Catalysis

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Chemical Engineering, Carnegie Mellon University
Ph.D., Massachusetts Institute of Technology, 2015
Summary:

Our research work is focused on study of chemical, mechanical, electronic, and thermal properties of nano sized materials. At nano scales, entropic fluctuations become more prominent and materials behave differently. Our work is on capturing these effects in real devices and applications requires a range of modeling approaches, from hard theory (DFT and kinetics), to soft theory (continuum, statistical mechanics and molecular dynamics), and up through systems engineering approaches. There are various application to study such effect, including biomedical sensors (nanotube-based optical sensors)  and energy applications (CO2 to fuels, fuel cells, thermal catalysis). Following are our major projects:

  • Controlling selectivity of nanoscale interfaces with co-adsorbates and soft functionalizations
  • Machine-learning based approaches to accelerate materials screening
  • Bayesian methods for complex reaction mechanism reduction and elucidation
Most Cited Publications
  1. "Molecular recognition using corona phase complexes made of synthetic polymers adsorbed on carbon nanotubes." Jingqing Zhang, Markita P Landry, Paul W Barone, Jong-Ho Kim, Shangchao Lin, Zachary W Ulissi, Dahua Lin, Bin Mu, Ardemis A Boghossian, Andrew J Hilmer, Alina Rwei, Allison C Hinckley, Sebastian Kruss, Mia A Shandell, Nitish Nair, Steven Blake, Fatih Şen, Selda Şen, Robert G Croy, Deyu Li, Kyungsuk Yum, Jin-Ho Ahn, Hong Jin, Daniel A Heller, John M Essigmann, Daniel Blankschtein, Michael S Strano. Nature nanotechnology.
  2. "To address surface reaction network complexity using scaling relations machine learning and DFT calculations." Zachary W Ulissi, Andrew J Medford, Thomas Bligaard, Jens K Nørskov. Nature communications.
  3. "Diameter-dependent ion transport through the interior of isolated single-walled carbon nanotubes." Wonjoon Choi, Zachary W Ulissi, Steven FE Shimizu, Darin O Bellisario, Mark D Ellison, Michael S Strano. Nature communications.
  4. "Machine-Learning Methods Enable Exhaustive Searches for Active Bimetallic Facets and Reveal Active Site Motifs for CO2 Reduction." Zachary W Ulissi, Michael T Tang, Jianping Xiao, Xinyan Liu, Daniel A Torelli, Mohammadreza Karamad, Kyle Cummins, Christopher Hahn, Nathan S Lewis, Thomas F Jaramillo, Karen Chan, Jens K Nørskov. ACS Catalysis.
  5. "Active learning across intermetallics to guide discovery of electrocatalysts for CO 2 reduction and H 2 evolution." Kevin Tran, Zachary W Ulissi. Nature Catalysis.
Recent Publications
  1. "Multi-Task Machine Learning to Predict ORR Catalyst Descriptors and Performance across Surface Composition." Aini Palizhati, Seoin Back, Kevin Tran, Zachary Ulissi. 2019 AIChE Annual Meeting.
  2. "Graph Convolutional Machine Learning Methods for the Predictions of Adsorption and Thermochemistry and Surface Stability." Seoin Back, Aini Palizhati, Wen Zhong, Nianhan Tian, Kevin Tran, Zachary Ulissi. 2019 AIChE Annual Meeting.
  3. "Thermodynamic Techniques to Capture Non-Ideal Surfactant Assembly at Hard Nanoscale Interfaces." Junwoong Yoon, Zachary Ulissi. 2019 AIChE Annual Meeting.
  4. "Towards Predicting Intermetallics Surface Properties with High-Throughput DFT and Convolutional Neural Networks." Aini Palizhati, Wen Zhong, Kevin Tran, Seoin Back, Zachary W Ulissi. Journal of chemical information and modeling.
  5. "Convolutional neural network of atomic surface structures to predict binding energies for high-throughput screening of catalysts." Seoin Back, Junwoong Yoon, Nianhan Tian, Wen Zhong, Kevin Tran, Zachary W Ulissi. The journal of physical chemistry letters.
Department of Chemistry, Carnegie Mellon University
Ph.D. Chemistry, Northwestern University, Illinois, 2003
Summary:

