Source: UNIV OF WISCONSIN submitted to
PARTNERSHIP: SUSTAINABLE BIOPLASTIC PRODUCTION BY IMPROVED BIOSYNTHESIS AND CONTROLLED HYDROLYSIS OF DAIRY INDUSTRY AND PAPER MILL WASTE MIX
Sponsoring Institution
National Institute of Food and Agriculture
Project Status
ACTIVE
Funding Source
Reporting Frequency
Annual
Accession No.
1028654
Grant No.
2022-67021-37605
Cumulative Award Amt.
$747,793.00
Proposal No.
2021-10481
Multistate No.
(N/A)
Project Start Date
May 1, 2022
Project End Date
Apr 30, 2026
Grant Year
2022
Program Code
[A1531]- Biorefining and Biomanufacturing
Project Director
Majumder, E.
Recipient Organization
UNIV OF WISCONSIN
21 N PARK ST STE 6401
MADISON,WI 53715-1218
Performing Department
Bacteriology
Non Technical Summary
Biobased and easily biodegradable bioplastics, such as polyhydroxyalkanoates (PHAs), are alternatives to petroleum-based plastics which are difficult to degrade in the environment. and are rapidly gaining plastic market share. PHAs hold promise for a sustainable future owing to their biological origin, biodegradability, biocompatibility, and tunable properties. PHAs biodegrade entirely into carbon dioxide and water, and the degradation rate is faster compared to other bioplastics. Despite the environmental benefits and significant interest, the commercial success of PHAs is limited, mainly due to the high production cost and scalable supply of carbon sources. Currently, most of the PHAs are produced using carbon sources derived from food-based feedstocks, which contribute significantly to the production cost (> 50%) and also compete with food production. Agro-food and forest-product industries generate several million tons of various wastes and low-value co-product streams during their operations. Traditionally, most of the solid waste streams are disposed of at landfills and liquid waste streams are directed to wastewater treatment plants. Disposal of these waste is costly to food industries, and at the same time causes potential environmental problems, with direct and indirect emissions of greenhouse gasses, and contamination of groundwater. Agro-food processing industries are increasingly looking toward diversifying their product stream through the valorization of waste materials and achieving zero waste.Our goal is to establish an economically and environmentally sustainable bioprocess that converts agriculture and forest product low-value and underutilized waste streams into polymers for the production of more elastic and biodegradable biobased bioplastics. This project would use an innovative approach by developing a mixing strategy for waste streams from the dairy industry (acid whey and whey permeate phospholipid concentrate) and paper mills (waste fines) to produce a polymer with desired properties for improved bioplastics. Acid whey is a byproduct of the production of cream cheese and Greek yogurt. Currently, more than 4 million tons of acid whey are produced in the United States. The acid whey waste is hard to dispose of and thus poses serious problems for the dairy industry and the environment. Waste fines are fragments of fibers that are produced during the processing of recycled pulps into linerboard and similar paper products. A large amount of these fibers is rejected as a solid waste stream to avoid these challenges in the paper production process. Acid whey and waste fines burden dairy and paper industries economically and environmentally but contain desirable substrates for microbial growth during the bio-production of bioplastics. Besides increasing bioplastic feedstock availability and decreasing cost, mixing these waste streams and use as co-substrates addresses individual bioconversion challenges through less neutralization chemicals, better carbon utilization efficiency, and pretreatment elimination, all while improving economic and environmental sustainability of the process. We will optimize the bioprocess by converting the mixture of acid whey and waste fines to maximize a common PHA, polyhydroxybutyrate, yield by controlling hydrolysis conditions. While there are many uses for poluhydroxybutyrate, it is brittle and not suitable for all applications. To make a more flexible bioplastic, we will incorporate lipids from underutilized dairy industry co-product Whey Permeate Phospholipid Concentrate into the bioplastic polymer by metabolically engineering our production microbe. Process simulations, techno-economic analysis, and life cycle assessments will determine economic and commercial feasibility and the potential impact of the PHA production on the environment. Accomplishing this goal will enable future work in scaling the bioplastic production process towards industrial levels and testing other unexplored agricultural wastes as innovative bioproduct substrates.
Animal Health Component
25%
Research Effort Categories
Basic
50%
Applied
25%
Developmental
25%
Classification

