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At least 955 records · Page 53

Preliminary Analysis of Species Partitioning in the DWPF Melter - Sludge Batch 7b

The goal of the work described in this report is to provide additional off-gas carryover data from the Defense Waste Processing Facility (DWPF) melter to support the estimation of off-gas carryover rates from the Low Activity Waste (LAW) melter at the Hanford Site. Of particular interest is to determine the volatility of technetium-99 (Tc-99), which is a key isotope of concern for disposal and is a significant challenge to retain in glass in the Hanford waste treatment flowsheet. Since the DWPF melter is not equipped with routine offgas monitoring and/or sampling capabilities, the off-gas carryover data had to be extracted using component mass balance of the measured feed and pour stream (PS) glass compositions under time-averaged melter operating conditions over the duration of one canister-filling cycle, typically 20-25 hours. The method was first tested using the Sludge Batch 6 (SB6) PS sample data taken while Canister #3472 was being filled on 12/20/2010, approximately three months after the (argon) glass bubblers were installed. The method was tested again using the SB7a PS sample data taken while Canister #3619 was being filled on 8/5/2011 with the glass bubblers in operation.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Vitrification of Sellafield Wastes with High Metallic Magnesium Alloy Content - 17495

The Sellafield nuclear complex, located in northwest England, is the largest such site in the United Kingdom. Sellafield Limited, which is the operating contractor for the Nuclear Decommissioning Authority, is evaluating thermal treatment technologies for a potential future facility to process a variety of Intermediate Level Waste sludges and slurries accumulated from historical site operations. In support of that effort, Atkins and the Vitreous State Laboratory (VSL) of The Catholic University of America conducted studies to evaluate the feasibility and implications of installing a joule-heated ceramic melter (JHCM) vitrification system to process a variety of sludge and slurry radioactive wastes at the Sellafield site. These sludges have the potential to contain a significant proportion of reactive metals in localized regions. The metallic fraction derives from unreacted Magnox spent fuel cladding. Thus, an important objective of this work was to investigate the performance of JHCM technology for the treatment of streams with localized regions of high reactive metal contents. The present work was focused on Site Ion Exchange Effluent Plant (SIXEP) Magnox sludges, investigated previously. Suitable waste simulants were developed for the SIXEP Magnox sludge waste stream, which included surrogates for all important radionuclides. High waste-loading, fully compliant glass formulations were designed using a combination of previous experience, extensive waste glass data bases, and small-scale crucible melts. Glasses from the test melts were characterized for properties that are important for processability and product quality. The most viable compositions were then selected for small-scale melter trials to collect information on processing rates and behavior, off-gas and secondary waste compositions, and overall system mass balance. These data were used to support the technology evaluation, which considered such factors as minimization of inactive additions, waste volume reduction, retention of radionuclides, minimization of secondary wastes, and overall process efficiency and effectiveness. The data were also used to develop sizing estimates for the full-scale facility and to estimate treatment durations under various treatment scenarios. A series of tests was then performed with partial replacement of the magnesium hydroxide with a metallic magnesium alloy that is close in composition to Magnox alloy. A commercially available magnesium alloy, Elecktron AZ31B, which has a nominal magnesium content of 95.7%, was used for this purpose. The testing was performed on a DuraMelter 10 (DM10) JHCM system to characterize the melter off-gas, glass product, and the effects of magnesium alloy particle size on feed processing. Data on processing rate and any processing issues, product glass composition, off-gas composition including hydrogen, and system operating parameters, including flows, temperatures, pressures, etc., were collected and analyzed to evaluate the effects of magnesium alloy on the vitrification process. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Effect of Power Plant Capacity on the CAPEX, OPEX, and LCOC of the CO2 Capture Process in Pre-Combustion Applications - Abstract

