Characterization and Evaluation of Methane Oxidation Catalysts for Dual-Fuel Diesel and Natural Gas Engines

The UK has incentivized the use of natural gas in heavy goods vehicles (HGVs) by converting to dual-fuel (DF) diesel-natural gas systems to reduce noxious and greenhouse gas emissions. Laboratory and on-road measurements of DF vehicles have demonstrated a decrease in CO$_2$ emissions relative to diesel, but there is an increase in greenhouse gas (CO$_2$e) emissions because of unburned methane. Decreasing tailpipe emissions of methane via after-treatment devices in lean-burn compression ignition engines is a challenge because of low exhaust temperatures (~400 °C) and the presence of water vapor. In this study, six commercially available methane oxidation catalysts (MOCs) were tested for their application in DF HGV vehicles. Each MOC was characterized in terms of the catalyst platinum group metal (PGM) loading (both Pd and Pt), particle size, catalytic surface area, and Pd:Pt ratio. In addition, the washcoat surface area, pore volume, and pore size were evaluated. The MOC conversion efficiency was evaluated in controlled methane-oxidation experiments with varying temperatures, flow rates, and gas compositions. Characteristic-conversion efficiency correlations demonstrate that the influential MOC characteristics were PGM loading (both Pd and Pt), Pd:Pt ratio, washcoat surface area, and washcoat pore volume. With 90 % methane oxidation at less than 400 °C in DF HGV exhaust conditions, sample 1 had the highest conversion efficiency because of a high PGM loading (330 g/ft$^3$, 12,000 g/m$^3$), a 5.9 Pd:Pt ratio, a high alumina washcoat surface area of 20 m$^2$/cm$^3$, and 74-mm$^3$/cm$^3$ pore volume. Additional studies showed increased MOC conversion efficiency with decreasing gas hourly space velocities (GHSVs) and increasing methane concentrations.We acknowledge support from the UK Engineering and Physical Sciences Research Council (EP/K00915X/1), the UK Department for Transport, the Office for Low Emission Vehicles and Innovate UK (project reference 400266), and the industrial partners of the Centre for Sustainable Road Freight. GreenUrban Technologies Ltd. (3) and Prins Autogas UK Ltd. (1) provided the samples for testing in this study

One particle interchain hopping in coupled Hubbard chains

Interchain hopping in systems of coupled chains of correlated electrons is investigated by exact diagonalizations and Quantum-Monte-Carlo methods. For two weakly coupled Hubbard chains at commensurate densities (e.g. n=1/3) the splitting at the Fermi level between bonding and antibonding bands is strongly reduced (but not suppressed) by repulsive interactions extending to a few lattice spacings. The magnitude of this reduction is directly connected to the exponent $\alpha$ of the 1D Luttinger liquid. However, we show that the incoherent part of the single particle spectral function is much less affected by the interchain coupling. This suggests that incoherent interchain hopping could occur for intermediate $\alpha$ values.Comment: 4 pages, LaTeX 3.0, 7 PostScript figures in uuencoded for

Spin-Density-Wave Phase Transitions in Quasi-One-Dimensional Dimerized Quarter-Filled Organic Conductors

We have studied spin density wave (SDW) phase transitions in dimerized quarter-filled Hubbard chains weakly coupled via interchain one-particle hopping, $t_{b0}$. It is shown that there exists a critical value of $t_{b0}$, $t_{b}^\ast$, between the incoherent metal regime ($t_{b0}<t_{b}^\ast$) and the Fermi liquid regime ($t_{b0}>t_{b}^\ast$) in the metallic phase above the SDW transition temperature. By using the 2-loop perturbative renormalization-group approach together with the random-phase-approximation, we propose a SDW phase diagram covering both of the regimes. The SDW phase transition from the incoherent metal phase for $t_{b0}<t_{b}^\ast$ is caused by growth of the intrachain electron-electron umklapp scattering toward low temperatures, which is regarded as preformation of the Mott gap. We discuss relevance of the present result to the SDW phase transitions in the quasi-one-dimensional dimerized quarter-filled organic conductors, (TMTTF)$_2$X and (TMTSF)$_2$X.Comment: 19 pages, 13 eps figures, uses jpsj.sty, corrected typo in the text and figures, no changes to the paper, to appear in J. Phys. Soc. Jpn. 68, No.8 (1999

Impurity-induced stabilization of Luttinger liquid in quasi-one-dimensional conductors

It is shown theoretically that the Luttinger liquid phase in quasi-one-dimensional conductors can exist in the presence of impurities in a form of a collection of bounded Luttinger liquids. The conclusion is based upon the observation by Kane and Fisher that a local impurity potential in Luttinger liquid acts, at low energies, as an infinite barrier. This leads to a discrete spectrum of collective charge and spin density fluctuations, so that interchain hopping can be considered as a small parameter at temperatures below the minimum excitation energy of the collective modes. The results are compared with recent experimental observation of a Luttinger-liquid-like behavior in thin NbSe$_3$ and TaS$_3$ wires.Comment: 11 pages, revtex, final version published in JETP Lett

Superconductivuty versus Tunneling in a Doped Antiferromagnetic Ladder

The low-energy charge excitations of a doped antiferromagnetic ladder are modeled by a system of interacting spinless fermions that live on the same ladder. A relatively large spin gap is assumed to ``freeze out'' all spin fluctuations. We find that the formation of rung hole pairs coincides with the opening of a single-particle gap for charge excitations along chains and with the absence of coherent tunneling in between chains. We also find that such hole pairs condense into either a crystalline or superconducting state as a function of the binding energy.Comment: 15 pgs. in PLAIN TeX, 2 figs. in postscript, to appear in Phys. Rev.

