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At least 919 records · Page 51
All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

Reduction of water content in calcium aluminate cement with/out phosphate modification for alternative cementation technique

Cementation of the secondary aqueous wastes from TEPCO Fukushima Daiichi Nuclear Power Plant is challenging due to the significant strontium content and radioactivity, leading to a potential risk of hydrogen gas generation via radiolysis of water content. The present study investigates the reduction of water content in calcium aluminate cement (CAC) with/out phosphate modification by a heat-treatment during the solidification. The reduction of water in the CAC was found restricted by the rapid formation of crystalline hydration phases, whereas the phosphate-modified system allowed the gradual reduction of water, achieving the reduction of 60% water content at 95 °C. Curing at 60–95 °C also eliminated the significant cracks found at 35 °C in the phosphate system. The possible difference in the amorphous products, NaCaPO{sub 4}·nH{sub 2}O type at 35°C and Ca(HPO{sub 4})·xH{sub 2}O type at 60–95 °C, may have contributed to the improvement in the microstructure together with the change in the pore size distribution.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Revisiting the electrochemical reduction of CO 2 on Au 25 (SR)$\overline{_{18}}$ nanocluster

Experiments show that Au25(SR)$\overline{_{18}}$ is a potential electrocatalyst for the electrochemical reduction of CO 2 , but elucidation of the reaction mechanisms remain challenging experimentally. We evaluate key steps in the active site formation, CO 2 reduction, and H 2 evolution on the nanocluster employing density functional theory coupled with an explicit solvent model of the electrochemical interface to calculate activation barriers. The predicted preferred pathway for activating the nanocluster involves dethiolation, resulting in an exposed Au site that is both active and selective for CO 2 reduction. Finally, the alternative S site is found to be kinetically prohibitive and does not facilitate CO 2 reduction.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Evaluating the causes of cost reduction in photovoltaic modules

Photovoltaic (PV) module costs have declined rapidly over forty years but the reasons remain elusive. Here we advance a conceptual framework and quantitative method for quantifying the causes of cost changes in a technology, and apply it to PV modules. Our method begins with a cost model that breaks down cost into variables that changed over time. Cost change equations are then derived to quantify each variable's contribution. We distinguish between changes observed in variables of the cost model – which we term low-level mechanisms of cost reduction – and research and development, learning-by-doing, and scale economies, which we refer to as high-level mechanisms. We find that increased module efficiency was the leading low-level cause of cost reduction in 1980–2012, contributing almost 25% of the decline. Government-funded and private R&D was the most important high-level mechanism over this period. After 2001, however, scale economies became a more significant cause of cost reduction, approaching R&D in importance. Policies that stimulate market growth have played a key role in enabling PV's cost reduction, through privately-funded R&D and scale economies, and to a lesser extent learning-by-doing. The method presented here can be adapted to retrospectively or prospectively study many technologies, and performance metrics besides cost.

14 SOLAR ENERGY↗
DOE OSTI2016

Selective recovery of pure copper nanopowder from indium-tin-oxide etching wastewater by various wet chemical reduction process: Understanding their chemistry and comparisons of sustainable valorization processes

Sustainable valorization processes for selective recovery of pure copper nanopowder from Indium-Tin-Oxide (ITO) etching wastewater by various wet chemical reduction processes, their chemistry has been investigated and compared. After the indium recovery by solvent extraction from ITO etching wastewater, the same is also an environmental challenge, needs to be treated before disposal. After the indium recovery, ITO etching wastewater contains 6.11 kg/m{sup 3} of copper and 1.35 kg/m{sup 3} of aluminum, pH of the solution is very low converging to 0 and contain a significant amount of chlorine in the media. In this study, pure copper nanopowder was recovered using various reducing reagents by wet chemical reduction and characterized. Different reducing agents like a metallic, an inorganic acid and an organic acid were used to understand reduction behavior of copper in the presence of aluminum in a strong chloride medium of the ITO etching wastewater. The effect of a polymer surfactant Polyvinylpyrrolidone (PVP), which was included to prevent aggregation, to provide dispersion stability and control the size of copper nanopowder was investigated and compared. The developed copper nanopowder recovery techniques are techno-economical feasible processes for commercial production of copper nanopowder in the range of 100–500 nm size from the reported facilities through a one-pot synthesis. By all the process reported pure copper nanopowder can be recovered with>99% efficiency. After the copper recovery, copper concentration in the wastewater reduced to acceptable limit recommended by WHO for wastewater disposal. The process is not only beneficial for recycling of copper, but also helps to address environment challenged posed by ITO etching wastewater. From a complex wastewater, synthesis of pure copper nanopowder using various wet chemical reduction route and their comparison is the novelty of this recovery process. - Highlights: • From the Indium-Tin-Oxide etching wastewater, copper nanopowder was synthesized. • Solution chemistry of ITO etching wastewater is addressed. • A techno-economical feasible, environment friendly and occupational safe process. • Brings back the material to production stream and address the circular economy. • A cradle to cradle technology management lowers the futuristic carbon economy.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2018

