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At least 1,639 records · Page 91

Scale-up of microwave-assisted, continuous flow, liquid phase reactors: Application to 5-Hydroxymethylfurfural production

Microwave (MW) technology can be powerful for the electrification and intensification of chemical manufacturing. However, very few examples of scaled MW processes exist. In this work, we build a scaled, MW-assisted, continuous flow reactor for the processing of liquid phase chemistries with specific application to 5-hydroxymethylfurfural (HMF) production. Here, we demonstrate a corresponding computational fluid dynamics model to simulate the reactor’s temperature profile and performance, both of which are in good agreement with experiments. We construct a surrogate model to relate operating parameters to performance for guiding experiments, without demanding simulations, via active learning. Heat recirculation is demonstrated in this scaled reactor, further extending its scale and reducing the energy demand. An HMF yield of ~55 % and a productivity of 0.1 kg/hr, 8x higher than any other reactor, at a flowrate >20x than prior work, are demonstrated while maintaining energy efficiency of >98 %. A basic economic analysis estimates a $1.85/kg cost of HMF from fructose and >60 % reduction in CO 2 emissions than a conventional system without considering the impact of green electricity. We demonstrate that MW technology is well-applied to systems larger than the laboratory scale, and strategies to further reduction in cost and CO 2 are discussed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Online residence time distribution measurement of thermochemical biomass pretreatment reactors

Residence time is a critical parameter that strongly affects the product profile and overall yield achieved from thermochemical pretreatment of lignocellulosic biomass during production of liquid transportation fuels. The residence time distribution (RTD) is one important measure of reactor performance and provides a metric to use when evaluating changes in reactor design and operating parameters. An inexpensive and rapid RTD measurement technique was developed to measure the residence time characteristics in biomass pretreatment reactors and similar equipment processing wet-granular slurries. Sodium chloride was pulsed into the feed entering a 600 kg/d pilot-scale reactor operated at various conditions, and aqueous salt concentration was measured in the discharge using specially fabricated electrical conductivity instrumentation. This online conductivity method was superior in both measurement accuracy and resource requirements compared to offline analysis. Experimentally measured mean residence time values were longer than estimated by simple calculation and screw speed and throughput rate were investigated as contributing factors. In conclusion, a semi-empirical model was developed to predict the mean residence time as a function of operating parameters and enabled improved agreement.

09 BIOMASS FUELS↗

Quantifying transport and electrocatalytic reaction processes in a gastight rotating cylinder electrode reactor via integration of Computational Fluid Dynamics modeling and experiments

Understanding the complexity of the multiple processes of mass, momentum, charge, and heat transport, and how these affect reaction kinetics at the electrode/electrolyte interface is one of the major challenges in the field of energy and catalysis. The rapid and rational scale-up of electrocatalytic systems to industrial scales require a detailed understanding of nonlinear transport-reaction processes, accessible only through the building of multi-physics models that capture with high fidelity the complexity of real-world devices. The gastight rotating cylinder electrode (RCE) reactor is a promising lab-scale tool that can decouple transport from intrinsic kinetics to generate data for first-principle models useful in the design of industrial, electrochemical reactors. Computational Fluid Dynamics (CFD) studies have previously been used to investigate the bulk flow in RCE reactors for simple corrosion and electroplating processes. However, the quantification of changes in local concentration within the viscous layer where catalysis takes place requires capturing the correct flow conditions inside the hydrodynamic boundary layer near the surface of the electrode. Further, this requires simulations with spatial resolution in the nm and μm scale and temporal resolutions between ms and s scales that are similar to the timescales for reactions on the electrode surface. In this study, experimental electrocatalysis is combined with CFD modeling to elucidate and parameterize the hydrodynamics in a gastight RCE reactor. CFD simulations of the electrochemical ferricyanide reduction reaction under mass transport limited conditions are used to evaluate the validity of the CFD model parameters by comparing calculated dimensionless mass transport descriptors to dimensionless correlations obtained experimentally. Justifications for assumptions and details of the simulation methods used in this study are presented to provide a detailed understanding of the effect that each model parameter has on the ability to accurately simulate electrocatalysis in RCE systems. The simulation methodology reported here is a first step towards the development of multi-scale models for the study of transport dependent electrocatalytic processes, such as the electrochemical transformation of CO 2 to fuels and chemicals.

