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Bell, David C.

Publications and source records attributed to Bell, David C..

A simultaneous depolymerization and hydrodeoxygenation process to produce lignin-based jet fuel in continuous flow reactor

Economical production of lignin-based jet fuel (LJF) can improve the sustainability of sustainable aviation fuels (SAFs) as well as can reduce the overall greenhouse gas emissions. However, the challenge lies in converting technical lignin polymer from biorefinery directly to jet fuel in a continuous operation. In this work, we demonstrate a simultaneous depolymerization and hydrodeoxygenation (SDHDO) process to produce lignin-based jet fuel from the alkali corn stover lignin (ACSL) using engineered Ru-HY-60-MI catalyst in a continuous flow reactor at first time. The maximum carbon yield of LJF of 17.9wt% was obtained, and it comprised of 60.2wt% monocycloalkanes, and 21.6wt% polycycloalkanes. Catalyst characterization of Ru-HY-60-MI suggested there was no significant change in HY zeolite structure and its crystallinity after catalyst engineering. Catalyst characterizations performed post the SDHDO experiments indicate presence of carbon and K content in the catalyst. K content presence in the spent catalyst was due to K + ion was exchanged between lignin solution and HY-60 while carbon presence validated the SDHDO chemistry on the catalyst surface. Tier a fuel property testing indicates that LJF production using SDHDO chemistry can offer SAF with high compatibility, good sealing properties, low emissions, and high energy density for aircraft.

09 BIOMASS FUELS↗

An antiferromagnetic diode effect in even-layered MnBi 2 Te 4

In a p–n junction, the separation of positive and negative charges leads to diode transport, in which charge flows in only one direction. Non-centrosymmetric polar conductors are intrinsic diodes that could be of use in the development of nonlinear applications. Such systems have recently been extended to non-centrosymmetric superconductors, and the superconducting diode effect has been observed. Here, in this paper, we report an antiferromagnetic diode effect in a centrosymmetric crystal without directional charge separation. We observed large second-harmonic transport in a nonlinear electronic device enabled by the compensated antiferromagnetic state of even-layered MnBi 2 Te 4 . We show that this antiferromagnetic diode effect can be used to create in-plane field-effect transistors and microwave-energy-harvesting devices. We also show that electrical sum-frequency generation can be used as a tool to detect nonlinear responses in quantum materials.

electronic properties and materials↗

Dual quantum spin Hall insulator by density-tuned correlations in TaIrTe 4

The convergence of topology and correlations represents a highly coveted realm in the pursuit of new quantum states of matter. Introducing electron correlations to a quantum spin Hall (QSH) insulator can lead to the emergence of a fractional topological insulator and other exotic time-reversal-symmetric topological order, not possible in quantum Hall and Chern insulator systems. Here, in this study, we report a new dual QSH insulator within the intrinsic monolayer crystal of TaIrTe 4 , arising from the interplay of its single-particle topology and density-tuned electron correlations. At charge neutrality, monolayer TaIrTe 4 demonstrates the QSH insulator, manifesting enhanced nonlocal transport and quantized helical edge conductance. After introducing electrons from charge neutrality, TaIrTe 4 shows metallic behaviour in only a small range of charge densities but quickly goes into a new insulating state, entirely unexpected on the basis of the single-particle band structure of TaIrTe 4 . This insulating state could arise from a strong electronic instability near the van Hove singularities, probably leading to a charge density wave (CDW). Remarkably, within this correlated insulating gap, we observe a resurgence of the QSH state. The observation of helical edge conduction in a CDW gap could bridge spin physics and charge orders. The discovery of a dual QSH insulator introduces a new method for creating topological flat minibands through CDW superlattices, which offer a promising platform for exploring time-reversal-symmetric fractional phases and electromagnetism.

