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At least 253 records · Page 14
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

High-Fidelity and High-Performance Computational Simulations for Rapid Design Optimization of Sulfur Thermal Energy Storage

Industrial process heating (IPH) accounts for approximately 70% of US manufacturing energy use and is primarily produced by fossil fuel combustion. Approximately 1500 TWht (approximately 60%) of IPH demand is in the temperature range of 100-300. Industrial applications in this temperature range include drying, hydrothermal processing, thermal enhanced oil recovery, food and beverage, bioethanol production, etc. Cost-effective thermal energy storage (TES) that increases the utilization of waste and renewable heat (solar, geothermal, etc.) could provide significant energy savings and reliable heat sources, decrease emissions, and increase US manufacturing competitiveness through reductions in fuel consumption. TES development has historically been dominated by technologies suitable for deployment with concentrating solar power (CSP). State-of-the-art thermal storage deployed commercially with power tower CSP plants uses a 60%/40% NaNO3/KNO3 molten salt and operates between temperatures of approximately 280 degrees Celsius and 570 degrees Celsius using a two-tank configuration. However, these nitrate salts are unsuitable for operation outside of this temperature range due to a high freezing point of approximately 220 degrees Celsius, and limits on high-temperature salt stability and corrosion resistance of containment alloys. Other materials being investigated for TES include those based on: (1) sensible energy storage (various molten salt compositions, inert solid particles, rocks or pebble beds, sulfur, water, concrete, graphite, etc.), (2) latent energy storage in materials that undergo solid-liquid phase change at relevant temperatures (organic materials for low-temperature applications, inorganic salts and/or metals for high-temperature applications), or (3) thermochemical energy storage (hydrides, hydroxides, carbonates, metal oxides, etc.). The application temperature and challenges pertaining to storage material and/or containment cost, energy density, long-term thermal and cyclic stability, and charge/discharge heat transfer effectiveness drive material selection for a given IPH or electricity generation application. Sulfur is a cheap commodity at $80/ton compared to $1100 - 1300/ton for conventional salts. When using a metric of storage cost per kWh, sulfur costs around 2-3 $/kWh. Previous sulfur TES development focused on high temperature (>600 degrees) concentrated solar power applications with sulfur encapsulated in pipes and flow of gaseous HTF (air) in the shell side. However, for lower-temperature IPH applications in the range of approximately 100-300 degrees Celsius Element 16 adopted a compact and scalable TES design with molten sulfur in the shell and HTF pipes submerged in the molten sulfur bath. The low-cost molten sulfur TES for dispatchable IPH has deployment potential for broad applications. The spatial and temporal evolution of the HTF and sulfur temperature is critical to the TES system performance, and thus detailed modeling can improve understanding of the performance and facilitate design improvements. Using high performance computing and computational fluid dynamics (CFD) a low-cost molten sulfur thermal energy storage (TES) system for industrial process heating (IPH) applications was developed. The unique challenges in CFD modeling of sulfur TES are the sharp property changes of sulfur relevant to the working temperatures. Above 159, liquid sulfur undergoes polymerization, and the viscosity of sulfur rapidly increases by several orders of magnitude between 159 degrees Celsius and 188 degrees Celsius, followed by a decrease in viscosity beyond 188 degrees Celsius due to thermal bound dissociation. In addition, various concentrations of H2S impurities can also modify sulfur viscosity. This numerical challenge is especially relevant to transient simulation of the sulfur TES charging and discharging processes as the extreme property variations limit the applicability of traditional heat transfer correlations. Transient CFD simulations including the temperature-dependent sulfur properties and geometric complexity of the TES design were used to predict the effect of natural convection during charging and discharging on the heat transfer process, sulfur temperature uniformity, charge/discharge rates, and performance of the storage devices. The CFD model was validated with experimental results for a full charge and discharge cycle. The work will show 3D and 2D simulation comparisons aimed to facilitate rapid design iterations and a machine learning based design optimization approach.