Contribution of climate and land cover changes to reduction in soil erosion rates within small cultivated catchments in the eastern part of the Russian Plain during the last 60 years

Highlights: • The soil erosion has decreased at least 2–3 times over the last 30 years at the RP. • The increase in winter air temperature is the key reason for the soil loss reduction. • The crop rotation changes is the factor of erosion rate reduction at the forest zone. The eastern part of the Russian Plain is an important agricultural region of European Russia with high proportion of cultivated lands in the steppe, forest-steppe and forest (southern part) landscape zones. Soil erosion is the main process of land degradation and surface water contamination there. Climate and land cover changes have been observed in this region during the last 30 years. However, field quantitative assessments of soil erosion rates are not available for the eastern part of European Russia due to the lack of monitoring data as well as the evaluation of erosion/deposition processes in cultivated catchments using other field methods. Three representative small cultivated catchments with high (> 80%) proportion of cultivated lands were selected in the forest (southern part), forest-steppe and steppe zones of the study region to evaluate sedimentation rates in dry valley bottoms of the catchments for two-time intervals (1963–1986 and 1987–2016) based on the application of the bomb-derived and Chernobyl-derived {sup 137}Cs isotope for sediment dating. The 3–4 depth {sup 137}Cs profiles were used to assess the sedimentation rates within the each investigated catchment. It was established that the sedimentation rates have considerably decreased (at least 2–3 times) over the last 30 years compared to 1963–1986 in all the investigated catchments. This is in agreement with results of erosion rate calculations using erosion models for the forest zone, however not consistent with erosion rates assessments for the forest-steppe and steppe zones. According to the model calculations, erosion rates show a slight decrease in the forest-steppe zone and increase in the steppe zone. The reduction in surface runoff during snowmelt period is one of the reasons for decrease in erosion rates within cultivated slopes for all the investigated catchments. The increase in proportion of perennial grasses in the regional crop rotation is another important reason for the decrease in erosion rates for the catchment located in the south of the forest zone. The importance of land cover changes in a major decrease of soil losses from the cultivated fields of the investigated catchments located in the forest-steppe and steppe zones cannot be identified due to the lack detailed information about crop rotation for those particular sites. However, available regional information about crop rotation changes for the two-time intervals (1960–1980 and 1996–2012) do not explain very high reduction in sedimentation rates in the dry valley bottoms after 1986.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2014

Clinical Evaluation of Normalized Metal Artifact Reduction in kVCT Using MVCT Prior Images (MVCT-NMAR) for Radiation Therapy Treatment Planning

Purpose: To evaluate the metal artifacts in diagnostic kilovoltage computed tomography (kVCT) images of patients that are corrected by use of a normalized metal artifact reduction (NMAR) method with megavoltage CT (MVCT) prior images: MVCT-NMAR. Methods and Materials: MVCT-NMAR was applied to images from 5 patients: 3 with dual hip prostheses, 1 with a single hip prosthesis, and 1 with dental fillings. The corrected images were evaluated for visualization of tissue structures and their interfaces and for radiation therapy dose calculations. They were compared against the corresponding images corrected by the commercial orthopedic metal artifact reduction algorithm in a Phillips CT scanner. Results: The use of MVCT images for correcting kVCT images in the MVCT-NMAR technique greatly reduces metal artifacts, avoids secondary artifacts, and makes patient images more useful for correct dose calculation in radiation therapy. These improvements are significant, provided the MVCT and kVCT images are correctly registered. The remaining and the secondary artifacts (soft tissue blurring, eroded bones, false bones or air pockets, CT number cupping within the metal) present in orthopedic metal artifact reduction corrected images are removed in the MVCT-NMAR corrected images. A large dose reduction was possible outside the planning target volume (eg, 59.2 Gy to 52.5 Gy in pubic bone) when these MVCT-NMAR corrected images were used in TomoTherapy treatment plans without directional blocks for a prostate cancer patient. Conclusions: The use of MVCT-NMAR corrected images in radiation therapy treatment planning could improve the treatment plan quality for patients with metallic implants.