Aspen Plus v8.8 was used to simulate the pre-combustion CO2 capture process from a typical fuel gas stream at different power plant capacities ranging from 54.3 to 543 MW. Polyethylene glycol polydimethyl siloxane (PEGPDMS-1) was used as a physical solvent to capture CO2 in a countercurrent packed-bed absorber containing a structured packing (Mellapak 250Y). The process pressure was 51.4 bar and the solvent temperature was varied from 10 to 40 <sup>o</sup>C. The internal diameter of the absorber ranged from 1.9 to 7 m and the packing height from 13.9 to 45.5 m. The physico-chemical properties were obtained and modeled using the Perturbed Chain-Statistical Associating Fluid Theory (PC-SAFT) Equation-of-State (EOS).<p> Four process constraints were imposed in Aspen Plus: (1) no flooding in the absorber, (2) the absorber height to diameter ratio (H/D) is greater than or equal 6, (3) at least 90 mol% of the CO2 capture from the fuel gas stream, and (4) the CO2 stream destined to sequestration sites should contain less than 600 ppm water concentration and less than or equal 0.5 mol% of fuel gases (H2, CO, CH4). The plant lifetime was assumed to be 30 years with an annual discount rate of 10% and an annual maintenance cost of 4% of the total capital expenses.</p><p> Seven power plants with different capacities were used and for each plant, the corresponding CO2 capture process was simulated. The absorber flooding was checked using the generalized pressure drop correlation (GPDC) by Leva [1] and the capital expenditure (CAPEX), operating expenditure (OPEX), and levelized costs per ton of CO2 captured (LCOC) were calculated [2-5]. Normalized by the largest power plant capacity (543 MW) used in the simulation, the results indicated that the capital and operating expenditures increased, however, the LCOC decreased with increasing plant capacity. This behavior was due to the increased annual tonnage of the CO2 captured with plant capacity as shown in Figure 1. The calculated CAPEX, OPEX, LCOC and the tonnage of CO2 captured for the 543 MW power plant were about 52 MM$, 22 MM$/year, 7.46 $/ton and 4 MM ton/year.</p>

Ashkanani, Husain↗

Levelized Cost of CO 2 Captured Using Five Physical Solvents in Pre-combustion Applications

Aspen Plus v8.8 was used to perform techno-economic analysis (TEA) of a CO 2 capture process from a typical fuel gas stream in a 543-MW pre-combustion power plant using five different physical solvents (Selexol, PEGPDMS-1, NMP, [aPy][Tf 2 N] and [hmim][Tf 2 N]). The process included a countercurrent packed-bed absorber operating under high-pressure over a wide range of temperatures and three pressure-swing flash drums for solvent regeneration. Furthermore, two packings, Mellapak 250Y and IMTP50, were used and the Levelized costs of CO 2 captured (LCOC) were calculated. The simulation results indicated that using Mellapak 250Y exhibited lower LCOC values than those when using IMTP50 for the five solvents under all conditions used as it offered better mass transfer. The CO 2 capture process carried out at low temperatures showed lower LCOC values than those at higher temperatures due to the increased CO 2 solubility in the solvents at lower temperatures, requiring smaller absorber diameter and lower solvent circulation rates, which offset the cooling requirements. Comparing the lowest LCOC values for the five solvents, the hydrophobic PEGPDMS-1 solvent was the most promising one compared to the other four solvents, due to its lowest capital and operating costs and noncorrosive, which enabled using less expensive materials for the process equipment.

42 ENGINEERING↗

Predictive Chemical Kinetic Modeling: Where We Succeed, Where We Struggle, and What Comes Next

Chemical kinetic modeling plays a foundational role in fields ranging from energy to environmental science, pharmaceuticals, and advanced materials. The past two decades have seen remarkable progress, particularly in modeling gas-phase reactions for thermochemical processes, leading to impactful industrial applications such as steam cracking and air quality management. However, new challenges are emerging. The successful development of systematic methodologies for the description of gas-phase kinetics opens the possibility to apply the same approach to the study of more challenging systems. Here, we review recent advances, including ab initio transition state theory-based master equation estimation of elementary rates, automated mechanism generation, machine-learning-assisted kinetics, and uncertainty quantification, and discuss the advances needed to apply the same methodological approach in areas such as heterogeneous catalysis, electrochemistry, liquid-phase and solid-state reactivity, and multiscale model integration. We advocate for the development of targeted tools, especially methods that go beyond empirical tuning toward first-principles-based predictions. We highlight the need for accessible software and AIaugmented workflows to democratize modeling for industry and academia alike. In this perspective, we call attention to not only what has worked but also what remains unsolved, advocating to avoid overemphasizing successes in scientific works at the expense of realism. The next decade should focus on predictive capability, physical accuracy, and community infrastructure (e.g., databases and services) to enable innovation across diverse fields. We argue that kinetic modeling, properly equipped, can accelerate discovery far beyond its traditional domains.

