Mechanical Properties of Interlocked-ring Polymers: A Molecular Dynamics Simulation Study

Wu, Zheng-Tao; Zhou, Jiajia

doi:10.1007/s10118-019-2279-z

Cited by 18 publications

(11 citation statements)

References 17 publications

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“…Due to the huge fossil energy consumption in the past 100 years, the CO 2 concentration in the eath's atmosphere has continued to rise, and now it has exceeded 410 ppm. [ 1,2 ] Knowing that the greenhouse effect is destructive to human society, a group of top scientists proposed some concepts of “liquid sunlight”, [ 3–5 ] “artificial photosynthesis”, [ 6–9 ] and “futuristic solar refinery”. [ 10,11 ] Actually, these concepts essentially follow this formula: CO 2 + water + sunlight = green fuel + oxygen.…”

Section: Introductionmentioning

confidence: 99%

Revealing the Sudden Alternation in Pt@h‐BN Nanoreactors for Nearly 100% CO₂‐to‐CH₄ Photoreduction

Jiang

et al. 2021

Adv Funct Materials

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How to develop an efficient photocatalyst with high activity and high selectivity is the biggest challenge limiting the application of photocatalysis. A reasonable design of the nanoreactor model is an effective strategy. Herein, a series of Pt nanoparticles coated with hexagonal boron nitride (Pt@h-BN) nanoreactors highly dispersed on a photochemically inert carrier, Al 2 O 3 substrate, are synthesized. The results show that as the number of h-BN coating layers increases, the selectivity of photocatalysis is altered from nearly 100% CO 2 -to-CO to nearly 100% CO 2 -to-CH 4 , and the optimized space-time yield of CH 4 is up to 184.7 μmol g (Pt) −1 h −1 with three-layer coating. The in situ characterizations reveal the cleavage of the CO on Pt to be the rate determining step and the existence of the key intermediate CO 2 − species on the surface of Pt@h-BN facilitates CH 4 formation. Notably, combined with detailed simulation calculations, this work reveals that the confinement effect in Pt@h-BN attributes the electrons mobility behavior and alleviate the interaction of COPt. What is more, the change of the reaction site is the essence for the sudden alternation. This work will bring a new insight to the selective catalysis of noble metals in the gas-solid phase.

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Section: Introductionmentioning

confidence: 99%

Revealing the Sudden Alternation in Pt@h‐BN Nanoreactors for Nearly 100% CO₂‐to‐CH₄ Photoreduction

Jiang

et al. 2021

Adv Funct Materials

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“…However, at short length scales, the conformations of the rings within catenanes are strongly affected by the mechanical bonds, which are quantified in terms of the Rouse mode amplitudes. , More specifically, the rings are expanded at large length scales but compressed at smaller ones compared to rings without threadings. Since then, additional simulations were conducted by other researchers also using the KG model, extending the chain lengths up to n = 100 rings. These extremely long poly[ n ]catenanes showed highly unusual structural properties including unexpected scaling behavior and large, long-lived orientational correlations along the chain.…”

Section: Introductionmentioning

confidence: 99%

Thermodynamics and Structure of Poly[n]catenane Melts

et al. 2020

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Motivated by recent achievements in the synthesis of interlocking polymers, the structural features of poly[n]catenanes, polymers composed entirely of interlocking rings (or macrocycles), are studied by extensive molecular dynamics simulations in the melt state. The degree of polymerization (number of links) is varied from n = 1–25 and the number of beads per macrocycle is varied from m = 15–50; the results are compared to linear chains of degrees of polymerization N = 15–175. The mechanical bonds in the system cause significant topological contributions to the pressure and potential energy density not seen in other polymer systems. The polymers themselves possess many unusual structural features at short and intermediate length scales, which can be attributed to density inhomogeneities along the polymer contour. Furthermore, the conformations of the individual macrocycles within poly[n]catenanes are quite different from those of ordinary ring polymers and depend on the topology of the macrocycle, that is, whether it is threaded by one ring (chain end) or two (chain center). At larger length scales, the poly[n]catenanes are conformationally similar to ideal linear chains, but unlike traditional (covalent) polymers, they are highly globular at low degrees of polymerization and are extremely flexible relative to their size, which inhibits interchain entanglement. Implications for poly[n]catenane material properties and synthesis are discussed.

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“…The increasing CO 2 emissions due to the over‐consumption of fossil fuels have resulted in the deterioration of environment [1,2] . As a promising way to mitigate environmental challenges, electroreduction of CO 2 has attracted a huge amount of attention [3,4] .…”

Section: Introductionmentioning

confidence: 99%

DFT‐based Machine Learning for Ensemble Effect of Pd@Au Electrocatalysts on CO₂ Reduction Reaction

Liu

Gao

et al. 2023

ChemPhysChem

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The ensemble effect due to variation of Pd content in Pd−Au alloys have been widely investigated for several important reactions, including CO2 reduction reaction (CO2RR), however, identifying the stable Pd arrangements on the alloyed surface and picking out the active sites are still challenging. Here we use a density functional theory (DFT) based machine‐learning (ML) approach to efficiently find the low‐energy configurations of Pd−Au(111) surface alloys and the potentially active sites for CO2RR, fully covering the Pd content from 0 to 100 %. The ML model is actively learning process to improve the predicting accuracy for the configuration formation energy and to find the stable Pd−Au(111) alloyed surfaces, respectively. The local surface properties of adsorption sites are classified into two classes by the K‐means clustering approach, which are closely related to the Pd content on Au surface. The classification is reflected in the variation of adsorption energy of CO and H: In the low Pd content range (0–60 %) the adsorption energies over the surface alloys can be tuned significantly, and in the medium Pd content (37‐68 %), the catalytic activity of surface alloys for CO2RR can be increased by increase the Pd content and attributed to the meta‐stable active site over the surface. Thus, the active site‐dependent reaction mechanism is elucidated based on the ensemble effect, which provides new physical insights to understand the surface‐related properties of catalysts.

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Mechanical Properties of Interlocked-ring Polymers: A Molecular Dynamics Simulation Study

Cited by 18 publications

References 17 publications

Revealing the Sudden Alternation in Pt@h‐BN Nanoreactors for Nearly 100% CO₂‐to‐CH₄ Photoreduction

Revealing the Sudden Alternation in Pt@h‐BN Nanoreactors for Nearly 100% CO₂‐to‐CH₄ Photoreduction

Thermodynamics and Structure of Poly[n]catenane Melts

DFT‐based Machine Learning for Ensemble Effect of Pd@Au Electrocatalysts on CO₂ Reduction Reaction

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Mechanical Properties of Interlocked-ring Polymers: A Molecular Dynamics Simulation Study

Cited by 18 publications

References 17 publications

Revealing the Sudden Alternation in Pt@h‐BN Nanoreactors for Nearly 100% CO2‐to‐CH4 Photoreduction

Revealing the Sudden Alternation in Pt@h‐BN Nanoreactors for Nearly 100% CO2‐to‐CH4 Photoreduction

Thermodynamics and Structure of Poly[n]catenane Melts

DFT‐based Machine Learning for Ensemble Effect of Pd@Au Electrocatalysts on CO2 Reduction Reaction

Contact Info

Product

Resources

About

Revealing the Sudden Alternation in Pt@h‐BN Nanoreactors for Nearly 100% CO₂‐to‐CH₄ Photoreduction

Revealing the Sudden Alternation in Pt@h‐BN Nanoreactors for Nearly 100% CO₂‐to‐CH₄ Photoreduction

DFT‐based Machine Learning for Ensemble Effect of Pd@Au Electrocatalysts on CO₂ Reduction Reaction