62 RADIOLOGY AND NUCLEAR MEDICINE↗
DOE OSTI2021

Process modeling, techno-economic assessment, and life cycle assessment of the electrochemical reduction of CO 2 : a review

The electrochemical reduction of CO 2 has emerged as a promising alternative to traditional fossil-based technologies for the synthesis of chemicals. Its industrial implementation could lead to a reduction in the carbon footprint of chemicals and the mitigation of climate change impacts caused by hard-to-decarbonize industrial applications, among other benefits. However, the current low technology readiness levels of such emerging technologies make it hard to predict their performance at industrial scales. During the past few years, researchers have developed diverse techniques to model and assess the electrochemical reduction of CO 2 toward its industrial implementation. The aim of this literature review is to provide a comprehensive overview of techno-economic and life cycle assessment methods and pave the way for future assessment approaches. First, we identify which modeling approaches have been conducted to extend analysis to the production scale. Next, we explore the metrics used to evaluate such systems, regarding technical, environmental, and economic aspects. Finally, we assess the challenges and research opportunities for the industrial implementation of CO 2 reduction via electrolysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Windowed least-squares model reduction for dynamical systems

Here we propose a windowed least-squares (WLS) approach for model reduction of dynamical systems. The proposed approach sequentially minimizes the time-continuous full-order-model residual within a low-dimensional space–time trial subspace over time windows. The approach comprises a generalization of existing model reduction approaches, as particular instances of the methodology recover Galerkin, least-squares Petrov–Galerkin (LSPG), and space–time LSPG projection. In addition, the approach addresses key deficiencies in existing model reduction techniques, e.g., the dependence of LSPG and space–time LSPG projection on the time discretization and the exponential growth in time exhibited by a posteriori error bounds for both Galerkin and LSPG projection. We consider two types of space–time trial subspaces within the proposed approach: one that reduces only the spatial dimension of the full-order model, and one that reduces both the spatial and temporal dimensions of the full-order model. For each type of trial subspace, we consider two different solution techniques: direct (i.e., discretize then optimize) and indirect (i.e., optimize then discretize). Numerical experiments conducted using trial subspaces characterized by spatial dimension reduction demonstrate that the WLS approach can yield more accurate solutions with lower space–time residuals than Galerkin and LSPG projection.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2023

DRIPS: A framework for dimension reduction and interpolation in parameter space

Reduced-order models are often used to describe the behavior of complex systems, whose simulation with a full model is too expensive, or to extract salient features from the full model’s output. We introduce a new model-reduction framework DRIPS (dimension reduction and interpolation in parameter space) that combines the offline local model reduction with the online parameter interpolation of reduced-order bases (ROBs). The offline step of this framework relies on dynamic mode decomposition (DMD) to build a low-rank linear surrogate model, equipped with a local ROB, for quantities of interest derived from the training data generated by repeatedly solving the (nonlinear) high-fidelity model for multiple parameter points. The online step consists of the construction of a parametric reduced-order model for each target/test point in the parameter space, with the interpolation of ROBs done on a Grassman manifold and the interpolation of reduced-order operators done on a matrix manifold. The DMD component enables DRIPS to model (typically low-dimensional) quantities of interest directly, without having to access the (typically high-dimensional and possibly nonlinear) operators in a high-fidelity model that governs the dynamics of the underlying high-dimensional state variables, as required in projection-based reduced-order modeling. A series of numerical experiments suggests that DRIPS yields a model reduction, which is computationally more efficient than the commonly used projection-based proper orthogonal decomposition; it does so without requiring a prior knowledge of the governing equation for quantities of interest. Furthermore, for the nonlinear systems considered, DRIPS is more accurate than Gaussian-process interpolation (Kriging).

