, and their interface play. Current projects include:
●Selective oxidation of methanol to dimethoxymethane over bifunctional hybrid oxides
●Mechanism and kinetics of selective oxidation of alcohols on supported metal clusters

Photocatalysis

1. Hydrogen production via photoelectrochemical water splitting

Hydrogen generation from photoelectrochemical (PEC) water splitting represents a holy grail in chemistry and energy science. Compared to bulk semiconductors, nanostructured photoelectrodes  could potentially improve the solar-to-hydrogen conversion efficiency due to their large surface area and short diffusion length for minority carriers. We conduct a new line of research directed towards (1) designing PEC devices using dense and vertically aligned metal oxide nanowire arrays as photoanodes, and (2) creating novel hybrid semiconductors with high solar-to-hydrogen conversion efficiency. 
Current projects include:
●Rational design of self-assembled colloids as photoanodes
●Hierarchical bottom-up approach to a new generation of photoanodes
●Fabrication of nanostructured photoanodes via reactive angle deposition

2. Fuel generation by photocatalytic CO2 reduction

Utilizing the abundant solar energy to convert CO2 into fuels such as methane or methanol could provide a convenient means of energy storage and positively impact the global carbon balance. There remain great challenges in the selectivity of photogenerated electrons for CO2 reduction in the presence of H2O. We are interested in (1) designing online detection devices for CO2 photoreduction (2) creating novel semiconductors with high conversion efficiency and selectivity for CO2 reduction. Current projects include:
●Rational design of mesoporous photoanodes to achieve a high adsorption ability of CO2
●Investigation on the relationship between selectivity and CO2 reduction co-catalyst
●Surface modification of the photocatalysts to reduce the activation energy or overpotential for CO2 reduction

3. Well-controlled nanocatalysts for fuel cell-related reactions

Fuel cells are receiving extensive attention owing to their numerous advantages, including high efficiency, high specific energy density, and low pollution. The performance of a fuel cell is directly determined by the activity of its catalysts. Among various types of catalysts, the platinum-group metals (PGMs) are broadly used as the key catalysts in several kinds of fuel cells, such as proton exchange membrane fuel cell (PEMFC), direct formic acid fuel cell (DFAFC) and direct methanol fuel cell (DMFC). However, their low abundance in the earth’s crust and their ever increasing prices have created a major roadblock for the large-scale commercialization of PGMs-related fuel cells. We aimed to develop more active catalysts through tuning the utilization efficiency, exposed surfaces and composition of Pt- or Pd- based nanocrystals. The mechanism for relationship between the well-controlled nanocrystals and their performance in fuel cell-related electrocatalytic reactions are carefully investigated via DFT calculations. Current projects include:
●Shape-controlled synthesis of Pd-Au alloy with high-energy surfaces
●Preparation of Pt-based core-shell structure to achieve a high mass activity towards oxidation reduction reaction
●Rational design of Pt-free catalysts for oxidation reduction reaction

4. Selective oxidation of alcohols via photocatalysis

Selective oxidation of alcohols with molecular oxygen (O2) is an essential process for the synthesis of various chemicals. Traditionally, toxic oxidants or harsh conditions are needed during the oxidation of alcohols. The photocatalytic selective oxidation provides an alternative green and sustainable process for the chemical synthesis under mild conditions. We aim to develop photocatalysts with wide absorption range of light and efficient separation of electrons and holes. In addition, we also work on the mechanism illustration of selective oxidation via various photocatalysts, which is helpful to design catalysts with high efficiency rationally. Current project includes:
●Photocatalytic oxidation of benzyl alcohol over metal-oxides with expanded absorption range of irradiation
●Mechanism of photocatalytic oxidation over various photocatalysts
●Photocatalytic oxidation over oxides with oxidation and reduction cocatalysts which could improve the separation of electrons and holes.

Electrocatalysis

1. Electrocatalytic CO2 Reduction

Facing the shortage of fossil resources and the environmental issues caused by excessive CO2 emission, it is of great significance to develop strategies to utilize CO2 in a sustainable manner. We are investigating electrocatalytic CO2 reduction technologies to synthesize carbon-neutral chemical fuels and feedstocks using renewable electricity. We perform theoretical calculations to screen novel catalysts. The results of theoretical calculations guide the synthesis of catalysts with finely tuned reaction sites and high performance. Based on the development of outstanding electrocatalysts, we optimize the integrating methods of the catalysts into electrolyzers. We design gas diffusion electrodes and membrane electrode assemblies to enable CO2 reduction to achieve industrially relevant performance metrics.
Current projects include:
●Synthesis of highly active electrocatalysts to convert CO2 into chemical feedstocks (e.g., ethylene, syngas) and renewable fuels (e.g., methane, methanol, and ethanol)
●Investigation of electrocatalysts and manipulation of multi-physics fields within CO2 reduction devices
●Design of novel reactors to break mass transfer limitations for the industrialization of CO2 reduction systems

