Development and Application of Suspect and Nontarget Screening to Characterize Organic Micropollutants in Aquatic Environments of New York State

Organic micropollutants (OMPs) have presented a global challenge to water resources management due to concerns over their adverse impacts on aquatic biota and human health at low exposure concentrations (e.g., at ng/L to μg/L levels in aquatic systems). OMPs encompass an extensive array of synthetic organic compounds (e.g., pharmaceuticals, pesticides, personal care products, household chemicals, industrial additives) and their transformation products. My research has been centered around establishing analytical methods based on liquid chromatography-high-resolution mass spectrometry (LC-HRMS), with a focus on the development and application of suspect and nontarget screening workflows for the identification and prioritization of OMPs in inland lakes, streams, and urban wastewater in New York State. In Chapter 1, I collaborated with volunteers from the Citizens Statewide Lake Assessment Program and scientists at the Upstate Freshwater Institute to conduct the first statewide investigation of OMP occurrence in New York inland lakes. Through this project, I developed a suspect screening method based on LC-HRMS to identify and quantify 65 OMPs in 314 lake water samples collected by volunteers from 111 lakes, ponds, and reservoirs across the state. I also performed partial least squares regression and multiple linear regression analyses to prioritize total dissolved nitrogen, specific conductance, and a wastewater-derived fluorescent organic matter component as the best combination of explanatory predictors for the inter-lake variability in OMP occurrence patterns. I further applied the exposure-activity ratio approach to estimate the potential for biological effects associated with OMPs. My work demonstrated that engaging an established network of citizen volunteers offers a viable approach to increasing the spatiotemporal coverage of OMP monitoring while raising public awareness of their prevalence. In Chapter 2, I collaborated with Drs. Christa Kelleher and Rebecca Schewe to investigate the occurrence patterns of OMPs in streams draining mixed-use watersheds in central New York. I combined the use of polar organic chemical integrative samplers (POCIS) with suspect screening and nontarget screening based on LC-HRMS to identify and quantify 133 OMPs in samples collected from 20 stream sites over two sampling seasons. I also performed hierarchical clustering to establish the co-occurrence profiles of OMPs in connection with watershed attributes indicative of anthropogenic influences. I further evaluated the feasibility of deploying POCIS for estimating daily average loads of OMPs and their potential for biological effects in streams via screening-level risk assessments. My work supported the prospect of combining passive sampling with high-resolution accurate mass screening for the multi-watershed characterization of OMP contamination status in streams. In Chapter 3, I collaborated with colleagues from the School of Public Health to pursue one of the earliest wastewater-based epidemiology studies on population-level substance use during the COVID-19 pandemic. I developed and validated an online solid-phase extraction method for sample preconcentration before LC-HRMS analyses to achieve rapid screening of health and lifestyle-related substances in urban wastewater. I applied this method to quantify the levels of 26 pharmaceuticals and lifestyle chemicals in wastewater influent samples collected from six sewersheds in central New York over a period spanning the rising and falling of COVID-19 prevalence. I back-calculated the population-level consumption rates of antidepressants, antiepileptics, antihistamines, antihypertensives, and central nervous system stimulants and further identified their co-variation with disparities in household income, marital status, and/or age of the contributing populations as well as the detection frequency of SARS-CoV-2 RNA in wastewater and the COVID-19 test positivity within the sewersheds. My work highlighted the utility of high-throughput wastewater analysis for assessing substance use patterns during a public health crisis such as COVID-19

Occurrence and Mass Flows of Organic Micropollutants in the Onondaga Lake – Three Rivers System

Organic micropollutants (OMPs) are synthetic and naturally occurring organic compounds that may pose long-term ecotoxicological risks to the aquatic life occur at low levels. This work seeks to characterize the spatiotemporal occurrence and mass flows of OMPs in the Onondaga Lake-Three Rivers system in central New York. In collaboration with the Upstate Freshwater Institute, multiple batches of water samples were collected from the lake-river system between June and October 2017 and analyzed for OMPs using a suspect screening workflow developed on liquid chromatography-high resolution mass spectrometry. To date, a total of 52, 31, and 37 OMPs were identified and quantified in Onondaga Lake, its four major tributaries, and the Three Rivers, respectively. Lamotrigine, estradiol, benzotriazole, methyl benzotriazole, sucralose, and atrazine were measured in every sample, suggesting their ubiquitous presence in the lake-river system. Over the study period, the horizontal concentration profiles of OMPs in Onondaga Lake showed relatively consistent patterns, but the vertical distribution of OMPs in the lake was influenced by thermal stratification and wastewater discharge from a regional WWTP serving the Syracuse metropolitan area. Specifically, OMPs derived from point source wastewater discharge exhibited peak concentrations in the thermocline in July 2017, but such phenomenon disappeared in October 2017, likely due to changes in lake stratification. OMPs were generally detected at lower levels in the lake tributaries and the Three Rivers, suggesting diffuse inputs from agricultural activities or irregular wastewater discharge. Further calculations of the OMP mass flow revealed that the WWTP might account for up to 67-86% of the OMP mass flow entering the lake, which is in line with its high percentage of wastewater inflow. Onondaga Lake itself contributed 12-24% of the OMP mass flow entering the Three Rivers, confirming its role as a regionally important source of OMPs