ab initio calculations↗

Improving the Work Function of Nitrogen-Doped Niobium Surfaces for SRF Cavities by Plasma Processing

Work function and surface chemistries of SiC-polished, electropolished, and nitrogen-doped niobium coupons were analyzed before and after plasma processing using a neon-oxygen gas mixture. These studies represent an initial enquiry into the feasibility of applying the plasma processing technique designed at ORNL for the Spallation Neutron Source (SNS) to the nitrogen-doped Nb cavities for the Coherent Light Source II (LCLS-II). Work function of all measured samples was increased after plasma processing, which indicates the strong potential of the plasma processing technique as a tool for increasing the accelerating gradient of nitrogen-doped cavities.

43 PARTICLE ACCELERATORS↗

Isolated Single Metal Atoms Supported on Silica for One Step Non-Oxidative Methane Upgrading to Hydrogen and Value-Added Hydrocarbons

Natural gas in the United States offers substantial economic opportunities due to its abundance but its transportation is challenging because its primary component, methane (CH 4 ), does not liquefy at ambient temperature and typical pressures. As a result, a significant portion of natural gas is either used for heat, flared in remote locations, or remains unutilized, presenting a lost economic opportunity and an environmental harm. Converting natural gas to larger hydrocarbons in an economically competitive manner would enable transportation of products and further boost the economy and reduce environmental footprint. Our research goal is to enable efficient non-oxidative methane conversion (NMC) via catalyst innovation to convert CH 4 in one-step to olefins and aromatics and hydrogen (H 2 ) co-product. The catalysts are made of supported single metal atoms and operated at medium-high temperatures. The single metal atoms achieve methane activation by heterogeneous surface dehydrogenation to generate a hydrocarbon pool and importantly limit coke formation. The integration of novel single atom catalysts in a short contact time microreactor enable unprecedented NMC performance that could lead to economically-feasible, distributed natural gas upgrading by advanced manufacturing and process intensification. Our innovated catalyst and reactor technology promise to tap into previously uneconomic natural gas resources, such as stranded, vented, and flared methane.

03 NATURAL GAS↗

Single Crystal Casting with Fluidized Carbon Bed Cooling: A Process Innovation for Quality Improvement and Cost Reduction

Superalloy gas turbine blades are being produced by investment casting and directional solidification. A new process, Fluidized Carbon Bed Cooling (FCBC), has been developed and is now being optimized in a prototype casting unit with 10 kg pouring weight. In early test runs with still rather simple mold cluster geometries, a reduction of the primary dendrite arm spacing of around 40 pct compared to the standard radiation cooling process (HRS) could be demonstrated. The improvement is mainly attributed to higher temperature gradients driving solidification, made possible by a functioning Dynamic Baffle. Compared to earlier development efforts in the literature, contamination of the melt and damage to the equipment are avoided using carbon-based fluidized bed materials and the so-called “counter pressure concept.”.

36 MATERIALS SCIENCE↗

Implications of Underground Nuclear Explosion Cavity Evolution for Radioxenon Isotopic Composition

Abstract Isotopic ratios of radioxenons sampled in the atmosphere or subsurface can be used to verify the occurrence of an underground nuclear explosion (UNE). Differences in the half-lives of radioactive xenon precursors and their decay-chain networks produce different time-dependent concentration profiles of xenon isotopes allowing isotopic ratios to be used for tracking UNE histories including estimating the time of detonation. In this study, we explore the potential effects of post-detonation cavity processes: precipitation of iodine precursors, gas seepage, and prompt venting on radioxenon isotopic evolution which influences UNE histories. Simplified analytical models and closed-form solutions yielding a potentially idealized radioactive decay/ingrowth chain in a closed and well-mixed system typically have limited application by not including the partitioning of the radionuclide inventory between a gas phase and rock melt created by the detonation and by ignoring gas transport from the cavity to host rock or ground surface. In reality, either subsurface transport or prompt release that is principally responsible for gas signatures violates the closed-system (or batch-mode) assumption. A closed-form solution representing time-dependent source-term activities is extended by considering the cavity partitioning process, slow seepage, and/or prompt release of gases from the cavity and applied to realistic systems.

