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At least 397 records · Page 22

Spatial distributions of X CO 2 seasonal cycle amplitude and phase over northern high-latitude regions

Satellite-based observations of atmospheric carbon dioxide (CO 2 ) provide measurements in remote regions, such as the biologically sensitive but undersampled northern high latitudes, and are progressing toward true global data coverage. Recent improvements in satellite retrievals of total column-averaged dry air mole fractions of CO 2 (X CO 2 ) from the NASA Orbiting Carbon Observatory 2 (OCO-2) have allowed for unprecedented data coverage of northern high-latitude regions, while maintaining acceptable accuracy and consistency relative to ground-based observations, and finally providing sufficient data in spring and autumn for analysis of satellite-observed X CO 2 seasonal cycles across a majority of terrestrial northern high-latitude regions. Here, we present an analysis of X CO 2 seasonal cycles calculated from OCO-2 data for temperate, boreal, and tundra regions, subdivided into 5° latitude by 20° longitude zones. We quantify the seasonal cycle amplitudes (SCAs) and the annual half drawdown day (HDD). OCO-2 SCAs are in good agreement with ground-based observations at five high-latitude sites, and OCO-2 SCAs show very close agreement with SCAs calculated for model estimates of X CO 2 from the Copernicus Atmosphere Monitoring Services (CAMS) global inversion-optimized greenhouse gas flux model v19r1 and the CarbonTracker2019 model (CT2019B). Model estimates of X CO 2 from the GEOS-Chem CO 2 simulation version 12.7.2 with underlying biospheric fluxes from CarbonTracker2019 (GC-CT2019) yield SCAs of larger magnitude and spread over a larger range than those from CAMS, CT2019B, or OCO-2; however, GC-CT2019 SCAs still exhibit a very similar spatial distribution across northern high-latitude regions to that from CAMS, CT2019B, and OCO-2. Zones in the Asian boreal forest were found to have exceptionally large SCA and early HDD, and both OCO-2 data and model estimates yield a distinct longitudinal gradient of increasing SCA from west to east across the Eurasian continent. In northern high-latitude regions, spanning latitudes from 47 to 72° N, longitudinal gradients in both SCA and HDD are at least as pronounced as latitudinal gradients, suggesting a role for global atmospheric transport patterns in defining spatial distributions of X CO2 seasonality across these regions. GEOS-Chem surface contact tracers show that the largest X CO 2 SCAs occur in areas with the greatest contact with land surfaces, integrated over 15–30d. The correlation of X CO 2 SCA with these land surface contact tracers is stronger than the correlation of X CO 2 SCA with the SCA of CO 2 fluxes or the total annual CO 2 flux within each 5° latitude by 20° longitude zone. This indicates that accumulation of terrestrial CO 2 flux during atmospheric transport is a major driver of regional variations in X CO 2 SCA.

54 ENVIRONMENTAL SCIENCES↗

Optimization of Residential Air Source Heat Pump using Low–Global Warming Potential Refrigerants

We report low–global warming potential refrigerants can significantly reduce the direct emissions of CO 2 originating from HVAC systems. However, high-efficiency systems are needed to reduce indirect CO 2 emissions. In this study, an R410A residential 5-Ton heat pump was optimized using R32, R454A, R454B, R454C, and R455A. Among these options, R455A and R454C have the lowest global warming potential but have lower volumetric capacity and high glide. Optimization results using 5 mm tube heat exchangers showed 12.4% to 19.1% efficiency improvements and 13% to 33% reduction in CO 2 emissions.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

Improving Global Analysis and Short-Range Forecast Using Rainfall and Moisture Observations Derived from TRMM and SSM/I Passive Microwave Instruments

