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...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 geochem展开更多
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 de...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.展开更多
After the investigation on partial remelting of thixotropic magnesium serial alloys (ZK60) by near non-equilibrium liquidus casting (NNLC), the primary solid grains of ZK60-2Ca alloy spheroidized notably during pa...After the investigation on partial remelting of thixotropic magnesium serial alloys (ZK60) by near non-equilibrium liquidus casting (NNLC), the primary solid grains of ZK60-2Ca alloy spheroidized notably during partial remelting processing, however, coarsening and polygonization as occurred holding time prolonged. The refining and globularity of the thixotropic alloys are promoted after further alloyed by Y, RE, Nd and/or Ag, and the results vary with those addition. The remelting structure of ZK60-2Ca-1Y alloy is finer than its base alloy. And the effect of RE, especially Ag, on the refinement of microstrueture is notable, but Nd does nothing on it. There is little impact of remelting temperature fluctuation on partial remelted microstrueture as holding time in general. On the contrary, it is more sensitive at longer holding time. The quality thixotropic silver-contained alloy can be achieved by remelted partially at 600℃ for 10 min.展开更多
基金partially supported by U.S. National Science Foundation grants EAR-2221907partly sponsored by agencies of the United States Government。
文摘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 geochem
基金supported by the National Natural Science Foundation of China (22125101)the fellowship of the China Postdoctoral Science Foundation Funded Project (2020M680193)the China Postdoctoral Science Special Foundation Funded Project (2021T140008)
文摘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.
文摘After the investigation on partial remelting of thixotropic magnesium serial alloys (ZK60) by near non-equilibrium liquidus casting (NNLC), the primary solid grains of ZK60-2Ca alloy spheroidized notably during partial remelting processing, however, coarsening and polygonization as occurred holding time prolonged. The refining and globularity of the thixotropic alloys are promoted after further alloyed by Y, RE, Nd and/or Ag, and the results vary with those addition. The remelting structure of ZK60-2Ca-1Y alloy is finer than its base alloy. And the effect of RE, especially Ag, on the refinement of microstrueture is notable, but Nd does nothing on it. There is little impact of remelting temperature fluctuation on partial remelted microstrueture as holding time in general. On the contrary, it is more sensitive at longer holding time. The quality thixotropic silver-contained alloy can be achieved by remelted partially at 600℃ for 10 min.