skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.


Title: Machine learning-assisted ammonium detection using zinc oxide/multi-walled carbon nanotube composite based impedance sensors
Abstract We report a machine learning approach to accurately correlate the impedance variations in zinc oxide/multi walled carbon nanotube nanocomposite (F-MWCNT/ZnO-NFs) to NH4+ions concentrations. Impedance response of F-MWCNT/ZnO-NFs nanocomposites with varying ZnO:MWCNT compositions were evaluated for its sensitivity and selectivity to NH4+ions in the presence of structurally similar analytes. A decision-making model was built, trained and tested using important features of the impedance response of F-MWCNT/ZnO-NF to varying NH4+concentrations. Different algorithms such as kNN, random forest, neural network, Naïve Bayes and logistic regression are compared and discussed. ML analysis have led to identify the most prominent features of an impedance spectrum that can be used as the ML predictors to estimate the real concentration of NH4+ion levels. The proposed NH4+sensor along with the decision-making model can identify and operate at specific operating frequencies to continuously collect the most relevant information from a system.  more » « less
Award ID(s):
2100930
PAR ID:
10361034
Author(s) / Creator(s):
; ; ; ; ; ; ;
Publisher / Repository:
Nature Publishing Group
Date Published:
Journal Name:
Scientific Reports
Volume:
11
Issue:
1
ISSN:
2045-2322
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract The seasonal controls of hydrology, temperature, hypoxia, and biogeochemical conditions for groundwater ammonium–N (NH4+) concentrations are not well understood. Here we investigated these controls for riparian groundwaters located upstream of two milldams over a period of 4 years. Groundwater chemistry was sampled monthly while groundwater elevations, hydraulic gradients, and temperatures were recorded sub‐hourly. Distinct seasonal patterns for NH4+were observed which differed among the wells. For wells that displayed a strong seasonal pattern, NH4+concentrations increased through the summer and peaked in October–November. These elevated concentrations were attributed to ammonification, suppression of nitrification, and/or dissimilatory nitrate reduction to ammonium (DNRA). These processes were driven by high groundwater temperatures, low hydraulic gradients (or long residence times), hypoxic/anoxic groundwater conditions, and increased availability of dissolved organic carbon as an electron donor. In contrast, NH4+concentrations decreased in the riparian groundwater from January to April during cool and wet conditions. A groundwater well with elevated total dissolved iron (TdFe) concentrations had elevated NH4+concentrations but displayed a muted seasonal response. In addition to hydrologic controls, we attributed this response to additional NH4+contribution from Fe‐driven autotrophic DNRA and/or ammonification linked to dissimilatory Fe reduction. Understanding the temporal patterns and factors controlling NH4+in riparian groundwaters is important for making appropriate watershed management decisions and implementing appropriate best management practices. 
    more » « less
  2. Abstract This work reports important fundamental advancements in multiwall carbon nanotube (MWCNT) rectenna devices by creating and optimizing new diode structures to allow optical rectification with air‐stable devices. The incorporation of double‐insulator layer tunnel diodes, fabricated for the first time on MWCNT arrays, enables the use of air‐stable top metals (Al and Ag) with excellent asymmetry for rectification applications. Asymmetry is increased by as much as 10 times, demonstrating the effectiveness of incorporating multiple dielectric layers to control electron tunneling in MWCNT diode structures. MWCNT tip opening also reduces device resistance up to 75% due to an increase in diode contact area to MWCNT inner walls. This effect is consistent for different oxide materials and thicknesses. A number of insulator layers, including Al2O3, HfO2, TiO2, ZnO, and ZrO2, in both single‐ and then double‐insulator configurations are tested. Resistance increases exponentially with insulator thickness and decreases with electron affinity. These results are used to characterize double‐insulator diode performance. Finally, for the most asymmetric device structure, Al2O3‐HfO2(4/4 nm), optical rectification at a frequency of 470 THz (638 nm) is demonstrated. These results open the door for designing efficient MWCNT rectenna devices with more material flexibility, including air‐stable, transparent, and conductive top electrode materials. 