Our research focuses on fundamental science and engineering questions motivated by the creation of materials on the nanometer scale (1 nm=10-9 m). Our research themes include the synthesis, characterization, and applications of nanoparticles (typically 1-100 nm in size). We are developing chemical methods for synthesizing well defined nanoparticles, including atomically precise nanoclusters, shape- and size-controlled nanocrystals, hybrid nano-architectures, and inorganic/polymer nanocomposites. In-depth characterizations of the physical and chemical properties of nanoparticles and self-assembled nanomaterials are carried out with microscopy and spectroscopy techniques, such as electron microscopy, atomic force microscopy, X-ray crystallography, steady-state and ultrafast spectroscopies, etc. We also develop applications of nanoparticles in areas of catalysis, optics, chemo- and bio-sensing, and photovoltaics, etc.

Selected Publications: 
  1. “Correlating second harmonic optical responses of single Ag nanoparticles with morphology”, Jin, R.; Jureller, J.E.; Kim, H.Y.; Scherer, N.F. J. Am. Chem. Soc.127, 12482 (2005).
  2. “Synthesis of open-ended, cylindrical Au-Ag alloy nanostructures on a Si/SiOx surface”, Zhang, H.; Jin, R.; Mirkin, C.A. Nano Lett., 4, 1493 (2004).
  3. “Thermally-induced formation of atomic Au clusters and conversion into nanocubes”, Jin, R.; Egusa, S.; Scherer, N.F. J. Am. Chem. Soc.126, 9900 (2004).
  4. “Controlling anisotropic nanoparticle growth through plasmon excitation”, Jin, R.; Cao, Y.W.;  Hao, E.; Metraux, G.S.; Schatz, G.C.; Mirkin, C.A.; Nature425, 487 (2003).
  5. “Raman dye-labeled nanoparticle probes for proteins”, Cao, Y.C.; Jin, R.; Nam, J.M.; Thaxton, C.S.; Mirkin, C.A. J. Am. Chem. Soc.125, 14676 (2003).
Most Cited Publications
  1. "Photoinduced conversion of silver nanospheres to nanoprisms", R Jin, YW Cao, CA Mirkin, KL Kelly, GC Schatz, JG Zheng, science, 294, 1901 (2001).
  2. "Nanoparticles with Raman spectroscopic fingerprints for DNA and RNA detection", YWC Cao, R Jin, CA Mirkin, Science 297, 1536 (2002).
  3. "Controlling anisotropic nanoparticle growth through plasmon excitation", R Jin, YC Cao, E Hao, GS Métraux, GC Schatz, CA Mirkin, Nature 425, 487 (2003).
  4. "Correlating the crystal structure of a thiol-protected Au25 cluster and optical properties", M Zhu, CM Aikens, FJ Hollander, GC Schatz, R Jin, Journal of the American Chemical Society 130 , 5883 (2008).
  5. "What controls the melting properties of DNA-linked gold nanoparticle assemblies?", R Jin, G Wu, Z Li, CA Mirkin, GC Schatz, Journal of the American Chemical Society 125, 1643 (2003).
Recent Publications
  1. "Rational construction of a library of M29 nanoclusters from monometallic to tetrametallic." Kang, Xi, Xiao Wei, Shan Jin, Qianqin Yuan, Xinqi Luan, Yong Pei, Shuxin Wang, Manzhou Zhu, and Rongchao Jin. Proceedings of the National Academy of Sciences 116, no. 38 (2019): 18834-18840.
  2. "New Advances in Atomically Precise Silver Nanoclusters." Yang, Jie, and Rongchao Jin. ACS Materials Letters (2019).
  3. "Understanding the Solubility Behavior of Atomically Precise Gold Nanoclusters." Cowan, Michael J., Tatsuya Higaki, Rongchao Jin, and Giannis Mpourmpakis. The Journal of Physical Chemistry C 123, no. 32 (2019): 20006-20012.
  4. "Theoretical Prediction of Optical Absorption and Emission in Thiolated Gold Clusters." Day, Paul N., Ruth Pachter, Kiet A. Nguyen, and Rongchao Jin. The Journal of Physical Chemistry A 123, no. 30 (2019): 6472-6481.
  5. "Gold Nanoclusters: Bridging Gold Complexes and Plasmonic Nanoparticles in Photophysical Properties,"  M Zhou, C Zeng, Q Li, T Higaki, and R JinNanomaterials 9.7 (2019)

