Article
Engineering, Environmental
Bryan Parnitzke, Tochukwu Nwoko, Kate G. E. Bradford, Nethmi De Alwis Watuthanthrige, Kevin Yehl, Cyrille Boyer, Dominik Konkolewicz
Summary: The kinetics of photoinduced electron/energy transfer reversible addition fragmentation chain transfer (PET-RAFT) polymerization were investigated using a model system. Efficient PET-RAFT occurred under blue, violet, and green light, while minimal polymerization was observed under orange or red light. A universal scaling law was developed for Ir(ppy)3 and other energy transfer catalyzed PET-RAFT, allowing a description of polymerization across a range of light intensities, reaction conditions, and geometries.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Physical
Fuqiang Lan, Junle Zhang, Yuying Li, Yaxuan Shi, Yuancheng Zhang, Ge Shi, Xiaomeng Zhang, Zhe Cui, Peng Fu, Minying Liu, Xiaoguang Qiao, Yanjie He, Wenjie Zhang, Xinchang Pang
Summary: Highly ordered TiO2 nanotube arrays (TNTAs) and their heterostructure nanocomposites were used as photocatalysts for efficient broadband photoinduced controlled radical polymerization (photoCRP). The combination of electron transfer acceleration from TNTAs' structure and the localized surface plasmon resonance (LSPR) effect with the formation of Schottky barrier via Au nanoparticle modification enabled efficient UV-visible light responsive photoCRP. The resulting polymers exhibited high conversion, living chain-ends, tightly regulated molecular weights, and excellent temporal control properties.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Yang Xiao, Wanchao Hu, Zhinan Xia, Bingfeng Shi, Changli Lu
Summary: Phenanthroline is a stable p-electron acceptor with a large conjugated chromophore and its derivatives are widely used in various applications. Designing efficient organic photocatalysts (OPCs) for reversible-deactivation radical polymerization (RDRP) is still a challenge. In this study, donor-acceptor (D-A) type OPCs based on phenanthroline were used for the first time in photoinduced electron transfer-reversible addition-fragmentation chain transfer (PET-RAFT) polymerization. By combining donor groups and weak acceptor groups, highly controlled polymerization of conjugated and unconjugated monomers was achieved.
CHINESE JOURNAL OF CHEMISTRY
(2023)
Article
Chemistry, Physical
Chunyu Zhao, Haixia Song, Yinghao Chen, Wei Xiong, Mingyou Hu, Youshen Wu, Yanfeng Zhang, Ling He, Yi Liu, Aizhao Pan
Summary: This study introduces a photocatalytic reaction called photoinduced electron transfer reversible addition-fragmentation chain transfer (PET-RAFT) polymerization using a CsPbBr3@MSNs nanocomposite as the photocatalyst. The embedded CsPbBr3 nanocrystals in dendritic mesoporous silica nanospheres (MSNs) successfully initiate the polymerization reaction, and the reaction variables are controlled to achieve polymers with desired characteristics.
ACS ENERGY LETTERS
(2022)
Article
Chemistry, Multidisciplinary
Shannon M. North, Steven P. Armes
Summary: In this study, zwitterionic diblock copolymers were successfully synthesized using RAFT polymerization in a wholly aqueous environment, with the isoelectric point in aqueous solution tunable by varying monomer proportions. These copolymers show promise for potential applications.
Article
Engineering, Environmental
Wan Lin Guo, Yan Zhou, Bo Duan, Wen Fang Wei, Chen Chen, Xue Li, Tao Cai
Summary: This study utilized nanofibrous chitin microspheres to prepare NCPNIEY microspheres, which were used for surface conjugation of eosin Y-bound copolymers via activated ester-amine reaction. These microspheres hold great potential for high throughput polymerizations, demonstrating the advantages of PET-RAFT polymerization.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Materials Science, Multidisciplinary
Longqiang Xiao, Zhishun Yang, Hongjie Yang, Zhen Lu, Rui Zhao, Linxi Hou
Summary: D-A conjugated organic polymers (COP) photocatalysts have great potential due to their tunable structure and diverse species. D-A conjugated organic polymers composed of relatively weak donor units and strong acceptor units are more favorable for photogenerated charge migration and exhibit better photocatalytic activity.
