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  1. Symposium on the 60th Anniversary of the Life-Saving Technetium-99m

    Wednesday, November 7, 2018, 3 pm
    Hamilton Seminar Room, Bldg. 555

    Speakers will present talks on technetium and nuclear medicine, including the history of the development of the Tc-99m generator at Brookhaven. The talks will be followed by a reception in the Chemistry Lobby.

  2. Chemistry Department Seminar

    "Synchrotron-based X-ray Absorption Spectroscopy for In Situ and Operando Studies of Nanoporous Catalysts"

    Presented by Kirill A. Lomachenko, European Synchrotron Radiation Facility (ESRF), Grenoble, France, France

    Monday, November 5, 2018, 11 am
    Room 300, Chemistry Bldg. 555

    Hosted by: Anatoly Frenkel

    X-ray absorption spectroscopy (XAS) has proven to be a very powerful tool for rationalization of catalytic processes because of the possibility to determine oxidation state and coordination geometry of catalytically active species in operando regime. The seminar will be focused on the advanced facilities for chemical XAS studies available at BM23 and ID24 beamlines of the ESRF synchrotron, which allow to exploit simultaneously a wide range of complementary techniques, make use of flexible sample environment, and obtain high-quality data in the timescale from minutes down to milliseconds. As a case study, recent work on the investigation of the local environment and electronic structure of the active centers of Cu-zeolites in deNOx and methane-to-methanol processes will be discussed.

  3. NSLS-II Friday Lunchtime Seminar

    "Materials Tribology: An Application-Driven Field with Rich Opportunities for Fundamental Studies of Surface Chemistry, Physics, Structure"

    Presented by Brandon A. Krick, Department of Mechanical Engineering and Mechanics, Lehigh University

    Friday, November 2, 2018, 12 pm
    NSLS-II Bldg. 743 Rm 156

    Hosted by: Ignace Jarrige

    The significant economic (~3-6% of developed countries GDP) and environmental (several percent of our annual energy consumption) impacts of friction and wear make tribology is an important, application-driven field. However, there is an opportunity and need for inherently fundamental studies on surface chemistry, physics and structure to elucidate fundamental mechanisms for friction and wear. The non-equilibrium and transient nature of shear-induced changes caused by contacting surfaces in relative motion requires both in situ and ex situ advanced characterization techniques; many of these only available at the light source at Brookhaven. A brief overview of shear-induced (sliding friction/wear) alterations of surfaces will be presented for material systems including: - environmental and tribochemistry molybdenum disulphide based coatings for space applications - shear-induced band bending in GaN - mechanochemistry of polymer nanocomposites

  4. Chemistry Department Seminar

    ""Size control of supported metals for catalysis""

    Presented by Xiao Yan Liu, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023 (China), China

    Tuesday, October 30, 2018, 11 am
    Room 300 - 3rd Flr. Chemistry Bldg. 555

    Hosted by: Sanjaya Senanayake

    Catalysis by supported metals is size sensitive, so the size control is extremely important. Here, I will present two examples for the size control of catalysis. One is the size control of gold catalysts by tuning the metal support interaction. In the last decade, we've developed several methods to control the particle size of gold, for example, adding a second metal to form alloy with gold, using the thiolated gold nanoclusters as the precursor of gold catalysts, and so on. The other example focuses on single-atom catalysis that has emerged as a new frontier in heterogeneous catalysis and shown distinctive performances in a series of oxidation and hydrogenation reactions. The ways we developed to stabilize the single atoms will be introduced. The mechanism for the stabilization of the nanoparticles/single atoms were proposed based on the characterization by aberration-corrected HAADF-STEM, in situ EXAFS and DFT calculations.