Knowledge Area (KA)Subject of Investigation (SOI)Field of Science (FOS)Percent
1330660202025%
4033470202025%
5114099104025%
5116199301025%
Goals / Objectives
Development of technologies to valorize agricultural and forest industrial waste streams through conversion to high value bioplastics can provide green and sustainable alternative to petroleum-based plastics and improve profitability to agricultural product and bioplastic producers. Our long-term goal aims to design a sustainable bioprocessing system utilizing agro-processing waste streams as feedstock for production of bio-based and biodegradable plastic precursors. This project is based on extensive preliminary data on the bioconversion of acid whey (AW), a major liquid waste (5-7% solids) from the dairy industry, and waste fines (WF), a solid waste from the recycled paper mills, into bioplastics which enables us to focus on engineering solutions to specific limitations we identified in the system. Our process is hindered by ratio of substrates and nutrients and in the type of biopolymer being produced. In Objective 1, we will optimize i) the mixing of AW and WF, and ii) the performance of a controlled hydrolysis combined with the fermentation to produce high yields of bioplastic poly(3-hydroxybutyrate) (PHB). In Objective 2, we will employ metabolic engineering methods to biosynthesize a novel bioplastic co-polymer by incorporating underutilized Whey Permeate Phospholipid Concentrate (WPPC), which supplies the necessary fatty acids into the process. In Objective 3, we will evaluate the commercial scale economic feasibility and environmental impact of the process through techno-economic assessment (TEA) and life cycle analysis (LCA) approaches. Besides increasing the feedstock availability for bioplastic production, this innovative approach of utilizing AW and WF as co-substrates for bioplastic production addresses several challenges associated with bioconversion of these individual streams, maximizes carbon utilization efficiency, and improves economic and environmental sustainability of the process. Altogether, the results of these efforts will give a lab scale demonstration of this sustainable bioprocess for generating two types of bioplastics from negative-cost wastes and have prepared the system to be ready for future testing at pilot scale. This approach also addresses concerns of environmental and human health, waste disposal, and the need to diversify products and markets for the forest product and dairy industries.
Project Methods
The methods in this project span bioprocess engineering, microbiology metabolic engineering and economic assessment of the process. Efforts and their respective Evaluations are herein described chronologically.Objective 1: Optimization of fermentation for maximizing PHB production from acid whey and waste fines mixThe first part of this objective involves optimizing the media composition during fermentation by investigating several important experimental factors, including the total carbon, carbon/nitrogen (C/N) ratio, and sugar/lactate ratio. The effect of parameters will be evaluated on the PHB yield, and the parameters will optimized. Initial experiments will be performed using pure sugars (glucose and lactose) and lactic acid. The nitrogen content will be controlled by adding bovine serum albumin (BSA). The fermentation will be performed for 48 h using recombinant E. coli. The microbial biomass (containing PHB) will be harvested at the end of fermentation and the cell yield will be determined using gravimetric methods. The PHB content of the cell biomass will be measured using GC-FID (gas chromatograph equipped with a flame ionization detector) using standard protocols. The second part of this objective focuses on producing desired media through controlled hydrolysis of acid whey (AW) and waste fines (FW) mix. The ratio of sugars to lactate in the solution will be controlled by adjusting the mixture of acid whey and waste fines at the start of hydrolysis. Various enzyme dosages will also be investigated to evaluate their impact on the carbohydrate conversion during hydrolysis. The next part involves PHB production using this hydrolysate. The media composition will be adjusted to achieve similar PHB yields as that with the fermentation of pure sugars and lactic acid. In the last part, the