Sun, Yunwei (ORCID:0000000194801439)↗

In Stream Monitoring of Off-Gasses from Plutonium Fluorination

Technology enabling real-time analysis is currently being developed to assess and advance processes used for the fluorination of actinides, which have increasing demands in the fields of forensics and molten salt reactor applications. Well established methods of fluorination use HF, a toxic and corrosive gas, which greatly limits materials of construction for probes and interfaces and is typically incompatible with detectors at greater than part per million quantities. The technology being developed utilizes Raman spectroscopy interrogation of the off-gas stream, providing detailed instantaneous process information in conditions up to 100% HF. The real-time data not only provides detailed reaction information, but also allows for a reduction, via process optimization, in the use of HF benefitting worker health and safety, minimizing waste, and prolonging equipment life.

PuF4, actinide fluorination, Raman↗

EXPLORING SYSTEMATIC EFFECTS IN THE RELATION BETWEEN STELLAR MASS, GAS PHASE METALLICITY, AND STAR FORMATION RATE

There is evidence that the well-established mass–metallicity relation in galaxies is correlated with a third parameter: star formation rate (SFR). The strength of this correlation may be used to disentangle the relative importance of different physical processes (e.g., infall of pristine gas, metal-enriched outflows) in governing chemical evolution. However, all three parameters are susceptible to biases that might affect the observed strength of the relation between them. We analyze possible sources of systematic error, including sample bias, application of signal-to-noise ratio cuts on emission lines, choice of metallicity calibration, uncertainty in stellar mass determination, aperture effects, and dust. We present the first analysis of the relation between stellar mass, gas phase metallicity, and SFR using strong line abundance diagnostics from Dopita et al. for ∼130,000 star-forming galaxies in the Sloan Digital Sky Survey and provide a detailed comparison of these diagnostics in an appendix. Using these new abundance diagnostics yields a 30%–55% weaker anti-correlation between metallicity and SFR at fixed stellar mass than that reported by Mannucci et al. We find that, for all abundance diagnostics, the anti-correlation with SFR is stronger for the relatively few galaxies whose current SFRs are elevated above their past average SFRs. This is also true for the new abundance diagnostic of Dopita et al., which gives anti-correlation between Z and SFR only in the high specific star formation rate (sSFR) regime, in contrast to the recent results of Kashino et al. The poorly constrained strength of the relation between stellar mass, metallicity, and SFR must be carefully accounted for in theoretical studies of chemical evolution.

79 ASTRONOMY AND ASTROPHYSICS↗

High Temperature Thermal Barrier Coating Evaluation of Yttrium Aluminum Garnet for Gas Turbine Applications

The Solution Precursor Spray Process (SPPS) process has been shown to overcome the durability and property challenges of applying yttrium aluminum garnet (YAG) coating for high temperature thermal barrier coating (TBC) applications (1200°C+) but only limited testing has been performed in representative application environments. In this study, YAG coatings were developed to optimize microstructure and tailor properties for combustion components in an industrial gas turbine. Thermal conductivity, erosion resistance and furnace cycling durability were used to validate YAG properties against the standard yttria-stabilized zirconia coating (YSZ). Graded and multi-layered microstructures were applied to enhance performance while maintaining durability. Further YAG process development was required to replicate coating properties and optimize deposition on more complex fuel injector nozzle and combustion liner components. Rig testing of both components was performed and compared against the baseline YSZ coating validating the high temperature capability and lower thermal conductivity of the SPPS YAG coating. The components in both tests were cycled for a minimum of ten cycles with the fuel injector test targeting a higher operating temperature while the combustor liner operated at standard conditions. A development engine test is planned to further validate performance in a gas turbine engine of this promising material.