42 ENGINEERING↗

Zigzag flow reactor for weekly thermochemical energy storage

This paper describes theoretical models and experimental performance of a novel Zigzag Flow Reactor (ZFR) for weekly thermochemical energy storage. The ZFR reduces redox-active metal oxide (MO x ) particles at high temperature (up to ~1100 °C) under inert gas sweep. A physical model demonstrates the approach to process equilibrium by minimizing the associated exergy destruction in a finite number of reaction steps, establishing the thermodynamic requirements for a practical reactor. The model results show several cost-relevant parameter tradeoffs, and the tradeoff analysis implies a cost-optimized set of boundary conditions. Numerical models and prototypes show that the ZFR enables significant gas phase homogenization while simultaneously enabling a customizable MO x residence time in the reactor, both key requirements for approaching an equilibrium process. A scaling model demonstrates the simplicity and affordability of sizing the ZFR to grid-scale levels, with fabrication costs at least five times lower than previously proposed scalable reactor concepts. As a result, a laboratory ZFR prototype achieved an energy storage density of ~90 Wh/kg with CaAl 0.2 Mn 0.8 O 3-δ as the MO x , at temperatures of ~850 °C in >10 h of total runtime.

Thermochemical energy storage↗

MELCOR-TMAP: The integration of MELCOR for fusion and TMAP4 for fusion reactor systems safety analysis and tritium inventory tracking

The design of fusion reactors requires the prediction of radioactive tritium migration during normal operating conditions and accident scenarios. Safety standards such as those from the U.S. Department of Energy (DOE) require that fusion reactor designs limit the release of hazardous material to the environment. In addition to safety requirements, the rarity of tritium supplies for burning D-T fusion plasma requires tritium breeding blankets. Computational modeling of migration of tritium and various reaction products throughout the fusion reactor serves to create designs that fulfill these requirements. MELCOR-TMAP, owned and developed at Idaho National Laboratory (INL), is an integrated system-level engineering code adapted for the analysis of fusion reactor systems. The history of the conception and evolution of the MELCOR-TMAP code, as well as its current capabilities, recent updates including a corrected composite material wall nodalization scheme, and plans for future development, are discussed here.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

A machine-learning-aided data recovery approach for predicting multi-material thermal behaviors in advanced test reactor capsules

Instrumented experiments conducted at test reactors are essential to the deployment of new advanced reactor systems. Designing new experiments and generating data on specific reactor conditions require significant investments in terms of both time and cost. Finite element analysis software can be used to create high-fidelity models of experiment environments in order to support the actual experiments, but computation time remains a concern in terms of applying outcomes to real-time usage of data (e.g., a digital twin [DT]). Here, the present research proposes a machine-learning (ML) aided approach to making temperature and displacement predictions based on the thickness of the outer gas gap on the experimental capsule used for in-pile demonstration of a novel new thermal conductivity probe in the Advanced Test Reactor (ATR). This capsule consisted of U10Zr fuel, a rodlet, sodium, and inner and outer capsules. Gas gaps existed between the fuel and the rodlet, and between the inner and the outer capsule. The learning data pertained to an experimental capsule's radial distributions of temperature and displacement, as obtained based on Abaqus and the physical features. For the first step of ML sequence, the temperature was predicted using three positional parameters. Next, the displacement was predicted using seven additional parameters. Each physical feature was normalized in order to be both nondimensional and standardized. The temperature and displacement predictions showed good agreement with the simulation results in all cases involving interpolation and extrapolation. Furthermore, data similarity enhancement increased the similarity between the training and the target data, thereby increasing the predictive accuracy of the ML models. In certain extrapolation cases involving limited original ML model accuracy, data similarity enhancement and data recovery was able to somewhat improve this accuracy.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Modeling of a direct solar receiver reactor for decomposition of sulfuric acid in thermochemical hydrogen production cycles