The Global Precipitation Mission, a satellite project under consideration as a follow-on to the Tropical Rainfall Measuring Mission (TRMM) by the National Aeronautics and Space Agency (NASA) in the United States, the National Space Development Agency (NASDA) in Japan, and other international partners, comprises an improved TRMM-like satellite and a constellation of 8 satellites carrying passive microwave radiometers to provide global rainfall measurements at 3-hour intervals. The success of this concept relies on the merits of rainfall estimates derived from passive microwave radiometers. This article offers a proof-of-concept demonstration of the benefits of using, rainfall and total precipitable water (TPW) information derived from such instruments in global data assimilation with observations from the TRMM Microwave Imager (TMI) and 2 Special Sensor Microwave/Imager (SSM/I) instruments. Global analyses that optimally combine observations from diverse sources with physical models of atmospheric and land processes can provide a comprehensive description of the climate systems. Currently, such data analyses contain significant errors in primary hydrological fields such as precipitation and evaporation, especially in the tropics. We show that assimilating the 6-h averaged TMI and SSM/I surface rainrate and TPW retrievals improves not only the hydrological cycle but also key climate parameters such as clouds, radiation, and the upper tropospheric moisture in the analysis produced by the Goddard Earth Observing System (GEOS) Data Assimilation System, as verified against radiation measurements by the Clouds and the Earth's Radiant Energy System (CERES) instrument and brightness temperature observations by the TIROS Operational Vertical Sounder (TOVS) instruments. Typically, rainfall assimilation improves clouds and radiation in areas of active convection, as well as the latent heating and large-scale motions in the tropics, while TPW assimilation leads to reduced moisture biases and improved radiative fluxes in clear-sky regions. Ensemble forecasts initialized with analyses that incorporate TMI and SSM/I rainfall and TPW data also yield better short-range predictions of geopotential heights, winds, and precipitation in the tropics. This study offers a compelling illustration of the potential of using rainfall and TPW information derived from passive microwave instruments to significantly improve the quality of 4-dimensional global datasets for climate analysis and weather forecasting applications.

Hou, Arthur Y.↗

Improving Assimilated Global Data Sets using TMI Rainfall and Columnar Moisture Observations

A global analysis that optimally combine observations from diverse sources with physical models of atmospheric and land processes can provide a comprehensive description of the climate systems. Currently, such data products contain significant errors in primary hydrological fields such as precipitation and evaporation, especially in the tropics. In this study, we show that assimilating precipitation and total precipitable water (TPW) retrievals derived from the TRMM Microwave Imager (TMI) improves not only the hydrological cycle but also key climate parameters such as clouds, radiation, and the large-scale circulation produced by the Goddard Earth Observing System (GEOS) data assimilation system (DAS). In particular, assimilating TMI rain improves clouds and radiation in areas of active convection, as well as the latent heating distribution and the large-scale motion field in the tropics, while assimilating TMI TPW heating distribution and the large-scale motion field in the tropics, while assimilating TMI TPW retrievals leads to reduced moisture biases and improved radiative fluxes in clear-sky regions. The improved analysis also improves short-range forecasts in the tropics. Ensemble forecasts initialized with the GEOS analysis incorporating TMI rain rates and TPW yield smaller biases in tropical precipitation forecasts beyond 1 day and better 500 hPa geopotential height forecasts up to 5 days. Results of this study demonstrate the potential of using high-quality space-borne rainfall and moisture observations to improve the quality of assimilated global data for climate analysis and weather forecasting applications

Hou, Arthur Y.↗

On optimizing a constellation of altimetric satellites for measuring global oceanic mesoscale

The orbital configuration of the Eos polar-platform constellation is examined to determine if baseline orbital parameters are appropriately specified to meet the mission goal of measuring global oceanic mesoscale variability. Using the Nyquist sampling theorem, spatial and temporal measurement requirements are first established for the constellation. Based upon these requirements, the optimum solution indicates that a total of five spacecraft are required to meet the mesoscale mapping task. Additional analyses are performed on both a two-platform configuration as well as the complete four-platform Eos constellation. The results of these calculations show that an optimized configuration of four properly-phased Eos platforms, placed into identical 835-km sun-synchronous orbits with 13-day repeat periods, can very nearly meet statistically significant sampling criteria for mapping global oceanic mesoscale variability.

Chase, Robert↗

Multi-spatio-temporal scales PIV in a turbulent buoyant jet discharging in a linearly stratified environment

Time-resolved particle image velocimetry is implemented with a camera array and several laser sheets; this results in a multi-spatio-temporal scale system that is modular and flexible. The setup is optimized to capture global flow features, while locally resolving in space and time near the Kolmogorov scale. The apparatus relies extensively on machine vision CMOS cameras; they are inexpensive and stream to computer hard drive with virtually continuous time-resolved records (up to one hour for the current system). This leads to statistically converged data and also helps in minimizing down time between experimental runs. Details of the implementation and design of experiment are reported. The system instruments a vertical buoyant jet discharging in a linearly stratified environment. Refractive index matched aqueous solutions enable precise optical deployment. The density difference is 3% and the fluids have similar dynamic viscosity. The jet Reynolds number is 2.00 x 10 4 and is above the mixing transition. Such flows are typically challenging to instrument and few velocity field data are available to date. The velocity statistics are reported as well as first insights gained from the campaign.