36 MATERIALS SCIENCE↗

Analysis of gas membrane ultra-high purification of small quantities of mono-isotopic silane

A small quantity of high-value, crude, mono-isotopic silane is a prospective gas for a small-scale, high-recovery, ultra-high membrane purification process. This is an unusual application of gas membrane separation for which we provide a comprehensive analysis of a simple purification model. The goal is to develop direct analytic expressions for estimating the feasibility and efficiency of the method, and guide process design; this is only possible for binary mixtures of silane in the dilute limit which is a somewhat realistic case. In addition, analytic solutions are invaluable to verify numerical solutions obtained from computer-aided methods. Hence, in this paper we provide new analytic solutions for the purification loops proposed. Among the common impurities in crude silane, methane poses a special membrane separation challenge since it is chemically similar to silane. Other potential problematic compounds are: ethylene, diborane and ethane (in this order). Nevertheless, we demonstrate, theoretically, that a carefully designed membrane system may be able to purify mono-isotopic, crude silane to electronics-grade level in a reasonable amount of time and expenses. We advocate a combination of membrane materials that preferentially reject heavy impurities based on mobility selectivity, and light impurities based on solubility selectivity. We provide estimates for the purification of significant contaminants of interest. In this study, we suggest cellulose acetate and polydimethylsiloxane as examples of membrane materials on the basis of limited permeability data found in the open literature. We provide estimates on the membrane area needed and priming volume of the cell enclosure for fabrication purposes when using the suggested membrane materials. These estimates are largely theoretical in view of the absence of reliable experimental data for the permeability of silane. And finally, future extension of this work to the non-dilute limit may apply to the recovery of silane from rejected streams of natural silicon semi-conductor processes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Characterizing the Effect of Thermal Processing on Feedstock Al Alloy Powder for Additive Manufacturing Applications

Gas-atomized metallic powders are commonly used in additive manufacturing processes. Research has shown that, for certain AM techniques, the chemistry and microstructural properties of the feedstock powders significantly affect the properties of the consolidated material. Understanding the powder characteristics before use in additive manufacturing can lead to optimizing properties of additively manufactured materials as well as determining the recyclability of feedstock powders. This research studies the effect of various solution treatment processes on the characteristics and microstructural evolution of powder aluminum alloy 6061. Solution treatment times and temperatures were guided by thermodynamic and kinetic modeling. Light microscopy, scanning electron microscopy, and hardness were used to evaluate each condition in both two and three dimensions. Results indicate that the Mg{sub 2}Si present in the untreated condition dissolves after 60 min of solution treatment, while there are competing effects from the dissolution and concurrent growth of various Fe-containing phases. Additionally, it is shown that both granular and sub-granular structures exist in these rapidly solidified powders, and the sub-grains reorient themselves during solution treatment.

36 MATERIALS SCIENCE↗

Simulation of Binary-single Interactions in AGN Disk. I. Gas-enhanced Binary Orbital Hardening

Stellar-mass binary black hole (BBH) mergers within the accretion disks of active galactic nuclei may contribute to gravitational wave (GW) events detected by ground-based GW detectors. In particular, the interaction between a BBH and a single stellar-mass black hole (sBH), known as the binary-single interaction (BSI) process, can potentially lead to GW events with detectable nonzero eccentricity. Previous studies of the BSI process, which neglected the effects of gas, showed that BSIs contribute non-negligibly to GW events in a coplanar disk environment. In this work, we conduct a series of two-dimensional hydrodynamical and N-body simulations to explore the BSI in a gas environment by coupling REBOUND with Athena++. We perform 360 simulation runs, spanning parameters in disk surface density Σ 0 and impact parameter b. We find that the gas-induced energy dissipation within the three-body system becomes significant if the encounter velocity between the sBHs is sufficiently large (≫c s ). Our simulation results indicate that approximately half of the end states of the BSI are changed by gas. Furthermore, at higher gas density, the number of close encounters during the BSI process will increase, and the end-state BBHs tend to be more compact. Consequently, the presence of gas may shorten the GW merger timescale for end-state BBHs and increase the three-body merger rate.

