Engineering topics

Gu, Siyong

Publications and source records attributed to Gu, Siyong.

6 records

DOE OSTI2021

Effect of Solvent on Fluorescence Emission from Polyethylene Glycol-Coated Graphene Quantum Dots under Blue Light Illumination

To explore aggregate-induced emission (AIE) properties, this study adopts a one-pot hydrothermal route for synthesizing polyethylene glycol (PEG)-coated graphene quantum dot (GQD) clusters, enabling the emission of highly intense photoluminescence under blue light illumination. The hydrothermal synthesis was performed at 300 °C using o-phenylenediamine as the nitrogen and carbon sources in the presence of PEG. Three different solvents, propylene glycol methyl ether acetate (PGMEA), ethanol, and water, were used for dispersing the PEG-coated GQDs, where extremely high fluorescent emission was achieved at 530–550 nm. It was shown that the quantum yield (QY) of PEG-coated GQD suspensions is strongly dependent on the solvent type. The pristine GQD suspension tends to be quenched (i.e., QY: ~1%) when dispersed in PGMEA (aggregation-caused quenching). However, coating GQD nanoparticles with polyethylene glycol results in substantial enhancement of the quantum yield. When investigating the photoluminescence emission from PEG-coated GQD clusters, the surface tension of the solvents was within the range of from 26.9 to 46.0 mN/m. This critical index can be tuned for assessing the transition point needed to activate the AIE mechanism which ultimately boosts the fluorescence intensity. The one-pot hydrothermal route established in this study can be adopted to engineer PEG-coated GQD clusters with solid-state PL emission capabilities, which are needed for next-generation optical, bio-sensing, and energy storage/conversion devices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Roll-To-Roll Atomic Layer Deposition of Titania Nanocoating on Thermally Stabilizing Lithium Nickel Cobalt Manganese Oxide Cathodes for Lithium Ion Batteries

Conformal coating of ceramic layers (nm-thick) on Ni-rich layered cathode materials is an effective strategy for improving high-temperature longevity of Li-ion batteries (LIBs). In this work, we develop a roll-to-roll atomic layer deposition (R2R ALD) apparatus for growing uniform nanolayers of TiO 2 . We explore the effect of ALD parameters (temperature: 120–180 °C and line speed: 2–40 mm s –1 ) on the TiO 2 surface coating and subsequently investigate the electrochemical performance of the as-prepared cathodes. The capacity retention of TiO 2 -coated porous electrodes is substantially improved compared to that of the pristine cathode material for high-temperature cycling. Electrochemical impedance spectroscopy confirms that the ALD-TiO 2 coating suppresses the undesired side reactions initiated at the electrode/electrolyte interface, reduces charge transfer resistance, and ultimately facilitates the Li + transport through the composite cathode nanostructure. The robust design of the ALD-TiO 2 cathode material enables high-temperature operation (>55 °C) with enhanced specific capacity, superior rate capability, excellent cyclability, and ultra-high coulombic efficiency within a wide potential window (3.0–4.35 V). Furthermore, the R2R ALD technique developed in this work paves the way for large-scale fabrication of ceramic-coated cathode sheets with a production rate reaching 2.4 m min –1 for a continuous coating operation.

25 ENERGY STORAGE↗

DOE OSTI2020

Improved lithium storage capacity and high rate capability of nitrogen-doped graphite-like electrode materials prepared from thermal pyrolysis of graphene quantum dots

Adopting a solid-phase microwave-assisted technique followed by thermal pyrolysis of N-functionalized graphene quantum dots, novel nitrogen-doped graphite-like (NGL) electrode materials were synthesized in this work and served as the anode for Li-ion batteries. The NGL anode demonstrated reversible capacity of 530 mAh g -1 at 0.1C, superior rate capability at high C rate operation (420 mAh g -1 at 5C), remarkable initial coulombic efficiency (>95.7%), and excellent cyclic stability along with high efficiency (>99.1%) during entire cycling. The NGL anode nanostructure enables improved lithium ion mobility and reversible Li + storage during cycling. The analysis of the Ragone plots revealed that the specific energy of NGL anode reaches to ca. 840 Wh kg -1 at the power density of 4200 W kg -1 . The diffusion coefficient of Li ions was measured as 1.69 × 10 -9 cm 2 s -1 for the NGL anode material, substantially improving over commonly used graphite electrodes (15–26 times higher Li + diffusivity). The high-rate cyclability as well as the cyclic stability of the NGL anodes were also confirmed via long-term cycling of full pouch cells assembled with ternary cathode and NGL anode. The robust design of the NGL anode materials introduced in this work, paves the way for designing next-generation lithium-ion batteries operating at ultra-high C rates.

