- A wide-ranging suite of experimental and computation facilities are available for IMASC research, including shared facilities at Harvard and at IMASC partner institutions. While many of the specific facilities available reside in the laboratories of individual Senior Investigators (SIs), they are often shared and jointly used by the team. IMASC research has been using national facilities, such as synchrotrons and supercomputing facilities, with resources allocated based on proposals submitted to each facility. An overview of shared and individual facilities is provided below with more detail about the facilities in each of the Sr. Investigators lab follow.
- Funding from DOE was utilized strategically to build instrumentation for in situ interrogation of reactions and surfaces under catalytic conditions. We have invested in: (i) a Hummingbird gas-cell holder to image morphological changes on nanoporous catalyst surfaces, at atmospheric pressures, using the scanning and transmission electron microscopes (STEMs & TEMs) at Harvard. (ii) a custom-build X-ray absorption system that will be used to probe materials composition and intermediates on the surface under reaction conditions. (iii) An Agilent HPLC coupled to ATRIR and the combined instrumentation, available at Tufts, as a means of probing liquid reactions. In addition we are in the process of purchasing Ion-scattering set-up/XPS upgrade as a new capability. The IMASC equipment have started creating value to the overall center based on usage by a large number of PIs involved and wider availability.
Shared Experimental Facilities
- Center for Nanoscale Systems (CNS) at Harvard (http://www.cns.fas.harvard.edu)
- Center for Functional Nanomaterials (CFN, BNL) (https://www.bnl.gov/cfn/)
- Nanoscale Synthesis and Characterization Laboratory (NSCL) at Lawrence Livermore National Labs (https://pls.llnl.gov/resources/materials-science/nanoscale-synthesis-and...)
- Advanced Manufacturing Laboratory- Custom tools for directed synthesis of functional architectures at LLNL (https://engineering.llnl.gov/content/assets/docs/aml_brochureweb.pdf)
- DOE Synchrotron facilities: IMASC researchers have a track record of successful proposals for beam time at ALS(Berkeley) and NSLS II (via CFN). New proposals will be written as needed, including atSSRL (SLAC).
- Mass spectrometer facility at Harvard (https://massspec.fas.harvard.edu): This facility houses the following mass spectrometers: Agilent 6210 Time-of-FlightLC/MS, Waters Quattro micro GC/MS/MS, Waters Micro MX MALDI-TOF, Bruker MaxisImpact LC-q-TOF Mass Spectrometer, Agilent 6460 Triple Quadrupole Mass Spectrometerwith Agilent 1290 uHPLC (Two Systems in-House), UltrafleXtreme MALDI-TOF/TOF MassSpectrometer, Agilent 6550 q-TOF-NEW high resolution tandem mass spectrometer, Thermoq-Exactive Plus with Protein Mode-New
- NMR facilities at Harvard (Chemistry) are available for analysis of liquid phase reactions: The NMR Facility contains 8 NMR (Agilent DD2 600/(DD2-600); Varian- Unity/Inova500(I500), Unity/Inova500B (I500B), Unity/Inova500C (I500C), Mercury400 (M400),Mercury400B (M400B), Mercury300 (M300); Bruker - ElexSys E500 EPR (E500), Avance700 (A700), microTOFII ESI LCMS, Bruker ALPHA FT-IR and Quantum Design MPMS).
Facilities in individual SI labs and available to the broader community
- Facilities for single-crystal studies using surface science techniques are available atHarvard (Friend, Madix), Tufts (Sykes), Univ. of FL (Weaver) and BNL (see above for CFNand NSLS II). See below for details for each lab.
- Catalysis testing facilities, including flow reactors and transient pulsed experiments, areavailable at Harvard (Friend, Madix), Tufts (Flytzani-Stephanopoulos), and Frenkel (SUNY,Stony Brook)
- Materials Synthesis and Growth Facilities include wet chemical, colloidal assembly and3-D printing facilities at Harvard (Lewis, Aizenberg) and capability for synthesis of sol-gelmaterials and the Advanced Manufacturing Laboratory- Custom tools for directed synthesisof functional architectures at LLNL.
- Transient Analysis of Products (TAP) reactors are available (Madix, Harvard andRedekop, UiO) for transient pulse-response kinetic and mechanistic studies of catalyticreactions.
- Harvard University (Kaxiras and Kosinsky) : Odyssey cluster of the Harvard FAS Research Computing (18 nodes).
- UCLA : The Sautet group has co-sponsored the University shared computational cluster, Hoffman2,by acquiring 400 cores.