electronic devices↗

Hopping frustration-induced flat band and strange metallicity in a kagome metal

The introduction of localized electronic states into a metal can alter its physical properties, for example enabling exotic metal physics including heavy fermion and strange metal behaviour. A common source of localized states in such systems are partially filled 4f and 5f shells because of the inherently compact nature of those orbitals. The interaction of electrons in these orbitals with the conduction sea is well described by the Kondo framework. However, there have also been observations of Kondo-like behaviour in 3d transition metal oxides and in 4d- and 5d-containing van der Waals heterostructures. This calls for a broader consideration of the physical requirements for Kondo systems. Here we show transport and thermodynamic hallmarks of heavy fermion and strange metal behaviour that arise in the kagome metal Ni3In, wherein the source of localized states is destructive interference-induced band flattening of partially filled Ni 3d states. With magnetic field and pressure tuning, here we also find evidence that the system is proximate to quantum criticality, extending the analogy to f-electron Kondo lattices. These observations highlight the role of hopping frustration in metallic systems as a potential source for strong correlations. Additionally, this suggests a lattice-driven approach to realizing correlated metals with non-trivial band topology.

36 MATERIALS SCIENCE↗

Quantum metric nonlinear Hall effect in a topological antiferromagnetic heterostructure

Quantum geometry in condensed matter physics has two components: the real part quantum metric and the imaginary part Berry curvature. Whereas the effects of Berry curvature have been observed through phenomena such as the quantum Hall effect in 2D electron gases and the anomalous Hall effect (AHE) in ferromagnets, quantum metric has rarely been explored. Here, in this paper, we report a nonlinear Hall effect induced by quantum metric dipole by interfacing even-layered MnBi 2 Te 4 with black phosphorus. The quantum metric nonlinear Hall effect switches direction upon reversing the AFM spins and exhibits distinct scaling that is independent of the scattering time. Our results open the door to discovering quantum metric responses predicted theoretically and pave the way for applications that bridge nonlinear electronics with AFM spintronics.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Axion optical induction of antiferromagnetic order

Using circularly polarized light to control quantum matter is a highly intriguing topic in physics, chemistry and biology. Previous studies have demonstrated helicity-dependent optical control of chirality and magnetization, with important implications in asymmetric synthesis in chemistry; homochirality in biomolecules; and ferromagnetic spintronics. We report the surprising observation of helicity-dependent optical control of fully compensated antiferromagnetic order in two-dimensional even-layered MnBi 2 Te 4 , a topological axion insulator with neither chirality nor magnetization. Furthermore, to understand this control, we study an antiferromagnetic circular dichroism, which appears only in reflection but is absent in transmission. We show that the optical control and circular dichroism both arise from the optical axion electrodynamics. Our axion induction provides the possibility to optically control a family of PT-symmetric antiferromagnets (P, inversion; T, time-reversal) such as Cr 2 O 3 , even-layered CrI3 and possibly the pseudo-gap state in cuprates. In MnBi 2 Te 4 , this further opens the door for optical writing of a dissipationless circuit formed by topological edge states.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Continuous hydrodeoxygenation of lignin to jet-range aromatic hydrocarbons

Sustainable aviation fuel (SAF) is essential to decrease the carbon footprint of the aviation industry. Although many strategies have been developed to provide the branched, aliphatic components of SAF, few viable strategies have been demonstrated to supply the aromatic and cycloalkane fraction of SAF at the necessary scale from bio-based feedstocks. Lignin is the largest natural source of renewable aromatic compounds, yet major challenges in deoxygenation have prevented its use as a feedstock for SAF. Here we report a continuous, two-stage catalytic process using molybdenum carbide to deoxygenate lignin from poplar into aromatic hydrocarbons with 87.5% selectivity towards aromatic hydrocarbons at 86% of the theoretical carbon recovery. This work demonstrates an effective approach to convert lignin into aromatic SAF blendstocks.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Synthetic aromatic kerosene property prediction improvements with isomer specific characterization via GCxGC and vacuum ultraviolet spectroscopy

