Source: TEXAS A&M UNIVERSITY submitted to NRP
DEVELOPMENT OF CELLULAR DELIVERY TOOLS FOR BIOTECHNOLOGICAL AND THERAPEUTIC APPLICATIONS IN ANIMALS AND PLANTS.
Sponsoring Institution
National Institute of Food and Agriculture
Project Status
COMPLETE
Funding Source
Reporting Frequency
Annual
Accession No.
1020411
Grant No.
(N/A)
Cumulative Award Amt.
(N/A)
Proposal No.
(N/A)
Multistate No.
(N/A)
Project Start Date
Aug 5, 2019
Project End Date
Jul 18, 2024
Grant Year
(N/A)
Program Code
[(N/A)]- (N/A)
Recipient Organization
TEXAS A&M UNIVERSITY
750 AGRONOMY RD STE 2701
COLLEGE STATION,TX 77843-0001
Performing Department
Biochemistry & Biophysics
Non Technical Summary
Controlled manipulation of cells through the precise intracellular delivery of biologically active materials has been a long-term goal for biotechnological and therapeutic applications. Our ongoing research program aims to enable efficient delivery of macromolecules into animal or plant cells, through control of endosomal membrane permeability. Cellular delivery is a problem that has not yet been solved. Most techniques remain inefficient, are disruptive to cells and can be toxic. Furthermore, no single approach works for all macromolecular cargo, across cell types, or in every context (e.g. cell cultures vs in vivo). This problem is exacerbated by emerging biological applications continually pushing the boundaries of required delivery efficiencies and versatility. For example, effective macromolecular delivery would greatly amplify the therapeutic potentials of CRISPR-Cas9 technologies, wherein a large ribonucleoprotein complex provides challenges to current delivery systems, and of the manipulation of stem or immune system cells. We aim to reveal fundamental mechanisms of how to permeate cellular membranes, enabling precise control of the molecules that achieve this cell permeation, and to develop new platforms for cellular delivery. Thus, our studies will significantly advance both understanding and solutions to the cell delivery problem. In turn, the new delivery tools developed as part of this research program will be useful to perform gene editing in plants or in animals, thereby enhancing agricultural competitiveness.
Animal Health Component
(N/A)
Research Effort Categories
Basic
100%
Applied
(N/A)
Developmental
(N/A)
Classification

Knowledge Area (KA)Subject of Investigation (SOI)Field of Science (FOS)Percent
2067299100050%
3037299100050%
Goals / Objectives
We have made the discovery of dfTAT, a peptide that enters cells with remarkably high efficiencies and without any toxicity. This reagent has two major benefits. First, it can be used to introduce a variety of molecules into the cytosol and nucleus of cells, including small molecules, peptides, enzymes, transcription factors, and nanoparticles. Second, it is uniquely suited as a molecular probe for revelation of membrane permeation mechanisms in unprecedented detail. In particular, we have established that dfTAT traffics to late endosomes after endocytic uptake, subsequently causing leakage specifically of late endosomes. This leakage occurs via dfTAT interactions with the late-endosome enriched lipid bis(monoacylglycero)phosphate (BMP, aka LBPA) and is critical for the delivery process as it is this step that permits cytosolic entry. Notably, this new mechanism likely extends to other delivery systems (e.g. cationic lipids, viral and polymer nanoparticles).Critically, to rationally design improved delivery agents and to maximize the utility of a variety of delivery systems, it becomes essential for us to understand the mechanisms of endosomal escape. The following specific aims will be pursued:objective 1: Determine how endosomal leakage is achieved by dfTAT and how this impacts the endocytic pathway. The interplay discovered between dfTAT and BMP has revealed that late endosomes can serve as useful gateways for efficient cell entry. First, we will dissect the molecular requirements for dfTAT-mediated endosomal leakage. Second, we will determine how BMP, a poorly characterized lipid selectively enriched in late endosomes, confers leakiness to the late endosomal membrane in response to dfTAT. Third, while endosomal leakage appears relatively innocuous to cells, our preliminary data suggest that endosomal leakage triggers a membrane damage response and transiently impacts endocytic trafficking. We will characterize this response as it pertains to the development of minimally disruptive delivery agents and reveals new membrane biology.objective 2: Determine how small molecule membrane modulators enhance endosomal escape. We have established that a newly discovered small molecule UNC7938 can augment the efficiency of dfTAT-mediated delivery. In particular, UNC7938 appears to prime late endosomal membranes for dfTAT-mediated leakage. Herein, we will uncover the molecular basis for this previously undiscovered synergy between membrane-disrupting compounds. These studies will enable exploration of the chemical space of molecules that can promote cell entry.objective 3: Development of a surface-modified viral delivery platform for macromolecular complexes. Our data indicate that endosomolytic dfTAT-like moieties can be incorporated into viral capsids to improve the cell penetration of virus-like particles (VLP), a potential delivery platform with numerous advantages for tailoring in vivo delivery of cargo. We will decorate the surface of VLP with membrane-active peptides and establish how surface density impacts membrane permeation. We seek to optimize the membrane-permeation of these agents. CRISPR-Cas9 delivery and gene editing activity will serve as a highly attractive model cargo system for manipulating cells, particularly immune cells resistant to current delivery approaches. VLP will be a learning platform for other encapsulation strategies (e.g. liposomes, nanoparticles).A second area of research consists in learning how to exploit exosomes as molecular delivery tools. Exosomes - membrane-bound vesicles secreted by animal cells - signal between cells, alter tissue physiology, and contribute to disease states. Exosomes signal by transferring bioactive lipids, proteins and nucleic acids from one cell to another.[8, 9] Here, we will address this problem by uncovering how exosomes deliver their content into recipient cells and by establishing what controls their transport properties.objective 5: Determine the mechanisms of exosomal trafficking and their modulation by exosome composition We will determine the cellular sites at which exosomes deliver their luminal cargos by using exosomes labeled with probes that report on cytosolic penetration. We will couple monitored exosome delivery with pharmacological or genetic manipulation of the endocytic pathway to identify the step(s) at which contents are delivered for distinct exosomal populations. Furthermore, our studies will determine how subpopulations of exosomes alter their transport properties depending on their membrane composition, their cells of origin, or the recipient cells they enter. These experiments will establish composition-trafficking relationships that control exosomal cell entry and lead to the potential identification of factors that control delivery.objective 6: Determine the mechanisms of exosomal fusogenicity and their modulation by cellular signaling or exosome composition To deliver signaling molecules into cells, exosomal membranes fuse with those of recipient cells. Our working hypothesis is that it takes place within the endocytic pathway and that exosomal membranes respond to the endosomal milieu to initiate fusion. We will determine how exosomal membranes are impacted in vitro by potential triggers of fusion using BAS. The same triggers will also be modulated in the endosomal milieu to determine how exosomal delivery is impacted in live cells. Moreover, because exosome secretion is a dynamic process, we will determine how the membrane and delivery properties of exosomes change under stimulatory conditions known to activate exosomal secretion and signaling of cancer cells. We will then ask how changes in these properties correlate with fusion, delivery efficiency, and trafficking route. These experiments will establish the biological ground rules of exosome function, which we will then manipulate to dissect mechanisms further.
Project Methods
Our methods involve the use of in vitro models (e.g. liposomes), cells (human, animal, plants), and organisms (e.g. mouse).We use a plethora of assays to monitor the process of cell penetration. They include fluorescence microscopy, flow cytometry, and bioactivity assays.