ACS APPLIED POLYMER MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Athanasios Smponias, Dionisis Stefanatos, Emmanuel Paspalakis
Summary: In this study, a hybrid nanostructure composed of a semiconductor quantum dot coupled to a metallic nanoparticle was investigated for the efficient creation of biexciton state using linearly polarized laser pulses. Numerical simulations showed that a simple on-off-on pulse-sequence can efficiently prepare the biexciton state even in the presence of the nanoparticle, for various interparticle distances and biexciton energy shifts. The pulse durations in the sequence were determined by solving a transcendental equation.
Article
Polymer Science
Meng Chen, Jingyi Hao, Wenjie Zhang, Ge Shi, Xiaomeng Zhang, Zhe Cui, Peng Fu, Minying Liu, Xiaoguang Qiao, Yanjie He, Xinchang Pang
Summary: In this study, the NIR region was extended up to 980 nm by introducing upconversion nanocrystals into PET-RAFT polymerization. Well-defined polymers with predictable molecular weight and narrow dispersity were prepared within a few hours by NIR light-regulated PET-RAFT polymerization. This photopolymerization showed livingness feature and could be performed under different conditions, demonstrating its multiple advantages.
Article
Chemistry, Physical
Changhoon Yu, Jaejung Song, Tae In Kim, Yungyeong Lee, Yonghwan Kwon, Jongkyoung Kim, Jeehun Park, Jinho Choi, Junsang Doh, Seung Kyu Min, Seungho Cho, Min Sang Kwon
Summary: Due to current global environmental concerns, the development of eco-friendly and sustainable polymerization methods is crucial. In this study, the use of Ag2S nanocrystals as photocatalysts enabled the efficient photoinduced energy/electron transfer reversible addition-fragmentation chain-transfer (PET-RAFT) polymerization of acrylic monomers under ambient/aqueous conditions without any additives. The Ag2S nanocrystals exhibited excellent reducing power, water solubility, and biocompatibility, making them promising candidates as photocatalysts for polymer synthesis.
Article
Chemistry, Physical
Kirsten Bell, Brock Hunter, Marvin Alvarez, Sai Dileep Kumar Seera, Yiwen Guo, Yen-Ting Lin, Seong H. Kim, Christian W. Pester
Summary: Solid-supported organic photocatalysts offer great potential for sustainable chemical syntheses and the development of novel (super)hydrophilic materials. This study presents a hydrolysis-resistant heterogeneous photocatalysis platform based on photocatalytic polymer brushes attached to solid glass supports. The materials overcome the limitations of silane hydrolysis in aqueous conditions and enable well-controlled light-mediated radical polymerization. The addition of hydrophobic protective layers improves longevity and recyclability by mitigating silane hydrolysis and limiting water diffusion to reactive sites. The influence of this hydrophobic protective layer and the hydrophilicity of the photoactive polymer brush on the photocatalytic efficacy of the platform is investigated.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Review
Chemistry, Multidisciplinary
Irvin Veloz Martinez, Jackeline Iturbe Ek, Ethan C. Ahn, Alan O. Sustaita
Summary: Molecularly imprinted polymers (MIP) have demonstrated their potential as artificial and selective receptors for environmental monitoring. By tailoring these materials through specific binding mechanisms, MIP can mimic the recognition capacity of biological receptors while offering superior stability and versatility in sensing platforms. Controlled/living radical polymerization (CRP) techniques, such as RAFT, have been used to overcome the limitations of traditional polymerization methods, resulting in MIP with enhanced selectivity, sensitivity, and sorption capacity when incorporated as transducing elements in sensors. This study focuses on the design and synthesis strategies of RAFT-MIP to improve binding affinities and their application in environmental contaminant sensing.
