Source: CONNECTICUT AGRICULTURAL EXPERIMENT STATION submitted to NRP
USING HIGH RESOLUTION MASS SPECTROMETRY TO ASSESS THE IMPACTS OF RECLAIMED WASTEWATER USE FOR CROP IRRIGATION
Sponsoring Institution
National Institute of Food and Agriculture
Project Status
COMPLETE
Funding Source
Reporting Frequency
Annual
Accession No.
1019602
Grant No.
(N/A)
Cumulative Award Amt.
(N/A)
Proposal No.
(N/A)
Multistate No.
(N/A)
Project Start Date
May 29, 2019
Project End Date
May 16, 2022
Grant Year
(N/A)
Program Code
[(N/A)]- (N/A)
Recipient Organization
CONNECTICUT AGRICULTURAL EXPERIMENT STATION
PO BOX 1106
NEW HAVEN,CT 06504
Performing Department
Environmental Sciences
Non Technical Summary
Water scarcity is a problem throughout the modern world and is expected to increase as human population expands and climate change intensifies. Wastewater reuse for agricultural irrigation is an important strategy to reduce demand from surface and ground water sources and is gaining momentum as obtaining freshwater from other sources becomes more difficult. While an important strategy for combating water scarcity, wastewater reuse for agriculture is not without risks. Wastewater can contain higher levels of bacteria, heavy metals, salts, and other contaminants than conventional water sources. Specifically, there is increasing concern over organic microcontaminants (OMCs) such as pharmaceuticals, pesticides, and endocrine disrupting compounds that may be taken up into irrigated crop plants. Designing methods to detect new and emerging OMCs will be increasingly important as water recycling continues to expand.High Resolution Mass Spectrometry (HRMS), often coupled with liquid chromatography (LC), is a new technology that can be used to detect OMCs in water, soil, and food crops. HRMS data can be used for suspect screening, which searches databases of past measurements to find matches for chemicals present in new samples, and for non-targeted analysis (NTA) which identifies features in the data without necessarily matching them to known chemicals. The USFDA and USEPA do not yet have standardized methods for suspect screening and NTA, but use of these types of data analysis could greatly improve recognition of new and unexpected OMCs in food and in the environment.This project will focus on developing suspect screening and NTA methods for use at the Connecticut Agricultural Experiment Station (CAES) and analyzing crops irrigated with recycled water. The first portion of the project will focus on substantial method development and validation experiments with LC-HRMS, and the second portion will be a greenhouse experiment where we grow and compare tomatoes, celery, and lettuce irrigated with fresh water and recycled wastewater. We will measure OMC and heavy metal accumulation in the plants and also assess plant health. At CAES, we have the knowledge and resources available to develop and implement these methods, and to grow crops and assess plant health effects. Our project will result in knowledge and publications about new analytical methods, as well as the effects of water reuse for agricultural irrigation.
Animal Health Component
10%
Research Effort Categories
Basic
30%
Applied
10%
Developmental
60%
Classification