CFD↗
DOE OSTI2024

High-Fidelity and High-Performance Computational Simulations for Rapid Design Optimization of Sulfur Thermal Energy Storage (CRADA Report)

NREL and Element 16 collaborated on sulfur thermal energy storage modeling using NREL’s high performance computing (HPC) resources to assist its application in industrial processes. Industrial process heat (IPH) accounts for ~70% of US manufacturing energy use and is primarily produced by fossil fuel combustion. Approximately, 1500 TWht (~60% Terawatt hour thermal) of IPH demand is in the temperature range of 100-300°C. Industrial applications in this temperature range include drying, hydrothermal processing, thermal enhanced oil recovery, food and beverage, bioethanol production, etc. Cost-effective thermal energy storage (TES) that increases the utilization of waste and renewable heat (solar, geothermal, etc.) could provide significant energy savings and reliable heat sources, decrease emissions, and increase US manufacturing competitiveness through reductions in fuel consumption. This HPC4EI project facilitated Element 16’s development of low-cost and high-impact molten sulfur TES for dispatchable IPH. The development of a high-fidelity model validated by experimental data and HPC simulations enabled the successful resolution of the complex interplay between fluid dynamics and heat transfer processes during transient operation of sulfur TES, overcoming the numerical challenges posed by the non-linear temperature-dependent physical properties of sulfur. The project helped accelerate Element 16’s molten sulfur TES product design and support its broad applications.

25 ENERGY STORAGE↗
NASA NTRSDate not supplied

The Development and Use of a Natural Gas / Oxygen Burner Rig for Environmental Barrier Coating and Ceramic Matrix Composite Technology Maturation

This work outlines the development of a new natural gas/oxygen (NG/O2) fueled combustion rig located at the NASA Glenn Research Center for high-temperature environmental durability studies of advanced materials and components at atmospheric pressure. The NG/O2 burner rig can simulate the high-temperature, high-heat flux, and high-velocity thermal environments encountered in gas turbine engines. It also provides the capability to study environmental effects such as water vapor and other foreign contaminants relevant to these applications. The rig is anticipated to bridge the gap between other laboratory methods such as furnaces, jet-fueled burner rigs, high-heat flux lasers, and more expensive engine rig testing. The NG/O2 rig is expected to have maximum sample temperature capabilities over 3,000°F (1,649°C) and result in higher water vapor content compared to our Mach 0.3 to Mach 1.0 jet-A burner rigs which is important for characterizing current and next-generation environmental barrier coatings. This paper will provide an overview of the development of the NG/O2 burner rig, initial characterization, and current research and development efforts on environmental barrier coated ceramic matrix composites.

Burner rig↗
NASA NTRS2023

The Development and Use of a Natural Gas / Oxygen Burner Rig for Environmental Barrier Coating and Ceramic Matrix Composite Technology Maturation

This work outlines the development of a new natural gas/oxygen (NG/O 2 ) fueled combustion rig located at the NASA Glenn Research Center for high-temperature environmental durability studies of advanced materials and components at atmospheric pressure. The NG/O 2 burner rig can simulate the high-temperature, high-heat flux, and high-velocity thermal environments encountered in gas turbine engines. It also provides the capability to study environmental effects such as water vapor and other foreign contaminants relevant to these applications. The rig is anticipated to bridge the gap between other laboratory methods such as furnaces, jet-fueled burner rigs, high-heat flux lasers, and more expensive engine rig testing. The NG/O 2 rig is expected to have maximum sample temperature capabilities over 3,000°F (1,649°C) and result in higher water vapor content compared to our Mach 0.3 to Mach 1.0 jet-A burner rigs which is important for characterizing current and next-generation environmental barrier coatings. This paper will provide an overview of the development of the NG/O 2 burner rig, initial characterization, and current research and development efforts on environmental barrier coated ceramic matrix composites.

Burner rig↗
DOE OSTI2021

Life cycle energy and environmental impacts of hydroprocessed renewable jet fuel production from pennycress

There is a growing interest in making the overall aviation industry more environmentally-friendly by developing advanced biofuels. In this context, the main driver is establishing feedstocks with lower environmental loads and higher energy use efficiency. The objective of this study was to evaluate the energy requirement and environmental impacts of hydroprocessed renewable jet fuel (HRJ) production from pennycress. The system boundary included pennycress production, logistics, oil extraction and conversion to HRJ, wastewater treatment, and electricity and steam generation. Energy allocation method was used for the analysis. The functional unit was considered to be one GJ of HRJ, and the biorefinery size was considered to be 18.9 million l/yr (5 million gal/yr) HRJ. Energy use efficiency of pennycress-based HRJ production was estimated to be 3.9–5.5 (90% central range), which was higher than that of HRJ from other oilseeds, such as canola. Global warming potential of pennycress-based HRJ (35–49 kgCO 2 eq/GJ of HRJ (90% central range)) was also lower than those of HRJ from similar oilseeds and the commercial jet fuel baseline. Pennycress production was the main contributor to the total energy use and environmental impacts of HRJ production, mainly due to the use of nitrogen fertilizer for production, and fuel combustion for farm operations. Pennycress yield was identified as the most sensitive parameter affecting the energy use efficiency and environmental impacts of HRJ production. Furthermore, the outcomes of this study are useful for identifying the performance targets towards improving energy use efficiency and environmental performance of pennycress-based HRJ production at the commercial scale.

