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DOE OSTI2025

Supported Single‐Atom Manganese Catalysts for the Trimerization of Ethylene

Selective ethylene oligomerization via oxidative cyclization, forming metallacyclic intermediates, is typically catalyzed by molecular titanium and chromium complexes to produce butenes, hexenes, or octenes, depending on the supporting ligand framework. However, this mechanism requires significant electron density at the metal active site and is not known to be generalizable to other first-row transition metals. In this work, we computationally investigate the electronic modulation of five transition metals (Mn, Fe, Co, Ni, and Cu) supported on titania (TiO₂) through reductive lithium intercalation to promote selective oligomerization via oxidative cyclization, using density functional theory (DFT). Our findings predict that Mn/LiTiO₂ exhibits high catalytic activity due to the exergonic nature of oxidative cyclization with two ethylene molecules. Additionally, lithium titanate (LiTiO₂) supports enhance catalytic performance compared to TiO₂. Experimental validation confirms that Mn/LiTiO₂ achieves higher conversion rates and improved selectivity toward hexene (C₄:C₆ = 1:2.6). The enhanced activity is attributed to lithiation, which alters the electronic environment around Mn active sites. Mechanistic studies reveal that the formation of a seven-membered ring, a key intermediate for hexene formation, is more favorable on LiTiO₂ than TiO₂. This work provides the first evidence of Mn catalyzing selective ethylene oligomerization via oxidative cyclization in either homogeneous or heterogeneous catalysis.

Kim, Yu Lim [Argonne National Laboratory (ANL), Ar↗

DOE OSTI2025

In situ deformation of antigorite-olivine two-phase mixtures: Implications for dynamics and seismic anisotropy in the mantle wedge

Water released from hydrous minerals in subducting slabs reacts with the overlying plate, resulting in widespread serpentinization in the mantle wedge. Deformation of serpentinized peridotites has been invoked to explain forearc seismic anisotropy, yet studies of the mechanical properties and deformation behaviors of serpentine-bearing multiphase aggregates remain limited. Here we deformed olivine-antigorite mixtures containing 70, 50, and 20 vol.% of antigorite at 2.5 – 7.6 GPa, 673 K and strain rates of ∼10 –5 –10 –4 s –1 . Elasto-viscoplastic self-consistent simulations, constrained by synchrotron X-ray diffraction (XRD) data, were used to estimate lattice strain, stress–strain partitioning, crystallographic preferred orientations (CPO) development, and aggregate strength. Selected run products were also analyzed by electron backscatter diffraction for comparison with the CPO results obtained from XRD experiments. We found olivine transitions from A- or B-type to C-type when antigorite fraction drops to 20 vol.%, coinciding with a microstructural change from interconnected weak layers to a load-bearing framework (LBF). An additional run on a sample Atg50/Ol50 with preexisting microstructures suggested the formation of LBF was promoted by these microstructures, although the preexisting antigorite CPO has been overprinted at 20.8 % strain and could be erased completely by subsequent deformation in nature. Estimated viscosity of the two-phase mixtures suggests that low-degree serpentinization (≤20 %) in the mantle wedge may increase the strength of olivine-rich peridotite and hinder slab-mantle decoupling, whereas high-degree serpentinization (≥50–70 %) weakens the peridotite and favors decoupling if sufficient viscosity contrast (>10) develops. Seismic anisotropy shows a nonlinear dependence on antigorite fraction: antigorite CPO governs the anisotropy of the mixtures with ≥50 vol.% antigorite, whereas olivine CPO dominates at low fractions (∼20 vol.%). The presence of pre-existing microstructures reduces seismic anisotropy of the deformed mixtures, however the persistence of pre-existing CPO in actively subducting slabs remains uncertain, making their significance over geological timescales questionable.

Crystallographic preferred orientation↗

DOE OSTI2026

Results from the last DD and DT JET campaigns in the framework of the EUROfusion Tokamak Exploitation Work Package activity

JET, the only tokamak capable of operating with deuterium–tritium (D–T) fuel (since TFTR was shutdown in 1999), has provided essential experimental data to support ITER and DEMO design and operation. Within the EUROfusion Tokamak Exploitation Work Package, JET completed its final campaigns (2022–2023), culminating in the third D–T campaign (DTE3). These experiments addressed key challenges in plasma scenarios, exhaust control, and tritium management under reactor-relevant conditions. Significant progress was achieved in demonstrating ITER-like integrated scenarios with impurity seeding, achieving partial divertor detachment and high confinement ($H_{98}(y,2)$ ≈ 0.85) at 3 MA in D–T plasmas. Advanced exhaust regimes such as quasi-continuous exhaust (QCE) and X-point radiator (XPR) were successfully achieved first in D–D and then extended to D–T operation, confirming their relevance for mixed isotope operation. Operational milestones included a new world record of 69 MJ fusion energy in tritium-rich hybrid plasmas and long-pulse H-mode operation up to 60 s, contributing with unique data to the CICLOP database. Physics studies focused on peeling-limited pedestals in support of ITER and improved understanding of edge stability and impurity screening in metallic environments. Extensive usage of the shattered pellet injector (SPI) on JET provided critical information for the design of the ITER disruption mitigation system (DMS). Real-time control systems for D/T ratio control and plasma exhaust were deployed and demonstrated in D–D and D–T, while energetic particle physics investigations unfolded the role of fast ions in turbulence suppression mechanisms. Comprehensive tritium retention studies using gas balance method, post-mortem analysis, and ITER-relevant laser induced desorption spectroscopy (LIDS) diagnostics provided essential input for tritium accountancy strategies. These results are validating the ITER operational concepts, inform DEMO design, and deliver critical experience in nuclear operation and scenario integration.

disruptions↗