Hydrogen production thermochemical cycles, based on the recirculation of sulfur-based compounds, are among the best suited processes to produce hydrogen using concentrated solar power. The sulfuric acid decomposition section is common to each sulfur-based cycle and represents one of the fundamental steps. A new direct solar receiver reactor concept is conceived, conceptually designed and simulated. A detailed transport phenomena model, including mass, energy and momentum balance expressions as well as suitable decomposition kinetics, is described adopting a finite volume approach. A single unit reactor is simulated with an inlet flow rate of 0.28 kg/s (corresponding to a production of approximately 11 kg H2 /h in a Hybrid Sulfur process) and a direct solar irradiation at a constant power of 143 kW/m 2 . Results, obtained for the high temperature catalytic decomposition of SO 3 into SO 2 and O 2 , demonstrate the effectiveness of the proposed concept, operating at pressures of 14 bar. A maximum temperature of 879 C is achieved in the reactor body, with a corresponding average SO 2 mass fraction of 27.8%. The overall pressure drop value is 1.7 bar. The reactor allows the SO 3 decomposition into SO 2 and O 2 to be realized effectively, requiring an external high temperature solar power input of 123.6 kJ/molSO 2 (i.e. 123.6 kJ/mol H2 ).

14 SOLAR ENERGY↗

A composite position independent monitor of reactor fuel irradiation using Pu, Cs, and Ba isotope ratios

When post-irradiation materials from the nuclear fuel cycle are released to the environment, certain isotopes of actinides and fission products carry signatures of irradiation history that can potentially aid a nuclear forensic investigation into the material's provenance. In this study, combinations of Pu, Cs, and Ba isotope ratios that produce position (in the reactor core) independent monitors of irradiation history in spent light water reactor fuel are identified and explored. These position independent monitors (PIMs) are modeled for various irradiation scenarios using automated depletion codes as well as ordinary differential equation solutions to approximate nuclear physics models. Experimental validation was performed using irradiated low enriched uranium oxide fuel from a light water reactor, which was sampled at 8 axial positions from a single rod. Plutonium, barium and cesium were chemically separated and isotope ratio measurements of the separated solutions were made by quadrupole and multi-collector inductively coupled mass spectrometry (Cs and Pu, respectively) and thermal ionization mass spectrometry (Ba). The effect of axial variations in neutron fluence and energy spectrum are evident in the measured isotope ratios. Furthermore, two versions of a combined Pu and Cs based PIM are developed. A linear PIM model, which can be used to solve for irradiation time is found to work well for natural U fuel with <10% 240 Pu and known or short cooling times. A non-linear PIM model, which cannot be solved explicitly for irradiation time without additional information, can nonetheless still group samples by irradiation history, including high burnup LEU fuel with unknown cooling time. 137 Ba/ 138 Ba is also observed to act as a position independent monitor; it is nearly single valued across the sampled fuel rod, indicating that samples sharing an irradiation history (same irradiation time and cooling time) in a reactor despite experiencing different neutron fluxes will have a common 137 Ba/ 138 Ba ratio. Modeling of this Ba PIM shows it increases monotonically with irradiation and cooling time, and a confirmatory first order analytical solution is also presented.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Possible impacts of molten salt reactors on the International Monitoring System

Molten salt reactors (MSRs) are gaining support as many countries look for ways to increase power generation and replace aging nuclear energy production facilities. MSRs have inherently safe designs, are scalable in size, can burn transuranic wastes from traditional solid fuel nuclear reactors, can store excess heat in thermal reservoirs for water desalination, and can be used to produce medical isotopes as part of the real-time liquid-fuel recycling process. The ability to remove 135 Xe in real time from the fuel improves the power production in an MSR because 135 Xe is the most significant neutron-absorbing isotope generated by nuclear fission. Xenon-135, and other radioactive gases, are removed by sparging the fuel with an inert gas while the liquid fuel is recirculated from the reactor inner core through the heat exchangers. Without effective abatement technologies, large amounts of radioactive gas could be released during the sparging process. This work examines the potential impact of radioxenon releases on samplers used by the International Monitoring System (IMS) to detect nuclear explosions. Here, atmospheric transport simulations from seven hypothetical MSRs on different continents were used to evaluate the holdup time needed before release of radioxenon so IMS samplers would register few detections. Abatement technologies that retain radioxenon isotopes for at least 120 d before their release will be needed to mitigate the impacts from a molten salt breeder reactor used to replace a nuclear power plant. A holdup time of about 150 d is needed to reduce emissions to the average level of current nuclear power plants.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Performance of low smeared density sodium-cooled fast reactor metal fuel