09 BIOMASS FUELS↗
DOE OSTI2026

Large-Scale Carbon Removal Will Create Public Health, Economic, and Climate Tradeoffs

Economy-wide efforts to achieve net-zero emissions offer both climate and air quality-related public health benefits from reducing fossil fuel combustion. We explore the expected costs and benefits if carbon dioxide removal (CDR) is deployed at scale in support of these efforts. Six leading forms of CDR at two levels of deployment are compared to a scenario with no U.S. climate action. We find that heavy reliance on CDR avoids a $2.5-5.8 trillion USD2020 in climate damages, provides $2.8-6.5 trillion USD2020 public health benefits, returns $5-6 trillion USD2020 in CDR revenues, but requires $11-13 trillion USD2020 CO2 mitigation cost, cumulatively by 2050 in the U.S. In contrast, lower reliance on CDR requires much deeper near-term fossil-fuel reductions, which increases mitigation costs by 52% but also creates 26% higher public health benefits from reductions in particulate matter- and ozone-related mortality and morbidity, preventing about 12,600 premature deaths by mid-century in the U.S.

Javadi, Parisa↗
NASA NTRS2021

Reductions in NO2 Burden Over North Equatorial Africa from Decline in Biomass Burning in Spite of Growing Fossil Fuel Use, 2005 to 2017

Socioeconomic development in low- and middle-income countries has been accompanied by increased emissions of air pollutants, such as nitrogen oxides [NOx: nitrogen dioxide (NO2) + nitric oxide (NO)], which affect human health. In sub-Saharan Africa, fossil fuel combustion has nearly doubled since 2000. At the same time, landscape biomass burning—another important NOx source—has declined in north equatorial Africa, attributed to changes in climate and anthropogenic fire management. Here, we use satellite observations of tropospheric NO2 vertical column densities (VCDs) and burned area to identify NO2 trends and drivers over Africa. Across the northern ecosystems where biomass burning occurs—home to hundreds of millions of people—mean annual tropospheric NO2 VCDs decreased by 4.5% from 2005 through 2017 during the dry season of November through February. Reductions in burned area explained the majority of variation in NO2 VCDs, though changes in fossil fuel emissions also explained some variation. Over Africa’s biomass burning regions, raising mean GDP density (USD·km−2) above its lowest levels is associated with lower NO2 VCDs during the dry season, suggesting that economic development mitigates net NO2 emissions during these highly polluted months. In contrast to the traditional notion that socioeconomic development increases air pollutant concentrations in low- and middle-income nations, our results suggest that countries in Africa’s northern biomass-burning region are following a different pathway during the fire season, resulting in potential air quality benefits. However, these benefits may be lost with increasing fossil fuel use and are absent during the rainy season.

air pollution↗
DOE OSTI2025

Towards stabilization of pressurized oxy-coal diffusion flames

Designing an effective burner is vital for the development of pressurized oxy-fuel combustion technologies. Turbulent jet diffusion burners are adopted for the pressurized oxy-combustor in this research and a bluff-body is employed to create a recirculation zone to stabilize the flame in pressurized oxy-combustor. The objective of this numerical work is to perform a systematic analysis of the characteristics of this pressurized non-premixed flame. Specifically, a 15-bar POFC combustor of power 100 kWth is modeled employing the Ansys FLUENT commercial platform, using Reynolds-averaged Navier-Stokes (RANS) modeling. The present computational work focuses on identifying the aerothermodynamic features of the isothermal and reacting flow with a disk-shape bluff-body. Results show that fuel-oxidizer stream momentum ratio has great impacts on the temperature profile of the down-fired, co-axial, pressurized oxy-coal, diffusion flame. Parametric study of the width of the burner tip identifies an optimal range for this pressurized burner.