Article
Polymer Science
Yifan Zhu, Emira Ramadani, Eilaf Egap
Summary: By utilizing thiol ligand capped CdSe quantum dots at low concentrations, we achieved rapid visible-light-induced radical polymerization in aqueous media, showcasing excellent oxygen tolerance and broad applications potential.
Article
Polymer Science
Maoji Zhao, Shuaishuai Zhu, Xue Yang, Yong Wang, Xingping Zhou, Xiaolin Xie
Summary: A heterogeneous catalyst with a unique structure synthesized by the Debus-Radziszewski reaction shows improved catalytic activity compared to small molecular analogs in polymerization reactions, producing polymers with narrow distribution and high chain-end fidelity. The catalyst can be easily separated and recycled multiple times.
MACROMOLECULAR RAPID COMMUNICATIONS
(2022)
Article
Pharmacology & Pharmacy
Jana Solomun, Gizem Cinar, Prosper Mapfumo, Friederike Richter, Elisabeth Moek, Franziska Hausig, Liam Martin, Stephanie Hoeppener, Ivo Nischang, Anja Traeger
Summary: The study presented a mild, aqueous formulation method for encapsulating high amounts of genetic material and successfully synthesized a pH-responsive hydrophobic copolymer, demonstrating high transfection efficiency and compatibility in cells.
INTERNATIONAL JOURNAL OF PHARMACEUTICS
(2021)
Article
Chemistry, Multidisciplinary
Poonam Mahendia, Gayatri Chauhan, Heena Wadhwa, Geeta Kandhol, Suman Mahendia, Ritu Srivastava, O. P. Sinha, Tristan D. Clemons, Shyam Kumar
Summary: Graphene composites with P3HT, PCBM, and their blends were successfully prepared via a chemical mixing approach, showing good dispersion and charge transfer within the polymers. Spectroscopic analysis revealed the doping effect of graphene and potential for designing optoelectronic devices with optimized photovoltaic performance.
JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS
(2021)
Article
Chemistry, Multidisciplinary
Naneki C. McCallum, Florencia A. Son, Tristan D. Clemons, Steven J. Weigand, Karthikeyan Gnanasekaran, Claudia Battistella, Brooke E. Barnes, Hashanthi Abeyratne-Perera, Zofia E. Siwicka, Christopher J. Forman, Xuhao Zhou, Martin H. Moore, Daniel A. Savin, Samuel Stupp, Zheng Wang, Gary J. Vora, Brandy J. Johnson, Omar K. Farha, Nathan C. Gianneschi
Summary: Research on artificial allomelanin analogues reveals high intrinsic microporosity and high BET surface area achievable through a simplified method. These synthetic allomelanin particles exhibit functions such as adsorbing ammonia and nerve agent simulants, as well as preventing agent breakthrough on breathable fabrics. Compared to naturally derived fungal melanin, synthetic analogues have higher porosity.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Multidisciplinary
Alexandra N. Edelbrock, Tristan D. Clemons, Stacey M. Chin, Joshua J. W. Roan, Eric P. Bruckner, Zaida Alvarez, Jack F. Edelbrock, Kristen S. Wek, Samuel I. Stupp
Summary: The study reports a supramolecular system where interactions between peptide amphiphiles and beta-cyclodextrin with adamantane lead to the formation of a mechanically robust hydrogel with highly porous architecture, which can be 3D printed and exhibits significant bioactivity towards neurons. This nanostructured hydrogel based on supramolecular assembly has potential applications in neuronal research and biomaterial design.
Article
Engineering, Biomedical
Alexandra I. Mercel, Kathleen Marulanda, David C. Gillis, Kui Sun, Tristan D. Clemons, Smaranda Willcox, Jack Griffith, Erica B. Peters, Mark R. Karver, Nick D. Tsihlis, Rob Maile, Samuel I. Stupp, Melina R. Kibbe
Summary: This study successfully identified proteins upregulated in the lung after smoke inhalation injury and developed nanofibers that target these proteins, showing promising lung localization effects in vivo, especially with angiotensin-converting enzyme-targeted nanofibers.