An experiment was performed in the Experimental Breeder Rector-II (EBR-II) in the 1990s to show that metallic fast reactor fuel could be used in reactors with a single, once-through core. To prove the long duration, high burnup, high neutron exposure capability an experiment where the fuel pin was designed with a very large fission gas plenum and very low fuel smeared density (SD). The experiment, X496, operated to only 8.3 at. % burnup because the EBR-II reactor was scheduled for shut-down at that time. Many of the examinations of the fuel pins only funded recently with the resurgence of reactor designs using very high-burnup fuel. The results showed that, despite the low smeared density of 59% the fuel swelled radially to contact the cladding, fission gas release appeared to be slightly higher than demonstrated in conventional 75%SD fuel tests and axial growth was about the same as 75% SD fuel. There were axial positions in some of the fuel pins which showed evidence of fuel restructuring and an absence of fission products with low metaling points and gaseous precursors (Cs and Rb). Lastly, a model to investigate whether these areas may have overheated due to a loss of bond sodium indicates that it is a possible explanation for the fuel restructuring and something to be considered for fuel performance modeling of low SD fuel.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Effect of reactor radiation on the thermal conductivity of TREAT fuel

The Transient Reactor Test Facility (TREAT) at the Idaho National Laboratory is resuming operations after more than 20 years in latency in order to produce high-neutron-flux transients for investigating transient-induced behavior of reactor fuels and their interactions with other materials and structures. A parallel program is ongoing to develop a replacement core in which the fuel, historically containing highly-enriched uranium (HEU), is replaced by low-enriched uranium (LEU). Both the HEU and prospective LEU fuels are in the form of UO 2 particles dispersed in a graphite matrix, but the LEU fuel will contain a much higher volume of UO 2 particles, which may create a larger area of interphase boundaries between the particles and the graphite. This may lead to a higher volume fraction of graphite exposed to the fission fragments escaping from the UO 2 particles, and thus may induce a higher volume of fission-fragment damage on the fuel graphite. In this work, we analyzed the reactor-radiation induced thermal conductivity degradation of graphite-based dispersion fuel. A semi-empirical method to model the relative thermal conductivity with reactor radiation was proposed and validated based on the available experimental data. Prediction of thermal conductivity degradation of LEU TREAT fuel during a long-term operation was performed, with a focus on the effect of UO 2 particle size on fission-fragment damage. Lastly, the proposed method can be further adjusted to evaluate the degradation of other properties of graphite-based dispersion fuel.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Development of the technological process for the IGR reactor's highly-enriched irradiated uranium-graphite fuel immobilization

The immobilization of irradiated highly enriched uranium (HEU) fuel is a critical component of nuclear waste management and non-proliferation efforts. In Kazakhstan, at National Nuclear Center of the Republic of Kazakhstan special attention is given to managing legacy HEU fuel from research reactors. One such case involves the IGR research reactor, whose first core containing irradiated HEU uranium-graphite fuel was operated from 1961 to 1966 and removed following reactor modernization. This fuel now requires a reliable and secure immobilization strategy. Here, this paper presents the development of a technological process for immobilizing this fuel to reduce its enrichment to below 20 % in terms of 235U content. The proposed method involves down-blending irradiated HEU fuel with depleted uranium, followed by encapsulation in a Portland cement matrix. Full-scale experiments were conducted to assess the uniformity of uranium distribution within the matrix. The results confirm the effectiveness of this approach, ensuring reliable immobilization of fuel in accordance with international requirements, including IAEA standards and Kazakhstan's regulatory framework. These findings contribute to the broader effort of adapting immobilization strategies for the safe management of spent fuel from research reactors.