Li, Lei↗
NASA NTRSDate not supplied

Biomass burning declines lead to large net reductions in NO2 concentrations over north equatorial Africa in spite of growing fossil fuel emissions

Socio-economic development in low and middle-income countries has been accompanied by increased emissions of air pollutants such as nitrogen oxides (NOx: nitrogen dioxide (NO2) + nitric oxide (NO)), which affect human health. In sub-Saharan Africa, fossil fuel combustion has nearly doubled since 2000. At the same time, biomass burning—another important NOx source—has declined in Africa’s northern biomass burning region, attributed to changes in climate and anthropogenic fire management associated with agricultural development. Here we use satellite observations of tropospheric NO2 vertical column densities (VCDs) and burned area to identify NO2 trends and drivers over Africa. Across the northern ecosystems where biomass burning occurs—home to over 350 million people—mean annual tropospheric NO2 VCDs decreased by 4.5% from 2005 through 2017 during the biomass burning season of November through February. Reductions in burned area explained the majority of these change in NO2 VCDs, but there were also weaker relationships between changes in NO2 VCDs and fossil fuel emissions over parts of West Africa, which were stronger during rainy season. Over Africa’s biomass burning regions, NO2 VCDs tended to decrease with increasing population density up to a threshold of approximately 180 people per km2, suggesting that anthropogenic activity causes a net reduction in NO2 emissions across roughly 90% of the continent’s biomass burning regions. In contrast to the widely-held perception that socio-economic development worsens air quality in low and middle-income nations, our results suggest that countries in Africa’s northern biomass burning region are following a different pathway, resulting in regional air quality benefits. However, these benefits may be lost with increasing fossil fuel use.

Biomass burning↗
DOE OSTI2026

Rate constants and third-body collision efficiencies for recombination of Na with OH and O2: Implications for flame inhibition by alkali salts

Flame inhibition by alkali metals has implications for solid fuel combustion, fire safety, and a number of industrial processes. While the mechanism of inhibition is fairly well understood, details related to thermodynamic properties and rate constants are still in question. In the present work, the recombination of Na with OH (R5) and O2 (R7), respectively, was characterized theoretically, and the implications for modeling laminar premixed hydrogen flames doped with sodium species were examined. Third-body collision efficiencies and low-pressure-limit rate constants were obtained using newly fitted ab initio-based potential energy surfaces, classical trajectories, and one-dimensional master equation calculations. The results are consistent with available experimental results and aid in the present modeling study by providing rate information for bath gases and conditions that remain unexplored experimentally. Chemical kinetic modeling of relative Na and absolute H and OH profiles in H2-fueled laminar, premixed flames doped with a sodium salt shows that the most important radical removal cycle is the sequence Na + OH (+M) → NaOH (+M) (R5), NaOH + H → Na + H2O (R12), even under oxidizing conditions. A secondary cycle, Na + O2 (+M) ⇄ NaO2 (+M) (R7), NaO2 + OH → NaOH + O2 (R14), is less important due to the low thermal stability of NaO2. In most flames, reaction R7 is partially equilibrated, and reaction R14 becomes rate-limiting for the second cycle. The flame analysis supports a lower value of k14 than indicated by recent work on KO2 + OH, but more work is required to confirm this.

Jasper, Ahren W.↗
NASA NTRS2003

Black Carbon in Estuarine (Coastal) High-molecular-weight Dissolved Organic Matter

Dissolved organic matter (DOM) in the ocean constitutes one of the largest pools of organic carbon in the biosphere, yet much of its composition is uncharacterized. Observations of black carbon (BC) particles (by-products of fossil fuel combustion and biomass burning) in the atmosphere, ice, rivers, soils and marine sediments suggest that this material is ubiquitous, yet the contribution of BC to the ocean s DOM pool remains unknown. Analysis of high-molecular-weight DOM isolated from surface waters of two estuaries in the northwest Atlantic Ocean finds that BC is a significant component of DOM, suggesting that river-estuary systems are important exporters of BC to the ocean through DOM. We show that BC comprises 4-7% of the dissolved organic carbon (DOC) at coastal ocean sites, which supports the hypothesis that the DOC pool is the intermediate reservoir in which BC ages prior to sedimentary deposition. Flux calculations suggest that BC could be as important as vascular plant-derived lignin in terms of carbon inputs to the ocean. Production of BC sequesters fossil fuel- and biomass-derived carbon into a refractory carbon pool. Hence, BC may represent a significant sink for carbon to the ocean.

