Source: UNIV OF MASSACHUSETTS submitted to NRP
DEVELOPMENT OF ANTIMICROBIAL FOOD PROCESSING SURFACES BY NANOSCALE SURFACE MODIFICATION
Sponsoring Institution
National Institute of Food and Agriculture
Project Status
COMPLETE
Funding Source
Reporting Frequency
Annual
Accession No.
0223785
Grant No.
2011-65210-20059
Cumulative Award Amt.
$488,000.00
Proposal No.
2010-03455
Multistate No.
(N/A)
Project Start Date
Dec 15, 2010
Project End Date
Dec 14, 2015
Grant Year
2011
Program Code
[A1511]- Agriculture Systems and Technology: Nanotechnology for Agricultural and Food Systems
Recipient Organization
UNIV OF MASSACHUSETTS
(N/A)
AMHERST,MA 01003
Performing Department
Food Science
Non Technical Summary
Research in this project will design and characterize self-sanitizing processing surfaces through nanoscale surface modification. By making nanoscale changes to the surface of common materials, we introduce antimicrobial nanostructures, which can repeatedly recharge antimicrobial activity after rinsing in chlorine sanitizing solution. The resulting materials exert antimicrobial activity against a broad range of food pathogens and spoilage organisms. Materials regain antimicrobial activity during sanitization, making them practical for use in food processing environments.
Animal Health Component
60%
Research Effort Categories
Basic
40%
Applied
60%
Developmental
(N/A)
Classification

Knowledge Area (KA)Subject of Investigation (SOI)Field of Science (FOS)Percent
51150102000100%
Knowledge Area
511 - New and Improved Non-Food Products and Processes;

Subject Of Investigation
5010 - Food;

Field Of Science
2000 - Chemistry;
Goals / Objectives
1. Improve our demonstrated nanoscale N-halamine surface functionalization methodology. Our current technology has been shown to regenerate antimicrobial N-halamine structures, but uses a wet chemical process for initial functionalization. We will explore UV irradiation for initial functionalization of polymer and stainless steel substrates. We will also investigate methods to increase the density of N-halamine forming moieties in order to increase antimicrobial activity. Finally, we will adapt our surface functionalization chemistries (successful on polyethylene) to perform on elastomeric (EPDM) and stainless steel substrates. 2. Demonstrate repeated antimicrobial activity of the self-sanitizing food processing surfaces against food borne pathogens. Surfaces that have been functionalized with N-halamine nanostructures will be tested against isolates of E. coli, Vibrio spp., Salmonella spp., and L. monocytogenes to demonstrate the broad spectrum activity against a range of food borne pathogens. We will test antimicrobial activity of surfaces against cells in both planktonic and biofilm state. 3. Establish the practical effectiveness of our rechargeable self-sanitizing food processing surfaces under stresses typical in a food processing environment. We will evaluate the effectiveness of our novel antimicrobial materials after long-term repeated use, after exposure to mechanical stress, and after contact with food components. Experiments will be performed to demonstrate that the covalently-linked N-halamine structures do not migrate from the surfaces during food production. Completing this objective will demonstrate the practical stability and activity of our N-halamine functionalized surfaces.
Project Methods
Use ultraviolet light to functionalize gasket material and stainless steel. Introduce halamine containing moieties onto functionalized gasket and stainless steel substrates using a range of bioconjugation techniques. Alternate deposition of polyacrylic acid and polyethylenimine to increase the number of halamine moieties per unit area. Activate halamines by washing in dilute bleach (sodium hypochlorite). Quantify number of halamines by diethyl-p-phenylenediamine assay. Demonstrate long-term stability and rechargeability of halamine modified materials. Characterize surface morphology and chemistry of control and modified materials using infrared spectroscopy, atomic force microscopy, and scanning electron microscopy. Because of their prevalence in food borne disease, and because they represent both gram positive and gram negative organisms, E. coli, Vibrio spp., Salmonella spp., and L. monocytogenes will be used as challenge organisms in testing antimicrobial activity of the newly developed surfaces. At least two different strains of each organism will be tested, including isolates from a food processing environment and/or a food source when possible. We will obtain such isolates from the American Type Culture Collection (ATCC, Manassus, VA) as well as environmental isolates from the culture collection of Dr. Lynne McLandsborough (co-PI). Viability of microorganisms after contact with control and modified materials will be tested in both planktonic and biofilm form. Materials will be functionalized, wash in industrial sanitizers, and tested for halamine activation. This cycle of antimicrobial activity analysis, cleaning, and sanitization will be repeated up to 100 times. A Taber abrasion apparatus will be used to simulate repeated brushing of the N-halamine functionalized materials, per standardized test methodology ASTM D406079. Coupons of N-halamine modified EPDM or stainless steel will be placed on the abrasion apparatus, and an abrading wheel will be spun on the surface under a defined load. Unmodified materials will be similarly tested as a control. At intervals up to 5000 rotations, the materials will be removed and tested for N-halamine activity using the DPD assay described in Objective 1, as well as antimicrobial activity assays described in Objective 2. Roughness will be quantified at each interval using atomic force microscopy for nanoscale roughness and scanning electron microscopy for mesoscale roughness. As model food components, rolled oats, texturized vegetable protein, and coarsely chopped vegetables will be used. Coupons of N-halamine modified EPDM or stainless steel will be shaken in dry, sterile vials with the test food components for periods up to 6 hours. At 30-60 minute intervals, the materials will be removed and tested for N-halamine activity using the DPD assay described in Objective 1, as well as antimicrobial activity assays described in Objective 2. Unmodified materials will be similarly tested as a control.