42 ENGINEERING↗

Development of a hybrid neural network and transfer learning model for optimized ICP-MS/MS operation

Correct function and calibration of instrumentation is a crucial assumption for any scientific experiment. One such instrument, tandem inductively coupled plasma mass spectrometer (ICP-MS/MS), has in-depth calibration settings that range across 30+ different parameters, making it difficult to determine optimal conditions without expertise and some degree of trial and error. Often, these settings are hand-tuned, a time-intensive process prone to local maxima and human error. While some automation is available, the automation also may favor local optimizations over a global optimum. In addition to these difficulties, day to day instrument variability can further complicate the calibration process. We propose a solution to this problem as a machine learning (ML) algorithm that learns how each parameter helps determine the calibration sensitivity across several elements, and re-weights parameters over time as instrument variability changes (e.g., a global neural network (NN) with a time-dependent transfer learning (TL) component). This model would be able to generate a surface of predicted calibration sensitivities and their respective parameters, and a simple multivariate algorithm would be able to pull out the optimum results with the settings associated with them. Here-in, we describe our initial findings in working towards this goal, including data extraction from historical files, exploratory data analysis, and some initial model building to better describe the data and the feasibility of our goal.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Abstract for CRADA among NETL, Mälardalen University, University College Cork (acting through its Tyndall National Institute), and Micro Electricity Generation Association

GeoCoHorT aims to accelerate the transition to 4 th generation district heating and cooling (4GDHC) in Europe and globally, by assessing, optimizing, and demonstrating the integration of shallow geothermal heat extraction with other renewable sources and smart buildings. The target geo-source is ground water from River Shannon (Limerick, Ireland), which will provide both an efficiency and noise-reduction benefit to the micro-district and a method of combatting climate-change-warming of the Shannon Estuary. The heat from this low-temperature source will be recycled and supplied to a smart district located in Limerick, Ireland, through heat pumps powered by renewable electricity and by means of a suitable DH network design. The mandate is to find solutions that work for entire communities in a fair and sustainable manner, with the involvement of the communities themselves to highlight their needs. The project brings together four partners from Ireland, Sweden, and the U.S.A. with strong multi-disciplinary competencies. The Tyndall Institute at University of Cork (UCC) and Mälardalen University (MDU) will design and optimize the 4GDH micro-district system, and the Micro Electricity Generation Association (MEGA) will work with the community to build a sense of ownership of the Climate Challenge and ensure close community involvement. The National Energy Technology Laboratory of the U.S. Department of Energy (NETL) will design the prospective geo-fluid loop to optimize heat-extraction effectiveness with ecological safety and assess the environmental benefits of the proposed solutions. Industrial advisors (Eskilstuna Strängnäs Energi och Miljö (ESEM) and Mimer in Sweden, and Smart MPOWER in Ireland) will steer the technology development to meet the needs of public utilities and consumers. Current infrastructure in the smart district in Limerick (demonstration site of an EU Lighthouse project) will be exploited and modified with support of MEGA, UCC, and MPOWER to integrate micro-DH from low-temperature heat sources, such as the river heat, and to allow increasing penetration of prosumers in the grid. Additional case studies will be developed with the help of industrial advisors to extend the results to other regions (e.g., Sweden and USA) and provide valuable insights for the development of 4GDH worldwide.

15 GEOTHERMAL ENERGY↗

Modeling and Characterization of Surface Discharges in Insulating Material for Spacers: Electrode Shape, Discharge Mode, and Revision of the Creepage Concept

In the design of MV AC and DC spacers, the predominant factors are surface and interface conditions. Design is generally carried out on specifications and standards which are based on long-term experience and lab testing. However, the diffusion of power electronics with a trend to increase electric field, switching frequency, and rise time to achieve higher power density calls for an innovative, global approach to optimized insulation system design. A new methodology, based on field simulation, discharge modeling, and partial discharge inception measurements, called the three-leg approach, can form the basis to optimize insulation design for any type of supply voltage waveform. This paper focuses on the influence of the type of electrode on the inception and phenomenology of surface discharges and, as a consequence, on the interpretation of the results used for application of the three-leg approach. It is demonstrated that a typical electrode system used for insulating material testing can generate both gas and surface discharges at the triple point, when the electrodes have a smooth profile that is used to avoid corona or flashover. Hence, testing partial discharge may not provide a straightforward indication of the surface discharge inception and, thus, be partially misleading for insulation design. Another takeover is that such analysis must benefit from PD testing tools endowed with analytics able to provide automatic identification of the type of defect generating PD, i.e., internal, surface, and corona, since design and remedy actions can be taken, and adequate insulating materials developed, only knowing the type of source generating PD. Hence, testing partial discharge may not provide a straightforward indication of surface discharge inception and, thus, be partially misleading for insulation design. In addition to the importance of the three-leg approach to favor reliable and optimized design of insulation systems, there is a clear need to have a PD testing tool endowed with analytics. It should preferably be able to provide automatic identification of the type of defect generating PD, i.e., internal, surface, and corona.

