ACS polymers Au最新文献

{"title":"Plasticization of a Semicrystalline Metallosupramolecular Polymer Network","authors":"Franziska Marx,&nbsp;Subhajit Pal,&nbsp;Julien Sautaux,&nbsp;Nazim Pallab,&nbsp;Grégory Stoclet,&nbsp;Christoph Weder* and Stephen Schrettl*,&nbsp;","doi":"10.1021/acspolymersau.2c00044","DOIUrl":"10.1021/acspolymersau.2c00044","url":null,"abstract":"<p >The assembly of ligand-functionalized (macro)monomers with suitable metal ions affords metallosupramolecular polymers (MSPs). On account of the reversible and dynamic nature of the metal–ligand complexes, these materials can be temporarily (dis-)assembled upon exposure to a suitable stimulus, and this effect can be exploited to heal damaged samples, to facilitate processing and recycling, or to enable reversible adhesion. We here report on the plasticization of a semicrystalline, stimuli-responsive MSP network that was assembled by combining a low-molecular-weight building block carrying three 2,6-bis(1′-methylbenzimidazolyl) pyridine (Mebip) ligands and zinc bis(trifluoromethylsulfonyl)imide (Zn(NTf₂)₂). The pristine material exhibits high melting (<i>T</i>_m = 230 °C) and glass transition (<i>T</i>_g ≈ 157 °C) temperatures and offers robust mechanical properties between these temperatures. We show that this regime can be substantially extended through plasticization. To achieve this, the MSP network was blended with diisodecyl phthalate. The weight fraction of this plasticizer was systematically varied, and the thermal and mechanical properties of the resulting materials were investigated. We show that the <i>T</i>_g can be lowered by more than 60 °C and the toughness above the <i>T</i>_g is considerably increased.</p>","PeriodicalId":72049,"journal":{"name":"ACS polymers Au","volume":"3 1","pages":"132–140"},"PeriodicalIF":0.0,"publicationDate":"2022-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acspolymersau.2c00044","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"10773343","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Self-Healing Thermosensitive Hydrogel for Sustained Release of Dexamethasone for Ocular Therapy","authors":"Ada Annala,&nbsp;Blessing C. Ilochonwu,&nbsp;Danny Wilbie,&nbsp;Amir Sadeghi,&nbsp;Wim E. Hennink and Tina Vermonden*,&nbsp;","doi":"10.1021/acspolymersau.2c00038","DOIUrl":"10.1021/acspolymersau.2c00038","url":null,"abstract":"<p >The aim of this study was to develop an injectable hydrogel delivery system for sustained ocular delivery of dexamethasone. To this end, a self-healing hydrogel consisting of a thermosensitive ABA triblock copolymer was designed. The drug was covalently linked to the polymer by copolymerization of methacrylated dexamethasone with <i>N</i>-isopropylacrylamide (NIPAM) and <i>N</i>-acryloxysuccinimide (NAS) through reversible addition–fragmentation chain transfer (RAFT) polymerization, using poly(ethylene glycol) (PEG) functionalized at both ends with a chain transfer agent (CTA). Hydrogel formation was achieved by mixing aqueous solutions of the formed thermosensitive polymer (with a cloud point of 23 °C) with cystamine at 37 °C, to result in covalent cross-linking due to the reaction of the <i>N</i>-hydroxysuccimide (NHS) functionality of the polymer and the primary amines of cystamine. Rheological analysis showed both thermogelation and covalent cross-linking at 37 °C, as well as the self-healing properties of the formed network, which was attributed to the presence of disulfide bonds in the cystamine cross-links, making the system injectable. The release of dexamethasone from the hydrogel occurred through ester hydrolysis following first-order kinetics in an aqueous medium at pH 7.4 over 430 days at 37 °C. Based on simulations, administration of 100 mg of hydrogel would be sufficient for maintaining therapeutic levels of dexamethasone in the vitreous for at least 500 days. Importantly, dexamethasone was released from the hydrogel in its native form as determined by LC–MS analysis. Cytocompatibility studies showed that at clinically relevant concentrations, both the polymer and the cross-linker were well tolerated by adult retinal pigment epithelium (ARPE-19) cells. Moreover, the hydrogel did not show any toxicity to ARPE-19 cells. The injectability of the hydrogel, together with the long-lasting release of dexamethasone and good cytocompatibility with a retinal cell line, makes this delivery system an attractive candidate for treatment of ocular inflammatory diseases.