Doctor of Philosophy, Zhejiang University (2018)
Bachelor of Science, Zhejiang University (2013)
All-Solid-State Lithium-Sulfur Batteries Enhanced by Redox Mediators.
Journal of the American Chemical Society
Redox mediators (RMs) play a vital role in some liquid electrolyte-based electrochemical energy storage systems. However, the concept of redox mediator in solid-state batteries remains unexplored. Here, we selected a group of RM candidates and investigated their behaviors and roles in all-solid-state lithium-sulfur batteries (ASSLSBs). The soluble-type quinone-based RM (AQT) shows the most favorable redox potential and the best redox reversibility that functions well for lithium sulfide (Li2S) oxidation in solid polymer electrolytes. Accordingly, Li2S cathodes with AQT RMs present a significantly reduced energy barrier (average oxidation potential of 2.4 V) during initial charging at 0.1 C at 60 °C and the following discharge capacity of 1133 mAh gs-1. Using operando sulfur K-edge X-ray absorption spectroscopy, we directly tracked the sulfur speciation in ASSLSBs and proved that the solid-polysulfide-solid reaction of Li2S cathodes with RMs facilitated Li2S oxidation. In contrast, for bare Li2S cathodes, the solid-solid Li2S-sulfur direct conversion in the first charge cycle results in a high energy barrier for activation (charge to 4 V) and low sulfur utilization. The Li2S@AQT cell demonstrates superior cycling stability (average Coulombic efficiency 98.9% for 150 cycles) and rate capability owing to the effective AQT-enhanced Li-S reaction kinetics. This work reveals the evolution of sulfur species in ASSLSBs and realizes the fast Li-S reaction kinetics by designing an effective sulfur speciation pathway.
View details for DOI 10.1021/jacs.1c07754
View details for PubMedID 34677957
- Sensitive, portable heavy-metal-ion detection by the sulfidation method on a superhydrophobic concentrator (SPOT) ONE EARTH 2021; 4 (5): 756-766
Air-Filtering Masks for Respiratory Protection from PM2.5 and Pandemic Pathogens.
One earth (Cambridge, Mass.)
2020; 3 (5): 574–89
Air-filtering masks, also known as respirators, protect wearers from inhaling fine particulate matter (PM2.5) in polluted air, as well as airborne pathogens during a pandemic, such as the ongoing COVID-19 pandemic. Fibrous medium, used as the filtration layer, is the most essential component of an air-filtering mask. This article presents an overview of the development of fibrous media for air filtration. We first synthesize the literature on several key factors that affect the filtration performance of fibrous media. We then concentrate on two major techniques for fabricating fibrous media, namely, meltblown and electrospinning. In addition, we underscore the importance of electret filters by reviewing various methods for imparting electrostatic charge on fibrous media. Finally, this article concludes with a perspective on the emerging research opportunities amid the COVID-19 crisis.
View details for DOI 10.1016/j.oneear.2020.10.014
View details for PubMedID 33748744
Designing a Nanoscale Three-phase Electrochemical Pathway to Promote Pt-catalyzed Formaldehyde Oxidation.
Gas-phase heterogeneous catalysis is a process spatially constrained on the two-dimensional surface of a solid catalyst. Here, we introduce a new toolkit to open up the third dimension. We discovered that the activity of a solid catalyst can be dramatically promoted by covering its surface with a nanoscale-thin layer of liquid electrolyte while maintaining efficient delivery of gas reactants, a strategy we call three-phase catalysis. Introducing the liquid electrolyte converts the original surface catalytic reaction into an electrochemical pathway with mass transfer facilitated by free ions in a three-dimensional space. We chose the oxidation of formaldehyde as a model reaction and observed a 25000-times enhancement in the turnover frequency of Pt in three-phase catalysis as compared to conventional heterogeneous catalysis. We envision three-phase catalysis as a new dimension for catalyst design and anticipate its applications in more chemical reactions from pollution control to the petrochemical industry.