36 MATERIALS SCIENCE↗

Kinetics Modeling and Reactor Design Study of Glucose-to-Terpenes Cell-Free Conversion

Cell-free systems offer many advantages over traditional biological conversion by eliminating biological growth constraints. It also offers easy manipulation and finetuning of the reaction conditions for each individual enzyme. The conversion of cellulosic glucose to Limonene, a terpene, is a promising pathway for producing fuels and chemicals. Recent advances in developing cell-free systems focuses on bench scale optimization of terpene yield and to demonstrate its feasibility towards commercialization [1,2]. There is significant knowledge gap regarding reaction kinetics of these cell-free systems to further study how it will perform at larger scale. We present here, our studies on reaction kinetics and reactor design implications of cell-free glucose to Limonene conversion to facilitate the further development and commercialization of this process. We developed a novel kinetic model based on the metabolic-network structure of the cell-free system with multi-substrate reversible Michaelis-Menten rate law. To estimate kinetic parameters for this system of rate equations, we employed Bayesian optimization to perform global search with the assistance of gaussian processes to balance exploration and exploitation. The model parameters estimated showed good results compared with experimental data. The estimated parameters were used to perform sensitivity analysis. We found that Hexokinase is one of the most critical enzymes that affect the conversion of the glucose. We also observed that abundance of co-factors is also critical to the conversion of glucose to limonene. We investigated packed bed reactors with enzymes immobilized on the surface of particles to convert glucose stream into Limonene for larger scale production. The reactor design such as particle size, enzyme loading, and flow rate are found to be critical for improving yields. [1] Dudley, Q.M., Nash, C.J. and Jewett, M.C., 2019. Synthetic Biology, 4(1), p.ysz003. [2] Korman, T.P., Opgenorth, P.H. and Bowie, J.U., 2017. Nature communications, 8(1), p.15526.

09 BIOMASS FUELS↗

Adaptive analog video signal conditioner

This paper presents an adaptive analog video signal conditioner. This system supplements conventional irises and automatic gain controls to condition video signals for digitizing with a uniform analog-to-digital converter. Employing two degree of freedom, this circuit adjusts an analog gain and analog offset to increase the average information content of digitized images as defined by an entropy measure. The globally near-optimized implementation tracks smoothly to adapt to changing scene conditions.

Jeong, Cheol-Ho↗

Collectives for Multiple Resource Job Scheduling Across Heterogeneous Servers

Efficient management of large-scale, distributed data storage and processing systems is a major challenge for many computational applications. Many of these systems are characterized by multi-resource tasks processed across a heterogeneous network. Conventional approaches, such as load balancing, work well for centralized, single resource problems, but breakdown in the more general case. In addition, most approaches are often based on heuristics which do not directly attempt to optimize the world utility. In this paper, we propose an agent based control system using the theory of collectives. We configure the servers of our network with agents who make local job scheduling decisions. These decisions are based on local goals which are constructed to be aligned with the objective of optimizing the overall efficiency of the system. We demonstrate that multi-agent systems in which all the agents attempt to optimize the same global utility function (team game) only marginally outperform conventional load balancing. On the other hand, agents configured using collectives outperform both team games and load balancing (by up to four times for the latter), despite their distributed nature and their limited access to information.