  5. PubSci at the Parrish

    "Illumination: Revealing the Secret Chemistry of Oil Paintings"

    Friday, September 21, 2018, 7 pm
    Parrish Art Museum 279 Montauk Hwy., Water Mill, N

  6. Chemistry Department Colloquium

    "Proton-Coupled Electron Transfer in Catalysis and Energy Conversion"

    Presented by Dr. Sharon Hammes-Schiffer, Department of Chemistry, Yale University

    Monday, September 10, 2018, 11 am
    Hamilton Seminar Room, Bldg. 555

    Hosted by: Mehmed Zahid Ertem

    Proton-coupled electron transfer (PCET) reactions play a vital role in a wide range of chemical and biological processes. This talk will focus on recent advances in the theory of PCET and applications to catalysis and energy conversion. The quantum mechanical effects of the active electrons and transferring proton, as well as the motions of the proton donor-acceptor mode and solvent or protein environment, are included in a general theoretical formulation. This formulation enables the calculation of rate constants and kinetic isotope effects for comparison to experiment. Recent extensions enable the study of heterogeneous as well as homogeneous interfacial PCET processes. Applications to PCET in molecular electrocatalysts for hydrogen production and water splitting, photoreduced zinc-oxide nanocrystals, and the Volmer reaction will be discussed. These studies have identified the thermodynamically and kinetically favorable mechanisms, as well as the role of proton relays, and are guiding the theoretical design of more effective catalysts. In addition, recent developments of theoretical approaches for simulating the ultrafast dynamics of photoinduced PCET, along with applications to solvated molecular systems and photoreceptor proteins, will be discussed.

  7. Chemistry Department Seminar

    "Synthesis of Fuels and Chemicals by Electroreduction over Copper Catalysts"

    Presented by Elizabeth J. Biddinger, The City College of New York, CUNY

    Monday, August 6, 2018, 11 am
    Room 300 - 3rd Flr. Chemistry Bldg. 555

    Hosted by: Sanjaya Senanayake

    Electrochemical synthesis methods offer opportunities to perform reactions under benign reaction conditions (at or near room temperature and pressure), use less harmful or waste-generating reaction steps, and perform selective reactions. In electroreduction reactions, externally-supplied hydrogen that is generally needed for reduction is not required. Rather, electrons, frequently paired with the electrolyte, are the reducing agents. New opportunities for utilization of electrochemical reactions exist with the emerging renewable electricity generation market. Due to the intermittent supply sources for many renewable electricity systems, excess electricity gets generated when peak generation (sunny or windy periods) does not match with demand. Electrochemical reactions can be performed at relatively low costs with this excess electricity to synthesize fuels for later use or chemicals. The work presented here will illustrate two synthesis systems via electroreduction – carbon dioxide electroreduction to hydrocarbons and furfural (a biomass-derived species) electrochemical hydrogenation and hydrogenolysis (ECH) to fuels and chemicals. Both of these reactions are performed over copper electrodes, serving as the catalysts for the system. Copper is utilized because of its unique balance between being active for the electroreduction and less active for the undesired side reaction hydrogen evolution. In CO2 electroreduction, copper is the only known metal to produce significant quantities of hydrocarbons. By tuning the morphology, the selectivity between ethylene and methane can be tuned. The results of morphological differences and the dynamic nature of copper surfaces will be discussed in terms of electrodeposition and the resulting CO2 electroreduction performance. In furfural ECH, both 2-methyl furan and furfuryl alcohol can be formed, while over many other metals 2-methyl furan is not formed. The reaction conditions for furfural ECH si

  8. Chemistry Department Seminar

    "Triggered Reversible Phase Transformation between Layered and Spinel Structure via Intercalated Hetero Species in Sodium Birnessite"

    Presented by Yong-Mook Kang, Department of Energy and Materials Engineering, Dongguk University-Seoul, Seoul, 04620, Republic of Korea., Korea, Republic of (South)

    Monday, July 23, 2018, 11 am
    Room 300, 3rd Flr. Chemistry Bldg. 555

    Hosted by: Xiao-Qing Yang

    Phase transformation of layered structure into spinel structure has been detrimental for most of layered oxide cathodes. Even if a lot of efforts have been made to relieve this highly irreversible phase transformation, there have been few successful results. However, we firstly observed the possibility to make this irreversible phase transformation extremely reversible by utilizing Na- birnessite (NaxMnO2•yH2O; Na-bir) as a basic structural unit, which has distinctive layered structure containing crystal water. Herein, the crystal water in the structure contributes to generating metastable spinel-like phase, which is the key factor for making this unusual reversibility happen. The reversible structural rearrangement between layered and spinel-like phases during electrochemical reaction could activate new cation sites and enhance ion diffusion with higher structural stability. This unprecedented reversible phase transformation between spinel and layered structure was deeply analyzed via combined ex situ soft and hard X-ray absorption spectroscopy (XAS) analysis with in situ X-ray diffraction (XRD). Fundamental mechanism on this reversible phase transformation was theoretically elucidated and confirmed by kinetic investigation using first-principle calculation. These results provide deep insight into novel class of intercalating materials which can deal with highly reversible framework changes, and thus it can pave an innovative way for the development of cathode materials for next- generation rechargeable batteries.

