Design of Microstructure-Engineered Polymers for Energy and Environmental Conservation

Yang, Xue; Cao, Mengxue; Chen, Charles; Zhong, Mingjiang

doi:10.1021/jacsau.3c00081

Cited by 11 publications

(3 citation statements)

References 275 publications

(415 reference statements)

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“…Among the diverse topological polymers, hyperbranched polymers, including hyperbranched polyesters (HBPEs), have garnered considerable interest due to their distinctive 3D globular structures, intriguing physical and chemical properties, and abundant functional end groups. − ,− Unlike their perfectly symmetrical counterparts, dendrimers, , hyperbranched polymers can be produced on a commercially viable scale using a streamlined one-step process while preserving key features of dendrimers, such as excellent solubility, low solution/melt viscosity (which facilitates processing), and a high degree of functionality. These attributes render them appealing for various biological applications such as drug delivery, tissue engineering, and bioimaging. − , Furthermore, branching is a pervasive and crucial phenomenon that can lead to accelerated, more efficient transfer, dissipation, and distribution of energy or matter …”

Section: Introductionmentioning

confidence: 99%

Topology-Accelerated and Selective Cascade Depolymerization of Architecturally Complex Polyesters

Shi,

Rorrer,

Shaw

et al. 2024

J. Am. Chem. Soc.

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Despite considerable recent advances already made in developing chemically circular polymers (CPs), the current framework predominantly focuses on CPs with linear-chain structures of different monomer types. As polymer properties are determined by not only composition but also topology, manipulating the topology of the single-monomer-based CP systems from linear-chain structures to architecturally complex polymers could potentially modulate the resulting polymer properties without changing the chemical composition, thereby advancing the concept of monomaterial product design. To that end, here, we introduce a chemically circular hyperbranched polyester (HBPE), synthesized by a mixed chain-growth and stepgrowth polymerization of a rationally designed bicyclic lactone with a pendent hydroxyl group (BiL OH ). This HBPE exhibits full chemical recyclability despite its architectural complexity, showing quantitative selectivity for regeneration of BiL OH , via a unique cascade depolymerization mechanism. Moreover, distinct differences in materials properties and performance arising from topological variations between HBPE, hb-PBiL OH , and its linear analogue, l-PBiL OH , have been revealed where generally the branched structure led to more favorable interchain interactions, and topologyamplified optical activity has also been observed for chiral (1S, 4S, 5S)-hb-PBiL OH . More intriguingly, depolymerization of l-PBiL OH proceeds through an unexpected, initial topological transformation to the HBPE polymer, followed by the faster cascade depolymerization pathway adopted by hb-PBiL OH . Overall, these results demonstrate that CP design can go beyond typical linear polymers, and rationally redesigned, architecturally complex polymers for their unique properties may synergistically impart advantages in topology-augmented depolymerization acceleration and selectivity for exclusive monomer regeneration.

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Section: Introductionmentioning

confidence: 99%

Topology-Accelerated and Selective Cascade Depolymerization of Architecturally Complex Polyesters

Shi,

Rorrer,

Shaw

et al. 2024

J. Am. Chem. Soc.

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“…They are stacked together by weak van der Waals forces. MoS 2 /C with monolayers has been proven to be a promising material for a wide range of energy storage applications including supercapacitors (SCs) and secondary batteries. − SCs combine the technical characteristics of common capacitors and secondary batteries, providing higher specific energy than common capacitors, higher specific power than secondary batteries, and longer cycle life. − For example, Han et al designed an independent core–shell heterostructure supported on carbon nanotube fibers by anchoring MoS 2 nanosheets on nanowires (MoS 2 @TiN/CNTF) as the anode of AASCs, which has great advantages in wearable water-based SCs. Abbas et al reported “one-step” liquid phase coexfoliation of graphene (G) and MoS 2 together, i.e., graphene nanoplatelet (GNP)/MoS 2 using high-temperature ultrasonication and gelatin.…”

Section: Introductionmentioning

confidence: 99%

Mesoporous Iron Family Element (Fe, Co, Ni) Molybdenum Disulfide/Carbon Nanohybrids for High-Performance Supercapacitors

Yao,

Zhang,

Zhang

et al. 2023

Inorg. Chem.