</p>","PeriodicalId":72049,"journal":{"name":"ACS polymers Au","volume":"3 1","pages":"118–131"},"PeriodicalIF":0.0,"publicationDate":"2022-11-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://ftp.ncbi.nlm.nih.gov/pub/pmc/oa_pdf/f4/2a/lg2c00038.PMC9912331.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"9267589","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"There is Signal in Your Noise: A Case for Advanced Mass Analysis","authors":"Benjamin A. Suslick*,&nbsp;Harm-Anton Klok and Jeffrey S. Moore,&nbsp;","doi":"10.1021/acspolymersau.2c00057","DOIUrl":"10.1021/acspolymersau.2c00057","url":null,"abstract":"■ WHY WE NEED NEW ANALYTICAL TOOLS Synthetic chemists often take modern characterization techniques for granted and do not appreciate the fortuitous process of analytical development. Imagine yourself as a 1950s chemist without easy access to spectroscopic instrumentation: how would you unambiguously assign chemical structures to small molecules? This question fueled an explosive growth of technologies that provide molecule-specific fingerprints. The advent of classical characterization tools (e.g., NMR spectroscopy, mass spectrometry) accelerated the rate of discovery in organic chemistry as they provide sufficient information to deduce the identity and purity of a sample. In the context of polymer synthesis, however, these classical tools only provide insights related to bulk composition and often fail to fully capture terminal group speciation. As an unintended consequence, many graphical representations omit the chainends. Despite the lack of comprehensive knowledge, ambitious research programs have sparked a renaissance of renewed interest in developing new analytical methodologies. Postpolymerization reactions, for example, often exploit end-groups for practical applications (e.g., upcycling, dynamic network cross-linking). A need, therefore, exists for new tools that uncover currently elusive structural details. Advanced mass analysis has begun to reemerge as an effective solution to these problems. While the initial development of Kendrick analysis dates to the early 1960s, only recent work from Fouquet and co-workers developed the tools necessary for adaptation to polymer characterization. The power of this mass spectral method is readily apparent in Figure 1. Signals are elegantly pulled from the noise in a traditional mass spectrum by deconvoluting the data and rendering it across multiple dimensions. The resultant Kendrick plot extracts compositional information within a homologous series of polymers. Despite its obvious utility, Kendrick analysis has not yet received the attention it deserves nor is it a common-place technique. Indeed, synthetic polymer chemists are often unaware of its existence despite routinely acquiring mass spectra (e.g., MALDI). Indeed, we only learned of Kendrick analysis from an enlightening tutorial by Fouquet entitled “The Kendrick analysis for polymer mass spectrometry”. Our serendipitous introduction to this technique occurred while we were characterizing complex mixtures of oligomers derived from dicyclopentadiene (DCPD). Monomer resins with the second generation Grubbs catalyst (G2, [(SIMes)Ru(�CHPh)(PCy3)Cl2]) produced short chain oligomers when in the presence of a chain-transfer agent (CTA; e.g., styrene). Traditional characterization techniques approximated the molecular weights of the resultant materials but did not report on the chain-end speciation or fate of the pendent cyclopentene groups. While the MALDI pattern revealed the existence of multiple species, only Kendrick analysis provided defini","PeriodicalId":72049,"journal":{"name":"ACS polymers Au","volume":"2 6","pages":"392–396"},"PeriodicalIF":0.0,"publicationDate":"2022-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://ftp.ncbi.nlm.nih.gov/pub/pmc/oa_pdf/f6/bd/lg2c00057.PMC9954250.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"9363064","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"N-Coordinated Organoboron in Polymer Synthesis and Material Science","authors":"Congze He,&nbsp;Jin Dong,&nbsp;Chaoran Xu and Xiangcheng Pan*,&nbsp;","doi":"10.1021/acspolymersau.2c00046","DOIUrl":"10.1021/acspolymersau.2c00046","url":null,"abstract":"<p >Organoboron chemistry has been widely explored and developed in synthetic chemistry for over half a century and provides various elegant synthetic protocols in polymer synthesis. Compared with most trivalent bare organoboron compounds, N-coordinated organoboron shows better performances, such as air and moisture stability. This review summarizes the application of various N-coordinated boranes and boronic acid/esters in polymer synthesis and materials science. We introduce the significance of N-coordinated boranes and boronate esters for controllable polymer synthesis and systematically summarize the structures and properties of polymers containing N-coordinated boronate esters. Furthermore, we highlight the effect of N→B dative bonds on improving the performance of self-healing materials. We hope that, through this review, more researchers will realize the advantages of N-coordinated organoboron and promote the development of this direction in polymer synthesis and materials science.