Article
Engineering, Biomedical
Kathleen Marulanda, Alexandra Mercel, David C. Gillis, Kui Sun, Maria Gambarian, Joshua Roark, Jenna Weiss, Nick D. Tsihlis, Mark R. Karver, S. Ruben Centeno, Erica B. Peters, Tristan D. Clemons, Samuel I. Stupp, Sean E. McLean, Melina R. Kibbe
Summary: The study developed peptide amphiphile nanofibers that target lung tissue with pulmonary hypertension, demonstrating the potential of a RAGE-targeted nanomaterial as a drug delivery platform to treat the disease. The targeted nanofibers significantly accumulated in the lungs, showing specific localization to diseased pulmonary tissue and reduced off-target toxicity.
ADVANCED HEALTHCARE MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Benjamin T. Ledford, Adam W. Akerman, Kui Sun, David C. Gillis, Jenna M. Weiss, Johnny Vang, Smaranda Willcox, Tristan D. Clemons, Hiroaki Sai, Ruomeng Qiu, Mark R. Karver, Jack D. Griffith, Nick D. Tsihlis, Samuel Stupp, John S. Ikonomidis, Melina R. Kibbe
Summary: This study reports the development of injectable supramolecular nanofibers that target fragmented elastin, matrix metalloproteinase 2, and membrane type 1 matrix metalloproteinase to reduce the risks associated with a ruptured abdominal aortic aneurysm. The results show that one of the nanofibers was able to better localize to the aneurysm tissue and had an optimal dose.
Article
Polymer Science
Alexander W. Fortenberry, Penelope E. Jankoski, Evan K. Stacy, Charles L. McCormick, Adam E. Smith, Tristan D. Clemons
Summary: Reversible addition-fragmentation chain transfer (RAFT) polymerization is a powerful polymerization technique, suitable for water as a solvent, with the ability to control molecular weight, molecular weight distribution, and structure. Combining water as a non-toxic, cheap, and environmentally friendly solvent with RAFT polymerization yields powerful potential in polymer science.
MACROMOLECULAR RAPID COMMUNICATIONS
(2022)
Article
Multidisciplinary Sciences
Nutan Chaudhari, Alison Findlay, Andrew Stevenson, Tristan Clemons, Yimin Yao, Amar Joshi, Sepidar Sayyar, Gordon Wallace, Suzanne Rea, Priyanka Toshniwal, Zhenjun Deng, Philip Melton, Nicole Hortin, Swaminatha Iyer, Wolfgang Jarolimek, Fiona Wood, Mark Fear
Summary: Scarring is a lifelong consequence of skin injury. This study develops a topical drug that reduces collagen stability and improves scar appearance and stiffness in preclinical models.
NATURE COMMUNICATIONS
(2022)
Correction
Multidisciplinary Sciences
Nutan Chaudhari, Alison D. Findlay, Andrew W. Stevenson, Tristan D. Clemons, Yimin Yao, Amar Joshi, Sepidar Sayyar, Gordon Wallace, Suzanne Rea, Priyanka Toshniwal, Zhenjun Deng, Philip E. Melton, Nicole Hortin, K. Swaminathan Iyer, Wolfgang Jarolimek, Fiona M. Wood, Mark W. Fear
NATURE COMMUNICATIONS
(2023)
Article
Nanoscience & Nanotechnology
Ruomeng Qiu, Feng Chen, Zaida Alvarez, Tristan D. Clemons, Suvendu Biswas, Mark R. Karver, Nozomu Takata, Hiroaki Sai, Han Peng, Steven Weigand, Liam C. Palmer, Samuel I. Stupp
Summary: This study reports a method that blocks the interaction between SARS-CoV-2 and ACE2 by displaying ACE2 sequence on the surface of supramolecular nanofibers, offering promising therapeutic opportunities to prevent viral infection. The results demonstrate that this method maintains the secondary structure of ACE2 and blocks the entry of pseudovirus and its variants into human cells, while enhancing the chemical stability of bioactive structures in the supramolecular environment. These findings reveal the unique advantages of supramolecular peptide therapies for preventing viral infections and other targets.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Multidisciplinary
Cara S. Smith, Zaida Alvarez, Ruomeng Qiu, Ivan R. Sasselli, Tristan Clemons, J. Alberto Ortega, Marcos Vilela-Picos, Haley Wellman, Evangelos Kiskinis, Samuel I. Stupp
Summary: This study reports the development of a nanofiber-shaped supramolecular mimetic of a neurotrophic factor, Netrin-1, which can promote neuronal growth and synaptogenesis through the activation of DCC receptors. The results suggest the potential use of this supramolecular structure as a therapeutic approach for promoting regenerative bioactivity in central nervous system injuries.