This research explores an advanced method of fuel composition determination and builds upon typical hydrocarbon group type analyses performed with two-dimensional gas chromatography (GCxGC). In this study, structural information of individual species within Virent’s Synthetic Aromatic Kerosene (SAK) is identified by vacuum ultraviolet (VUV) spectroscopy. By mass, 71.3% of the components elute within six peaks of the chromatogram, from which 12 unique species are identified through a novel deconvolution method. Overall, the identification of 93.6%m across 26 structural isomers is made by the methods described in this work. With 93.6%m ascribed to specific isomers, the precision of fuel property predictions improves dramatically. For example, the absolute error of the viscosity prediction is reduced by 90% because of this advancement in diagnostic capability, and its 95-percentile confidence interval (precision only) is reduced by 93%. Additionally, the properties of SAK, blended with hydro processed esters fatty acids (HEFA), are demonstrated to have blended properties consistent with conventional jet fuel.

10 SYNTHETIC FUELS↗

Replication Data for: On the Origin of Sinter-Resistance and Catalyst Accessibility in Raspberry-Colloid-Templated Catalyst Design

The data underlying this published work have been made publicly available in this repository as part of the IMASC Data Management Plan. This work was supported as part of the Integrated Mesoscale Architectures for Sustainable Catalysis (IMASC), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award # DE-SC0012573.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

On the Origin of Sinter‐Resistance and Catalyst Accessibility in Raspberry‐Colloid‐Templated Catalyst Design

Abstract Nanoparticle (NP) sintering is a major cause of the deactivation of supported catalysts. Raspberry‐colloid‐templated (RCT) catalysts are an emerging class of materials that show an unprecedented level of sinter‐resistance and exhibit high catalytic activity. Here a comprehensive study of the origin of NP stability and accessibility in RCT catalysts using theoretical modeling, 3D electron microscopy, and epitaxial overgrowth is reported. The approach is showcased for silica‐based RCT catalysts containing dilute Pd‐in‐Au NPs previously used in hydrogenation and oxidation catalysis. Modeling of the contact line of the silica precursor infiltrating into the assembled raspberry colloids suggests that a large part of the particles must be embedded into silica, which is confirmed by quantitative visualization of >200 individual NPs by dual‐axis electron tomography. The RCT catalysts have a unique structure in which all NPs reside at the pore wall but have >50% of their surface embedded in the matrix, giving rise to the strongly enhanced thermal and mechanical stability. Importantly, epitaxial overgrowth of Ag on the supported NPs reveals that not only the NP surface exposed to the pore but the embedded interface as well remained chemically accessible. This mechanistic understanding provides valuable guidance in the design of stable catalytic materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Layer Hall effect in a 2D topological axion antiferromagnet

While ferromagnets have been known and exploited for millennia, antiferromagnets (AFMs) were only discovered in the 1930s. The elusive nature indicates AFMs' unique properties: At large scale, due to the absence of global magnetization, AFMs may appear to behave like any non-magnetic material; However, such a seemingly mundane macroscopic magnetic property is highly nontrivial at microscopic level, where opposite spin alignment within the AFM unit cell forms a rich internal structure. In topological AFMs, such an internal structure leads to a new possibility, where topology and Berry phase can acquire distinct spatial textures. Here, we study this exciting possibility in an AFM Axion insulator, even-layered MnBi 2 Te 4 flakes, where spatial degrees of freedom correspond to different layers. Remarkably, we report the observation of a new type of Hall effect, the layer Hall effect, where electrons from the top and bottom layers spontaneously deflect in opposite directions. Specifically, under no net electric field, even-layered MnBi 2 Te 4 shows no anomalous Hall effect (AHE); However, applying an electric field isolates the response from one layer and leads to the surprising emergence of a large layer-polarized AHE (~50e 2 /h). Such a layer Hall effect uncovers a highly rare layer-locked Berry curvature, which serves as a unique character of the space-time PT-symmetric AFM topological insulator state. Moreover, we found that the layer-locked Berry curvature can be manipulated by the Axion field, E∙B, which drives the system between the opposite AFM states. Our results achieve previously unavailable pathways to detect and manipulate the rich internal spatial structure of fully-compensated topological AFMs. The layer-locked Berry curvature represents a first step towards spatial engineering of Berry phase, such as through layer-specific moiré potential.