  9. Chemistry Department Colloquium

    "Turning Base Metals into Precious Metals: Nanostructured Early Transition Metal Carbides and Nitrides"

    Presented by Levi Thompson, University of Michigan, Department of Chemical Engineering,

    Monday, July 9, 2018, 11 am
    Hamilton Seminar Room, Bldg. 555

    Hosted by: Sanjaya Senanayake

    The addition of carbon and nitrogen to early transition metals like molybdenum and vanadium can result in materials with properties that are similar to those of platinum group metals (PGMs). In the mid-1970s, for example, it was discovered that tungsten carbides can catalyze hydrogenation reactions that previously were only known for PGMs, and more recently we observed that molybdenum nitrides are capable of bulk hydrogen storage like Pd. Since then, early transition metal carbides and nitrides have been investigated for a variety of reactions. This paper will describe our work to design and synthesize nanostructured early transition metal carbides and nitrides for reactions including selective hydrogenations. Our research has focused on understanding the genesis of the materials, unraveling the reaction mechanisms and determining structure-function relationships that will enable the rational design of these materials. Of particular interest are CO2 hydrogenation and ammonia synthesis, reactions for which new catalysts are needed to reduce energy consumption.

  10. Chemistry Department Seminar

    "Nanowires Devices for Emerging Energy Storage"

    Presented by Liqiang Mai, Wuhan University of Technology, China

    Friday, June 15, 2018, 11 am
    Room 300 - Third Floor - Chemistry Bldg. 555

    Hosted by: Xiao-Qing Yang

    One-dimensional nanomaterials can offer large surface area, facile strain relaxation upon cycling and efficient electron transport pathway to achieve high electrochemical performance. Hence, nanowires have attracted increasing interest in energy related fields. We designed the single nanowire electrochemical device for in situ probing the direct relationship between electrical transport, structure, and electrochemical properties of the single nanowire electrode to understand intrinsic reason of capacity fading. The results show that during the electrochemical reaction, conductivity of the nanowire electrode decreased, which limits the cycle life of the devices. We have developed a facile and high-yield strategy for the oriented formation of CNTs from metal−organic frameworks (MOFs). The appropriate graphitic N doping and the confined metal nanoparticles in CNTs both increase the densities of states near the Fermi level and reduce the work function, hence efficiently enhancing its oxygen reduction activity. Then, we fabricated a field-tuned hydrogen evolution reaction (HER) device with an individual MoS2 nanosheet to explore the impact of field effect on catalysis. In addition, we demonstrated the critical role of structural H2O on Zn2+ intercalation into bilayer V2O5·nH2O. The results suggest that the H2O-solvated Zn2+ possesses largely reduced effective charge and thus reduced electrostatic interactions with the V2O5 framework, effectively promoting its diffusion. We also identified the exciting electrochemical properties (including high electric conductivity, small volume change and self-preserving effect) and superior sodium storage performance of alkaline earth metal vanadates through preparing CaV4O9 nanowires. Our work presented here can inspire new thought in constructing novel one-dimensional structures and accelerate the development of energy storage applications.

  11. Chemistry Department Seminar

    "Astrochemistry in the Laboratory – Combining Theory and Experiment"

    Presented by Kelvin Lee, Harvard-Smithsonian Center for Astrophysics

    Monday, June 11, 2018, 11 am
    Room 300, 3rd Floor, Chemistry Bldg. 555

    Hosted by: Greg Hall

    Brief overview of the laboratory and theoretical efforts in astrochemistry at the Harvard Smithsonian Center for Astrophysics. Will highlight one of our areas of research – the characterization and spectroscopy of molecular isomers in space by showcasing two recent projects (1) the rotational spectroscopy of ethynethiol (HCCSH), a higher energy isomer of thioketene, and (2) the first-principles high accuracy chemical network we are developing for the production and destruction of hydrogen (iso)cyanide in space.