    more » « less
  3. Abstract Ammonia (NH3) from animal feeding operations (AFOs) is an important source of reactive nitrogen in the US, but despite its ramifications for air quality and ecosystem health, its near‐source evolution remains understudied. To this end, Phase I of the Transport and Transformation of Ammonia (TRANS2Am) field campaign was conducted in the northeastern Colorado Front Range in summer 2021 and characterized atmospheric composition downwind of AFOs during 10 research flights. Airborne measurements of NH3, nitric acid (HNO3), and a suite of water‐soluble aerosol species collected onboard the University of Wyoming King Air research aircraft present an opportunity to investigate the sensitivity of particulate matter (PM) formation to AFO emissions. We couple the observations with thermodynamic modeling to predict the seasonality of ammonium nitrate (NH4NO3) formation. We find that during TRANS2Am northeastern Colorado is consistently in the NH3‐rich and HNO3‐limited NH4NO3formation regime. Further investigation using the Extended Aerosol Inorganics Model reveals that summertime temperatures (mean: 23°C) of northeastern Colorado, especially near the surface, inhibit NH4NO3formation despite high NH3concentrations (max: ≤114 ppbv). Finally, we model spring/autumn and winter conditions to explore the seasonality of NH4NO3formation and find that cooler temperatures could support substantially more NH4NO3formation. Whereas NH4NO3only exceeds 1 μg m−3∼10% of the time in summer, modeled NH4NO3would exceed 1 μg m−361% (88%) of the time in spring/autumn (winter), with a 10°C (20°C) temperature decrease relative to the campaign. 
    more » « less
  4. Abstract Stream fluxes are commonly reported without a complete accounting for uncertainty in the estimates, which makes it difficult to evaluate the significance of findings or to identify where to direct efforts to improve monitoring programs. At the Hubbard Brook Experimental Forest in the White Mountains of New Hampshire, USA, stream flow has been monitored continuously and solute concentrations have been sampled approximately weekly in small, gaged headwater streams since 1963, yet comprehensive uncertainty analyses have not been reported. We propagated uncertainty in the stage height–discharge relationship, watershed area, analytical chemistry, the concentration–discharge relationship used to interpolate solute concentrations, and the streamflow gap‐filling procedure to estimate uncertainty for both streamflow and solute fluxes for a recent 6‐year period (2013–2018) using a Monte Carlo approach. As a percentage of solute fluxes, uncertainty was highest for NH4+(34%), total dissolved nitrogen (8.8%), NO3(8.1%), and K+(7.4%), and lowest for dissolved organic carbon (3.7%), SO42−(4.0%), and Mg2+(4.4%). In units of flux, uncertainties were highest for solutes in highest concentration (Si, DOC, SO42−, and Na+) and lowest for those lowest in concentration (H+and NH4+). Laboratory analysis of solute concentration was a greater source of uncertainty than streamflow for solute flux, with the exception of DOC. Our results suggest that uncertainty in solute fluxes could be reduced with more precise measurements of solute concentrations. Additionally, more discharge measurements during high flows are needed to better characterize the stage‐discharge relationship. Quantifying uncertainty in streamflow and element export is important because it allows for determination of significance of differences in fluxes, which can be used to assess watershed response to disturbance and environmental change. 
    more » « less
  5. Abstract Optical atomic clocks are the most accurate and precise measurement devices of any kind, enabling advances in international timekeeping, Earth science, fundamental physics, and more. However, there is a fundamental tradeoff between accuracy and precision, where higher precision is achieved by using more atoms, but this comes at the cost of larger interactions between the atoms that limit the accuracy. Here, we propose a many-ion optical atomic clock based on three-dimensional Coulomb crystals of order one thousand Sn2+ions confined in a linear RF Paul trap with the potential to overcome this limitation. Sn2+has a unique combination of features that is not available in previously considered ions: a1S0 ↔ 3P0clock transition between two states with zero electronic and nuclear angular momentum (I = J = F = 0) making it immune to nonscalar perturbations, a negative differential polarizability making it possible to operate the trap in a manner such that the two dominant shifts for three-dimensional ion crystals cancel each other, and a laser-accessible transition suitable for direct laser cooling and state readout. We present calculations of the differential polarizability, other relevant atomic properties, and the motion of ions in large Coulomb crystals, in order to estimate the achievable accuracy and precision of Sn2+Coulomb-crystal clocks. 
    more » « less