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Creators/Authors contains: "Peng, Zhenmeng"

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  1. Free, publicly-accessible full text available July 1, 2024
  2. Abstract

    The evergrowing plastic production and the caused concerns of plastic waste accumulation have stimulated the need for waste plastic chemical recycling/valorization. Current methods suffer from harsh reaction conditions and long reaction time. Herein we demonstrate a non-thermal plasma-assisted method for rapid hydrogenolysis of polystyrene (PS) at ambient temperature and atmospheric pressure, generating high yield (>40 wt%) of C1–C3hydrocarbons and ethylene being the dominant gas product (Selectivity of ethylene,SC2H4 > 70%) within ~10 min. The fast reaction kinetics is attributed to highly active hydrogen plasma, which can effectively break bonds in polymer and initiate hydrogenolysis under mild condition. Efficient hydrogenolysis of post-consumer PS materials using this method is also demonstrated, suggesting a promising approach for fast retrieval of small molecular hydrocarbon modules from plastic materials as well as a good capability to process waste plastics in complicated conditions.

     
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  4. Capacitive deionization (CDI) is an energy saving and environmentally friendly technology for water desalination. However, classical CDI is challenged by a low salt removal capacity. To improve the desalination capacity, electrode materials utilizing the battery mechanism for salt ion removal have emerged as a new direction more recently. In this work, we report a study of amorphous iron phosphate (FePO 4 ) as a promising electrode material for pseudocapacitive sodium ion removal. Sodium ions can be effectively, reversibly intercalated and de-intercalated upon its electrochemical reduction and oxidation, with an excellent sodium ion capacity under half-cell testing conditions. By assembling a hybrid CDI (HCDI) system utilizing the FePO 4 electrode for pseudocapacitive sodium ion removal and active carbon electrode for capacitive chloride ion removal, the cell exhibited a high salt removal capacity and good reversibility and durability, which was attributed to the advantageous features of amorphous FePO 4 . The HCDI system achieved a high deionization capacity (82 mg g −1 ) in 10 mM NaCl, a fast deionization rate (0.046 mg g −1 s −1 ), and good stability and cyclability. 
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  5. Formaldehyde is an essential building block for hundreds of chemicals and a promising liquid organic hydrogen carrier (LOHC), yet its indirect energy-intensive synthesis process prohibits it from playing a more significant role. Here we report a direct CO reduction to formaldehyde (CORTF) process that utilizes hydrogen underpotential deposition to overcome the thermodynamic barrier and the scaling relationship restriction. This is the first time that this reaction has been realized under ambient conditions. Using molybdenum phosphide as a catalyst, formaldehyde was produced with nearly a 100% faradaic efficiency in aqueous KOH solution, with its formation rate being one order of magnitude higher compared with the state-of-the-art thermal catalysis approach. Simultaneous tuning of the current density and reaction temperature led to a more selective and productive formaldehyde synthesis, indicating the electrochemical and thermal duality of this reaction. DFT calculations revealed that the desorption of the *H 2 CO intermediate likely served as the rate-limiting step, and the participation of H 2 O made the reaction thermodynamically favorable. Furthermore, a full-cell reaction set-up was demonstrated with CO hydrogenation to HCHO achieved without any energy input, which fully realized the spontaneous potential of the reaction. Our study shows the feasibility of combining thermal and electrochemical approaches for realizing the thermodynamics and for scaling relationship-confined reactions, which could serve as a new strategy in future reaction design. 
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