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

Alternative reductants for foam control during vitrification of high-iron High Level Waste (HLW) feeds

Foaming during vitrification of radioactive waste in Joule-Heated Ceramic Melters (JHCM) is exacerbated by trapping of evolving gases, such as CO 2 , NO x and O 2 , beneath a viscous reaction layer. Foaming restricts heat transfer during melting. Sucrose is employed as the baseline additive at the Hanford site in Washington State, USA to reduce foaming. Alternative carbon-based reductant additives were explored in simulated, inactive Hanford high-iron HLW-NG-Fe2 feeds, for both their effect on foaming and to give insight to the behaviour of multivalent species in glass melts under different redox conditions. Graphite, coke (93% C), formic acid and HEDTA additives were compared with sucrose, and a feed with no additive. Graphite and coke additions proved most effective in reducing the maximum foam volume by 51 ± 3% and 54 ± 2%, respectively, compared with 24 ± 5% for sucrose. Lower foaming could result in more efficient vitrification in JHCMs. Reductants also affected redox ratios in the multivalent species present in the feed. The order of reduction, Mn 3+ /Mn 2+ > Cr 6+ /Cr 3+ > Ce 3+ /Ce 4+ > Fe 3+ /Fe 2+ was as predicted on the basis of their redox potentials. There is less reduction overall, particularly in the Fe 3+ → Fe 2+ , than predicted by the calculations, attributed to the oxygenated atmosphere of the experiments.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2016

Effective reduction in the nanoparticle sizes of NiO obtained via the pyrolysis of nickel malonate precursor modified using oleylamine surfactant

Nickel oxide nanoparticles were synthesized via thermal decomposition of two precursors, the first, a simple nickel malonate and the second, a nickel malonate modified by oleylamine, a surfactant, both having been synthesized by precipitation. While FTIR, TGA and ToF-SIMS were used to characterize the two precursors and to show the presence of oleylamine in the modified precursor, XRD, SEM, TEM and BET were employed to investigate the structure, the morphology and the specific surface area of the decomposition products obtained after pyrolysis. The results showed that the modification of nickel malonate by oleylamine was effective. The XRD results, which showed a cubic structure for the NiO obtained, suggest with SEM an important particle size reduction (at least 54%) when oleylamine was used to modify the nickel malonate precursor. The SEM images also showed a well-defined spherical nanoparticle morphology in both cases, not affected by the presence of oleylamine. The TEM also confirmed the reduction of particle size and their spherical nature but at the same time showed that, in the presence of oleylamine, there was no agglomeration resulting in a more uniform particle size distribution. The specific surface area of the NiO obtained by the oleylamine-modified precursor was 4.7 times larger than that obtained with the regular precursor. This again confirms the particle size reduction. - Highlights: • Nickel malonate precursor has been synthesized by precipitation method. • This precursor was successfully modified by a surfactant (oleylamine). • NiO was identified as the decomposition products of the previous precursors. • Oleylamine has provoked around 54% of particle size reduction of the NiO.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Oxygen reduction reaction catalyzed by platinum nanonetwork prepared by template free one step synthesis for polymer electrolyte membrane fuel cells

Highlights: • Supportless Pt nanonetwork (Pt NN) synthesized by novel template free one step method as per our earlier reported procedure. • Electrocatalytic activity of Pt NN studied taking oxygen reduction reaction in acid medium. • Kinetic and thermodynamic parameters were deduced under hydrodynamic conditions. • ORR mechanistic pathway was proposed based on kinetic rate constants. • ADT analysis found enhanced stability (5000 cycles) for Pt NN than Pt NN/VC and reported Pt/C. - Abstract: The reduction reaction of molecular oxygen (ORR) was investigated using supportless Pt nanonetwork (Pt NN) electrocatalyst in sulfuric acid medium. Pt NN was prepared by template free borohydride reduction. The transmission electron microscope images revealed a network like nano-architecture having an average cluster size of 30 nm. The electrochemical characterization of supportless and Vulcan carbon supported Pt NN (Pt NN/VC) was carried out using rotating disc and ring disc electrodes at various temperatures. Kinetic and thermodynamic parameters were estimated under hydrodynamic conditions and compared with Pt NN/VC and reported Pt/C catalysts. The accelerated durability test revealed that supportless Pt NN is quite stable for 5000 potential cycles with 22% reduction in electrochemical surface area (ECSA). While the initial limiting current density has in fact increased by 11.6%, whereas Pt NN/VC suffered nearly 55% loss in ECSA and 13% loss in limiting current density confirming an enhanced stability of supportless Pt NN morphology for ORR compared to conventional Pt/C ORR catalysts in acid medium.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Selective catalytic reduction of NO by ammonia and NO oxidation Over CoO x /CeO 2 catalysts

