DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Hierarchical Self–Assembly of Multidimensional Functional Materials from Sequence–Defined Peptoids

Journal Article · · Angewandte Chemie (International Edition)
ORCiD logo [1];  [2];  [3];  [2];  [4];  [4];  [5];  [6]; ORCiD logo [6]
  1. Zhejiang Sci-Tech University, Hangzhou (China); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
  2. Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
  3. Harvard University, Cambridge, MA (United States)
  4. University of Washington, Seattle, WA (United States)
  5. Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Binghamton University, NY (United States)
  6. Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); University of Washington, Seattle, WA (United States)

Hierarchical self-assembly represents a powerful strategy for the fabrication of functional materials across various length scales. However, achieving precise formation of functional hierarchical assemblies remains a significant challenge and requires a profound understanding of molecular assembly interactions. In this study, we present a molecular-level understanding of the hierarchical assembly of sequence-defined peptoids into multidimensional functional materials, including twisted nanotube bundles serving as a highly efficient artificial light harvesting system. By employing synchrotron-based powder X-ray diffraction and analyzing single crystal structures of model compounds, we elucidated the molecular packing and mechanisms underlying the assembly of peptoids into multidimensional nanostructures. Our findings demonstrate that incorporating aromatic functional groups, such as tetraphenyl ethylene (TPE), at the termini of assembling peptoid sequences promotes the formation of twisted bundles of nanotubes and nanosheets, thus enabling the creation of a highly efficient artificial light harvesting system. This research exemplifies the potential of leveraging sequence-defined synthetic polymers to translate microscopic molecular structures into macroscopic assemblies. It holds promise for the development of functional materials with precisely controlled hierarchical structures and designed functions.

Research Organization:
Univ. of Washington, Seattle, WA (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE
Grant/Contract Number:
SC0019288; AC05-76RL01830; AC02-05CH11231; FWP 65357; FWP 80124
OSTI ID:
2346260
Alternate ID(s):
OSTI ID: 2346261; OSTI ID: 2409176; OSTI ID: 2446795
Report Number(s):
PNNL-SA-193522
Journal Information:
Angewandte Chemie (International Edition), Vol. 63, Issue 24; ISSN 1433-7851
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

References (36)

Efficient light harvesting in self-assembled organic luminescent nanotubes journal January 2023
Peptide-Based Supramolecular Systems Chemistry journal September 2021
Smart activatable and traceable dual-prodrug for image-guided combination photodynamic and chemo-therapy journal November 2017
Hierarchical Nanomaterials Assembled from Peptoids and Other Sequence-Defined Synthetic Polymers journal August 2021
Aggregation‐Induced Emission: New Vistas at the Aggregate Level journal May 2020
Peptoid Polymers: A Highly Designable Bioinspired Material journal May 2013
Constructing Adaptive Photosensitizers via Supramolecular Modification Based on Pillararene Host–Guest Interactions journal May 2020
Programming Amphiphilic Peptoid Oligomers for Hierarchical Assembly and Inorganic Crystallization journal November 2020
Highly stable and self-repairing membrane-mimetic 2D nanomaterials assembled from lipid-like peptoids journal July 2016
Structural Elucidation of a Polypeptoid Chain in a Crystalline Lattice Reveals Key Morphology-Directing Role of the N-Terminus journal February 2023
Designing Sequence-Defined Peptoids for Biomimetic Control over Inorganic Crystallization journal April 2021
Designable and dynamic single-walled stiff nanotubes assembled from sequence-defined peptoids journal January 2018
Programmable two-dimensional nanocrystals assembled from POSS-containing peptoids as efficient artificial light-harvesting systems journal May 2021
Highly Bright and Photostable Two-Dimensional Nanomaterials Assembled from Sequence-Defined Peptoids journal March 2021
Nanoparticle-Mediated Assembly of Peptoid Nanosheets Functionalized with Solid-Binding Proteins: Designing Heterostructures for Hierarchy journal February 2021
Universal Relationship between Molecular Structure and Crystal Structure in Peptoid Polymers and Prevalence of the cis Backbone Conformation journal January 2018
Designing sequence-defined peptoids for fibrillar self-assembly and silicification journal March 2023
Insights into the Biomimetic Synthesis of 2D ZnO Nanomaterials through Peptoid Engineering journal October 2023
Hierarchical Materials from High Information Content Macromolecular Building Blocks: Construction, Dynamic Interventions, and Prediction journal October 2022
Efficient method for the preparation of peptoids [oligo(N-substituted glycines)] by submonomer solid-phase synthesis journal December 1992
Hierarchical Assembly of Peptoid‐Based Cylindrical Micelles Exhibiting Efficient Resonance Energy Transfer in Aqueous Solution journal August 2019
Peptide-Based Methods for the Preparation of Nanostructured Inorganic Materials journal February 2010
Pillar[5]arene-Based Solid-State Supramolecular Polymers with Suppressed Aggregation-Caused Quenching Effects and Two-Photon Excited Emission journal September 2020
Very strong hydrogen bonding journal January 1980
Multidimensional Frameworks Assembled from Silver(I) Coordination Polymers Containing Flexible Bis(thioquinolyl) Ligands:  Role of the Intra- and Intermolecular Aromatic Stacking Interactions journal June 2003
Bioinspired Peptoid Nanotubes for Targeted Tumor Cell Imaging and Chemo‐Photodynamic Therapy journal August 2019
Highly stable and tunable peptoid/hemin enzymatic mimetics with natural peroxidase-like activities journal May 2022
Efficient Artificial Light-Harvesting System Based on Supramolecular Peptide Nanotubes in Water journal December 2020
Assembly of highly efficient aqueous light-harvesting system from sequence-defined peptoids for cytosolic microRNA detection journal August 2023
Self-Assembling Nucleic Acid Nanostructures Functionalized with Aptamers journal June 2021
Biomimetic peptide self-assembly for functional materials journal September 2020
Self-Repair and Patterning of 2D Membrane-Like Peptoid Materials journal August 2016
Lessons from nature about solar light harvesting journal September 2011
Protein Assembly by Design journal August 2021
Helical Sulfono-γ-AApeptides with Aggregation-Induced Emission and Circularly Polarized Luminescence journal July 2019
Designed Metal-Containing Peptoid Membranes as Enzyme Mimetics for Catalytic Organophosphate Degradation journal October 2023