25 ENERGY STORAGE↗

DOE OSTI2019

Amino-functionalization on graphene oxide sheets using an atomic layer amidation technique

Nitrogen functionalization on graphene sheets has solely been demonstrated with a stepwise amidation implementation within the literature. The present work proposes an atomic layer amidation (ALN) technique to linearly adjust the surface amidation level on the carbon nanostructures. The ALN cycling protocol proposed in this work consists of an ammonia pulse, nitrogen pulse, and pumping at 100 and 150 °C. Both surface amidation and oxidation levels were linearly controlled by the ALN cycle number. The ALN technique was demonstrated as a self-limiting process capable of step-by-step N-functionalizing graphene oxide (GO) sheets on the atomic scale. The amidation reaction rates were ca. 0.023 (100 °C) and 0.028 atomic percent (at%) cycle–1 (150 °C), and the apparent activation energy was determined to be 14.3 kJ mol –1 (= 0.148 eV atom –1 ) from the Arrhenius equation. The amidation mechanism for forming the “chemical N” and “lattice N” at an atomic level was also proposed. Linearly controlling the optical band-gap with the ALN cycle number was suggested as a robust method for tuning the oxidation as well as the amidation level on the GO sheets. Here, nitrogen functionalization can be utilized for engineering any desirable properties within the graphene sheets.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2019

Synthesis of MgCo 2 O 4 -coated Li 4 Ti 5 O 12 composite anodes using co-precipitation method for lithium-ion batteries

In the present work, we report synthesis of MgCo 2 O 4 (MCO)/Li 4 Ti 5 O 12 (LTO) composites for Li-ion battery anodes by a co-precipitation method. The objective here is to replace expensive Co with Mg and also to exploit advantages of both MCO and LTO. Three samples of MCO/LTO particles with different MCO proportion have various average particle sizes of 38.1, 56.9, and 58.5 nm, confirmed by scanning electron microscopy. Electrochemical studies show that a MCO/LTO anode offers a discharge capacity of ca. 300 mAh g -1 , which is two times higher than that achieved by pristine LTO. The MCO/LTO anode also retains 75% of its initial capacity, even if the discharge rate is increased to 5 C. Cyclic stability test reveals that the composite anode still maintains nearly 85.5% of its initial capacity after 150 cycles. Electrochemical impedance spectroscopy indicates that the equivalent series resistance of MCO/LTO electrodes is significantly lower than that of LTO, i.e., from 35.5 to 9.9 Ω. The enhanced performance of the composite electrodes can be attributed to its improved conductivity as well as to the surface modification of LTO particles by MCO nanoparticle deposition which leads to increased number of active sites on the former.

25 ENERGY STORAGE↗

DOE OSTI2019

Tailoring Fluorescence Emissions, Quantum Yields, and White Light Emitting from Nitrogen-doped Graphene and Carbon Nitride Quantum Dots

Highly fluorescent N-doped graphene quantum dots (NGQDs) and graphitic carbon nitride quantum dots (CNQDs, g-C 3 N 4 ) were synthesized using a solid-phase microwave-assisted (SPMA) technique. The SPMA method, based on the pyrolysis of citric acid and urea with different recipes, is capable of producing quantum dots with coexisting NGQDs and CNQDs at 280°C within only five minutes. The photoluminescence (PL) emissions from NGQD and CNQDs are strongly dependent on excitation wavelength and the solvent type, i.e., water, ethanol, and N-methyl pyrrolidinone. The unique design of the quantum dots possesses a multiple chromophoric band-gap structure, originated from the presence of g-C 3 N 4 , defect-related emissive traps, and grain boundaries. Thus, an appropriate excitation wavelength induces a conjugated π electron system to fulfill the most probable absorption band, resulting in wavelength-dependent emissions including ultraviolet, visible and infrared light. Here, the quantum yield of the NGQD and CNQD samples can attain as high as 68.1%. Accordingly, one light-emitting device using the combination of the NGQD and CNQD powders embedded polymeric film can emit white-like light with high power conversion efficiency.

77 NANOSCIENCE AND NANOTECHNOLOGY↗