CDSD: Chinese Dysarthria Speech Database

We present the Chinese Dysarthria Speech Database (CDSD) as a valuable resource for dysarthria research. This database comprises speech data from 24 participants with dysarthria. Among these participants, one recorded an additional 10 hours of speech data, while each recorded one hour, resulting in 34 hours of speech material. To accommodate participants with varying cognitive levels, our text pool primarily consists of content from the AISHELL-1 dataset and speeches by primary and secondary school students. When participants read these texts, they must use a mobile device or the ZOOM F8n multi-track field recorder to record their speeches. In this paper, we elucidate the data collection and annotation processes and present an approach for establishing a baseline for dysarthric speech recognition. Furthermore, we conducted a speaker-dependent dysarthric speech recognition experiment using an additional 10 hours of speech data from one of our participants. Our research findings indicate that, through extensive data-driven model training, fine-tuning limited quantities of specific individual data yields commendable results in speaker-dependent dysarthric speech recognition. However, we observe significant variations in recognition results among different dysarthric speakers. These insights provide valuable reference points for speaker-dependent dysarthric speech recognition.Comment: 9 pages, 3 figure

Research on en route capacity evaluation model based on aircraft trajectory data

For the sake of refined assessment of airspace operation status, improvement of the en route air traffic management performance, and alleviation of the imbalance of demand-capacity and airspace congestion, an en route accessible capacity evaluation model (based on aircraft trajectory data) is proposed in this paper. Firstly, from the perspective of flux, the en route capacity is defined and expanded from a two-dimensional concept to a three-dimensional concept. Secondly, based on the indicators of spatial flow and instantaneous density, an evaluation model of en route capacity is given. Finally, a case study is performed to validate the applicability and feasibility of the model. Results show that the en route accessible capacity, instantaneous density, and spatial flow can describe the temporal and spatial distribution of air traffic flow more precisely, as compared to the conventional indicators, such as route capacity, density, and flow. The proposed model envisages three innovations: (ⅰ) the definition of airspace accessible capacity with reference to capacity of road traffic, (ⅱ) the computation model for flux-based airspace accessible capacity and en route accessible capacity, and (ⅲ) two indicators of en route characteristics named instantaneous density and spatial flow are introduced for evaluating the micro-state of the en route. Furthermore, because of the capacity depiction of the spatial and temporal distribution of air traffic congestion within an airspace unit, this model can also help air traffic controllers balance the distribution of traffic flow density, reduce the utilization rate of horizontal airspace, and resolve flight conflicts on air routes in advance

Genome Assembly and Annotation of a High-Polymalic Acid (PMLA) Producing Strain Aureobasidium melanogenum CGMCC18996 and Analysis of Its Key Proteins Related to PMLA Synthesis

In this study, we applied PacBio Sequel II and Illumina NovaSeq 6000 sequencing platforms to sequence the genome of a high-polymalic acid (PMLA)-producing strain, Aureobasidium melanogenum CGMCC18996, and used different assemblers to obtain a high-quality genome assembly, which was then annotated using transcriptomic data. The results indicated a total of 6 202 genes were found in the A. melanogenum genome, mainly involved in carbohydrate transport and metabolism, amino acid transport and metabolism, post-translational modification, RNA processing and modification. Meanwhile, functional annotation revealed that most genes in the genome were related to peroxisome in the strain. Transmission electron microscopy (TEM) indicated the existence of a circular peroxisome-like (glyoxysome) structure in the cells, demonstrating the ability to malic acid through the glyoxylate cycle. Finally, we predicted the protein structures of two enzymes related to PMLA biosynthesis, phosphoenolpyruvate carboxykinase (PCKA) and malate synthase (MASY). It was found that the enzymes could have the ability to synthesize malic acid. This study could provide a reference for metabolism regulation in A. melanogenum for improved PMLA production, and the assembled genome has been uploaded to the database, which could provide the basis for the future development and utilization of A. melanogenum CGMCC18996

Co-immobilization multienzyme nanoreactor with co-factor regeneration for conversion of CO2