Mannino, Antonio↗
NASA NTRS2005

Characterizing the Chemical Stability of High Temperature Materials for Application in Extreme Environments

The chemical stability of high temperature materials must be known for use in the extreme environments of combustion applications. The characterization techniques available at NASA Glenn Research Center vary from fundamental thermodynamic property determination to material durability testing in actual engine environments. In this paper some of the unique techniques and facilities available at NASA Glenn will be reviewed. Multiple cell Knudsen effusion mass spectrometry is used to determine thermodynamic data by sampling gas species formed by reaction or equilibration in a Knudsen cell held in a vacuum. The transpiration technique can also be used to determine thermodynamic data of volatile species but at atmospheric pressures. Thermodynamic data in the Si-O-H(g) system were determined with this technique. Free Jet Sampling Mass Spectrometry can be used to study gas-solid interactions at a pressure of one atmosphere. Volatile Si(OH)4(g) was identified by this mass spectrometry technique. A High Pressure Burner Rig is used to expose high temperature materials in hydrocarbon-fueled combustion environments. Silicon carbide (SiC) volatility rates were measured in the burner rig as a function of total pressure, gas velocity and temperature. Finally, the Research Combustion Lab Rocket Test Cell is used to expose high temperature materials in hydrogen/oxygen rocket engine environments to assess material durability. SiC recession due to rocket engine exposures was measured as a function of oxidant/fuel ratio, temperature, and total pressure. The emphasis of the discussion for all techniques will be placed on experimental factors that must be controlled for accurate acquisition of results and reliable prediction of high temperature material chemical stability.

Opila, Elizabeth↗
DOE OSTI2026

Life cycle analysis of dedicated energy crops for fuel production in the United States

Dedicated energy crops are promising feedstocks to make biofuels including jet fuels. This study applies life cycle analysis (LCA) to estimate direct well-to-wake (WTW) greenhouse gas (GHG) emissions (g CO 2 e/MJ) for jet fuel derived from five energy crops-biomass sorghum, miscanthus, switchgrass, poplar, and willow-via Fischer-Tropsch-to-Jet (FTJ) and Ethanol-to-Jet (ETJ) pathways. The WTW boundary includes direct emissions from biomass production, fuel production, and fuel combustion. The R&D GREET model is expanded to conduct the LCA, using national average biomass yields and farming inputs from the 2023 Billion-Ton Study. In addition, this study estimates emissions from market-mediated effects, including induced land-use change, induced other crop (non-feedstock) production changes, and induced livestock production changes using global economic and emissions factor models. On a per-dry U.S. ton basis, cultivation and harvest emissions are lowest for willow (51,565 g CO 2 e) and highest for biomass sorghum (104,488 g CO 2 e). Per-acre results show similarly high emissions for sorghum and lowest values for poplar and willow. Direct WTW emissions are substantially lower for FTJ (biomass sorghum: 5.5; miscanthus: 10.3; switchgrass: 11.7; poplar: 11.9; and willow: 8.7 g CO 2 e/MJ) than ETJ (33.2; 33.8; 34.8; 36.2; and 31.7 g CO 2 e/MJ, respectively). When market-mediated emissions are included, miscanthus exhibits the lowest total emissions across energy crop pathways. Although results are sensitive to modeling assumptions, they indicate that high-yielding perennial and woody crops, particularly when planted on marginal land, could significantly reduce WTW emissions for bio-jet fuels by combining low direct emissions with soil carbon gains and favorable market-mediated effects.

Billion-Ton Study↗
DOE OSTI2021

Study the thermal radiation effects in gas-solid flows with gray and non-gray P1 models implemented in MFiX

Thermal radiation is a dominant mode of heat transfer in combustion/gasification, packed/circulating bed reactors, and energy storage/conversion devices. In hydrocarbon fuel combustion, the high absorption and emission of product gases like CO 2 and H 2 O significantly affect the heat transfer characteristics. It is essential to understand the radiative energy propagation in such applications. In the present study, we developed a framework to implement the P-1 radiation model in MFiX for Eulerian-Eulerian (Two fluid-TFM) and Eulerian-Lagrangian (Discrete element-DEM and Particle in cell-PIC) models. The P-1 is a simplification of the spherical harmonics method. The framework has been verified on various flue gas conditions. The verified solver results are validated against the benchmark results available in the literature. The verified and validated gray and non-gray weighted sum of gray gas models is evaluated for dry and wet flue gas conditions. Further, they are also used to study gas-solid flows in a fluidized bed/riser.