Article
Polymer Science
Farbod Shirinichi, Chetna Karkera, Tarek Ibrahim, Hayat Khan, Tristan Clemons, Alireza G. Senejani, Hao Sun
Summary: This study presents a new class of near-infrared-sensitive nanoparticles by conjugating indocyanine green (ICG) to glycogen. The resulting ICG-glycogen conjugates imbue the ICG with two critical properties otherwise not inherent to the free ICG: significantly enhanced hydrolytic stability and improved cellular uptake. These unique properties of ICG-glycogen conjugates lead to an improved NIR-triggered anti-cancer performance in breast cancer cells.
MACROMOLECULAR CHEMISTRY AND PHYSICS
(2023)
Article
Chemistry, Physical
Hannah G. Abernathy, Jhinuk Saha, Lisa K. Kemp, Parvesh Wadhwani, Tristan D. Clemons, Sarah E. Morgan, Vijayaraghavan Rangachari
Summary: Proteinaceous amyloids have important roles in pathology and are also key components in biological functions. Amyloid fibers have robust enzymatic and structural stabilities due to their ability to form tightly packed conformations. Understanding the sensitivity of peptide sequence to subtle changes is crucial for designing customizable amyloid nanomaterials. Small changes in the sequence can affect the aggregation and nanomechanical properties of the fibrils formed by the amyloid peptides. Therefore, considering the tolerance of amyloid peptides to sequence changes is essential for effective design of customizable amyloid nanomaterials.
Article
Chemistry, Multidisciplinary
Chuang Li, Qinsi Xiong, Tristan D. D. Clemons, Hiroaki Sai, Yang Yang, M. Hussain Sangji, Aysenur Iscen, Liam C. C. Palmer, George C. C. Schatz, Samuel I. I. Stupp
Summary: Supramolecular-covalent hybrid polymers are interesting systems to generate robotic functions in soft materials in response to external stimuli. Recent work found that supramolecular components enhance the speed of reversible bending deformations and locomotion when exposed to light. This study reports on supramolecular-covalent hybrid materials that incorporate high-aspect-ratio peptide amphiphile (PA) ribbons and fibers, or low-aspect-ratio spherical peptide amphiphile micelles into photo-active spiropyran polymeric matrices. Molecular dynamics simulations show that the high-aspect-ratio supramolecular polymers effectively facilitate the transport of trapped water molecules by functioning as channels and therefore enhancing actuation of the hybrid system.
Article
Pharmacology & Pharmacy
Erica B. Peters, Mark R. Karver, Kui Sun, David C. Gillis, Suvendu Biswas, Tristan D. Clemons, Wenhan He, Nick D. Tsihlis, Samuel I. Stupp, Melina R. Kibbe
Summary: This study developed targeted self-assembled peptide amphiphile (PA) nanofibers that can respond to biochemical cues in atherosclerotic lesions to deliver a liver X receptor agonist (LXR) for enhancing macrophage cholesterol efflux. The PA nanofibers were shown to promote cholesterol efflux from macrophages in vitro with lower cytotoxicity, and target plaque within an atherosclerotic mouse model in vivo, demonstrating their potential for controlled therapeutic delivery to the atherosclerotic niche.
ADVANCED THERAPEUTICS
(2021)
