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Recyclable polythioesters and polydisulfides with near-equilibrium thermodynamics and dynamic covalent bonds

Science China Chemistry 2023年第3期66卷 725-738页

作者： Wei Xiong Hua Lu Beijing National Laboratory for Molecular Sciences Center for Soft Matter Science and EngineeringKey Laboratory of Polymer Chemistry and Physics of Ministry of EducationCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China

The accumulation of discarded petroleum-based plastics causes serious environmental crises.Currently,recyclable polymers with neutrality in thermodynamics,such as polyesters,polycarbonates,and polyolefins,have been developed as promising alternatives to traditional petroleum-based polymers.However,the chemical recycle of these polymers usually requires high energy input and expensive catalysts.Dynamic covalent bonds,such as thioester and disulfide bonds,have emerged as building blocks for constructing recyclable polymers that can be rapidly degraded/recycled under mild conditions.In this review,we introduce representative studies on recyclable polythioesters and polydisulfides with respect to their synthetic strategies,thermodynamic manipulation,physicochemical properties,and preliminary applications.We also highlight the important role of kinetic factors played in the design of recyclable polymers.Finally,major challenges,perspectives,and future opportunities in the synthesis and applications of polythioesters/polydisulfides are discussed.

关键词： polythioesters polydisulfides recyclable near-equilibrium thermodynamics dynamic covalent bond

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Geochemical modeling to aid experimental design for multiple isotope tracer studies of coupled dissolution and precipitation reaction kinetics

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Acta Geochimica 2024年第1期43卷 1-15页

作者： Mingkun Chen Peng Lu Yongchen Song Chen Zhu Department of Earth and Atmospheric Sciences Indiana UniversityBloomingtonIN 47405USA School of Energy and Power Engineering Dalian University of TechnologyDalian 116024China EXPEC Advanced Research Center Saudi Aramco31311 DhahranSaudi Arabia

It is a challenge to make thorough but efficient experimental designs for the coupled mineral dissolution and precipitation studies in a multi-mineral system, because it is difficult to speculate the best experimental duration, optimal sampling schedule, effects of different experimental conditions, and how to maximize the experimental outputs prior to the actual experiments. Geochemical modeling is an efficient and effective tool to assist the experimental design by virtually running all scenarios of interest for the studied system and predicting the experimental outcomes. Here we demonstrated an example of geochemical modeling assisted experimental design of coupled labradorite dissolution and calcite and clayey mineral precipitation using multiple isotope tracers. In this study, labradorite(plagioclase) was chosen as the reactant because it is both a major component and one of the most reactive minerals in basalt. Following our isotope doping studies of single minerals in the last ten years, initial solutions in the simulations were doped withmultiple isotopes(e.g., Ca and Si). Geochemical modeling results show that the use of isotope tracers gives us orders of magnitude more sensitivity than the conventional method based on concentrations and allows us to decouple dissolution and precipitation reactions at near-equilibrium condition. The simulations suggest that the precise unidirectional dissolution rates can inform us which rate laws plagioclase dissolution has followed. Calcite precipitation occurred at near-equilibrium and the multiple isotope tracer experiments would provide near-equilibrium precipitation rates, which was a challenge for the conventional concentration-based experiments. In addition, whether the precipitation of clayey phases is the rate-limiting step in some multi-mineral systems will be revealed. Overall, the modeling results of multimineral reaction kinetics will improve the understanding of the coupled dissolution–precipitation in the multi-mineral systems and the quality of geochemic

关键词： Kinetics Feldspar Isotope doping near-equilibrium CO_(2)sequestration Basalt

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