Computational Study of Ni-Catalyzed C−H Functionalization: Factors That Control the Competition of Oxidative Addition and Radical Pathways

  • By Aude Marjolin
  • 2 August 2017

To guide the development of a more diverse set of Ni-catalyzed C−H bond functionalizations, a thorough understanding of the mechanisms, reactivity, and selectivity of these reactions is required. Peng Liu and his student Humair Omer have undertaken a computational study of the functionalization of the C−H bonds in molecules that contain the N,N-bidentate directing group with Ni catalyst and various coupling  partners, e.g. phenyl iodide (Ph−I), which has been published in the July 26, 2017 issue of the Journal of the American Chemical Society.

Giannis Mpourmpakis Lands Cover of Catalysis Science & Technology

  • By Aude Marjolin
  • 31 May 2017

Research from Giannis Mpourmpakis' group was recently featured on the inside front cover of the Royal Society of Chemistry journal, Catalysis Science & Technology. The team’s investigations into a more energy-efficient catalytic process to produce olefins--the building blocks for polymer production--could impact potential applications in diverse technology areas from green energy and sustainable chemistry to materials engineering and catalysis. 
 

Structure-Activity Relations in Heterogeneous Catalysis – A View from Computational Chemistry

Speaker(s): 
Phillipe Sautet
Dates: 
Friday, March 17, 2017 - 9:30am to 10:30am

The understanding of the catalytic properties of nanoparticle catalysts and the design of optimal composition and structures demands fast methods for the calculation of adsorption energies. By exploring the adsorption of O and OR (R=OH, OOH, OCH3) adsorbates on a large range of surface sites with 9 transition metals, we propose new structure sensitive scaling relations between the adsorption energy of two adsorbates that are valid for all metals and for all surface sites.1 This opens the way for a new class of activity volcano plots where the descriptor is not an energy...

In Silico Searches for Efficient Renewable Energy Catalysts Through Chemical Compound Space

Speaker(s): 
John Keith
Dates: 
Friday, February 3, 2017 - 11:30am to 12:30pm

This talk will provide an overview of our group’s work using both standard and atypical high-performance computational chemistry modeling to elucidate atomic scale reaction mechanisms of catalytic reactions. I will introduce our toolkit of in silico methods for accurately modeling solvating environments and realistic nanoscale architectures. I will then present how these methods can be used for predictive insights into chemical and material design. The talk will then summarize our progress in unraveling reaction mechanisms for 1) electrochemical CO2 reduction with...

Department of Chemical and Petroleum Engineering, University of Pittsburgh
Ph.D., Theoretical and Computational Chemistry, University of Crete, 2006
Summary:

My research expertise is interdisciplinary, blending concepts and techniques from Chemistry, Physics, Materials Science and Chemical Engineering. I use theory and computation to investigate the physicochemical properties of nanomaterials with potential applications in diverse nanotechnological areas, ranging from energy generation and storage, to materials design, nanoparticle growth, magnetism, and catalysis.

In the Computer-Aided Nano and Energy Lab (C.A.N.E.LA.), led by Prof. Mpourmpakis, we use theory and computation to investigate the physicochemical properties of nanomaterials with potential applications in diverse nanotechnological areas, ranging from green energy generation and storage to materials engineering and catalysis. Our laboratory core expertise lies on "ab-initio" electronic-structure theoretical calculations. We develop structure-activity relationships and apply multiscale tools to elucidate complex chemical processes that take place on nanomaterials. Ultimately, we design novel nanostructures with increased, molecular-level precision and tailored multifunctionality. 