Knowledge Area (KA)Subject of Investigation (SOI)Field of Science (FOS)Percent
7111499200020%
4035370200010%
2031499115010%
7117310200025%
7117299200025%
4035360200010%
Goals / Objectives
This project will focus on developing liquid chromatography - high resolution mass spectrometry based suspect screening and non-targeted analysismethods for use at the Connecticut Agricultural Experiment Station and analyzing the effects of irrigation with recycled water on crop plants. Our project will result in knowledge and publications about new analytical methods, as well as the effects of water reuse for agricultural irrigation.Objective 1: Developand evaluatesuspect screening and non-targeted analysis methods for crop plants, soils, and recycled water.Objective 2: Investigate organic microcontaminant and heavy metal accumulation by crop plants irrigated with recycled water and relate the results to effects on plant health.
Project Methods
Objective 1:We will develop computational, analytical, and sample preparation methods for conducting suspect screening and non-targeted analysis (NTA) at the Connecticut Agricultural Experiment Station (CAES), and provide a validation framework for similar methods in other labs.The first step will be to ensure we have the computational abilities to conduct suspect screening and NTA. We will conduct three types of computational analysis: internal suspect screening, external suspect screening, and true NTA. Computational method development will require minimal collection of new data. CAES has collected data for many projects already using the orbitrap mass spectrometers, but only targeted data analysis has been done. Non-targeted analysis can be conducted on the same data. We will test our new computational methods by reanalyzing the files to see if our results are comparable. For example, we should be able to use the new suspect screening methods to identify pesticides that were previously spiked into a vegetable sample for targeted, quantitative method development. We will also use our new computational methods to search for additional information about previous samples. For example, we will look for evidence for the presence of pesticides that were not on the analyte lists for previous studies.We will also develop analytical and sample preparation methods for use in this project. We will use the Q-Exactive LC-MS in the CAES Analytical Chemistry department for all data collection and base our instrument methods on those that are commonly used here already. We will create a standard mixture of approximately 50 organic micro contaminants (OMCs) that are commonly found in reclaimed wastewater (including pharmaceuticals, personal care product ingredients, pesticides, disinfection byproducts, and food additives), and ensure that as many as possible can be successfully measured using our instrument method(s). We will develop sample preparation methods for plants, soil, and water, that are as universal as possible, sensitive, and similar to each other. We will conduct tests where our 50 compound mixture is spiked into to water at 10 µg·L-1 and to plant tissue and soil at 10 ng·g-1, and assess our ability to extract and measure the spiked compounds.As a complete method development test, we will have a CAES technician create an "unknown" spiking solution using a subset of compounds in the method development mixture, as well as some that were not included. Plant, soil, and water samples will be fortified with the mixture, then extracted and analyzed using the developed methods. We will then use our internal and external suspect screening methods to determine the compounds included in the spike solution. We will report information about which compounds we can detect, as well as those we cannot and those that we identify as false positives.No extraction and analysis method is truly universal, and we expect there will be compounds on our list of 50 that we are unable to detect. However, knowledge about the limitations of the methods used can help with the suspect screening and NTA process. Some candidate structures matched to detected masses can be eliminated based on knowledge about the detection methods used. Thus, the positive and negative data obtained will be useful as we move forward to studies using the methods developed.Objective 2:We will conduct a greenhouse experiment where we grow and compare tomatoes, celery, and lettuce irrigated with fresh water and recycled wastewater. We will obtain a supply of secondary treated wastewater from the Greater New Haven Area Water Pollution Control Authority. Our irrigation protocol will follow the policies established for recycled water use in California. Plants will be watered with their designated irrigation treatment starting when seeds are first germinated. No-plant controls will also be included for each irrigation treatment. Plants will be grown in field soil obtained from the CAES farm.Plants will be harvested after they produce viable fruit (tomato) or when they reach a standard harvest size for human consumption (celery and lettuce). We will use the methods developed in Objective 1 to analyze for OMCs in the irrigation water, harvested plants (roots, stems, fruit, and leaves), and irrigated soil. We will compare which OMCs are detected in water, soil, and the different plant species via suspect screening, and use NTA to compare the full analyte profile of the different types of samples. Many of the compounds that we detect in plants using our NTA and suspect screening methods will not be OMCs; it is likely we will find many chemicals related to plant health such as hormones and metabolites. Therefore, we will also investigate whether irrigation water affects the levels of any of these detected chemicals using a metabolomics type approach. The metabolomics analysis should provide us with some information about recycled water effects on plant health. We will also use more conventional methods for assessing plant health such as germination rate, emergence time, time to flower/fruit production, plant mass, length, and height, major elemental content, chlorophyll content, oxidative stress, and metabolic enzyme activity. We will also conduct heavy metal analysis on water, plants, and soil using ICP-MS.