2. Electrochemical Production of Green Hydrogen

Green hydrogen is the key to build up a carbon-neutral society. Electrochemical water splitting by renewable electricity is a promising way to obtain green hydrogen. We focus on the synthesis of inexpensive transition metal-based electrocatalysts to replace precious metal electrocatalysts for water splitting. Meanwhile, we study the direct electrolysis of seawater and design stable and corrosion-resistant catalysts to produce hydrogen. In order to improve the current density and stability of water splitting systems, our team also investigate the behavior of bubbles in the electrolyte. By regulating the fluid flow pattern, we seek to reduce the ohmic resistance drop, improve the energy conversion efficiency, and eventually achieve the long-term operation of the hydrogen production devices.
Current projects include:
●Electrochemical oxygen evolution reaction catalyzed by inexpensive transition metal-based electrocatalysts
●Corrosion-resistant catalysts for the electrolysis of seawater
●Modulation of the growth and desorption behaviors of bubbles

Interfacial & Surface Catalysis

1. Mechanistic study by computational chemistry

Exploration of catalyst reaction mechanisms is of fundamental importance in improving known catalysts or designing new catalysts. In recent years, a great number of the catalytic processes have been computationally studied using Density Functional Theory (DFT) calculations and other relative methods. Along with the development of computational chemistry methods, parallel computing and high-performance computing cluster, state-of-the-art computational chemistry researches not only uncover the essence of a known catalytic process, but also are used as a fast and low-cost pre-screening technic to assist new catalyst design.Currently, we are focusing on following projects

i. Mechanistic research on propane dehydrogenation to propylene: In order to gain deeper understanding of dehydrogenations of saturated hydrocarbons, we selected propane dehydrogenation reactions as our model reactions, which was catalyzed by Pt based catalyst. To facilitate determination of systematic trends in the propane dehydrogenationon Pt based catalyst, we will first investigate propane dehydrogenation on flat and stepped Pt and PtM alloy surfaces as well as interfaces of metal oxides, including MgO, Al2O3, and TiO2. They were selected for initial study as supports with at least one surface which matches the shape and size of the Pt(100) or Pt(111) surface. In a practical sense, the matched lattice dimensions provide a more uniform geometry between systems, thus facilitating initial development of correlations and Brønsted–Evans–Polanyi (BEP) relationships at the metal/support interfaces. By systematically permuting the alloy metal and nature of the substrates, we will establish correlations and reactivity patterns, including the development of BEP relationships. In the future, the analysis can be extended to other supported transition metal catalysts, and "volcano" relationships can be constructed between the predicted activity of different metal alloy/support structures and key catalytic parameters that are identified through the analysis.

ii. Development of Global Optimization Algorithm: One challenge to build a realistic catalyst model is to determining its most stable structure (global minimum) or set of lowest energy structures of a catalyst under reaction conditions. Although local minimum optimization technics have already been well developed, it could not guarantee the optimized structure to be the most stable one in case with complicated environment, like high adsorbate coverage, surface reconstruction, etc. Ideally, the global minimum can be located by exploring the whole potential energy surface with conducting numbers of local optimizations. We are interested in improvement of global optimization efficiency by reducing the number of local optimizations to obtain the desired global minimum with advanced computational algorithms like genetic algorithm, machine learning.

iii. Electrocatalysis of CO2 reduction: The insights of catalytic structures and exploration of candidate catalysts in our group mainly also focus on (photo)electrocatalysis for CO2 reduction (CO2RR). For example, atomic structure motifs for product-specific active sites on OD-Cu catalysts OD-Cu are detected by the molecular dynamic simulation with neural network (NN) potential. As for metal oxide, the surface defect was utilized to detect the regulatory factor for the catalytic performance. In detail, surface defects can control the adsorption strength of key intermediates of CO2RR by surface hydroxyl (Cu2O) or oxygen vacancies (SnOx), thereby providing theoretical guidance for improving the selectivity of target products. Our further analysis would continue to explore the influence on the reaction mechanisms around the regulation of surface morphology, electronic structure and extend to the model construction consistent with the realistic environment.

iv. Machine learning potentials: Recently, the data-driven ML technique is emerging as a useful tool and surrogate model to accelerate the time-consuming simulation. Machine learning potentials (MLP), which directly learns the potential surface from ab initio calculations, have been developed to act as an energy calculator with high accuracy while maintaining the large speedup. Using MLP as a surrogate model, not only the thermodynamics for active sites, the evaluation of kinetic properties like reaction rate can also be accelerated. MLP can significantly extend the spatial and time scale of atomistic simulations, providing more opportunities to simulate large-scale catalyst systems while maintaining high accuracy. Besides, MLP can accelerate enhanced sampling simulations to predict the long-time-scale surface reaction using ab initio calculation. In our group, we tend to develop and apply MLP to accelerate the time-consuming, large-scale, and long-term simulation of catalytic system.

Batteries

Current state of the art in battery technology significantly sacrifices high energy density, high power density and security. Energy storage devices such as advanced batteries, including Li-ion, Na-ion, K-ion batteries, lithium–sulfur batteries batteries, are important for portable electronics, vehicle electrification and smart grid. We develop novel materials including electrodes, electrolytes, binders, current collectors to address scientific problems, and improve the critical performance parameters related to energy storage such as energy density, power density, safety, cycle and calendar life and cost.
Current projects include:
●P-based anode for Li-ion, Na-ion, K-ion batteries
●Other Li-ion battery anodes: Si, Bi, Li
●Li-ion battery cathodes: metal oxides, sulfur
●Li-ion battery electrolytes: esters, ethers, high concentration salts
●Zn-ion battery: Zn metal anodes and metal oxides cathodes, respectively