Most Cited Publications
  1. "SiC nanotubes: a novel material for hydrogen storage." Giannis Mpourmpakis, George E Froudakis, George P Lithoxoos, Jannis Samios. Nano letters.
  2. "Carbon nanoscrolls: a promising material for hydrogen storage." Giannis Mpourmpakis, Emmanuel Tylianakis, George E Froudakis. Nano letters.
  3. "Correlating particle size and shape of supported Ru/γ-Al2O3 catalysts with NH3 decomposition activity." Ayman M Karim, Vinay Prasad, Giannis Mpourmpakis, William W Lonergan, Anatoly I Frenkel, Jingguang G Chen, Dionisios G Vlachos. Journal of the American Chemical Society.
  4. "Why boron nitride nanotubes are preferable to carbon nanotubes for hydrogen storage?: An ab initio theoretical study." Giannis Mpourmpakis, George E Froudakis. Catalysis today.
  5. "DFT study of furfural conversion to furan, furfuryl alcohol, and 2-methylfuran on Pd (111)." Vassili Vorotnikov, Giannis Mpourmpakis, Dionisios G Vlachos. Acs Catalysis.
Recent Publications
  1. "Identification of Stable Bimetallic Nanoclusters Via a Mathematical Optimization Framework." Xiangyu Yin, Natalie M Isenberg, Michael G Taylor, Giannis Mpourmpakis, Chrysanthos E Gounaris. 2019 AIChE Annual Meeting.
  2. "Generalized Adsorption Models on Metal Nanoparticles." James Dean, Michael G Taylor, Giannis Mpourmpakis. 2019 AIChE Annual Meeting.
  3. "Prediction of Nanoparticles Size Distribution: The Effects of Ligand Surface Coverage and Nanoparticle Size in Altering the Kinetics of Surface Growth." Saeed Mozaffari, Wenhui Li, Mudit Dixit, Giannis Mpourmpakis, Ayman M Karim. 2019 AIChE Annual Meeting.
  4. "Understanding Mixing Behavior of Bimetallic Nanoparticles through Genetic Algorithm Modeling." Michael Cowan, James Dean, Giannis Mpourmpakis. 2019 AIChE Annual Meeting.
  5. "Understanding Oligomerization Steps in Zeolite Growth Using Density Functional Theory." Emily Freeman, Jeffrey D Rimer, Giannis Mpourmpakis. 2019 AIChE Annual Meeting.

Oxide-metal Interfaces as Active Sites for Acid-base Catalysis: Oxidation State of Nanocatalyst Change with Decreasing Size, Conversion of Heterogeneous to Homogeneous Catalysis, Hybrid Systems

Speaker(s): 
Gábor A. Somorjai
Dates: 
Friday, May 6, 2016 - 9:30am to 10:30am

When metal nanoparticles are placed on different mezoporous or microporous oxide supports the catalytic turnover rates and selectivities markedly change.  The charge flow between the metal and the oxide ionizes the adsorbed molecules at the oxide-metal interfaces and alters the catalytic chemistry (acid-base catalysis). 

The oxidation state of metal nanoparticles becomes less metallic and assume higher oxidation states with decreasing size.  The...

Metal Nanocatalysts, Their Synthesis and Size Dependent Covalent Bond Catalysis: Instrumentation for Characterization under Reaction Conditions

Speaker(s): 
Gábor A. Somorjai
Dates: 
Thursday, May 5, 2016 - 5:00pm to 7:00pm

Colloidal chemistry is used to control the size, shape and composition of metal nanoparticles usually in the 1-10 nm range.  In-situ methods are used to characterize the size, structure (electronic and atomic), bonding, composition and oxidation states under reaction conditions.  These methods include sum frequency generation nonlinear optical spectroscopy (SFG), ambient pressure X-ray photoelectron spectroscopy (APXPS) and high pressure scanning tunneling...

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