ORCID Profile
0000-0002-0714-6710
Current Organisation
Worcester Polytechnic Institute
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Publisher: Royal Society of Chemistry (RSC)
Date: 2020
DOI: 10.1039/C9CP06792B
Abstract: In this paper, the performance of ab initio composite methods, and a wide range of DFT methods is assessed for the calculation of interaction energies of thermal clusters of a solute in water.
Publisher: American Chemical Society (ACS)
Date: 10-2018
Publisher: American Chemical Society (ACS)
Date: 06-06-2019
Abstract: In this work, contemporary quantum mechanical (QM) implicit solvent models (SMD, SM12, and COSMO-RS) and a molecular mechanical (MM) explicit solvent model were used to predict the aqueous free energy barrier of a simple Menschutkin reaction (NH
Publisher: Wiley
Date: 09-09-2021
Abstract: Proton is an ideal charge carrier for rechargeable batteries due to its small ionic radius, ultrafast diffusion kinetics and wide availability. However, in commonly used acid electrolytes, the co‐interaction of polarized water and proton (namely hydronium) with electrode materials often causes electrode structural distortions. The hydronium adsorption on electrode surfaces also facilitates hydrogen evolution as an unwanted side reaction. Here, a “water‐in‐sugar” electrolyte with high concentration of glucose dissolved in acid to enable the naked proton intercalation, as well as an extended 3.9 V working potential window, is shown. A glucose‐derived organic thin film is formed on electrode surface upon cycling. Molecular dynamics simulations reveal the significant decrease of free water in bulk electrolytes, while density functional theory calculations indicate that glucose preferentially binds to the electrode surface which can inhibit water adsorption. The scarcity of free water and the protective organic film work in synergy to suppress water interactions with the electrode surface, which enables the naked proton (de)intercalation. The “water‐in‐sugar” electrolyte significantly enhances a MoO 3 electrode for stable cycling over 100 000 times. This facile electrolyte approach opens new avenues to aqueous electrochemistry and energy storage devices.
Publisher: American Chemical Society (ACS)
Date: 06-08-2021
Publisher: American Chemical Society (ACS)
Date: 11-08-2022
Abstract: This paper introduces an economical approach for improving the accuracy and convergence of quantum mechanics/molecular mechanics (QM/MM) models. The approach is tested on a series of neutral and charged amino acids embedded in a 160-water cluster, where their intramolecular proton transfer energies (neutral amino acid → zwitterionic amino acid) were previously obtained at the ωB97X-D/6-31G(d) level of theory. When the charges on the MM atoms were replaced with those obtained at the same QM level of theory used to treat the QM atoms, this significantly improved the accuracy and convergence of the QM/MM models. In particular, the QM/MM model converged to within 1.4 kcal mol
Publisher: Royal Society of Chemistry (RSC)
Date: 2023
DOI: 10.1039/D3CC00475A
Abstract: The feasibility of various bespoke guanidine-based compounds as electrochemically regenerative biomimetic hydrides for reduction of carbon dioxide to formate were assessed by Density Functional Theory (DFT).
Publisher: Wiley
Date: 12-05-2022
Abstract: Rechargeable aqueous proton batteries are promising competitors for the next generation of energy storage systems with the fast diffusion kinetics and wide availability of protons. However, poor cycling stability is a big challenge for proton batteries due to the attachment of water molecules to the electrode surface in acid electrolytes. Here, a hydrogen‐bond disrupting electrolyte strategy to boost proton battery stability via simultaneously tuning the hydronium ion solvation sheath in the electrolyte and the electrode interface is reported. By mixing cryoprotectants such as glycerol with acids, hydrogen bonds involving water molecules are disrupted leading to a modified hydronium ion solvation sheaths and minimized water activity. Concomitantly, glycerol absorbs on the electrode surface and acts to protect the electrode surface from water. Fast and stable proton storage with high rate capability and long cycle life is thus achieved, even at temperatures as low as − 50 ° C. This electrolyte strategy may be universal and is likely to pave the way toward highly stable aqueous energy storage systems.
Publisher: American Chemical Society (ACS)
Date: 09-02-2021
Publisher: Wiley
Date: 26-09-2022
Abstract: Proton electrochemistry is promising for developing post‐lithium energy storage devices with high capacity and rate capability. However, some electrode materials are vulnerable because of the co‐intercalation of free water molecules in traditional acid electrolytes, resulting in rapid capacity fading. Here, the authors report a molecular crowding electrolyte with the usage of poly(ethylene glycol) (PEG) as a crowding agent, achieving fast and stable electrochemical proton storage and expanded working potential window (3.2 V). Spectroscopic characterisations reveal the formation of hydrogen bonds between water and PEG molecules, which is beneficial for confining the activity of water molecules. Molecular dynamics simulations confirm a significant decrease of free water fraction in the molecular crowding electrolyte. Dynamic structural evolution of the MoO 3 anode is studied by in‐situ synchrotron X‐ray diffraction (XRD), revealing a reversible multi‐step naked proton (de)intercalation mechanism. Surficial adsorption of PEG molecules on MoO 3 anode works in synergy to alleviate the destructive effect of concurrent water desolvation, thereby achieving enhanced cycling stability. This strategy offers possibilities of practical applications of proton electrochemistry thanks to the low‐cost and eco‐friendly nature of PEG additives.
No related grants have been discovered for Junbo Chen.