</p>","PeriodicalId":72049,"journal":{"name":"ACS polymers Au","volume":"3 1","pages":"5–27"},"PeriodicalIF":0.0,"publicationDate":"2022-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acspolymersau.2c00046","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"47847039","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Multiscale Modeling of Grain-Boundary Motion in Cylinder-Forming Block Copolymers","authors":"Niklas Blagojevic,&nbsp; and ,&nbsp;Marcus Müller*,&nbsp;","doi":"10.1021/acspolymersau.2c00048","DOIUrl":"10.1021/acspolymersau.2c00048","url":null,"abstract":"<p >Using the combination of a soft, coarse-grained, particle-based model, a free-energy functional that depends on the local composition, and a lattice model of local, metastable states, we study the structure and motion of a grain boundary between two orthogonal grains of cylindrical domains in asymmetric block copolymers. The particle-based model provides direct insights into the elementary class of transitions of the self-assembled morphology in the course of grain-boundary translation. These processes are correlated in space and time. We identify a minimal set of transitions, whose free-energy changes and barriers are obtained by describing the system by a free-energy functional of the local composition and calculating the minimum free-energy path (MFEP). The spatiotemporal correlation arises from the dependence of the free-energy characteristics on the local environment. We use this information to parametrize a lattice model of the correlated processes in the course of grain-boundary motion. This allows us to investigate the grain-boundary motion by kinetic Monte Carlo (kMC) simulation and determine its free-energy landscape. Grain-boundary motion proceeds by nucleating a two-dimensional, anisotropic cluster inside the plane of the grain boundary.</p>","PeriodicalId":72049,"journal":{"name":"ACS polymers Au","volume":"3 1","pages":"96–117"},"PeriodicalIF":0.0,"publicationDate":"2022-10-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acspolymersau.2c00048","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"42535749","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Greener Synthesis Route for Furanic-Aliphatic Polyester: Enzymatic Polymerization in Ionic Liquids and Deep Eutectic Solvents","authors":"Fitrilia Silvianti,&nbsp;Dina Maniar,&nbsp;Laura Boetje,&nbsp;Albert J. J. Woortman,&nbsp;Jur van Dijken and Katja Loos*,&nbsp;","doi":"10.1021/acspolymersau.2c00035","DOIUrl":"10.1021/acspolymersau.2c00035","url":null,"abstract":"<p >The development of bio-based polymers is growing not only due to their abundance in nature but also mainly because of the current issues with fossil-based plastics. Enzymatic polymerizations are a promising way to produce such polymers since they are known to be environmentally friendly. Sustainable polymers that require a greener production process can be realized easily via this polymerization route. However, the use of organic solvents is often one of the drawbacks in developing pathways toward fully green enzymatic polymerization methods. Therefore, in the present work, a series of fully bio-based polyesters based on 2,5-furandicarboxylic acid (FDCA), namely, furanic-aliphatic polyesters (FPEs), were enzymatically synthesized using greener solvents, such as ionic liquids (ILs) and deep eutectic solvents (DESs). The enzymatic polymerization in ILs and DESs effectively leads to the FDCA-based polyesters without any byproduct, which frequently causes coloration using traditional polymerization methods. FPEs with M_w up to 5.4 kg mol^–1 were successfully achieved by Novozyme 435-catalyzed polycondensation of dimethyl 2,5-furandicarboxylate (DMFDCA) with aliphatic diols in BMIMPF₆. Polymerization in DESs was also successfully conducted, resulting in the synthesis of bio-based polyesters, which can be further functionalized. Characterization using TGA, DSC, and WAXD showed that all obtained FPEs are semi-crystalline materials, which