Tumer, K.↗

Evolutionary Computing for Low-thrust Navigation

The development of new mission concepts requires efficient methodologies to analyze, design and simulate the concepts before implementation. New mission concepts are increasingly considering the use of ion thrusters for fuel-efficient navigation in deep space. This paper presents parallel, evolutionary computing methods to design trajectories of spacecraft propelled by ion thrusters and to assess the trade-off between delivered payload mass and required flight time. The developed methods utilize a distributed computing environment in order to speed up computation, and use evolutionary algorithms to find globally Pareto-optimal solutions. The methods are coupled with two main traditional trajectory design approaches, which are called direct and indirect. In the direct approach, thrust control is discretized in either arc time or arc length, and the resulting discrete thrust vectors are optimized. In the indirect approach, a thrust control problem is transformed into a costate control problem, and the initial values of the costate vector are optimized. The developed methods are applied to two problems: 1) an orbit transfer around the Earth and 2) a transfer between two distance retrograde orbits around Europa, the closest to Jupiter of the icy Galilean moons. The optimal solutions found with the present methods are comparable to other state-of-the-art trajectory optimizers and to analytical approximations for optimal transfers, while the required computational time is several orders of magnitude shorter than other optimizers thanks to an intelligent design of control vector discretization, advanced algorithmic parameterization, and parallel computing.

optimization↗

A Comparison of Methods for a Priori Bias Correction in Soil Moisture Data Assimilation

Data assimilation is being increasingly used to merge remotely sensed land surface variables such as soil moisture, snow and skin temperature with estimates from land models. Its success, however, depends on unbiased model predictions and unbiased observations. Here, a suite of continental-scale, synthetic soil moisture assimilation experiments is used to compare two approaches that address typical biases in soil moisture prior to data assimilation: (i) parameter estimation to calibrate the land model to the climatology of the soil moisture observations, and (ii) scaling of the observations to the model s soil moisture climatology. To enable this research, an optimization infrastructure was added to the NASA Land Information System (LIS) that includes gradient-based optimization methods and global, heuristic search algorithms. The land model calibration eliminates the bias but does not necessarily result in more realistic model parameters. Nevertheless, the experiments confirm that model calibration yields assimilation estimates of surface and root zone soil moisture that are as skillful as those obtained through scaling of the observations to the model s climatology. Analysis of innovation diagnostics underlines the importance of addressing bias in soil moisture assimilation and confirms that both approaches adequately address the issue.

Kumar, Sujay V.↗

An Assessment of Actual and Potential Building Climate Zone Change and Variability From the Last 30 Years Through 2100 Using NASA's MERRA and CMIP5 Simulations

Background: In the US, residential and commercial building infrastructure combined consumes about 40% of total energy usage and emits about 39% of total CO2 emission (DOE/EIA "Annual Energy Outlook 2013"). Building codes, as used by local and state enforcement entities are typically tied to the dominant climate within an enforcement jurisdiction classified according to various climate zones. These climate zones are based upon a 30-year average of local surface observations and are developed by DOE and ASHRAE. Establishing the current variability and potential changes to future building climate zones is very important for increasing the energy efficiency of buildings and reducing energy costs and emissions in the future. Objectives: This paper demonstrates the usefulness of using NASA's Modern Era Retrospective-analysis for Research and Applications (MERRA) atmospheric data assimilation to derive the DOE/ASHRAE building climate zone maps and then using MERRA to define the last 30 years of variability in climate zones for the Continental US. An atmospheric assimilation is a global atmospheric model optimized to satellite, atmospheric and surface in situ measurements. Using MERRA as a baseline, we then evaluate the latest Climate Model Inter-comparison Project (CMIP) climate model Version 5 runs to assess potential variability in future climate zones under various assumptions. Methods: We derive DOE/ASHRAE building climate zones using surface and temperature data products from MERRA. We assess these zones using the uncertainties derived by comparison to surface measurements. Using statistical tests, we evaluate variability of the climate zones in time and assess areas in the continental US for statistically significant trends by region. CMIP 5 produced a data base of over two dozen detailed climate model runs under various greenhouse gas forcing assumptions. We evaluate the variation in building climate zones for 3 different decades using an ensemble and quartile statistics to provide an assessment of potential building climate zone changes relative to the uncertainties demonstrated using MERRA. Findings and Conclusions: These results show that there is a statistically significant increase in the area covered by warmer climate zones and a tendency for a reduction of area in colder climate zones in some limited regions. The CMIP analysis shows that models vary from relatively little building climate zone change for the least sensitive and conservation assumptions to a warming of at most 3 zones for certain areas, particularly the north central US by the end of the 21st century.