79 ASTRONOMY AND ASTROPHYSICS↗

Multimodel simulation of vertical gas transfer in a temperate lake

In recent decades, several lake models of varying complexity have been developed and incorporated in numerical weather prediction systems and climate models. To foster enhanced forecasting ability and verification, improvement of these lake models remains essential. This especially applies to the limited simulation capabilities of biogeochemical processes in lakes and greenhouse gas exchanges with the atmosphere. Here we present multi-model simulations of physical variables and dissolved gas dynamics in a temperate lake (Harp Lake, Canada). The five models (ALBM, FLake, LAKE, LAKEoneD, MTCR-1) considered within this most recent round of the Lake Model Intercomparison Project (LakeMIP) all captured the seasonal temperature variability well. In contrast, none of the models is able to reproduce the exact dates of ice-cover and ice-off, leading to considerable errors in the simulation of eddy diffusivity around those dates.We then conducted an additional modeling experiment with a diffusing passive tracer to isolate the effect of the eddy diffusivity on gas concentration. Remarkably, sophisticated k -" models do not demonstrate a significant difference in the vertical diffusion of a passive tracer compared to models with much simpler turbulence closures. All models simulate less intensive spring overturn compared to autumn. Reduced mixing in the models consequently leads to the accumulation of the passive tracer distribution in the water column. The lake models with a comprehensive biogeochemical module, such as ALBM and LAKE, predict dissolved oxygen dynamics adequate to the observed data. However, for the surface carbon dioxide concentration the correlation between modeled (ALBM, LAKE) and observed data is weak (~0.3). Overall our results indicate the need to improve the representation of physical and biogeochemical processes in lake models, thereby contributing to enhanced weather prediction and climate projection capabilities.

Guseva, Sofya↗

Advanced spectrometric methods for characterizing bio-oils to enable refineries to reduce fuel carbon intensity during co-processing

A promising approach for supplementing petroleum-derived fuels to support reductions in green-house gas emissions is to convert abundant biomass feedstocks into renewable carbon-rich oils using pyrolysis. However, the resultant bio-oils contain various oxygenated compounds that can impart acidity, chemical and thermal instability, and immiscibility with petroleum derived fuels, necessitating further upgrading to derive fuel blendstocks. Co-processing bio-oils and petroleum-derived liquids in existing refineries is a potentially near-term, cost-effective approach for upgrading bio-oils while reducing refinery carbon intensities. However, one cause for hesitation in co-processing bio-oils is limited comprehensive characterization and speciation of the bio-oil components. Advanced analytical techniques are currently under investigation to enable identification of elusive species in bio-oils, enabling researchers to develop strategies to mitigate catalyst deactivation agents and contaminants. This review provides a brief overview of several analytical methods commonly used to analyze bio-oils and their limitations. In addition, advanced techniques currently under development are discussed to further elucidate bio-oil components that may limit its end use. This will help inform the technical and economic feasibility of co-processing bio-oils with petroleum-derived liquids, therefore, improving the overall downstream processes for biofuels blendstock production.

09 BIOMASS FUELS↗

Comparison of ammonia with methanol, liquefied natural gas and conventional marine transportation fuels through life cycle cost and emissions analysis

This work evaluates ammonia as a potential marine fuel for a SUEZMAX tanker and compares it with methanol, liquefied natural gas, and conventional fuel oils. The motivation arises from the need to identify low-emission, cost-competitive fuel options that can reduce greenhouse gas emissions from international shipping. The central hypothesis is that ammonia produced from renewable energy sources can achieve lower well-to-wake greenhouse gas emissions with varying life cycle costs based on the region. Life cycle assessment and techno-economic analysis were performed for a thirty-year vessel lifetime on two representative trade routes: from Saudi Arabia to Japan and from Saudi Arabia to the Netherlands. Four ammonia production pathways were assessed: natural gas, natural gas with carbon capture, natural gas pyrolysis, and renewable electricity–based synthesis. Results show that wind-based ammonia produced in Saudi Arabia achieved the lowest life cycle well-to-wake greenhouse gas emissions, between 0.58 and 0.64 million metric tons, among all fuels when using regional grid process electricity. With renewable process electricity, ammonia produced from natural gas pyrolysis in Saudi Arabia showed comparable emissions of 0.37 to 0.44 million metric tons with wind-based ammonia of 0.37 to 0.43 million metric tons. Liquefied natural gas exhibited the lowest life cycle cost, between 402 and 412 million United States dollars, and the only negative carbon abatement cost, ranging from −277 to –322 United States dollars per metric ton of greenhouse gas, compared with high sulfur fuel oil. The findings indicate that renewable ammonia offers a promising long-term pathway for reducing shipping emissions, while liquefied natural gas remains the most cost-effective option in the near term.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