decomposed around 390 °C with a <i>T</i>_m of 68–123 °C and <i>T</i>_g of 3–12 °C. With this, we successfully developed more eco-friendly enzymatic synthesis routes for the production of sustainable polyesters</p>","PeriodicalId":72049,"journal":{"name":"ACS polymers Au","volume":"3 1","pages":"82–95"},"PeriodicalIF":0.0,"publicationDate":"2022-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acspolymersau.2c00035","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"45527877","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Canonicalizing BigSMILES for Polymers with Defined Backbones","authors":"Tzyy-Shyang Lin,&nbsp;Nathan J. Rebello,&nbsp;Guang-He Lee,&nbsp;Melody A. Morris and Bradley D. Olsen*,&nbsp;","doi":"10.1021/acspolymersau.2c00009","DOIUrl":"10.1021/acspolymersau.2c00009","url":null,"abstract":"<p >BigSMILES, a line notation for encapsulating the molecular structure of stochastic molecules such as polymers, was recently proposed as a compact and readable solution for writing macromolecules. While BigSMILES strings serve as useful identifiers for reconstructing the molecular connectivity for polymers, in general, BigSMILES allows the same polymer to be codified into multiple equally valid representations. Having a canonicalization scheme that eliminates the multiplicity would be very useful in reducing time-intensive tasks like structural comparison and molecular search into simple string-matching tasks. Motivated by this, in this work, two strategies for deriving canonical representations for linear polymers are proposed. In the first approach, a canonicalization scheme is proposed to standardize the expression of BigSMILES stochastic objects, thereby standardizing the expression of overall BigSMILES strings. In the second approach, an analogy between formal language theory and the molecular ensemble of polymer molecules is drawn. Linear polymers can be converted into regular languages, and the minimal deterministic finite automaton uniquely associated with each prescribed language is used as the basis for constructing the unique text identifier associated with each distinct polymer. Overall, this work presents algorithms to convert linear polymers into unique structure-based text identifiers. The derived identifiers can be readily applied in chemical information systems for polymers and other polymer informatics applications.</p>","PeriodicalId":72049,"journal":{"name":"ACS polymers Au","volume":"2 6","pages":"486–500"},"PeriodicalIF":0.0,"publicationDate":"2022-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://ftp.ncbi.nlm.nih.gov/pub/pmc/oa_pdf/aa/f3/lg2c00009.PMC9761857.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"10421521","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Dithiol-yne Polymerization: Comb Polymers with Poly(ethylene glycol) Side chains","authors":"Brennan J. Curole,&nbsp;William J. Broussard,&nbsp;Amman Nadeem and Scott M. Grayson*,&nbsp;","doi":"10.1021/acspolymersau.2c00045","DOIUrl":"10.1021/acspolymersau.2c00045","url":null,"abstract":"<p >Recently dithiol-yne click chemistry and its role in the formation of cross-linked polymer networks and postpolymerization functionalizations has been studied; however, no research has considered this technique to form comb polymers with regular side chains. Here we report the first example of a grafted-through step-growth comb polymer via the utilization of dithiol-yne “click chemistry”. First, we exhibited the efficacy of this reaction to produce modest-molecular-weight combs (<i>M</i>_n = 16 kDa). Second, we displayed the ability to precisely control the length of the side chains of these combs along with the space between the side chains by using various molecular weights of propargylated PEG chains and a variety of alkanedithiol backbone spacers. The primary species of these reactions were macrocyclic comb polymers, with a smaller amount of dithiol-terminated comb polymers.