scale-up hydrolysis and fermentation experiments (6-L working volume) will be performed under the optimum conditions, and the results will be used to perform techno-economic analysis and further used for the life cycle analysis (Objective 3).Objective 2: Metabolic engineering of PHA co-polymer production with the addition of WPPCTo produce a co-polymer with more elastic properties than PHB from our mixed waste stream, we will add WPPC as a source of long-chain fatty acids in test flasks with our targeted bioplastic-producing microbes. We will perform growth and co-polymer production batch trials by inoculating the five targeted microbes into flasks containing at least three different WPPC to AW-PH ratios (0:100, 50:50, 100:0) held at 10 g/L sugar content, which promoted higher PHB yields in our preliminary data. After the cultures reach the stationary phase, the cells will be harvested, and biopolymers extracted and analyzed as described in Objective 1. To determine if a true co-polymer with desired properties has been biosynthesized compared to simultaneous homopolymer strands, we will perform chromatographic separation and collect fractions before identification by GCMS and NMR and other polymer analytical methods such as Elongation at Break. For our metabolic engineering strategy of our top PHA co-polymer-producing microbe, we will first determine which reaction in the biosynthesis pathway is the most limiting with our established PHA biosynthesis qPCR assay. Upregulation of gene expression during PHA co-polymer biosynthesis compared to non-polymer producing conditions will indicate which genes are involved in generating this co-polymer. We will generate a Flux balance Analysis Model (FBA) in KBase to predict which reactions are limiting. We will manually add any PHA biosynthesis genes or modifications. In the FBA model, we will run simulations varying substrates and nutrient loading, specifically carbon and nitrogen. Biosynthesis bottleneck reactions are identified by a lack of final PHA product and accumulation of initial substrate or intermediates. We then examine the responsible transporter or enzyme for that reaction. Based on the enzyme parameters listed in the BRENDA database, we can predict what is causing the inhibition or decreased turnover of limiting enzyme in specific AW-WF-WPPC process condition. We will then verify this limitation prediction by growing the microbe in that condition and perform our established enzyme activity or uptake assays. The magnitude of the polymer yield and change in enzyme activity should match the FBA model prediction. This will pinpoint which reaction and which protein contributes the most to the limitation of PHA co-polymer biosynthesis.Objective 3: Techno-economic analysis and life cycle assessment of the proposed processComprehensive process models will be developed for the complete process including hydrolysis, fermentation, PHB recovery, and other downstream operations, using SuperPro Designer (Intelligen, Inc., NJ, USA). The experimental results from objectives 1 and 2 will be used as inputs for the model simulations. The outcomes from the model simulations will include PHB and co-polymer yields, total capital investment, total operational cost and its breakdown, total energy consumption, and bioplastic production cost. The profitability will be estimated assuming a selling price of bioplastics, and results will be compared with alternate technologies. A sensitivity analysis will be performed by varying the purchase price of feedstocks to evaluate the potential gain to the agro-processing industries. A cradle-to-gate life cycle assessment model will be developed to quantify the environmental impact of the process. This assessment will follow the framework defined by the International Standardization Organization that includes goal and scope definition, inventory analysis, impact assessment, and results interpretation. The mass and energy balance data generated from process simulations and the existing life cycle inventory database (e.g., USLCI, Ecoinvent) will be used to conduct the analysis. The LCA results will be interpreted in relation to the double environmental benefits of biobased PHB: 1) utilization of a negative wastes stream that would otherwise create an environmental problem, and 2) substitution of fossil-based materials.