Progress 10/01/19 to 09/30/20

Outputs
Target Audience:Scientists at the Connecticut Agricultural Experiment Station: Project methods and progress were discused and shared with other CAES scientists. Scientific community: We published a manuscript on non-targeted methods for soil analysis. General public: We worked with high school students at the Sound School in New Haven on science fair projects about water pollution. We maintained contact we community groups and the Micmac Nationin Maine who grow hemp on contaminated land. We provided them updates on results from our analysis of their samples. Connecticut Government: Dr. Nason participated in Governor Lamont's PFAS Task Force with members of 17 other state agencies. Changes/Problems:The proposed project has expanded and split into two related projects with goals that are related to the original objectives. All work is still focuses on the general topics of organic microcontaminants in water, soil, and plants, and method development for non-targeted analysis. Per- and polyfluoroalkyl substances (PFAS) are an emerging class of organic microcontaminants that have received much attention in the press and from local governments. As concern over PFAS in the environment has expanded, our work has moved towards focusing on PFAS. We are working on method development for PFAS-specific non-targeted analysis methods in water, soil, and other matrices, and had one publication on this topic duringthisreportingperiod. We are also working with community collaborators in Maine on a project about plant uptake and phytoremediation of PFAS at the former Loring Air Force base - a site with PFAS soil contamination caused by former use of fire fighting foams. We are measuring PFAS in soil and plants from their site, and will publish a manuscript on the soil samples next year. The COVID-19 pandemic has caused increased interest in wastewater and sludge analysis, as levels of the SARS-CoV2 virus in wastewater can be used to track community spread of COVID-19. We are collaborating with the Peccia lab at Yale University to analyze primary sludge samples for both organic microcontaminants and the SARS-CoV2 virus. Our role is focused onorganic microcontaminants such as pharmaceuticals, illicit drug, and personal care products. Levels of these chemicals in sludge samples can reveal trends in usage for the population that the treatment plant serves, which can show important public health trends (for example - increasing fentanyl concentrations in sludge indicate higher levels of community use). This project shares many method development goals with the originally proposed work, including database development and evaluation of methods for measuring organic microcontaminants in wastewater. We anticipate at least on publication in the next reporting period as well as presentations to scientific audiences. We believe that these new projects will lead to results and outputs that are more valuable for the general public at this time. These changes have been discussed with Jason White, Director of the Connecticut Agricultural Experiment Station. What opportunities for training and professional development has the project provided?An undergraduate student from the University of New Haven served as an intern on this project from 9/2019-1/2020 and was trained in general labwork procedures and PFAS sample preparation. How have the results been disseminated to communities of interest?We published a bookchapter titledImportance of Soil Properties and Processes on Bioavailability of Organic Compounds that shares our knowledge with the scientific community. We also published a manuscript:Toward Comprehensive Per-and Polyfluoroalkyl Substances Annotation Using FluoroMatch Software and Intelligent High-Resolution Tandem Mass Spectrometry Acquisition that shares some of our method development progress with thescientific community. We coached high school science fair projects at the Sound School in New Haven on water pollution topics related to our research. We collaborated with the Micmac Nation (an indigenous people) and Upland Grassroots (a community science group) in Maine on a project about soil contamination and plant uptake of contaminants and regularly updated them on project progress and results. What do you plan to do during the next reporting period to accomplish the goals?We will publish an additional manuscripton FluoroMatch that usesthe data from our collaboratory project in Maine, as well as a manuscript onour analysis of wastewater and sludge from the first wave of the COVID-19 pandemic We will beging analyzing wastewater samples more regularly and expand our relationship with the New Haven Water Pollution authority, and move towards work that focuses more on irrigation water. We will coninue our work with our community colalborators in Maine and share our results with them using materials generated specifically for sharing outside the scientific community. We will continue to work with students from local universities and provide learning opportunities related to this project. We will continue to work on science fair projects with high school students at the Sound School.