  12. Chemistry Department Colloquium

    "Discovering Emergent Phenomena in Catalysis Through Large Scale Ab Initio Molecular Dynamics Simulations"

    Presented by Roger Rousseau, Pacific Northwest National Laboratory

    Tuesday, May 29, 2018, 11 am
    Hamilton Seminar Room, Bldg. 555

    Hosted by: Sanjaya Senanayake

    The current state of the art of electronic structure methods allows us to tackle model systems on the order of 100s to 1000s of atoms with suitable speed and efficiency to perform statistical mechanical sampling on millions of configurations. This has opened the door to using theoretical tools such as ab initio molecular dynamics (AIMD) combined with enhanced sampling techniques) to discover novel emergent phenomena that result from chemical complexity. Nowhere is this more needed than in catalysis, where models need to include support materials, the catalysts, the reactants and products all at elevated temperature and pressures. In this context, both global and local anharmonicities on the potential energy surface can lead to unexpected phenomena that can be discovered through large scale simulation yet are often not accounted for in current theoretical studies. This will be illustrated with examples drawn from the chemistry of metal particles on reducible supports [1-3], Brønsted acid chemistry in confined spaces [4] and reactivity at solid-liquid interfaces [5,6]. In the context of metal particles supported on reducible metal oxides (such as TiO2, CeO2 and RuO2), we have found that there is a strong coupling between the redox state of the support and the redox properties of the nanoparticle [1,2] such that unique catalytic processes can occur including: Redox state dependent reaction energies [2,3]; Formation of transient single atoms, which are themselves catalytic [1,3]; For prototypical reactions such as CO oxidation, a complex mechanistic landscape where catalysis can occur by competing mechanisms involving both the nanoparticle and single atom sites at the same time. Similar methods have been used to investigate the confinement effect in zeolite [4] and understand the free energetics of acid catalysis in confined media. It is shown that due to the large anharmonic effects associated with molecules, such as ethanol, interacting with the walls of a s

  13. HET/RIKEN Lunch Seminar

    "Quantum Simulation from Quantum Chemistry to Quantum Chromodynamics"

    Presented by Peter Love, Tufts

    Thursday, May 10, 2018, 12:30 pm
    Building 510, Room 2-160

    Hosted by: Mattia Bruno and Enrico Rinaldi

    Quantum simulation proposes to use future quantum computers to calculate properties of quantum systems. In the context of chemistry, the target is the electronic structure problem: determination of the electronic energy given the nuclear coordinates of a molecule. Since 2006 we have been studying quantum approaches to quantum chemical problems, and such approaches must face the challenges of high, but fixed, precision requirements, and fermion antisymmetry. I will describe several algorithmic developments in this area including improvements upon the Jordan Wigner transformation, alternatives to phase estimation, adiabatic quantum computing approaches to the electronic structure problem, methods based on sparse Hamiltonian simulation techniques and the potential for experiments realizing these algorithms in the near future. I will also briefly review work by others on the analog and digital simulation of lattice gauge theories using quantum simulators.

  14. Condensed-Matter Physics & Materials Science Seminar

    "Chemistry beyond the crystal- advanced Fourier techniques"

    Presented by Simon Kimber, Oak Ridge National Laboratory

    Monday, April 30, 2018, 1:30 pm
    ISB Bldg. 734 Conf. Rm. 201 (upstairs)

    Hosted by: Ian Robinson

    Chemical crystallography nowadays makes structure determination and refinement trivial. However, advances in x-ray and neutron sources mean that we should revisit some of the basic assumptions that shape our experiments. For example, most chemical reactivity in e.g. catalysis, self-assembly etc, occurs in the solution phase. Why are we as crystallographers then wedded to the solid state? In this presentation, I will show how total scattering can be used to determine changes in cluster structure during photochemical reactions and to probe the role of the solvent in 'magic size' cluster formation. I will then describe how neutron scattering techniques can be used to challenge another basic assumption- the static approximation in total scattering. We have successfully applied so-called 'dynamic-PDF' techniques to simple chalcogenide materials. This allows to determine the time scale on which local distortions appear, providing insight into the role of highly anharmonic phonons in e.g. phase change and thermoelectric materials. Time allowing, I will also provide a short update on progress at ORNL, including the upcoming restart of the SNS, and new instrumentation for diffraction, total and diffuse scattering.