Progress 12/15/10 to 12/14/15

Outputs
Target Audience:There are several target audiences who were served by this project in the past year. Graduate and undergraduate students learned experimental design, antimicrobial material chemistry, and food microbiology techniques through laboratory experience and instruction. Graduate students and postdoctoral researchers also gained technical writing experience as well as mentorship experience by mentoring undergraduate researchers who supported this project. The antimicrobial materials scientific community received new science-based knowledge through journal article publications and conference proceedings of results related to this work. The food industry received advances in the understanding of how different approaches to antimicrobial materials development can improve food safety and reduce spoilage in the processing environment. Changes/Problems: Nothing Reported What opportunities for training and professional development has the project provided?Through the course of the project, a total of four graduate students and two undergraduate students were involved in the execution of this project. As part of this project, they learn technical skills in nanotechnology, food microbiology, materials chemistry, and interdisciplinary life science. They are also given opportunities to present their findings at many levels: lab meetings, campus events, and national conferences, as well as in published technical journal articles. The postdoctoral researcher involved in this project was given additional mentorship responsibilities, providing technical guidance to the undergraduate and junior graduate students involved in the project. How have the results been disseminated to communities of interest?Knowledge from this project has been disseminated to scientific communities as well as the general public. Results were presented at the Fall 2015 American Chemical Society Meeting in Boston, MA, the 2015 Institute of Food Technologists' Annual Meeting in Chicago, IL, the 2015 Annual meeting of the International Association of Food Protection in Portland, OR, the 2015 Gordon Conference on Nanotechnology in Food and Agriculture in Waltham, MA, and the 2015 Dairy Ingredients Symposium in Shell Beach, CA. Results were published in four new peer-reviewed publication with one additional submitted publication. Technical consultations pertaining to the newly developed technology have been held with three private companies. What do you plan to do during the next reporting period to accomplish the goals? Nothing Reported

Impacts
What was accomplished under these goals? We have successfully demonstrated the broad spectrum efficacy of the newly developed antimicrobial coatings against both gram positive and negative pathogens of concern to food processing. Coating have been successfully applied to both polymer and steel solid supports, demonstrating their versatility in food processing and handling applications. We have further characterized their stability after extended exposure to alkaline, acid, and oxidizing conditions to support their potential commercial application. Using new synthetic approaches, we have enhanced the antimicrobial efficacy of the materials to both recharge after exposure to bleach as well as carry inherent antimicrobial character. We have further demonstrated that these coatings can exert significant antimicrobial and bacteriostatic character even in the presence of organic matter. By manipulating the coating application process and coating chemistry, we have designed a coating which can self-heal by a mild heat process.

