Browsing by Author "Mallick, Bikash Chandra"

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Amino-functionalization on graphene oxide sheets using an atomic layer amidation technique
(2020-01-14)
Gu, Siyong
;
Hsieh, Chien-Te
;
Mallick, Bikash Chandra
;
Gandomi, Yasser Ashraf
;
Chang, Jeng-Kuei
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 degrees 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 degrees C) and 0.028 atomic percent (at%) cycle(-1) (150 degrees 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. In this sense, nitrogen functionalization can be utilized for engineering any desirable properties within the graphene sheets.
Improved lithium storage capacity and high rate capability of nitrogen-doped graphite-like electrode materials prepared from thermal pyrolysis of graphene quantum dots
(2020-09-10)
Gu, Siyong
;
Christensen, Tommiejean
;
Hsieh, Chien-Te
;
Mallick, Bikash Chandra
;
Gandomi, Yasser Ashraf
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 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 x 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 ultrahigh C rates. (C) 2020 Elsevier Ltd. All rights reserved.