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

Outputs
Target Audience:The target audience is the scientific community. The delivery agents we have discovered are potected by a patent which has recently been licensed by TANA Therapeutics. The target audience to this commercialization efforts has been angel investors so far. Changes/Problems: Nothing Reported What opportunities for training and professional development has the project provided?The project has provided training opportunities for 6 graduate students. Two graduate students have graduated. One has been hired by Merck as a postdoctoral associate. The otehr graduate student is the recipient of aORISE Fellowship with the Biomedical Advanced Research and Development Authority (BARDA) at Health & Human Services. The project has also supported the development of an "oral communication in biochemistry" course for junior graduate students. The project has supported the development of a training workshop for undergraduate students interested in applying to graduate school. How have the results been disseminated to communities of interest?The results have been disseminated via publications (listed) and via virtual seminars. What do you plan to do during the next reporting period to accomplish the goals?The plan remains the same and we are on track to achieve our goals. I will hire a postdoctoral associate with a phage biology background to contribute to objective 3.

Impacts
What was accomplished under these goals? Significant progress was made for objective 1. In particular, we have develped of model for how cell penetration at the late endosome is achieved (Brock DJ, Kondow-McConaghy H, Allen J, Brklja?a Z, Kustigian L, Jiang M, Zhang J, Rye H, Vazdar M, Pellois JP. Mechanism of Cell Penetration by Permeabilization of Late Endosomes: Interplay between a Multivalent TAT Peptide and Bis(monoacylglycero)phosphate. Cell Chem Biol. 2020 Oct 15;27(10):1296-1307.e5.). We have also establish that little to no membrane damage response is engaged during the process of cell delivery by our reagents (Kondow-McConaghy HM, Muthukrishnan N, Erazo-Oliveras A, Najjar K, Juliano RL, Pellois JP. Impact of the Endosomal Escape Activity of Cell-Penetrating Peptides on the Endocytic Pathway. ACS Chem Biol. 2020 ). For objective 2, we have identified a small molecule as a powerful enhancer of cell penetration (Allen J, Najjar K, Erazo-Oliveras A, Kondow-McConaghy HM, Brock DJ, Graham K, Hager EC, Marschall ALJ, Dübel S, Juliano RL, Pellois JP. Cytosolic Delivery of Macromolecules in Live Human Cells Using the Combined Endosomal Escape Activities of a Small Molecule and Cell Penetrating Peptides. ACS Chem Biol. 2019 Dec 20;14(12):2641-2651). We are continuing in this direction by screening other molecules. Objectives 3, 4, and 5 are in progress. Reagents are being produced and protocols developed.