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As the demand for fuel continues to increase, the development of energy devices with excellent performance is crucial. Supercapacitors (SCs) are attracting attention for their advantages of high specific energy and a long cycle life. At present, the development of high-performance electrode materials is the main point for research and development of SCs. Transition metal sulfides have the advantages of a large interlayer space and high theoretical capacity, making them promising electrode materials. Herein, we reported a series of ultrathin mesoporous iron family element (Fe, Co, Ni) molybdenum disulfide (M x Mo 1−x S 2 /C, M = Fe, Co, and Ni) by a template method. The original monolayer mesoporous structure of MoS 2 /C was maintained, and accumulation and agglomeration of MoS 2 /C were avoided. Based on our investigations, the best performance was that of Co x Mo 1−x S 2 /C nanohybrids. Furthermore, the concentrations of Co and Mo ions were modulated to obtain the best performance, in which Mo and Co ions were released at 1:1, 1:2, and 1:3 ratios and they were named Co x Mo 1−x S 2 /C-1, Co x Mo 1−x S 2 /C-2, and Co x Mo 1−x S 2 /C-3, respectively. Overall, these materials represent a significant improvement and show promise as high-performance SC electrode materials due to their enhanced capacitance and stability. At a current density of 0.5 A g −1 , Co x Mo 1−x S 2 /C-2 has the optimal specific capacitance of 184 F g −1 . Co x Mo 1−x S 2 /C-2 as an SC electrode exhibited better reversible capacity and cycling stability than MoS 2 /C, which is an improvement over MoS 2 /C regarding reversible capacity and cycling stability.

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“…In recent decades, reversible-deactivation radical polymerization (RDRP) has revolutionized polymerization techniques by introducing a reversible activation/deactivation step into radical polymerization, − among which nitroxide-mediated polymerization (NMP), atom transfer radical polymerization (ATRP), , and reversible addition–fragmentation chain transfer (RAFT) polymerization are the three most frequently used ones. Several other RDRP systems have also been developed, which share similar kinetic behaviors with NMP, ATRP, or RAFT polymerizations, for example, organometallic-mediated radical polymerization (OMRP), organotellurium-mediated radical polymerization (TERP), and iodine transfer polymerization (ITP). , RDRP allows the precision synthesis of polymers with predictable M n and low Đ (<1.5) at gentler conditions than that of LAP, , and the manipulation of Đ is a significant topic for probing the dispersity–property relationships of the polymer materials in the RDRP community. ,, …”

Section: Introductionmentioning

confidence: 99%

Beauty of Explicit Dispersity (Đ) Equations in Controlled Polymerizations

Wang,

Zhou,

Luo

et al. 2023

ACS Macro Lett.

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Dispersity (Đ) as a critical parameter indicates the level of uniformity of the polymer molar mass or chain length. In the past several decades, the development of explicit equations for calculating Đ experiences a continual revolution. This viewpoint tracks the historical evolution of the explicit equations from living to reversible-deactivation polymerization systems. Emphasis is laid on displaying the charm of explicit Đ equations in batch reversible-deactivation radical polymerization (RDRP), with highlights of the relevant elegant mathematical manipulations. Some representative emerging applications enabled by the existing explicit equations are shown, involving nitroxide-mediated polymerization (NMP), atom transfer radical polymerization (ATRP), and reversible addition–fragmentation chain transfer (RAFT) polymerization systems. Stemming from the several outlined challenges and outlooks, sustained concerns about the explicit Đ equations are still highly deserved. It is expected that these equations will continue to play an important role not only in traditional polymerization kinetic simulation and design of experiments but also in modern intelligent manufacturing of precision polymers and classroom education.

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Design of Microstructure-Engineered Polymers for Energy and Environmental Conservation

Cited by 11 publications

References 275 publications

Topology-Accelerated and Selective Cascade Depolymerization of Architecturally Complex Polyesters

Topology-Accelerated and Selective Cascade Depolymerization of Architecturally Complex Polyesters

Mesoporous Iron Family Element (Fe, Co, Ni) Molybdenum Disulfide/Carbon Nanohybrids for High-Performance Supercapacitors

Beauty of Explicit Dispersity (Đ) Equations in Controlled Polymerizations

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