Publications

  • Type: Conference Papers and Presentations Status: Other Year Published: 2015 Citation: Bastarrachea, L, and Goddard, JM. Rechargeable antimicrobial N-halamine coatings for food contact surfaces. Poster in Division of Agricultural and Food Chemistry. August 18, 2015. American Chemical Society Fall Meeting in Boston, MA.
  • Type: Conference Papers and Presentations Status: Other Year Published: 2015 Citation: Bastarrachea, L, McLandsborough, L, and Goddard, JM. Development of Antimicrobial Food Processing Surfaces by Nanoscale Surface Modification. Gordon Research Conference: Nanoscale Science & Engineering for Agriculture and Food Systems. June 2015, Waltham, MA.
  • Type: Journal Articles Status: Submitted Year Published: 2016 Citation: Bastarrachea, LJ, and Goddard, JM. Hybrid Cationic and N-halamine Antimicrobial Coating with Self-Healing Properties and Efficacy in the Presence of Organic Matter. Submitted.
  • Type: Journal Articles Status: Published Year Published: 2015 Citation: Bastarrachea, LJ, Wong, DE, Roman, MJ, Lin, Z, Goddard, JM. 2015. Active Packaging Coatings. Coatings. 5(4) 771-791. DOI: 10/3390/coatings5040771.
  • Type: Journal Articles Status: Published Year Published: 2015 Citation: Bastarrachea, L. and Goddard, JM. 2015. Antimicrobial coatings with dual cationic and N-halamine character: characterization and biocidal efficacy. Journal of Agricultural and Food Chemistry. 63(16): 4243-51. DOI: 10.1021/acs.jafc.5b00445.
  • Type: Journal Articles Status: Published Year Published: 2015 Citation: Denis-Rohr, A, Bastarrachea, LJ, Goddard, JM. 2015. Antimicrobial Efficacy of N-Halamine Coatings Prepared via Dip and Spray Layer-by-Layer Deposition. Food and Bioproducts Processing. 96: 12-19. DOI: 10.1016/j.fbp.2015.06.002.
  • Type: Book Chapters Status: Published Year Published: 2015 Citation: Bastarrachea-Gutierrez, LJ, Denis-Rohr, A, Goddard, JM. 2015. Antimicrobial Food Equipment Coatings: Applications and Challenges. Annual Review of Food Science and Technology. 6: 97-118. DOI: 10.1146/annurev-food-022814-01543.
  • Type: Conference Papers and Presentations Status: Other Year Published: 2015 Citation: Bastarrachea, L, and Goddard, JM. Layer by Layer assembly of antimicrobial nanoscale polymeric coatings. Invited presentation in session: Nanotechnology-enabled technologies for food safety intervention. July 13, 2015. Institutes of Food Technologists Annual Meeting in Chicago, IL.
  • Type: Conference Papers and Presentations Status: Other Year Published: 2015 Citation: Huang, K, Barish, JA, and Goddard, JM. Scale-up of Non-Fouling Materials for Dairy Processing. Invited presentation in session: Advances in Dairy Processing with an Eye Towards Improving Sustainability. July 12, 2015. Institutes of Food Technologists Annual Meeting in Chicago, IL.
  • Type: Conference Papers and Presentations Status: Other Year Published: 2015 Citation: Bastarrachea, L, Huang, K, and Goddard, JM. Non-fouling and Antimicrobial Coatings to Improve Dairy Safety and Quality. Invited presentation at the 17th Annual Dairy Ingredients Symposium. February 18, 2015. Shell Beach, CA.
  • Type: Conference Papers and Presentations Status: Other Year Published: 2015 Citation: Bastarrachea, L, and Goddard, JM. Rechargeable Antimicrobial Coatings for Food Processing Equipment. July 27, 2015. Oral Presentation at the International Association for Food Protection Annual Meeting in Portland, Oregon.