Publications

  • Type: Book Chapters Status: Published Year Published: 2020 Citation: Diaz J, Pellois JP. Expressed Protein Ligation: General Experimental Protocols. Methods Mol Biol. 2020;2133:75-117. doi: 10.1007/978-1-0716-0434-2_5. PMID: 32144664.
  • Type: Journal Articles Status: Published Year Published: 2020 Citation: Brock DJ, Kondow-McConaghy H, Allen J, Brklja?a Z, Kustigian L, Jiang M, Zhang J, Rye H, Vazdar M, Pellois JP. Mechanism of Cell Penetration by Permeabilization of Late Endosomes: Interplay between a Multivalent TAT Peptide and Bis(monoacylglycero)phosphate. Cell Chem Biol. 2020 Oct 15;27(10):1296-1307.e5. doi: 10.1016/j.chembiol.2020.07.015. Epub 2020 Aug 11. PMID: 32783962; PMCID: PMC7572721.
  • Type: Journal Articles Status: Published Year Published: 2020 Citation: Impact of the Endosomal Escape Activity of Cell-Penetrating Peptides on the Endocytic Pathway. ACS Chem Biol. 2020 Sep 18;15(9):2355-2363. doi: 10.1021/acschembio.0c00319. Epub 2020 Aug 24. PMID: 32786263; PMCID: PMC7502533.


Progress 08/05/19 to 09/30/19

Outputs
Target Audience:The target audience for the reporting period are investigators within the scientific community. They include scientists from the fields of cell biology, chemical biology, and biotechnology. They also include students within these fields, with efforts consisting in classroom and laboratoryinstruction. The knowledge gained in this projects is also dessiminated through publications and participation at national and international meetings. Changes/Problems: Nothing Reported What opportunities for training and professional development has the project provided?The project has provided training opportunities for 6 graduate students. How have the results been disseminated to communities of interest?The results have been disseminated via publications (listed) and via seminars. What do you plan to do during the next reporting period to accomplish the goals?The plan remain the same and we are on track to achieve our goals.

Impacts
What was accomplished under these goals? Significant progress was made for objective 2. Our publication in ACS Chem Biol has indentified UNC7938 as a small molecule that can boost delivery efficiencies to a very high level.

Publications

  • Type: Journal Articles Status: Published Year Published: 2019 Citation: Brock DJ, Kondow-McConaghy HM, Hager EC, Pellois JP. Endosomal Escape and Cytosolic Penetration of Macromolecules Mediated by Synthetic Delivery Agents. Bioconjug Chem. 2019 Feb 20;30(2):293-304. doi: 10.1021/acs.bioconjchem.8b00799. Epub 2018 Dec 6. PMID: 30462487; PMCID: PMC6561124.
  • Type: Journal Articles Status: Published Year Published: 2019 Citation: Pellois JP. Efficient and Innocuous Live-Cell Delivery: Making Membrane Barriers Disappear to Enable Cellular Biochemistry: How Better Cellular Delivery Tools Can Contribute to Precise and Quantitative Cell Biology Assays. Bioessays. 2019 Jun;41(6):e1900031. doi: 10.1002/bies.201900031. Epub 2019 May 14. PMID: 31087674; PMCID: PMC6563813.
  • Type: Journal Articles Status: Published Year Published: 2019 Citation: Arora M, Ganugula R, Kumar N, Kaur G, Pellois JP, Garg P, Kumar MNVR. Next-Generation Noncompetitive Nanosystems Based on Gambogic Acid: In silico Identification of Transferrin Receptor Binding Sites, Regulatory Shelf Stability, and Their Preliminary Safety in Healthy Rodents. ACS Appl Bio Mater. 2019 Aug 19;2(8):3540-3550. doi: 10.1021/acsabm.9b00419. Epub 2019 Jul 4. PMID: 31440745; PMCID: PMC6705617.
  • Type: Journal Articles Status: Published Year Published: 2019 Citation: Park G, Brock DJ, Pellois JP, Gabba� FP. Heavy Pnictogenium Cations as Transmembrane Anion Transporters in Vesicles and Erythrocytes. Chem. 2019 Aug 8;5(8):2215-2227. doi: 10.1016/j.chempr.2019.06.013. Epub 2019 Jul 15. PMID: 31482145; PMCID: PMC6719792.
  • Type: Journal Articles Status: Published Year Published: 2019 Citation: Allen J, Najjar K, Erazo-Oliveras A, Kondow-McConaghy HM, Brock DJ, Graham K, Hager EC, Marschall ALJ, D�bel S, Juliano RL, Pellois JP. Cytosolic Delivery of Macromolecules in Live Human Cells Using the Combined Endosomal Escape Activities of a Small Molecule and Cell Penetrating Peptides. ACS Chem Biol. 2019 Dec 20;14(12):2641-2651. doi: 10.1021/acschembio.9b00585. Epub 2019 Oct 31. PMID: 31633910; PMCID: PMC7008471.