  15. Center for Functional Nanomaterials Seminar

    "Electrocatalysis: From nanoelectrochemistry to materials design"

    Presented by Professor Dr. Wolfgang Schuhmann, Ruhr-Universität Bochum, Analytical Chemistry and Center for Electrochemical Sciences (CES), Germany

    Friday, April 27, 2018, 11 am
    Bldg 735, CFN, Seminar Room 2nd Floor

    Hosted by: Huolin Xin

  16. Chemistry Department Seminar

    "Spectroscopy and Diabatization: Turning the GMH Method Upside Down to Study Butadiene"

    Presented by Robert Cave, Harvey Mudd College

    Friday, April 27, 2018, 11 am
    Room 300, 3rd Floor, Chemistry Bldg. 555

    Hosted by: John Miller

    The spectroscopy of the low-lying singlet states of butadiene has been a vexing problem for theorists for over forty years. The positions of the lowest-lying singlet states at the ground state geometry are something of a methodological Rorschach test and the planar stationary points of these states have seen modest attention. Important work has been done on the ultrafast dynamics of butadiene following excitation to the bright 11Bu but these studies are often forced to use simple wavefunctions that may lead to exaggerated couplings. We present new simulation results of its electronic spectrum based on Equations of Motion Coupled Cluster Theory in large basis sets using a vibronic coupling model involving many vibrational modes. We investigate the sensitivity of the results to the choice of vibronically-coupled states and test the dependence of the results on vertical excitation energies. We believe that butadiene should be considered somewhat less vexing than it has been before and our results can be used as a starting point for accurate explorations of its short-time excited state dynamics.

  17. Chemistry Department Seminar

    "In situ analysis of Ru-based catalysts under water oxidation conditions"

    Presented by Yulia Pushkar, Purdue University

    Tuesday, February 27, 2018, 10 am
    Room 300, 3rd Floor, Chemistry Bldg. 555

    Hosted by: Dmitry Polyansky

    Realization of artificial photosynthesis carries the promise of cheap and abundant energy. The water molecule is an ideal source of electrons and protons for fuel forming reactions, but the chemical complexity of water splitting makes practical realization challenging. To advance the catalyst's rational design, detailed information on the structure of the catalyst under reaction conditions and mechanisms of O-O bond formation are required. Here, we used a combination of EPR, freeze quench and stopped flow spectroscopy with ms-s time resolution, X-ray absorption spectroscopy (XAS), Resonance Raman (RR) and DFT to follow in situ catalyst dynamic under conditions of water oxidation.1-3 Two representative Ru –based catalysts were analyzed: [RuII(NPM)(4-pic)2(H2O)]2+ and [RuII(pic)2(dpp)]2+. First system has water coordinated to Ru center and forms [RuIV(NPM)(4-pic)2=O]2+ upon oxidation. This intermediate undergoes fast dynamics (on few sec time scale) of oxygen atom transfer from the RuIV=O oxo species to uncoordinated nitrogen of the NPM ligand. NPM ligand modification occurs on the time scale of catalyst activation and results in [RuIII(NPM-NO)(4-pic)2(H2O)]3+ and [RuIII(NPM-NO,NO)(4-pic)2]3+ complexes with unique EPR signals. [RuII(pic)2(dpp)]2+ complex was proposed to activate via formation of the 7-coordinate [RuV=O(pic)2(dpp)]3+ species. We report the first detection of the ligand protected 7-coordinate species in catalytic mixtures by combination of the spectroscopic techniques. Over a few minutes this intermediate transfers oxygen from the RuV=O group to a pyridyl nitrogen of the dpp ligand. This reaction proceeds twice resulting in the dpp-di-N-oxide ligand. This ligand modification results in the catalyst activation. [Ru(bda)(pic)2] complex is also proposed to activate via formation of 7-coordinate [RuV=O(bda)(pic)2]+ intermediate which is highly reactive in solution via radical coupling pathway. Site isolation of the catalyst on the electrode

  18. NSLS-II Friday Lunchtime Seminar Series

    "Using X-ray Fluorescence Microprobe to Elucidate the Chemistry of Trace Elements in Soils and Plants"