</p>","PeriodicalId":72049,"journal":{"name":"ACS polymers Au","volume":"3 1","pages":"70–81"},"PeriodicalIF":0.0,"publicationDate":"2022-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acspolymersau.2c00045","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"44603868","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Influence of Side Chain Interdigitation on Strain and Charge Mobility of Planar Indacenodithiophene Copolymers","authors":"Parker J. W. Sommerville,&nbsp;Alex H. Balzer,&nbsp;Garrett Lecroy,&nbsp;Lorenzo Guio,&nbsp;Yunfei Wang,&nbsp;Jonathan W. Onorato,&nbsp;Nadzeya A. Kukhta,&nbsp;Xiaodan Gu,&nbsp;Alberto Salleo,&nbsp;Natalie Stingelin and Christine K. Luscombe*,&nbsp;","doi":"10.1021/acspolymersau.2c00034","DOIUrl":"10.1021/acspolymersau.2c00034","url":null,"abstract":"<p >Indacenodithiophene (IDT) copolymers are a class of conjugated polymers that have limited long-range order and high hole mobilities, which makes them promising candidates for use in deformable electronic devices. Key to their high hole mobilities is the coplanar monomer repeat units within the backbone. Poly(indacenodithiophene-benzothiadiazole) (PIDT_C16-BT) and poly(indacenodithiophene-thiapyrollodione) (PIDT_C16-TPD_C1) are two IDT copolymers with planar backbones, but they are brittle at low molecular weight and have unsuitably high elastic moduli. Substitution of the hexadecane (C₁₆) side chains of the IDT monomer with isocane (C₂₀) side chains was performed to generate a new BT-containing IDT copolymer: PIDT_C20-BT. Substitution of the methyl (C₁) side chain on the TPD monomer for an octyl (C₈) and 6-ethylundecane (C_13B) afford two new TPD-containing IDT copolymers named PIDT_C16-TPD_C8 and PIDT_C16-TPD_C13B, respectively. Both PIDT_C16-TPD_C8 and PIDT_C16-TPD_C13B are relatively well deformable, have a low yield strain, and display significantly reduced elastic moduli. These mechanical properties manifest themselves because the lengthened side chains extending from the TPD-monomer inhibit precise intermolecular ordering. In PIDT_C16-BT, PIDT_C20-BT and PIDT_C16-TPD_C1 side chain ordering can occur because the side chains are only present on the IDT subunit, but this results in brittle thin films. In contrast, PIDT_C16-TPD_C8 and PIDT_C16-TPD_C13B have disordered side chains, which seems to lead to low hole mobilities. These results suggest that disrupting the interdigitation in IDT copolymers through comonomer side chain extension leads to more ductile thin films with lower elastic moduli, but decreased hole mobility because of altered local order in the respective thin films. Our work, thus, highlights the trade-off between molecular packing structure for deformable electronic materials and provides guidance for designing new conjugated polymers for stretchable electronics.</p>","PeriodicalId":72049,"journal":{"name":"ACS polymers Au","volume":"3 1","pages":"59–69"},"PeriodicalIF":0.0,"publicationDate":"2022-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://ftp.ncbi.nlm.nih.gov/pub/pmc/oa_pdf/db/ef/lg2c00034.PMC9912480.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"9267587","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Decoupling Ion Transport and Matrix Dynamics to Make High Performance Solid Polymer Electrolytes","authors":"Seamus D. Jones,&nbsp;James Bamford,&nbsp;Glenn H. Fredrickson and Rachel A. Segalman*,&nbsp;","doi":"10.1021/acspolymersau.2c00024","DOIUrl":"10.1021/acspolymersau.2c00024","url":null,"abstract":"<p >Transport of ions through solid polymeric electrolytes (SPEs) involves a complicated interplay of ion solvation, ion–ion interactions, ion-polymer interactions, and free volume. Nonetheless, prevailing viewpoints on the subject promote a significantly simplified picture, likening ion transport in a polymer to that in an unstructured fluid at low solute concentrations. Although this idealized liquid transport model has been successful in guiding the design of homogeneous electrolytes, structured electrolytes provide a promising alternate route to achieve high ionic conductivity and selectivity. In this perspective, we begin by describing the physical origins of the idealized liquid transport mechanism and then proceed to examine known cases of decoupling between the matrix dynamics and ionic transport in SPEs. Specifically we discuss conditions for “decoupled” mobility that include a highly polar electrolyte environment, a percolated path of free volume elements (either through structured or unstructured channels), high ion concentrations, and labile ion-electrolyte interactions. Finally, we proceed to reflect on the potential of these mechanisms to promote multivalent ion conductivity and the need for research into the interfacial properties of solid polymer electrolytes as well as their performance at elevated potentials.</p>","PeriodicalId":72049,"journal":{"name":"ACS polymers Au","volume":"2 6","pages":"430–448"},"PeriodicalIF":0.0,"publicationDate":"2022-09-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://ftp.ncbi.nlm.nih.gov/pub/pmc/oa_pdf/c8/e2/lg2c00024.PMC9761859.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"10414093","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}