- University College London (Stamatakis) : UCL provides access to the high-performance computing (HPC) facilities Legion (5680processor cores), and Grace (684 compute nodes hosting two Intel (Haswell); overall10,944 cores) and at no cost to academic staff. Stamatakis’s lab has access to the HPC facility “Thomas” (720 Lenovo Intel x86-64 nodes,giving 17.2k cores in total) managed by the UK Materials and Molecular Modelling Hub,which is partially funded by EPSRC (EP/P020194).
- National Computational Resources: XSEDE network of Supercomputers is used by Kaxiras and Sautet. NERSC DOE computing facilities(Kaxiras).
Prof. Friend's Surface Chemistry and analysis equipment
Several UHV systems all equipped with capability for Auger electron spectroscopy, LEED and temperature programmed reaction (mass spectrometry), and metal evaporators for formation of alloy surfaces. Each system has key capabilities for investigation of surface chemistry, outlined below.
- Variable temperature STM system (Omicron) for surface imaging.
- Variable temperature STM system (RHK) (Shared with Madix) for surface imaging.
- High resolution electron loss spectroscopy (LK) for surface vibrational spectroscopy usingelectron scattering.
- Infrared Spectrometer (Thermo-Fisher) for vibrational spectroscopy.
- X-ray photoelectron spectroscopy/Low Energy Ion Scattering for surface analysis, includingtransfer system for studies in ambient pressure (shared with Madix).
- Temperature programmed reaction/photodesorption system with capability for ambientpressure treatment in separate chamber.
Catalysis testing facilities
- Gas phase flow reactors (3) for catalyst testing are available, including controllers forintroduction of reactant and inert gases.
- Liquid phase flow reactor for pressures up to 10 bar.
- Gas chromatography/mass spectrometer system for product analysis.
Temporal Analysis of Products (TAP) reactor used for kinetic studies of catalysis
- Transient Analysis of Products (TAP) reactor is available for transient pulse-response kinetic and mechanistic studies of catalytic reactions.
Catalyst Synthesis facilities
- The Aizenberg's lab covers 3000 sq. ft. and has the tools required for the synthesis of colloidal particlesand their self-assembly, including fume hoods, laminar flow hoods, ovens, a calciner, aglove box (Braun), class 1000 clean room; vibration isolated humidity and temperaturecontrolled test enclosure, as well as microscopes and other relevant equipment for their characterization.
Lawrence Berkeley National Laboratory
- The following state-of-the-art Surface Science facilities equipped with various Microscopes, both home built, and commercial are available: Variable temperature (100 K-350 K) Scanning Tunneling Microscope (VT-STM), equipped with Low Energy Electron Diffraction (LEED), Ion Sputtering (IS), Mass Spectrometer (MS) and Auger Electron Spectroscopy (AES) in an ultra-high vacuum (UHV) chamber; A variable temperature (100 K- 350 K) Atomic Force Microscope (VT-AFM) in a UHV chamber with LEED, AES, IS and MS; A liquid He (4 K) cooled STM, with preparation chamber equipped with LEED, AES, IS and MS; A liquid He (4 K) cooled non-contact AFM, with preparation chamber equipped with LEED, AES, IS and MS; A Molecular Imaging AFM operating in air and in controlled gas environments; reaction cells for X-ray Absorption Spectroscopy (XAS), with gas circulation and laser assisted sample heating. Used in catalysis experiments at the Advanced Light Source (ALS); access to ALS allows in situ Ambient Pressure X-ray Photoelectron Spectroscopy (APXPS)
Lawrence Livermore National Lab
- LLNL Additive Micromanufacturing Laboratory with capabilities including a Projection Microstereolithography system (two new systems are in assembly), four Electrophoretic Deposition systems, and three Direct Ink Writing systems. This laboratory also houses a Stratasys Dimension 1200 SST 3D printer capable of printing 3D structures from ABS thermoplastic in a working volume of 10 Å~ 10 Å~ 12 inches, a 3D Systems Cube desktop fused deposition modeling 3D printer, and an Ultimaker desktop 3D printer capable of fabricating structures with multiple Polymers.
Prof. Stephanopoulos Nano Catalysis and Energy Laboratory
- These labs are equipped with several reactor systems, including two recycle reactors forlow-surface area sample tests and five tubular flow reactor systems; catalyst preparationapparatus; atomic layer deposition apparatus; gas and solid analysis systems, includingthree gas chromatographs, four mass spectrometers, two TGA assemblies, flow controllers,FTIR and NDIR gas analyzers, an ATR-IR analyzer for catalyst studies in both liquid andgas reaction mixtures, coupled with an HPLC for liquid effluent analysis; a UV-VISspectrophotometer, data acquisition systems.