Progress 05/01/23 to 04/30/24

Outputs
Target Audience:This past year, we have communicated with several target audiences per our project plan. This research has been discussed multiple times in formal classroom instruction such as BPE 300: Introduction to Industrial Bioprocessing at SUNY ESF and Micro526: Physiology of Microorganisms at UW-Madison. Faculty, graduate students and undergraduate students have presented their findings at local, regional and national conferences, this includes engineering and microbiology events as well as dairy industry events. Likewise, we have had discussions with stakeholders in the dairy, paper and bioplastic industries. The review paper in the products section was tangential to our work on this grant as it emphasizes lignin, which is why NIFA was not acknowledged, but we included it in this progress report because it highlights our overall philosophy in utilizing agricultural wastes as sustainable and low-cost feedstocks for bioproduction of valuable molecules and polymers. Changes/Problems: Nothing Reported What opportunities for training and professional development has the project provided?This project during this year has provided multiple opportunities for training and professional development.Training included graduate students being trained in many new skills including new to us uses of Gas Chromatography, better recombineering technology for strain development, culturing microbial communities for PHA production, bioreactor experiments and waste mixing. Rachel Rovinsky and PI Erica Majumder also attended a 4-day workshop on decolonizing microbiology. Additional professional development was met by students attending conferences and presenting posters such as ASABE and SIMB. The first PhD student graduating with work on this project will defend her thesis in early July 2024. How have the results been disseminated to communities of interest?To present our current findings to the scientific community, we presented at several relevant conferences during this reporting period. That included the USDA project director's meeting in Kansas City during summer 2023. Dr. Majumder presented at SBFC. A graduate and undergraduate student each presented at SIMB. Dr. Kumar and two graduate students presented at ASABE. We participated in a review paper on the bioconversion of lignin. We have also been in contact with different suppliers in both New York state and Wisconsin. In New York, our local dairy company Byrne Dairy made some production line changes, so we had to contact Chobani and explain our project to get acid whey. Dr. Kumar also met with Westrock, a paper mill from where we get fiber rejects. He also has a meeting with a start-up (Capro-X) working on dairy waste later in April at the end of this reporting period. In Wisconsin, Dr. Majumder has continued to work with the Center for Dairy Research to acquire WPPC and acid whey from various producers in the state. She also presented at the CDR's annual research forum and the World Cheese Expo about this project. More and more producers are getting excited about the dairy industry being a part of the bioeconomy and valorizing their waste streams. Dr. Majumder has also been meeting with bioplastic startup company OuroBio. What do you plan to do during the next reporting period to accomplish the goals?We anticipate the next reporting period will be very fruitful in terms of publishable data and subsequent publications. The first graduate student trained on the project is defending her thesis in July. All the method development and preliminary experiments are now primed to begin full experiments. Improvements to the microbial chassis will continue. Microbial communities are being tested for co-polymer production with WPPC. Scaling and fermentation conditions will be tested on the Acid Whey-waste fines hydrolysate mixture. TEA will be started.

Impacts
What was accomplished under these goals? The major issue that our project targets is the use of pure sugar feedstocks in the production of biobased and biodegradable plastics. Pure sugar feedstocks are the largest portion of the cost of bioplastics, which are too expensive to compete with petroleum-based plastics, and also compete with food production. Our project works to utilize and valorize current negative cost residues and waste streams from the dairy and paper industries as feedstock for bioplastic production, the groups that will most immediately benefit from our work. The outcomes of our project will help dairy processors and paper manufacturers turn a negative cost residue into a revenue-generating co-product. This will also help bioplastic companies to use these streams and reduce cost of bioplastics, ultimately helping all Americans to decrease the amount of petroleum-based plastics consumed by replacing them with biobased and biodegradable plastics. For Objective 1, Acid whey was collected from a commercial dairy facility (Chobani), and AW was stored in a freezer until use. Waste fiber rejects were collected from a local paper mill in Syracuse, New York. Fibers were dried (<10 moisture) and stored in a refrigerator at 4 °C until needed for experimentation. The chemical composition of both waste streams was analyzed. Then, Waste fibers were pretreated using an optimized two-step hydrothermal pretreatment (hot water treatment followed by disk refining) and hydrolyzed using commercial cellulase and hemicellulose enzymes yielding a good concentration of fermentable sugars.PHB fermentation experiments are in progress. This includes at least 5 sets of experiments: Pure AW, pure hydrolysate, 3 mix of AW and hydrolysate (1:1 mix, 1:2 mix, 2:1 mix, o mass basis). All fermentation experiments are being performed at 20 g/L sugar concentrations (sugars: glucose, xylose, lactose, galactose). Lactic acid and acetic acid are additional carbon sources, but experiments were performed keeping only the sugar concentrations fixed among all experiments. Flasks are harvested at various time points: 6,12, 18, 24, 30, 36, 48, 72 h to determine pH, OD, sugars and acid concentrations, cell dry weight and PHB inclusion. Preliminary results indicate improved fermentation with the AW-waste fines mixture. For Objective 2, we obtained WPPC from a local company. We determined the fatty acid composition of the WPPC with Gas Chromatography and the microbial community present with 16S rRNA gene community sequencing on a Miseq. We performed initial experiments testing for co-polymer production on a synthetic mixture of AW and waste fines with WPPC supplemented in the growth medium. Preliminary results indicate the presence of co-polymers of PHAs for some of the native producer bacteria and communities tested. We have also continued to improve our engineered E. coli strain for producing bioplastics. After some failures with gene insertion using our previous genome engineering method, we established a new to the Majumder lab method for gene insertion into the chromosome and are testing if the newly generated strains are capable of PHB and PHA production. For Objective 3, we plan to begin work during this reporting period as we have now acquired some of the necessary data to begin populating the TEA and LCA models. Key outcomes are in the validation of the waste mixing approach to neutralize the solution for better hydrolysis and fermentation. Likewise, use of WPPC was confirmed with initial evidence for incorporation into co-polymers, and microbial chassis strain engineering methods have been established.