The selective catalytic reduction of NOsub>x with NH 3 (NH 3 -SCR) at low temperatures is still a major challenge in environmental catalysis research. Metal oxide based catalysts have attracted great attention due to their excellent low-temperature activity. In this study, CeO 2 -supported cobalt (Co)-oxide with variable Co/Ce weight ratios were prepared by the incipient-wetness impregnation method. The effect of Co loading as well as the effect of temperature on catalytic behaviors have been studied for the NO reduction and NO oxidation reactions. Thorough characterization by means of BET, XRD, and Raman has shown the topological model of the catalyst and interpretation of the observed reactivity trends. The activity test of CoO x /CeO 2 catalysts showed that the addition of Co enhanced the activity of NO reduction as well as that of NO oxidation. The most active catalyst with 10 wt% Co loading showed 70% NO reduction and 85% NO oxidation activity. Catalyst characterization results indicated that Co was monodispersed on ceria surface with the low Co loading amount, while Co 3 O 4 was formed on ceria with high Co loading amounts that affected the overall catalytic activity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Variance Reduction Factor of Nuclear Data for Integral Neutronics Parameters

We propose a new quantity, a variance reduction factor, to identify nuclear data for which further improvements are required to reduce uncertainties of target integral neutronics parameters. Important energy ranges can be also identified with this variance reduction factor. Variance reduction factors are calculated for several integral neutronics parameters. The usefulness of the variance reduction factors is demonstrated.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2013

Contribution of cooperative sector recycling to greenhouse gas emissions reduction: A case study of Ribeirão Pires, Brazil

Highlights: • Cooperative recycling achieves environmental, economic and social objectives. • We calculate GHG emissions reduction for a recycling cooperative in São Paulo, Brazil. • The cooperative merits consideration as a Clean Development Mechanism (CDM) project. • A CDM project would enhance the achievements of the recycling cooperative. • National and local waste management policies support the recycling cooperative. - Abstract: Solid waste, including municipal waste and its management, is a major challenge for most cities and among the key contributors to climate change. Greenhouse gas emissions can be reduced through recovery and recycling of resources from the municipal solid waste stream. In São Paulo, Brazil, recycling cooperatives play a crucial role in providing recycling services including collection, separation, cleaning, stocking, and sale of recyclable resources. The present research attempts to measure the greenhouse gas emission reductions achieved by the recycling cooperative Cooperpires, as well as highlight its socioeconomic benefits. Methods include participant observation, structured interviews, questionnaire application, and greenhouse gas accounting of recycling using a Clean Development Mechanism methodology. The results show that recycling cooperatives can achieve important energy savings and reductions in greenhouse gas emissions, and suggest there is an opportunity for Cooperpires and other similar recycling groups to participate in the carbon credit market. Based on these findings, the authors created a simple greenhouse gas accounting calculator for recyclers to estimate their emissions reductions.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2014

