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1.
ACS Appl Mater Interfaces ; 15(33): 39351-39362, 2023 Aug 23.
Article in English | MEDLINE | ID: mdl-37552834

ABSTRACT

Sulfur (S) doping is an effective method for constructing high-performance carbon anodes for sodium-ion batteries. However, traditional designs of S-doped carbon often exhibit low initial Coulombic efficiency (ICE), poor rate capability, and impoverished cycle performance, limiting their practical applications. This study proposes an innovative design strategy to fabricate S-doped carbon using sulfonated sugar molecules as precursors via high-energy ball milling. The results show that the high-energy ball milling can immobilize S for sulfonated sugar molecules by modulating the chemical state of S atoms, thereby creating a S-rich carbon framework with a doping level of 15.5 wt %. In addition, the S atoms are present mainly in the form of C-S bonds, facilitating a stable electrochemical reaction; meanwhile, S atoms expand the spacing between carbon layers and contribute sufficient capacitance-type Na-storage sites. Consequently, the S-doped carbon exhibits a large capacity (>600 mAh g-1), a high ICE (>90%), superior cycling stability (490 mAh g-1 after 1100 cycles at 5 A g-1), and outstanding rate performance (420 mAh g-1 at a high current density of 50 A g-1). Such excellent Na-storage properties of S-doped carbon have rarely been reported in the literatures before.

2.
Small ; 19(34): e2301975, 2023 Aug.
Article in English | MEDLINE | ID: mdl-37165580

ABSTRACT

Oxygen doping is an effective strategy for constructing high-performance carbon anodes in Na ion batteries; however, current oxygen-doped carbons always exhibit low doping levels and high-defect surfaces, resulting in limited capacity improvement and low initial Coulombic efficiency (ICE). Herein, a stainless steel-assisted high-energy ball milling is exploited to achieve high-level oxygen doping (19.33%) in the carbon framework. The doped oxygen atoms exist dominantly in the form of carbon-oxygen double bonds, supplying sufficient Na storage sites through an addition reaction. More importantly, it is unexpected that the random carbon layers on the surface are reconstructed into a quasi-ordered arrangement by robust mechanical force, which is low-defect and favorable for suppressing the formation of thick solid electrolyte interfaces. As such, the obtained carbon presents a large reversible capacity of 363 mAh g-1 with a high ICE up to 83.1%. In addition, owing to the surface-dominated capacity contribution, an ultrafast Na storage is achieved that the capacity remains 139 mAh g-1 under a large current density of 100 A g-1 . Such good Na storage performance, especially outstanding rate capability, has rarely been achieved before.

3.
Environ Sci Technol ; 57(8): 3053-3061, 2023 02 28.
Article in English | MEDLINE | ID: mdl-36790355

ABSTRACT

Herein, we demonstrate the ability of a dual-purpose periodic mesoporous organosilica (PMO) probe to track the complex chlorinated paraffin (CP) composition in living animals by assembling it as an adsorbent-assisted atmospheric pressure chemical ionization Fourier-transform ion cyclotron resonance mass spectrometry (APCI-FT-ICR-MS) platform and synchronously performing it as the in vivo sampling device. First, synchronous solvent-free ionization and in-source thermal desorption of CP homologues were achieved by the introduction of the PMO adsorbent-assisted APCI module, generating exclusive adduct ions ([M - H]-) of individual CP homologues (CnClm) with enhanced ionization efficiency. Improved detection limits of short- and medium-chain CPs (0.10-24 and 0.48-5.0 pg/µL) were achieved versus those of the chloride-anion attachment APCI-MS methods. Second, the dual-purpose PMO probe was applied to extract the complex CP compositions in living animals, following APCI-FT-ICR-MS analysis. A modified pattern-deconvolution algorithm coupled with the sampling-rate calibration method was used for the quantification of CPs in living fish. In vivo quantification of a tilapia exposed to technical CPs for 7 days was successfully achieved, with ∑SCCPs and ∑MCCPs of the sampled fish calculated to be 1108 ± 289 and 831 ± 266 µg/kg, respectively. Meanwhile, 58 potential CP metabolites were identified in living fish for the first time during in vivo sampling of CPs, a capacity that could provide an important tool for future study regarding its expected risks to humans and its environmental fate.


Subject(s)
Hydrocarbons, Chlorinated , Paraffin , Humans , Animals , Paraffin/analysis , Paraffin/chemistry , Hydrocarbons, Chlorinated/analysis , Hydrocarbons, Chlorinated/chemistry , Environmental Monitoring/methods , Mass Spectrometry/methods , Fishes , Chlorides/analysis
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