12 - MGMT OF RADIOACTIVE AND NON-RADIOACTIVE WASTE↗

In situ observation of irradiation-induced enhancement to the desorption pressure of zirconium hydride in a nuclear reactor

We quantify the effect of a nuclear-reactor environment on the hydrogen isotope equilibrium vapor pressure over pure zirconium and zirconium hydride. A vacuum-sealed capsule containing a zirconium foil with 6 atom% deuterium was irradiated at a neutron flux of ~10 14 cm -2 s -1 at the University of Missouri Research Reactor (MURR). The internal stainless-steel (SS) sample holder acted as the heat source via gamma absorption. To measure low desorption pressures in a high-flux environment, we developed a method to transduce pressure from the measured sample temperature during irradiation, calibrating with known deuterium pressures in unirradiated capsules at various heating powers using an internal filament-heated system designed to mimic irradiation-induced heating. Our temperature-pressure transduction method operates similarly to a Pirani or thermocouple pressure gauge. The in-reactor measurements revealed a roughly 4-fold enhancement in desorption pressure after only 6 h of irradiation (~2 × 10 18 cm -2 neutron fluence) compared to thermal desorption in control experiments, indicating a nonthermal contribution from neutron irradiation. The slower temperature/pressure stabilization rate in the reactor suggests that desorption pressure enhancement increases with neutron fluence. Further, this enhancement signifies increased solubility of hydrogen isotopes in zirconium during irradiation. We propose that high-energy neutron collisions with hydrogen isotopes in hydrides lead to their decomposition at lower temperatures, supersaturating the surrounding αZr lattice and resulting in higher desorption pressure, which continues to rise as more hydrides dissolve with increasing neutron fluence.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Oxidative coupling of methane (OCM) conversion into C 2 products through a CO 2 /O 2 co-transport membrane reactor

Oxidative coupling of methane (OCM), which transforms CH 4 into C 2 products (C 2 H 6 and C 2 H 4 ) with molecular O 2 as the oxidant, is one of the most studied direct methane conversions (DMCs). However, a major technical hurdle to the OCM process is to achieve high CH 4 conversion at high C 2 (C 2 H 6 and C 2 H 4 ) selectivity. One rudimentary cause for this “tradeoff” behavior is the high chemical reactivity of the products (C 2 H 6 or C 2 H 4 ), which can be re-oxidized by O 2 . To overcome this thermodynamic challenge, minimizing the oxidizing power of the oxidant and lowering the local oxygen partial pressure are keys. Here, In this work, we demonstrate a new membrane reactor that capture CO 2 /O 2 from a flue gas and uses it for OCM conversion. The results show that the co-captured CO 2 /O 2 mixture converts CH 4 into C 2 H 6 in the presence of a 2%Mn–5%Na 2 WO 4 /SiO 2 catalyst, followed by thermal cracking of C 2 H 6 into C 2 H 4 and H 2 . The presence of CO 2 decreases the local partial pressure of O 2 , thus reducing the propensity of C 2 -products re-oxidation and leading to a higher C 2 selectivity. We show that a small button-type membrane reactor can achieve 12% C 2 yield with ~57% C 2 -selectivity using a diluted CH 4 -Ar mixture as the feedstock. We expect higher C 2 yield with tubular plug-flow membrane reactors in the future. We also highlight the unique advantage of the membrane reactor in intensifying CO 2 capture from both flue gas and OCM purification process into one single step.

42 ENGINEERING↗

Multi-principal element alloys for fast reactor cladding applications

Given the extensive list of multi-principal element alloys (MPEAs) within literature and the overwhelming number of alloys that can be made from only a handful of elements, this article proposes a methodology for prioritizing alloys for use as cladding within advanced reactors. This paper applies neutronic, mechanical, and chemical assessments to a collection of MPEAs available within literature for use as advanced reactor cladding. The results are compared to a reference design of HT9, a ferritic/martensitic steel, for employed in sodium-cooled fast reactor. Mechanical assessments determined pressure limits for a thin-walled tube pressure boundary, thus relating the material's mechanical properties to a minimum acceptable wall thickness. Neutronic analyses reveal a maximum allowable wall thickness that a given material must meet to provide a level of neutronic economy that is equivalent to than that of HT9. Lastly, each alloying element is compared to typical fission products found in a fast reactor fuels to mitigate deleterious phenomena such as fuel-cladding chemical interactions (FCCI). These analyses indicate that Mo-Nb-Ti-V-based alloys are likely to be advantageous and that the inclusion of elements with a high neutronic penalty (e.g., Hf) could be considered with minimal consequences.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