Progress 12/15/13 to 12/14/14

Outputs
Target Audience: There are several target audiences who were served by this project in the past year. Graduate and undergraduate students learned experimental design, antimicrobial material chemistry, and food microbiology techniques through laboratory experience and instruction. Graduate students also gained technical writing experience as well as mentorship experience by mentoring undergraduate researchers who supported this project. The antimicrobial materials scientific community received new science-based knowledge through journal article publications and conference proceedings of results related to this work. The food industry received advances in the understanding of how different approaches to antimicrobial materials development can improve food safety and reduce spoilage in the processing environment. Changes/Problems: Nothing Reported What opportunities for training and professional development has the project provided? Two graduate students and one undergraduate student are involved in the execution of this project. As part of this project, they learn technical skills in nanotechnology, food microbiology, materials chemistry, and interdisciplinary life science. They are also given opportunities to present their findings at many levels: lab meetings, campus events, and national conferences, as well as in published technical journal articles. How have the results been disseminated to communities of interest? Knowledge from this project has been disseminated to scientific communities as well as the general public. Results were presented at the Fall 2013 American Chemical Society Meeting in Indianapolis, IN and in University symposia. Results were published in one new peer-reviewed publication in Journal of Food Science. What do you plan to do during the next reporting period to accomplish the goals? In the next reporting period, we will have two major efforts. In the first, we will more thoroughly characterize the antimicrobial activity of our halamine materials in the presence of complex food matrix components. We will include growth inhibition assays as well as widen the range of organisms and growth environments. Exploration into coatings with both regenerable and natively antimicrobial character will support reduced contact time needed for microbial inactivation.

Impacts
What was accomplished under these goals? In the past year, several significant accomplishments were achieved towards the goal of designing rechargeably antimicrobial food processing surfaces by nanoscale surface modification. We have expanded our material synthesis work to better adapt coating technologies to larger-scale applications suitable for industrial use. Specifically, we adapted the layer-by-layer deposition technique using spray deposition (versus dip coating) to improve the commercial translatability of the technology. We have explored utilization of different polymers in the coating and demonstrated their antimicrobial effectiveness. Rigorous stability studies were performed in which materials were challenged against sanitizers and detergents used in the food industry and found to retain antimicrobial character. These results indicate the commercial potential for this nanoscale antimicrobial surface modification technique.

Publications

  • Type: Journal Articles Status: Published Year Published: 2014 Citation: Bastarrachea, L, McLandsborough, L, Peleg, M, Goddard, JM. 2014. Antimicrobial N-halamine modified polyethylene: characterization, biocidal efficacy, regeneration and stability. Journal of Food Science. 79 (5): 887-897. DOI: 10.1111/1750-3841.12455
  • Type: Conference Papers and Presentations Status: Published Year Published: 2013 Citation: Goddard, JM. Innovative Food Contact Materials. Young Scientist Competition, Division of Agricultural and Food Chemistry. September 2013. American Chemical Society National Meeting. Indianapolis, IN.
  • Type: Other Status: Other Year Published: 2013 Citation: Goddard, JM. Innovative Food Contact Materials. Seminar Presentation at Michigan State University School of Packaging, October 3, 2013, East Lansing, MI.
  • Type: Other Status: Other Year Published: 2014 Citation: Goddard, JM. Biointerfaces in Food and Bioprocessing. Cornell Food Science Seminar Series, March 18, 2014, Cornell University, Ithaca, NY.


Progress 12/15/12 to 12/14/13

Outputs
Target Audience: There are several target audiences who were served by this project in the past year. Graduate and undergraduate students learned experimental design, antimicrobial material chemistry, and food microbiology techniques through laboratory experience and instruction. Graduate students also gained technical writing experience as well as mentorship experience by mentoring undergraduate researchers who supported this project. The antimicrobial materials scientific community received new science-based knowledge through journal article publications and conference proceedings of results related to this work. The food industry received advances in the understanding of how different approaches to antimicrobial materials development can improve food safety and reduce spoilage in the processing environment. Changes/Problems: Nothing Reported What opportunities for training and professional development has the project provided? Two graduate students and one undergraduate student are involved in the execution of this project. As part of this project, they learn technical skills in nanotechnology, food microbiology, materials chemistry, and interdisciplinary life science. They are also given opportunities to present their findings at many levels: lab meetings, campus events, and national conferences, as well as in published technical journal articles. How have the results been disseminated to communities of interest? Knowledge from this project has been disseminated to scientific communities as well as the general public. Results were presented at the Spring 2013 American Chemical Society Meeting in New Orleans, LA and in regional conferences. Results were published in two peer-reviewed publications in Journal of Applied Polymer Science as well as Journal of Food Engineering. What do you plan to do during the next reporting period to accomplish the goals? In the next reporting period, we will have two major efforts. In the first, we will more thoroughly characterize the antimicrobial activity of our halamine materials in the presence of complex food matrix components. We will include growth inhibition assays as well as widen the range of organisms and growth environments. In the second effort, we will expand our material synthesis work to better adapt material coating technologies to larger-scale, potentially roll-to-roll, applications suitable for industrial use. A range of nanoscale surface modification techniques are being explored to maximize application simplicity and durability while retaining regenerably antimicrobial character.