Stackhouse, Paul W., Jr.↗

Adding GPU Support to the Markov Chain Monte Carlo Code Catmip

In geophysics, we are confronted with many under-determined inverse problems. For example, all of our observations of earthquakes are made at the Earth’s surface. So, when we try to infer how slip during an earthquake evolves in space and time, we find that there are many potential slip histories that are consistent with our limited observations and our understanding of earthquake physics. One way to approach these problems is with Bayesian analysis which allows us to infer the ensemble of all potential slip models that satisfy the observations and our prior knowledge of earthquake physics. In Bayesian analysis, our prior knowledge is known as the prior probability density function or prior PDF, the fit to the data is known as the data likelihood, and the target PDF that satisfies both the prior PDF and data likelihood is known as the posterior PDF. However, simulating the posterior PDF typically requires using Markov Chain Monte Carlo (MCMC) to draw tens of billions of random realizations of earthquake slip models, which may not be computationally feasible. To make this and similar geophysical inversions computationally tractable, we developed the Cascading Adaptive Transitional Metropolis In Parallel (CATMIP) algorithm. CATMIP is an efficient parallel Markov Chain Monte Carlo (MCMC) sampler that is used for model fitting and uncertainty quantification in geophysics. Example use cases are earthquake rupture modeling, determining mineral composition on Mars, reconstructing the history of ocean salinity, and historical earthquake relocation. CATMIP employs many parallel instances of the Metropolis algorithm for sampling in a transitioning framework. Transitioning is a process in which a set of random samples at equilibrium with a known probability density function (PDF) are used as seeds for the Markov chains to sample successive target PDFs that incrementally move the distribution from the starting seeds to the final desired PDF that describes the relative plausibility of potential values for the model parameters. The algorithm is implemented as a Master-Worker model employing MPI for communication. The worker processes are loosely coupled with global parameters periodically optimized by the master process. This provides a very high amount of parallelism with little communication between updates. During the presentation we will discuss the history of the algorithm and elaborate the earthquake rupture modeling use case for the CATMIP package. Our first step toward GPU optimization was to optimize the code for the CPU. CPU profiling revealed that most of the compute time is spent in calls to level 2 BLAS routines and calls to GSL random number generators. We revised the algorithm to employ level 3 BLAS routines instead. In our presentation we will describe how this was accomplished. Adding GPU support to CATMIP consisted mostly of replacing the calls to GSL with calls to GPU vendor-provided library routines. A small number of loops were directly implemented in CUDA. In the presentation will provide implementation details. Finally, we will discuss methods for profiling and opportunities for further optimizing GPU execution. By creating a code with the flexibility to run on either a CPU or GPU architecture, CATMIP can be used on systems ranging from large CPU-based HPC environments to single servers with GPU acceleration and everything in between.

HECC↗

Optimization of the Lunar Icecube Trajectory Using Stochastic Global Search and Multi-Point Shooting

Lunar IceCube is a 6U cubesat that will launch on NASA’s Artemis 1 mission in 2021. Lunar IceCube will separate from Artemis 1 shortly after trans-lunar injection (TLI) and travel to its science orbit about the moon using its Busek Ion Thruster 3 (BIT-3) propulsion system. This paper describes a technique to rapidly design Lunar IceCube trajectories using the monotonic basin hopping (MBH) stochastic global search algorithm, along with low- and high-fidelity multi-point shooting transcriptions. This technique allows the Lunar IceCube team to rapidly adapt to changing initial conditions, spacecraft properties, and operational constraints.

optimization↗

Adaptive learning-driven high-throughput synthesis of oxygen reduction reaction Fe–N–C electrocatalysts

Reducing human reliance on inefficient energy systems and fossil fuels has become more urgent due to the consequences of global climate change. However, traditional trial-and-error approaches have hampered our ability to accelerate the discovery and implementation of functional materials for efficient energy conversion devices, such as polymer electrolyte fuel cells (PEFCs). To address this, we develop an adaptive learning framework that integrates machine learning and state-of-the-art capabilities in high-throughput synthesis to achieve expedited optimization of iron-nitrogen-carbon PEFC oxygen reduction reaction (ORR) electrocatalysts. We use statistical inference, uncertainty quantification, and global optimization to build a computational design-of-experiment tool that identifies the optimum compositions to be investigated next to reduce the demands placed on experimental materials discovery. We benchmark the ability of the proposed strategy to discover optimum catalyst synthesis conditions in a six-dimensional search space when starting with a thirty-six-sample database. By following the adaptive learning strategy, we synthesize fourteen new catalysts from approximately ten billion unique compositions and discover four catalysts that outperform all original samples. The best machine learning-optimized catalyst is 33% more active than the highest-performing one in the initial database, showing an ORR activity seven times larger than those typically reported for the same class of materials.

36 MATERIALS SCIENCE↗