Landfill reduction experience in The Netherlands

Highlights: • ‘Zero waste’ initiatives never consider risks, side effects or experience of achieved low levels of landfill. • This paper provides insight into what works and what not. • Where strong gradients in regulations and tax occur between countries, waste will find its way to landfills across borders. • Strong landfill reduction can create a fierce competition over the remaining waste to be landfilled resulting in losses. • At some point a public organisation should take responsibility for the operation of a ‘safety net’ in waste management. - Abstract: Modern waste legislation aims at resource efficiency and landfill reduction. This paper analyses more than 20 years of landfill reduction in the Netherlands. The combination of landfill regulations, landfill tax and landfill bans resulted in the desired landfill reduction, but also had negative effects. A fierce competition developed over the remaining waste to be landfilled. In 2013 the Dutch landfill industry generated €40 million of annual revenue, had €58 million annual costs and therefore incurred an annual loss of €18 million. It is not an attractive option to prematurely end business. There is a risk that Dutch landfill operators will not be able to fulfil the financial obligations for closure and aftercare. Contrary to the polluter pays principle the burden may end up with society. EU regulations prohibiting export of waste for disposal are in place. Strong differentials in landfill tax rate between nations have nevertheless resulted in transboundary shipment of waste and in non-compliance with the self-sufficiency and proximity principles. During the transformation from a disposal society to a recycling society, it is important to carefully plan required capacity and to guide the reorganisation of the landfill sector. At some point, it is no longer profitable to provide landfill services. It may be necessary for public organisations or the state to take responsibility for the continued operation of a ‘safety net’ in waste management. Regulations have created a financial incentive to pass on the burden of monitoring and controlling the impact of waste to future generations. To prevent this, it is necessary to revise regulations on aftercare and create incentives to actively stabilise landfills.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2026

Estimating the Benefits of Sustainable Aviation Fuel Usage at Chicago O’Hare International Airport on Ultrafine Particle Exposure and Mortalities Reductions

The expanding commercial aviation sector necessitates diverse energy sources, and sustainable aviation fuels (SAFs) have emerged as a promising option. Widespread SAF adoption can help meet transportation fuel demand and offer health benefits for people residing near airports or along airport landing and takeoff (LTO) pathways, where elevated levels of aircraft-derived air pollution often exist. Blending SAF with traditional jet fuels can reduce ultrafine particle (UFP) emissions, which may improve health of near airport population. We analyzed a population of about 8 million people in 1925 census tracts around the Chicago O’Hare International Airport (ORD). We conducted a risk assessment to estimate anticipated UFP reductions for three adoption scenarios using blends of traditional jet fuels with 5, 25, and 50% SAF across all flights landing and taking off from ORD. We calculated baseline estimates of UFP emissions using ORD flight data, a dispersion model, and a calibration function derived from mobile monitoring data. We used this baseline UFP emission profile across the study area to estimate population-weighted UFP, as well as the attributable case reductions (ACRs) and attributable mortality rate reductions (AMRRs) across the demographic distribution around the airport, based on the SAF blending scenarios. We found a positive association of SAF blending with UFP reductions, particularly near the airport and along LTO flight pathways. Our study showed that the population-weighted UFP across different demographics was similar. ACRs were largely dependent on individual demographic populations, while AMRRs for all populations were relatively similar, with an estimated 0.3 (95% range: 0.2−0.3), 1.1 (0.9−1.4), and 1.8 (1.5−2.2) fewer mortalities per 100,000 people per year expected with the adoption of 5, 25, and 50% SAF blends, respectively. This study indicates that communities near ORD, across a range of demographics, may benefit similarly from SAF adoption, thus highlighting how SAF adoption may offer an opportunity to improve health outcomes like aviation UFP-related mortalities around airports.

10 SYNTHETIC FUELS↗
DOE OSTI2020

Production of C 2 /C 3 Oxygenates from Planar Copper Nitride-Derived Mesoporous Copper via Electrochemical Reduction of CO 2

Electrochemical reduction of CO 2 provides an opportunity to produce fuels and chemicals in a carbon-neutral manner, assuming that CO 2 can be captured from the atmosphere. To do so requires efficient, selective, and stable catalysts. In this study, we report a highly mesoporous metallic Cu catalyst prepared by electrochemical reduction of thermally nitrided Cu foil. Under aqueous saturated CO 2 reduction conditions, the Cu 3 N-derived Cu electrocatalyst produces virtually no CH 4 , very little CO, and exhibits a faradaic efficiency of 68% in C 2+ products (C 2 H 4 , C 2 H 5 OH, and C 3 H 7 OH) at a current density of ~18.5 mA cm –2 and a cathode potential of -1.0 V versus the reversible hydrogen electrode. Under these conditions, the catalyst produces more oxygenated products than hydrocarbons. We show that surface roughness is a good descriptor of catalytic performance. The roughest surface reached 98% CO utilization efficiency for C 2+ product formation from CO 2 reduction and the ratio of oxygenated to hydrocarbon products correlates with the degree of surface roughness. These effects of surface roughness are attributed to the high population of undercoordinated sites as well as a high pH environment within the mesopores and adjacent to the surface of the catalyst.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