Impacts
What was accomplished under these goals? In the past year, several significant accomplishments were achieved towards the goal of designing rechargeably antimicrobial food processing surfaces by nanoscale surface modification. Specifically, we adapted the layer-by-layer deposition technique to multiple polymer substrates. The kinetics of antimicrobial activity against Listeria monocytogenes were characterized in terms of rate of inactivation and the influence of the number of bilayers applied. Increasing the number of bilayers up to 5 reduced the time to total theoretical inactivation to less than an hour. On-going work has established the ability to successfully deposit up to 20 bilayers with shortened contact time needed for significant (6 log reduction) antimicrobial activity. We have further demonstrated the ability to recharge the materials with chlorine up to 100 times with retained antimicrobial activity. Materials were also shown to be stable against extended exposure to pH extremes and detergents, as quantified by X-Ray Photoelectron Spectroscopy, ability to recharge with chlorine after exposure, and antimicrobial activity. These results indicate the commercial potential for this nanoscale antimicrobial surface modification technique.

Publications

  • Type: Journal Articles Status: Published Year Published: 2012 Citation: Bastarrachea-Gutierrez, LJ, and Goddard, JM. 2012. Development of Antimicrobial Stainless Steel via Surface Modification: Characterization of Surface Chemistry and N-Halamine Chlorination. Journal of Applied Polymer Science. 127 (1): 821-831. DOI: 10.1002/APP.37806.
  • Type: Journal Articles Status: Published Year Published: 2013 Citation: Bastarrachea, LJ, Peleg, M, McLandsborough, LA, Goddard, JM. 2013. "Inactivation kinetics of Listeria monocytogenes on polyethylene modified by antimicrobial N-halamine multilayer deposition. Journal of Food Engineering. 117 (1): 52-58. DOI: 10.1016/j.jfoodeng.2013.02.004.
  • Type: Conference Papers and Presentations Status: Other Year Published: 2013 Citation: Bastarrachea, LJ, Peleg, M, McLandsborough, LA, Goddard, JM. Low density polyethylene modified with antimicrobial N-halamines: Kinetics of inactivation against Listeria monocytogenes and N-halamine regeneration. 245th ACS National Meeting, Division of Agricultural and Food Chemistry, Graduate Student Symposium. April 7th 2013. New Orleans, LA.
  • Type: Other Status: Other Year Published: 2013 Citation: Goddard, JM. Designing Materials to Improve Food Quality and Safety. Invited Seminar at Smith College, Chemistry Department, April 1, 2013, Northampton, MA.


Progress 12/15/11 to 12/14/12

Outputs
OUTPUTS: In the second year of the project, we successfully demonstrated that our antimicrobial N-halamine modification process can be adapted to stainless steel processing surfaces. A simple layer-by-layer deposition process was used along with an improved cross-linking chemistry to increase the amount of antimicrobial activity. The antimicrobial activity against Listeria monocytogenes was demonstrated with more than 4 log reduction in microbial populations. N-halamine modified steel was characterized by a colorimetric chlorine assay, FTIR spectroscopy, ellipsometry, and X-ray photoelectron spectroscopy. We are currently designing microbiological methodology to assess the antimicrobial effectiveness of our N-halamine modified stainless steel coupons. Knowledge from this project has been disseminated to scientific communities as well as the general public. Results were presented at the 2012 Annual meeting for the International Association of Food Protection in Providence Rhode Island, as well as at the annual grantees meeting in Orlando, FL. Outcomes were discussed at an invited talk on "New Approaches to Food Safety" at the 2011 regional meeting of the American Society of Microbiology in Randolph, MA as well as an invited talk on "Self-sanitizing Food Processing Surfaces" at the 2011 Annual Meeting of the Institute of Food Technologists in New Orleans, LA in the Session: Nanotechnology enabled food safety interventions. This work was shared in an international audience at Jiangnan University in Wuxi, China in the September 2011 symposium on "Nanotechnology - better food and better life". PARTICIPANTS: PI: Dr. Julie Goddard. Assistant Professor, Department of Food Science, UMass Amherst. PI Goddard provided overall project management, including administration of funds, mentorship of the graduate student hired as part of this project, and overall technical project direction. Partner Organization: Michigan State University is a collaborator (sub-contract) performing materials characterization and support of the objectives of this project. Collaborators: co-PI Dr Lynne McLandsborough (UMass Food Science) supports the microbiology aspects of this project. Co-PI Dr Joseph Hotchkiss (MSU) supports the material science aspects of this project. Training: Luis Bastarrachea-Guitierrez is a graduate student hired as part of this project to conduct research. He gets training and professional development through research, coursework, presentations, and collaboration opportunities. TARGET AUDIENCES: Not relevant to this project. PROJECT MODIFICATIONS: Not relevant to this project.