Impacts
What was accomplished under these goals? Our work focuses on organic microcontaminants - chemicals that are normally found in pharmaceuticals, cosmetics, and other household products but make their way into the environment. These contaminants are common in wastewater, as most are excreted and/or dumped down the drain after use. We are working on developing methods to identify and measure organic microcontaminants in wastewater and in the environment in matrices such as soil and plant tissue. Though these contaminants are present at very low levels, they may cause toxic effects if humans and other organisms are repeatedly exposed. Understanding contaminant presence and movement in the environment is important for ensuring safety of food and drinking water as well as protecting nature. Specifically, we work on suspect screening and non-targeted methods, which are designed to detect as many contaminants as possible in a single analysis. Objective 1: Develop and evaluate suspect screening and non-targeted analysis methods for crop plants, soils, and recycled water. Work on this objective has progressed in two directions. Part of our work focused heavily on per- and polyfluoroalkyl substances (PFAS) - a group of over 7,000 organic microcontaminants that are just beginning to be recognized as toxic. This year, we contributed to a scientific paper that introduces FluoroMatch a new software to use for detecting PFAS in environmental samples that have been analyzed using liquid chromatography coupled with high resolution tandem mass spectrometry (LC-HRMS). FluoroMatch uses non-targetedmethods to detect as many PFAS as possible in samples and does so more easily and quickly than previous software methods. We have also completed significant method development for detecting a broader range of contaminants via non-targeted analysis. We compiled a chemical database based on all of the previous LC-HRMS work at the Connecticut Agricultural Experiment Station and used it in preliminary analysis of wastewater sludge samples. The database is now functional, and we will be able to use it to identify organic microcontaminants in future samples that we analyze. Objective 2: Investigate organic microcontaminant and heavy metal accumulation by crop plants irrigated with recycled water and relate the results to effects on plant health. We have investigated plant accumulation of PFAS in collaboration with the Micmac Nation (and indigenous people) and Upland Grassroots (a community organization) in northern Maine. They are growing hemp on the contaminated land at the former Loring Airforce base as an investigation of the efficacy of hemp phytoremediation for PFAS. We found that four PFAS had significantly lower concentrations after the initial growing season. Hemp was planted at the site for a second growing season in 2020. We have also analyzed soil samples from the Loring site and used them to test the new FluoroMatch software described above. These results will be published next year and have been shared with our collaborators. Our work on wastewater has turned to a different focus. The chemical signature of wastewater can reveal a lot about the population of the area that a treatment plant serves. Wastewater analysis has become more popular during the COVID-19 pandemic, as RNA fragments present in wastewater and sludge can be used to trace clusters and outbreaks of the virus. We began working with the Peccia lab at Yale University on analysis of wastewater primary sludge samples collected during the first wave of the COVID-19 pandemic. The Peccia lab has focused on viral analysis, while we are using the database described above and other methods to screen for organic microcontaminants in the sludge. Preliminary results show trends over time fordisinfectant, opioid and antidepressant concentrations that are likely related to changes in use caused by the pandemic. This work is ongoing and will be published and presented to the scientific community and the public next year. Population level trends in chemical use can be difficult to measure - especially during a pandemic - and our analysis will help to reveal patterns that were affected by the pandemic and shutdown. After the pandemic, we plan to refocus our work on contaminants in irrigation water.

Publications

  • Type: Journal Articles Status: Published Year Published: 2020 Citation: Koelmel, J. P.; Paige, M.; Aristizabal-Henao, J. J.; Robey, N. M.; Nason, S. L.; Stelben, P.; Li, Y.; Kroeger, N. M.; Napolitano, M. P.; Savvaides, T.; Vasiliou, V.; Rostkowski, P.; Garrett, T.; Lin, E.; Diegl, C.; Jobst, K.; Townsend, T. G.; Pollitt, K. J. G.; Bowden, J. A. Towards Comprehensive PFAS Annotation Using FluoroMatch Software and Intelligent LC-HRMS/MS Acquisition Methods. Analytical Chemistry 2020, 92 (16), 1118611194.
  • Type: Book Chapters Status: Published Year Published: 2020 Citation: Pignatello J.J., Nason S.L. (2020) Importance of Soil Properties and Processes on Bioavailability of Organic Compounds. In: Ortega-Calvo J.J., Parsons J.R. (eds) Bioavailability of Organic Chemicals in Soil and Sediment. The Handbook of Environmental Chemistry, vol 100. Springer, Cham. https://doi.org/10.1007/698_2020_510


Progress 05/29/19 to 09/30/19

Outputs
Target Audience:Scientists at the Connecticut Agricultural Experiment Station: Project methods and progress were discused with other CAES scientists during initial data collection. General public: We built a relationship with the Greater New Haven Water Pollution ControlAuthority and communicatedthe goals of our research, and also made plans for collecting water samples. Changes/Problems: Nothing Reported What opportunities for training and professional development has the project provided? Nothing Reported How have the results been disseminated to communities of interest? Nothing Reported What do you plan to do during the next reporting period to accomplish the goals?We will continue our methhod development process, and conduct a full method validation experiment. We will begin work in the greenhouse and start to grow plants irrigate with recycled water.

Impacts
What was accomplished under these goals? We have begun method development for analyizing organic microcontaminants in recycled water, plants, and soil. We have preliminary data on contaminants found in wastewater from New Haven.

Publications