The radioactive source calibration system of the PROSPECT reactor antineutrino detector

The Precision Reactor Oscillation and Spectrum (PROSPECT) Experiment is a reactor neutrino experiment created to search for sterile neutrinos with a mass on the order of 1 eV/c 2 and to measure the spectrum of electron antineutrinos from a highly-enriched 235 U nuclear reactor. The PROSPECT detector consists of an 11 by 14 array of optical segments in 6 Li-loaded liquid scintillator at the High Flux Isotope Reactor in Oak Ridge National Laboratory. Antineutrino events are identified via inverse beta decay and read out by photomultiplier tubes located at the ends of each segment. The detector response is characterized using a radioactive source calibration system. Here, we describe the design, operation, and performance of the PROSPECT source calibration system.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

On the flow induced vibration of an externally excited nuclear reactor experiment

An in-pile, drop-in experiment design is presently being designed and studied for the near-term deployment within the Advanced Test Reactor (ATR) located at the Idaho National Laboratory (INL); this experiment is termed the Miniplate-1 Large-B (MP-1 LB) Experiment. A number of explicit studies are performed during the design- and safety-related stage. Traditionally, a clear and logical methodology has been developed and utilized for analyses such as hydraulics, thermal-loads, mechanical loads, and others for these experiments. Recently a small component from a different experiment assembly mechanically separated while in the reactor’s core. While this experiment didn’t compromise the safety of the reactor, it led to a higher-level question which centered on whether the appropriate level of consideration was being made toward the fluid–structure-interactions of these experiments. The outcome yielded separate flow test experiments of like-for-like geometry in an experimental loop located at Oregon State University which produces experimental data compliant with applicable parts and requirements to ASME’s NQA-1 2008, 2009a standard – suitable for benchmark evaluation. Here, the objectives of this study are to (1) develop a process for handling and interpreting the mechanical response of the test elements during hydraulic testing, to (2) characterize the motion of a specific test element during a flow test which imposes a wide range of hydraulic conditions, and (3) provide objective observations toward the potential safety related implications that are tied to the synthesized data. The outcome of this study has led to a confident process in inspecting the experimental data, synthesized it for interpretation, identified several unique hydraulic characteristics of the experiment design which were previously unknown, and demonstrated that the likelihood for mechanical failure resulting from fluid-structure-interactions in the reactor is far below any criterion for concern of the element’s safety.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Three-dimensional flow model development for thermal mixing and stratification modeling in reactor system transients analyses

Mixing, thermal-stratification, and mass transport phenomena in large pools or enclosures play major roles for the safety of reactor systems. Depending on the fidelity requirement and computational resources, various modeling methods, from the 0-D perfect mixing model to 3-D Computational Fluid Dynamics (CFD) models, are available. Each is associated with its own advantages and shortcomings. It is very desirable to develop an advanced and efficient thermal mixing and stratification modeling capability embedded in a modern system analysis code to improve the accuracy of reactor safety analyses and to reduce modeling uncertainties. An advanced system analysis tool, SAM, is being developed at Argonne National Laboratory for advanced non-LWR reactor safety analysis. While SAM is being developed as a system-level modeling and simulation tool, a reduced-order three-dimensional module is under development to model the mull-dimensional flow and thermal mixing and stratification in large enclosures of reactor systems. This paper provides an overview of the three-dimensional finite element flow model in SAM, including the governing equations, stabilization scheme, and solution methods. Additionally, several verification and validation tests are presented, including lid-driven cavity flow, natural convection inside a cavity, laminar flow in a channel of parallel plates. Here, based on the comparisons with the analytical solutions and experimental results, it is demonstrated that the developed 3-D fluid model can perform very well for a wide range of flow problems.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