Impacts
The results and findings of our refined and improved upon N-halamine modification technique have resulted in a change in knowledge. Increasing the stability, activity, and materials (e.g. stainless steel) of the N-halamine modification are examples of new applied knowledge that are presently being included in a publication. We have further characterized the inactivation kinetics of the N-halamine modified materials to better elucidate mechanisms of antimicrobial activity and improve the overall activity. Fundamental research in understanding the chemistry of chlorination has helped direct our research to improve the stability of the nanoscale coatings for continued use. On-going research will include these new techniques and methods, which will result in a change in actions, namely, the potential commercial adaptation of N-halamine modified materials as antimicrobial materials in the food industry.

Publications

  • Bastarrachea-Gutierrez, LJ, and Goddard, JM. 2012. Development of Antimicrobial Stainless Steel via Surface Modification: Characterization of Surface Chemistry and N-Halamine Chlorination. Journal of Applied Polymer Science. DOI: 10.1002/APP.37806.


Progress 12/15/10 to 12/14/11

Outputs
OUTPUTS: In the first year of the project, we successfully demonstrated that non-toxic UV irradiation can be used as a method for initial functionalization of polymer materials prior to antimicrobial N-halamine modification. Preliminary work was performed using a toxic wet chemical process (chromic acid) and we showed that UV irradiation can be used as a dry, high throughput, non toxic method to achieve the same results. We have improved on our prior N-halamine surface modification methodology by increasing the number and stability of N-halamines by using a covalently cross-linked layer-by-layer deposition technique. We have increased the number of antimicrobial N-halamines more than seven-fold. We further adapted our antimicrobial N-halamine surface modification methodology to perform on stainless steel substrates. N-halamine modified steel was characterized by a colorimetric chlorine assay, FTIR spectroscopy, ellipsometry, and X-ray photoelectron spectroscopy. We are currently designing microbiological methodology to assess the antimicrobial effectiveness of our N-halamine modified stainless steel coupons. PARTICIPANTS: PI: Dr. Julie Goddard. Assistant Professor, Department of Food Science, UMass Amherst. PI Goddard provided overall project management, including administration of funds, mentorship of the graduate student hired as part of this project, and overall technical project direction. Partner Organization: Michigan State University is a collaborator (sub-contract) performing materials characterization and support of the objectives of this project. Collaborators: co-PI Dr Lynne McLandsborough (UMass Food Science) supports the microbiology aspects of this project. Co-PI Dr Joseph Hotchkiss (MSU) supports the material science aspects of this project. Training: Luis Bastarrachea-Guitierrez is a graduate student hired as part of this project to conduct research. He gets training and professional development through research, coursework, and collaboration opportunities. TARGET AUDIENCES: Not relevant to this project. PROJECT MODIFICATIONS: Nothing significant to report during this reporting period.

Impacts
The results and findings of our refined and improved upon N-halamine modification technique have resulted in a change in knowledge. Increasing the stability, activity, and materials (e.g. stainless steel) of the N-halamine modification are examples of new applied knowledge that are presently being included in a publication. On-going research will include these new techniques and methods, which will result in a change in actions, namely, the potential commercial adaptation of N-halamine modified materials as antimicrobial materials in the food industry.

Publications

  • Goddard, JM. 2011. Improving the Sanitation of Food Processing Surfaces. Food Technology. October 2011 Issue, p. 40-46.