Strong-Coupling Expansion for the Hubbard Model

A strong-coupling expansion for models of correlated electrons in any dimension is presented. The method is applied to the Hubbard model in $d$ dimensions and compared with numerical results in $d=1$. Third order expansion of the Green function suffices to exhibit both the Mott metal-insulator transition and a low-temperature regime where antiferromagnetic correlations are strong. It is predicted that some of the weak photoemission signals observed in one-dimensional systems such as $SrCuO_2$ should become stronger as temperature increases away from the spin-charge separated state.Comment: 4 pages, RevTex, 3 epsf figures include

Dimensional Crossovers in the Doped Ladder System: Spin Gap, Superconductivity and Interladder Coherent Band Motion

Based on the perturbative renormalization group (PRG) approach, we have studied dimensional crossovers in Hubbard ladders coupled via weak interladder one-particle hopping, $t_{\perp}$. We found that the one-particle crossover is strongly suppressed through growth of the intraladder scattering processes which lead the isolated Hubbard ladder system toward the spin gap metal (SGM) phase. Consequently when $t_{\perp}$ sets in, there exists, for any finite intraladder Hubbard repulsion, $U>0$, the region where the two-particle crossover dominates the one-particle crossover and consequently the d-wave superconducting transition, which is regarded as a bipolaron condensation, occurs. By solving the scaling equations for the interladder one-particle and two-particle hopping amplitudes, we give phase diagrams of the system with respect to $U$, $t_{\perp0}$ (initial value of $t_{\perp}$) and the temperature, $T$. We compared the above dimensional crossovers with those in a weakly coupled chain system, clarifying the difference between them.Comment: 26 pages, 19 eps figures, to appear J. Phys. Soc. Jpn. Vol.67 No.

Interaction-induced Fermi surface deformations in quasi one-dimensional electronic systems

We consider serious conceptual problems with the application of standard perturbation theory, in its zero temperature version, to the computation of the dressed Fermi surface for an interacting electronic system. In order to overcome these difficulties, we set up a variational approach which is shown to be equivalent to the renormalized perturbation theory where the dressed Fermi surface is fixed by recursively computed counterterms. The physical picture that emerges is that couplings that are irrelevant tend to deform the Fermi surface in order to become more relevant (irrelevant couplings being those that do not exist at vanishing excitation energy because of kinematical constraints attached to the Fermi surface). These insights are incorporated in a renormalization group approach, which allows for a simple approximate computation of Fermi surface deformation in quasi one-dimensional electronic conductors. We also analyze flow equations for the effective couplings and quasiparticle weights. For systems away from half-filling, the flows show three regimes corresponding to a Luttinger liquid at high energies, a Fermi liquid, and a low-energy incommensurate spin-density wave. At half-filling Umklapp processes allow for a Mott insulator regime where the dressed Fermi surface is flat, implying a confined phase with vanishing effective transverse single-particle coherence. The boundary between the confined and Fermi liquid phases is found to occur for a bare transverse hopping amplitude of the order of the Mott charge gap of a single chain.Comment: 38 pages, 39 figures. Accepted for publication in Phys. Rev.

Dynamical Properties of one dimensional Mott Insulators

At low energies the charge sector of one dimensional Mott insulators can be described in terms of a quantum Sine-Gordon model. Using exact results derived from integrability it is possible to determine dynamical properties like the frequency dependent optical conductivity. We compare the exact results to perturbation theory and renormalisation group calculations. We also discuss the application of our results to experiments on quasi-1D organic conductors.Comment: 17 pages, 5 figures, to appear in the proceedings of the NATO ASI/EC summer school "New Theoretical Approaches to Strongly Correlated Systems" Newton Institute for Mathematical Sciences, Cambridge UK, April 200

On-chain electrodynamics of metallic (TMTSF)_2 X salts: Observation of Tomonaga-Luttinger liquid response

We have measured the electrodynamic response in the metallic state of three highly anisotropic conductors, (TMTSF)_2 X, where X=PF_6, AsF_6, or ClO_4, and TMTSF is the organic molecule tetramethyltetraselenofulvalene. In all three cases we find dramatic deviations from a simple Drude response. The optical conductivity has two features: a narrow mode at zero frequency, with a small spectral weight, and a mode centered around 200 cm^{-1}, with nearly all of the spectral weight expected for the relevant number of carriers and single particle bandmass. We argue that these features are characteristic of a nearly one-dimensional half- or quarter-filled band with Coulomb correlations, and evaluate the finite energy mode in terms of a one-dimensional Mott insulator. At high frequencies (\hbar\omega > t_\perp, the transfer integral perpendicular to the chains), the frequency dependence of the optical conductivity \sigma_1(\omega) is in agreement with calculations based on an interacting Tomonaga-Luttinger liquid, and is different from what is expected for an uncorrelated one-dimensional semiconductor. The zero frequency mode shows deviations from a simple Drude response, and can be adequately described with a frequency dependent mass and relaxation rate.Comment: 12 pages, 7 figures, RevTeX; minor corrections to text and references; To be published in Phys. Rev. B, 15 July 199