Publications

  • Type: Journal Articles Status: Accepted Year Published: 2024 Citation: Shilva Shrestha; Shubhasish Goswami; Deepanwita Banerjee; Valentina Garcia; Elizabeth Zhou; Charles N. Olmsted; Erica Majumder; Deepak Kumar; Deepika Awasthi; Aindrila Mukhopadhyay; Steven W. Singer; John M. Gladden; Blake A. Simmons; Hemant Choudhary. Perspective on Lignin Conversion Strategies that Enable Next Generation Biorefineries. Accepted. ChemSusChem.


Progress 05/01/22 to 04/30/23

Outputs
Target Audience:In the first few months of this project, we have begun to communicate with the various target audiences reached by this project. We have attended regional meetings with representatives from stakeholder industries including dairy, paper and plastics. We have reached out to several of these companies to provide samples of the residues and waste streams. We have presented posters atmicrobiology and bioengineering conferences. We have started training graduate students directly on this project and have presented in undergraduate and graduate seminars. Changes/Problems:There has not been a major change or problem with the work proposed. We did want to make one note on the timeline. The award was backdated to starting 5/1/22 even though we did not receive the award until autumn. So, this progress report only represents a few months of work rather than a full year. What opportunities for training and professional development has the project provided?To date, one new PhD graduate student has been recruited for the microbiology aspect. Rachel Rovinsky started in January of 2023 and is learning about strain engineering. Current graduate students at SUNYESF have been getting training on these waste streams and we plan to recruit 2 more students this fall at ESF for the process engineering and TEA and LCA aspects of the project. Joint group meetings have been established for professional development in interdisciplinary communication. How have the results been disseminated to communities of interest?In the first few months of the project, we have communicated the early findings to several of the audiences outlined in the proposal. Poster presentations were given at several national scientific conferences including American Society for Microbiology in June 2022, ASABE summer 2002 and SIMB SBFC spring 2023. Research presentations have also been given to local stakeholders such as the Center for Dairy Research Fall research forum in 2022 and NY Department of Environmental Conservation meetings.Results from our findings have been described in the courses we teach but also in guest lectures to graduate seminars other departments like Food Science and Materials Engineering. What do you plan to do during the next reporting period to accomplish the goals?For Objective 1, we will begin mixing the waste streams. We are also sourcing raw AW and WF from companies in WI and NY. For Objective 2, we will begin testing our newly engineered strains on the mixed waste and start testing which co-polymers are produced with inclusion of WPPC in with AW and WF. We are making a standard synthetic AW WF mixture to be able to compare across labs. For Objective 3, we are beginning to collect the data needed to start the TEA and LCA calculations. Manuscripts and presentations are in progress. We will also develop and activity for our courses that connects this research and teaching.

Impacts
What was accomplished under these goals? For Objective 1, we have improved the hydrolysis conditions and sugar release from the paper waste fines. Several pretreatment methods were tested, and a method was found that uses lower energy inputs. A paper manuscript is in progress.Mixing of acid whey and waste fines hydrolysates will start soon. For Objective 2, we have done proof of concept experiments that show conversion of WPPC phospholipids into PHA co-polymers. We have finally established a genome insertion method for our base strain and are currently integrating target genes of interest for better carbon conversion and production of unique PHA co-polymers. We contributed to a review paper in this topic area that is under review at Chemical Reviews (ACS) journal. Work on Objective 3 will begin in the next phase once baseline process parameters are established.

Publications