Multienzymatic conversion of carbon dioxide (CO2) into chemicals has been extensively studied. However, regeneration and reuse of co-factor are still the main problems for the efficient conversion of CO2. In this study, a nanoscale multienzyme reactor was constructed by encapsulating simultaneously carbonic anhydrase (CA), formate dehydrogenase (FateDH), co-factor (NADH), and glutamate dehydrogenases (GDH) into ZIF-8. In the multienzyme reactors, cationic polyelectrolyte (polyethyleneimine, PEI) was doped in the ZIF-8 by dissolving it in the precursors of ZIF-8. Co-factor (NADH) was anchored in ZIF-8 by ion exchange between PEI (positive charge) and co-factor (negative charge), and regenerated through GDH embedded in the ZIF-8, thus keeping high activity of FateDH. Activity recovery of FateDH in the multienzyme reactors reached 50%. Furthermore, the dissolution of CO2 in the reaction solution was increased significantly by the combination of CA and ZIF-8. As a result, the nanoscale multienzyme reactor exhibited superior capacity for conversion of CO2 to formate. Compared with free multienzyme system, formate yield was increased 4.6-fold by using the nanoscale multienzyme reactor. Furthermore, the nanoscale multienzyme reactor still retained 50% of its original productivity after 8 cycles, indicating excellent reusability

Rapid detection of porcine circovirus type 2 using a TaqMan-based real-time PCR

Porcine circovirus type 2 (PCV2) and the associated disease postweaning multisystemic wasting syndrome (PMWS) have caused heavy losses in global agriculture in recent decades. Rapid detection of PCV2 is very important for the effective prophylaxis and treatment of PMWS. To establish a sensitive, specific assay for the detection and quantitation of PCV2, we designed and synthesized specific primers and a probe in the open reading frame 2. The assay had a wide dynamic range with excellent linearity and reliable reproducibility, and detected between 102 and 1010 copies of the genomic DNA per reaction. The coefficient of variation for Ct values varied from 0.59% to 1.05% in the same assay and from 1.9% to 4.2% in 10 different assays. The assay did not cross-react with porcine circovirus type 1, porcine reproductive and respiratory, porcine epidemic diarrhea, transmissible gastroenteritis of pigs and rotavirus. The limits of detection and quantitation were 10 and 100 copies, respectively. Using the established real-time PCR system, 39 of the 40 samples we tested were detected as positive

Bimetal based inorganic-carbonic anhydrase hybrid hydrogel membrane for CO2 capture

In this study, we synthesized for the first time a bimetal-based inorganic-carbonic anhydrase (CA) hybrid nanoflower to immobilize CA using Cu2+ and Zn2+ instead of single metal ion. Subsequently, the synthesized bimetallic hybrid nanoflowers (CANF) were embedded into the poly(vinyl alcohol) (PVA)-chitosan (CS) hydrogel networks to obtain PVA/CS@CANF hydrogel membrane. The CANF exhibited a significantly higher activity recovery of 70 % compared with 35 % with CA/Zn3(PO4)2 hybrid nanoflowers and 10 % with CA/Cu3(PO4)2 hybrid nanoflowers. The PVA/CS@CANF hydrogel membrane possessed excellent mechanical strength, high catalytic activity, and were easy to flow out without centrifugation or filtration. At the same time, the PVA/CS@CANF displayed higher thermostability, storage stability, and pH stability than free CA and CANF, and superior reusability and CO2 capture capacity. The hydrogel membrane maintained more than 75 % of its original activity after 8 cycles. However, CANF only maintained 12 % of its original activity. Furthermore, the amount of CaCO3 produced by PVA/CS@CANF membrane was 9.0-fold and 2.0-fold compared with free CA and CANF, respectively. Therefore, This approach to synthesizing bimetallic-based protein hybrid hydrogel membrane could have a bright future in CO2 capture

Spatio-Temporal Pattern in the Changes in Availability and Sustainability of Water Resources in Afghanistan

Water is gradually becoming scarce in Afghanistan like in many other regions of the globe. The objective of this study was to evaluate the spatial changes in the availability and sustainability of water resources in Afghanistan. The Terrestrial Water Storage (TWS) data of the Gravity Recovery and Climate Experiment (GRACE) satellite obtained from three different institutes, having 1° × 1° spatial resolution for the period 2002–2016 was used for this purpose. Sen’s slope method was used to assess the rate of change, and the Modified Mann–Kendall test was used for the evaluation of the significance of trends in TWS. After, the concept of reliability–resiliency–vulnerability (RRV) was used for assessing the spatial distribution of sustainability in water resources. The results revealed a significant decrease in water availability in the country over the last 15 years. The decrease was found to be highest in the central region where most of the population of the country resides. The reliability in water resources was found high in the northeast Himalayan region and low in the southwest desert; resilience was found low in the central region, while the vulnerability was found high in the south and the southeast. Overall, the water resources of the country were found most sustainable in the northeast and southwest and least in the south and the central parts. The maps of water resource sustainability and the changes in water availability produced in the present study can be used for long-term planning of water resources for adaptation to global changes. Besides, those can be used for the management of water resources in a sustainable and judicious manner