20 FOSSIL-FUELED POWER PLANTS↗
DOE OSTI2024

Nitrogen acquisition and retention pathways in sustainable perennial bioenergy grass cropping systems

Abstract Perennial tall grasses show promise as bioenergy crops due to high productivity and efficient nutrient use. Ongoing research on bioenergy grasses seeks to reduce their reliance on synthetic nitrogen (N) fertilizer, the manufacture of which relies on fossil fuel combustion. Excessive use of fertilizers also causes adverse environmental consequences and leads to the evolutionary loss of plant traits beneficial to sustainable N cycle. Notably, perennial tall grasses have exhibited the potential to maintain high biomass yield without the need for N fertilizer or causing soil N depletion. Perennial grasses can be adept at interacting with their microbial partners to facilitate N acquisition and retention via mechanisms such as biological N fixation and nitrification inhibition. These inherent N management traits should be preserved and optimized at the this early stage of bioenergy grass breeding programs. This review examines the impact of external N on bioenergy grass production and explores the potential of leveraging advantageous N‐cycling attributes of perennial tall grasses, laying groundwork for future management and research efforts. With minimized dependency on external N input, the cultivation of perennial energy grasses will pave the way toward more resilient agricultural systems and play a significant role in addressing key global energy and environmental challenges.

Agriculture↗
DOE OSTI2024

Size Up or Size Down? National Analysis of Heat Pump Sizing and Impacts

Electrification of on-site fossil fuel combustion in buildings is recognized as a key component of achieving global greenhouse gas emissions targets. Air-source heat pumps are an efficient approach for space heating electrification. However, a major barrier to heat pump adoption is the high installation cost relative to furnaces and air conditioners. Because the installation cost of heat pumps - especially cold climate models - is dependent on their size, it is important to understand the distribution of heat pump sizes using different sizing methods and factors that impact heat pump sizing. In this study, we use sub-hourly physics simulations of 550,000 statistically representative dwelling units to analyze the distribution of heat pump size in the U.S. for three different efficiency levels of heat pumps, with and without building insulation and air sealing upgrades. We will present results from the national analysis of different factors affecting heat pump sizing along with the impact of sizing decisions on upgrade costs and operating costs.

electrification↗
DOE OSTI2022

Evaluation of the energy balance of chemical looping combustion of solid fuels using CuO-based oxygen carriers

Chemical looping combustion (CLC) can inherently capture the CO2 generated during thermal energy production. When using CuO-based oxygen carriers, the reactions in both the fuel reactor (FR) and air reactor (AR) are exothermic, facilitating autothermal operation. To prevent the oxygen carrier from becoming agglomerated while ensuring a sufficient oxygen release rate, it is necessary to predict the FR temperature and remove an appropriate amount of heat from the AR when burning high-rank fuels. Here in this work, the energy balance of a CuO-based CLC system firing various solid fuels (biomass, coal, and petroleum coke) was investigated by establishing a thermodynamic model using FactSage. The energy distribution characteristics of the FR were quantified based on a virtual five-step thermodynamic sequence. The effects of fuel properties, oxygen carrier properties, and operating conditions on the energy balance were evaluated systematically. The results indicate that the temperature difference between the FR and AR is not very sensitive to the heating value of the fuel, while the CuO loading of the oxygen carrier, the heat capacity of the support material, and the flow rate of the fluidizing gas have significant impact. The insights obtained in this work will help improve the design and heat management of CLC.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Ultrasmall Cu Nanoparticles Supported on Crystalline, Mesoporous ZnO for Selective CO 2 Hydrogenation

Converting CO 2 to value-added chemicals, e. g., CH 3 OH, is highly desirable in terms of the carbon cycling while reducing CO 2 emission from fossil fuel combustion. Cu-based nanocatalysts are among the most efficient for selective CO 2 -to-CH 3 OH transformation; this conversion, however, suffers from low reactivity especially in the thermodynamically favored low temperature range. We herein report ultrasmall copper (Cu) nanocatalysts supported on crystalline, mesoporous zinc oxide nanoplate (Cu@mZnO) with notable activity and selectivity of CO 2 -to-CH 3 OH in the low temperature range of 200–250 °C. Cu@mZnO nanoplates are prepared based on the crystal-crystal transition of mixed Cu and Zn basic carbonates to mesoporous metal oxides and subsequent hydrogen reduction. Under the nanoconfinement of mesopores in crystalline ZnO frameworks, ultrasmall Cu nanoparticles with an average diameter of 2.5 nm are produced. Cu@mZnO catalysts have a peak CH 3 OH formation rate of 1.13 mol h −1 per 1 kg under ambient pressure at 246 °C, about 25 °C lower as compared to that of the benchmark catalyst of Cu−Zn−Al oxides. In conclusion, our new synthetic strategy sheds some valuable insights into the design of porous catalysts for the important conversion of CO 2 -to-CH 3 OH.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