View details for DOI 10.1021/acs.nanolett.0c03560
View details for PubMedID 33201720
- Ultralight and fire-extinguishing current collectors for high-energy and high-safety lithium-ion batteries NATURE ENERGY 2020; 5 (10): 786–93
Incorporating the nanoscale encapsulation concept from liquid electrolytes into solid-state lithium-sulfur batteries.
Lithium-sulfur (Li-S) batteries are attractive due to their high specific energy and low-cost prospect. Most studies in the past decade are based on these batteries with liquid electrolytes, where many exciting material/structural designs are realized at the nanoscale to address problems of Li-S chemistry. Recently, there is a new promising direction to develop Li-S batteries with solid polymer electrolytes, although it is unclear whether the concepts from liquid electrolytes are applicable in the solid state to improve battery performance. Here we demonstrate that the nanoscale encapsulation concept based on Li2S-TiS2 core-shell particles, originally developed in liquid electrolytes, is very effective in solid polymer electrolytes. Using in situ optical cell measurement and sulfur K-edge X-ray absorption near edge spectroscopy, we find that polysulfides form and are well trapped inside individual particles by the nanoscale TiS2 encapsulation. This TiS2 encapsulation layer also functions to catalyze the oxidation reaction of Li2S to sulfur, even in solid-state electrolytes, proved by both experiments and density functional theory calculations. A high cell-level specific energy of 427 W∙h∙kg-1 at 60 °C (including the mass of the anode, cathode, and solid-state electrolyte, but excluding the current collector and packaging) is achieved by integrating TiS2 encapsulated Li2S cathode with ultrathin polyethylene oxide-based solid polymer electrolyte (10~20 m) and lithium metal anode. The solid-state cells show excellent stability over 150 charge/discharge cycles at 0.8 C at 80 °C. This study points to the fruitful direction of borrowing concepts from liquid electrolytes into solid-state Li-S batteries.
View details for DOI 10.1021/acs.nanolett.0c02033
View details for PubMedID 32515973
Destruction of Per- and Polyfluoroalkyl Substances (PFASs) in Aqueous Film-Forming Foam (AFFF) with UV-Sulfite Photoreductive Treatment.
Environmental science & technology
Ultraviolet photochemical reaction of sulfite (SO32-) photosensitizer generates strongly reducing hydrated electrons (eaq-; NHE = -2.9 V) that have been shown to effectively degrade individual per- and polyfluoroalkyl substances (PFASs), including perfluorooctanesulfonic acid (PFOS) and perfluorooctanoic acid (PFOA). However, treatment of complex PFAS mixtures in aqueous film-forming foam (AFFF) remains largely unknown. Here, UV-sulfite was applied to a diluted AFFF to characterize eaq- reactions with 15 PFASs identified by liquid chromatography quadrupole time-of-flight mass spectrometry (LC-QTOF-MS) targeted analysis. Results show that reactivity varies widely among PFASs, but reaction rates observed for individual PFASs in AFFF are similar to rates observed in single-solute experiments. While some structures, including long-chain perfluoroalkyl sulfonic acids (PFSAs) and perfluoroalkyl carboxylic acids (PFCAs) were readily degraded, other structures, most notably short-chain PFSAs and fluorotelomer sulfonic acids (FTSs), were more recalcitrant. This finding is consistent with results showing incomplete fluoride ion release (up to 53% of the F content in AFFF) during reactions. Furthermore, results show that selected PFSAs, PFCAs, and FTSs can form as transient intermediates or unreactive end-products via eaq- reactions with precursor structures in AFFF. These results indicate that while UV-sulfite treatment can be effective for treating PFOS and PFOA to meet health advisory levels, remediation of the wider range of PFASs in AFFF will prove more challenging.
View details for DOI 10.1021/acs.est.0c00961
View details for PubMedID 32343565