    Presented by Ryan Tappero, NSLS-II

    Friday, February 23, 2018, 12 pm
    NSLS-II Bldg. 743 Rm 156

    Hosted by: M. Abeykoon, S. Chodankar, B. Ocko, T. Tanabe, J. Thieme

  19. Chemistry Department Seminar

    "Learning the nanocatalyst structure "on the fly" using neural networks"

    Presented by Dr. Janis Timoshenko, Dept. of Material Science and Chemical Engineering, Stony Brook University

    Monday, February 12, 2018, 11 am
    Room 300, Chemistry Bldg. 555

    Hosted by: Sanjaya Senanayake

    Understanding of atomic structure in metallic nanoparticles (NPs) and its relation to the NPs properties is important for design of novel catalytic materials. In-situ studies are an essential element in such investigations, since the atomic structure of nanosized catalysts can change dramatically in reaction conditions. X-ray absorption spectroscopy is one of a few methods that are useful in this case, due to its sensitivity to the chemical state of absorbing atoms and to the types and arrangements of atoms around the absorber, and its suitability for in-situ and in-operando studies. While EXAFS spectroscopy is widely used in NPs structure studies, much less attention has been paid to the information encoded in X-ray absorption near edge structure (XANES). Analysis of XANES data has several advantages. First, XANES is less sensitive to disorder, which affects severely EXAFS quality and complicates EXAFS data interpretation. Secondly, XANES is more sensitive to the 3D geometry of the environment around absorbing atoms. Better signal-to-noise ratio in XANES region of absorption spectra also means that spectra can be collected with better time-resolution, for more diluted samples, on strongly attenuating support materials and/or in complex experimental setups. The main challenge that hinders the usage of XANES for quantitative analysis is the lack of methodology that would allow one to extract structural information from experimental data. Recent developments in data-enabled discovery methods provide a key to this problem. To correlate XANES features with the descriptors of 3D local structure of metallic NPs, we employed machine learning and ab-initio XANES calculations. Here we demonstrate the potentiality of this method on the example of XANES study of monometallic (Pt, Ag and Cu), as well as bimetallic (PdAu) particles. We use theoretical site-specific XANES spectra, calculated by ab-initio codes for a broad range of structure models, to train an artificial neura

  20. Chemistry Department Seminar

    "In situ Studies and Gas Phase Visulation of Model Catalysts at Work"

    Presented by Prof. Edvin Lundgren, Institute of Physics, Lund University, Sweden

    Wednesday, January 31, 2018, 11 am
    Hamilton Seminar Room, Bldg. 555

    Hosted by: Sanjaya Senanayake

    Motivated mainly by catalysis, gas-surface interaction between single crystal surfaces and molecules has been studied for decades. Most studies have been performed in well-controlled environments, and has been instrumental for the present day understanding of catalysis. We have for some years explored the possibilities to perform experiments at conditions closer to those of a technical catalyst, in particular at increased pressures. In this contribution we will show examples from catalytic CO oxidation over Pd single crystal surfaces using Ambient Pressure X-ray Photo emission Spectroscopy (APXPS) [1] and High Energy Surface X-Ray Diffraction (HESXRD) [2] at more realistic conditions. However, the detected surface structure during the reaction is sensitive to the composition of the gas phase close to the catalyst surface [3-4]. Therefore, the catalytic activity of the sample will itself affect the surface structure, which may complicate the assignment of the active phase. For this reason, we have applied 2D Planar Laser Induced Fluorescence (PLIF) to the gas phase in the vicinity of an active model catalysts [5-7]. In particular, these measurements enables a direct view of the onset and location of the catalytic activity. Further, the gas phase distribution during a catalytic reaction from more complicated samples, such as a curved single crystal upon ignition [8] may be explored, see Fig. 1. [1] S. Blomberg et al; Phys. Rev. Lett. 110, 117601 (2013). [2] J. Gustafson et al; Science, 343, 758 (2014). [3] S. Matera and K. Reuter, Phys. Rev. B 82, (2010) 085446. [4] S. Matera et al; ACS Catalysis 5, 4514 (2015). [5] J. Zetterberg et al; Rev.Sci. Instrum. 83, 053104 (2012). [6] J. Zetterberg et al; Nat. Comm. 6, 7076 (2015). [7] S. Blomberg et al; ACS catalysis 5, 2028 (2015). [8] S. Blomberg et al; ACS Catalysis 7, 110 (2016).

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