- Attenuated Total Reflection-Infra-Red (ATR-IR) coupled with HPLC: An ATR-IRinstrument in our lab was coupled with an HPLC system for liquid effluent analysis basedon part funding from IMASC 1.0. Our Thermo Fisher Scientific iS50 IR was equipped witha SMART ARK accessory for the ATR-IR cell.
- The laboratories are well equipped to conduct reaction rate measurements, parametricreaction studies, and life tests with catalysts in powder or pellet form in flow microreactorassemblies coupled with gas chromatographs and mass spectrometers.
- The catalysts of interest in this project wills be screened in a state-of-the-art AutoChem II2920 reactor system (Micromeritics) coupled with a mass spectrometer available at Tufts.A CryoCooler used in conjunction with the furnace allows us to continuously ramp thetemperature from -120 oC to 1100 oC.
- Temperature-programmed-reduction (TPR), using CO or H2 as the reductant, andtemperature-programmed surface reaction (TPSR) coupled with mass spectrometry studiesare routinely performed at the MF-S labs.
Reactor set-up for TPSR/MS studies
- Selective hydrogenation, deoxygenation, and hydrogenolysis reactions in the liquid phaseare carried out at Tufts in batch and semi-batch reactor systems.
- Liquid-phase hydrogenation and deoxygenation reactions are performed in a high-pressureflow reactor system.
- The following equipment and facilities have been identified specifically for the proposedproject.
- Fume hoods with glassware, vacuum oven, muffle furnace, etc. for catalystpreparation.
- Atomic-layer deposition apparatus (Cambridge NanoTech, Savannah 100)
- Micromeritics AutoChem II 2920 Catalyst Characterization System for BET-N2physisorption, chemisorption, and TPR/TPSR evaluation of catalysts.
- Stainless steel tube microreactor assembly capable of high-pressure operation,including an electric furnace with temperature controller, gas manifold, and flowcontrollers.
- Hewlett Packard 6890 dual detector (FID/TCD) gas chromatograph equipped withautomatic gas sampling valve and integrator.
- Hewlett Packard 5890 FID detector gas chromatograph with manual injection portfor offline analysis.
- Beckman-Model 864 non-dispersive-infrared (NDIR) CO2 analyzer.
- Hewlett Packard Model 8452A Diode Array UV-visible spectrophotometer withHarrick diffuse reflectance cell for in-situ redox catalyst studies up to 600 °C.
Prof. E. Charles H. Sykes Surface Science laboratory:
The laboratory contains five state of the art surfacescience/scanning probe instruments with the following capabilities:
- Low- and variable-temperature scanning tunneling microscopes (LT-STM andVTSTM). The LT-STM is located in a vibrationally stable area in the basement ofthe building and is housed inside a custom designed “quiet room” that shields theinstrument from acoustical noise (Dz < 2 pm rms noise). This isolation from theenvironment, coupled with the thermal stability afforded by operating attemperatures as low as 5 K, allows individual molecules to be probed for longperiods of time without thermal drift (Dz < 0.01 nm/h). This instrument has beenmodified in order to deposit molecules on the sample while it is at 5 K inside theSTM. This molecular doser has been built and tested and allows one to dosebetween fractions of a monolayer to multilayers of a chosen molecule directly onthe sample. The LT-STM chamber is coupled to a sample preparation chamberequipped with metal and molecule sources, as well as heating and sputteringcapabilities. The VT-STM is a more recent acquisition that has extended the group’satomic-scale imaging capabilities to a much wider range of temperatures: 30-500K.
- X-Ray Photoelectron Spectroscopy (XPS) allows the elemental composition ofSTMsamples be monitored in situ. The rotatable sample mount offers theopportunity to perform angle-resolved XPS measurements and hence depth profilesof the top ~7 atomic layers of samples. This instrument is interfaced with the VT-STM.
- Auger Electron Spectroscopy (AES), Low Energy Electron Diffraction (LEED),Temperature Programmed Reaction (TPR) and Reflection Absorption InfraredSpectroscopy (RAIRS) Apparatus have been installed on custom built chambers inthe Sykes lab. Sample preparation procedures and techniques are identical to thoseused on both UHV STMs. The three TPR instruments allow the sample temperatureto be controlled between 75 and 825 K. Hiden 3F 300 AMU mass spectrometersare mounted so as to approach within ~1 mm of the sample face, and a feedback-controlled power supply offers linear heating ramps for highquality TPR spectra.AES, XPS, LEED and RAIRS allow for the probing of sample structure,composition and adsorbate binding configuration.