36 MATERIALS SCIENCE↗

Replication Data for: Aggregated nanoparticles: Sample preparation and analysis by atom probe tomography

The data underlying this published work have been made publicly available in this repository as part of the IMASC Data Management Plan. This work was supported as part of the Integrated Mesoscale Architectures for Sustainable Catalysis (IMASC), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award # DE-SC0012573.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Imaging Electrons in Two Dimensional Materials (Final report)

Two-dimensional (2D) materials have extraordinary characteristics that offer promising new approaches for science and technology. Electrons in graphene can move ballistically through a sheet, even though it is only a single atom thick. And transition metal dichalcogenide materials can be cleaved into 2D flakes of all types – metals, semiconductors, insulators, magnetic materials, and superconductors. To benefit from these discoveries, the science needs to be understood to transform 2D materials into useful new devices and systems. The evolution in time of atomic scale graphene structures has been studied in time with a transmission electron microscope (TEM), and ballistic transport of electrons in graphene was been imaged using a cooled scanning probe microscope (SPM), as well as electron motion in MoS 2 . Graphene is only one atom thick but is extremely strong, creating the opportunity to fabricate atomic scale structures in the lateral direction. Using an atomic resolution TEM, a suspended sheet of graphene can be shaped by a Si impurity atom on its surface that acts like a chisel to open up apertures, one atom at a time. The electrons in the TEM provide both the chiseling energy and the ability to image the results. Electrons and holes in graphene form a new type of electronic system with conical conduction and valence bands that meet at the Dirac point, with no energy gap. For moderate densities, the carriers form a Fermi liquid with ballistic transport over micron-scale distances. Using a cooled SPM the cyclotron orbit of electrons in graphene has been imaged. In the magnetic focusing regime, electrons leaving a point contact circle around and leave from a second point contact when the cyclotron diameter is equal to the contact spacing. The paths of electrons are focused - they enter at different angles but converge again at the exiting contact. When the SPM tip knocks an electron out of its orbit, an imaging signal is created. The ballistic motion of carriers in graphene opens the way for ballistic devices that manipulate beams of electrons and holes. Our collaborator Gil-Ho Lee, in Philip Kim's group, created a collimating contact by placing zig-zag absorbers on either side of entering electrons. Our cooled SPM was used to image the electron beam and determine its 9-degree halfwidth. By changing the gate voltage, a collimated beam of holes was also created, opening the way for colliding beam experiments. Coherent beams of carriers are desirable for quantum information processing. Via Andreev reflection, superconducting contacts can covert Cooper pairs in a superconductor to an ingoing and outgoing electrons and holes. Using our cooled SPM, Andreev reflection was imaged from a superconducting contact on a graphene device. Magnetic focusing was used to create an incoming beam of electrons and an outgoing beam of holes, detected by a third point contact. The images show a clear transition from normal reflection above the superconducting transition temperature to Andreev reflection as the device is cooled. Transition metal dichalcogenides offer a wide array of materials that can be exfoliated into ultrathin 2D sheets. A cooled SPM can be used to detect quantum dots as well as to image electron flow. The tip charge capacitively couples to electrons on the dot, acting as a gate to tune the dot conductance. Coulomb blockade peaks appear as a bullseye pattern in an SPM image as the tip is raster scanned above the dot. This approach was used to detect quantum dots in a MoS 2 channel as the carrier density was reduced and electrons pooled in low energy points. Through our DOE supported research, cooled SPM imaging has proven to be a very useful tool to uncover the motion of electrons and holes in the new quantum materials graphene and MoS 2 .

36 MATERIALS SCIENCE↗