“…48,49 With increasing pyrolysis temperatures, the ICE of LHCs and CHCs showed an overall increasing trend, which benefited from the reduced specific surface area and defects leading to a lower irreversible capacity. 50 At low pyrolysis temperatures of 1000 °C, the ICEs of L-1000 and C-1000 were 51.4% and 29.9%, respectively. This is attributed to the fact that L-1000 already has a microcrystalline carbon stacking structure, whereas C-1000 is still mainly amorphous carbon.…”
Section: Resultsmentioning
confidence: 92%
“…The sodium storage performance of LHCs and CHCs was tested in half-cells (Table S3). The initial coulometric efficiency (ICE) is the ratio of the sodium deintercalation capacity (charging) to the sodium intercalation capacity (discharging) during the first charging and discharging process, in which the first discharging capacity consists of reversible and irreversible capacities and the first charging capacity is mainly the reversible capacity, so the ICE is commonly used as a measure of the utilization rate of the sodium storage active sites of HCs. , With increasing pyrolysis temperatures, the ICE of LHCs and CHCs showed an overall increasing trend, which benefited from the reduced specific surface area and defects leading to a lower irreversible capacity . At low pyrolysis temperatures of 1000 °C, the ICEs of L-1000 and C-1000 were 51.4% and 29.9%, respectively.…”
Microcrystalline carbon is the essential constituent unit that constitutes the hard carbon material for sodium-ion batteries. However, the evolution mechanism of microcrystalline carbon remains controversial, on account of the diversity of biomass composition. Here, we conducted a systematic study of the evolutionary mechanism of microcrystalline carbon using lignin and cellulose as models. It was found that lignin is more readily converted into microcrystalline carbon structures than cellulose. Owing to the differences in pyrolysis processes, lignin-derived microcrystalline carbon exhibits isotropic arrangement properties and evolves into long-range ordered graphite-like structures with increasing pyrolysis temperatures. In contrast, the anisotropic arrangement of cellulose-derived microcrystalline carbon allows them to maintain long-range disordered structures under high-temperature pyrolysis. Upon further analysis using four forestry biomass wastes with different compositional ratios to prepare hard carbon, we found that proper ratios of lignin and cellulose ensure a sufficient amount of microcrystalline carbon while avoiding overgrowth of microcrystalline carbon, where the tightness of the microcrystalline carbon stacking structure was positively correlated with lignin content. Besides, coconut-shell-derived hard carbon has a long-range disordered and short-range ordered microcrystalline stacking structure and exhibits a high capacity of 329.3 mAh g −1 .
“…48,49 With increasing pyrolysis temperatures, the ICE of LHCs and CHCs showed an overall increasing trend, which benefited from the reduced specific surface area and defects leading to a lower irreversible capacity. 50 At low pyrolysis temperatures of 1000 °C, the ICEs of L-1000 and C-1000 were 51.4% and 29.9%, respectively. This is attributed to the fact that L-1000 already has a microcrystalline carbon stacking structure, whereas C-1000 is still mainly amorphous carbon.…”
Section: Resultsmentioning
confidence: 92%
“…The sodium storage performance of LHCs and CHCs was tested in half-cells (Table S3). The initial coulometric efficiency (ICE) is the ratio of the sodium deintercalation capacity (charging) to the sodium intercalation capacity (discharging) during the first charging and discharging process, in which the first discharging capacity consists of reversible and irreversible capacities and the first charging capacity is mainly the reversible capacity, so the ICE is commonly used as a measure of the utilization rate of the sodium storage active sites of HCs. , With increasing pyrolysis temperatures, the ICE of LHCs and CHCs showed an overall increasing trend, which benefited from the reduced specific surface area and defects leading to a lower irreversible capacity . At low pyrolysis temperatures of 1000 °C, the ICEs of L-1000 and C-1000 were 51.4% and 29.9%, respectively.…”
Microcrystalline carbon is the essential constituent unit that constitutes the hard carbon material for sodium-ion batteries. However, the evolution mechanism of microcrystalline carbon remains controversial, on account of the diversity of biomass composition. Here, we conducted a systematic study of the evolutionary mechanism of microcrystalline carbon using lignin and cellulose as models. It was found that lignin is more readily converted into microcrystalline carbon structures than cellulose. Owing to the differences in pyrolysis processes, lignin-derived microcrystalline carbon exhibits isotropic arrangement properties and evolves into long-range ordered graphite-like structures with increasing pyrolysis temperatures. In contrast, the anisotropic arrangement of cellulose-derived microcrystalline carbon allows them to maintain long-range disordered structures under high-temperature pyrolysis. Upon further analysis using four forestry biomass wastes with different compositional ratios to prepare hard carbon, we found that proper ratios of lignin and cellulose ensure a sufficient amount of microcrystalline carbon while avoiding overgrowth of microcrystalline carbon, where the tightness of the microcrystalline carbon stacking structure was positively correlated with lignin content. Besides, coconut-shell-derived hard carbon has a long-range disordered and short-range ordered microcrystalline stacking structure and exhibits a high capacity of 329.3 mAh g −1 .
“…A large body of research suggests that closed pores (inaccessible by gases) in disordered carbons play a crucial role in the storage of sodium. [31][32][33][34] Distinct from N 2 adsorption/desorption measurement, in which it is difficult to detect closed pores in carbons, small-angle X-ray scattering (SAXS) can provide information on full pores including both open and closed pores. 30 Fig.…”
The cross-linking reaction tends to produce more sp3-hybrid carbon, which finally results in more curved and shorter carbon layers as well as much more closed pores. Therefore, we can regulate the closed pores and platform capacity.
“…Doping heteroatoms (such as nitrogen [ 17 , 18 ], fluorine [ 19 ], boron [ 7 ], sulfur [ 20 , 21 ], and phosphorus [ 5 , 6 , 22 , 23 ]) can effectively improve the Na-storage performance of carbon anodes, which could not only change the microstructure of carbon but also enlarge the interlayer spacing. Compared with other forms of heteroatom doping, phosphorus doping can achieve the enhancement of both plateau capacity and slope capacity, because it can enlarge interlayer spacing to facilitate adsorbing/inserting more Na + [ 24 , 25 ] and increase defect sites to achieve a higher adsorption amount of Na + [ 26 ].…”
The use of coal as a precursor for producing hard carbon is favored due to its abundance, low cost, and high carbon yield. To further optimize the sodium storage performance of hard carbon, the introduction of heteroatoms has been shown to be an effective approach. However, the inert structure in coal limits the development of heteroatom-doped coal-based hard carbon. Herein, coal-based P-doped hard carbon was synthesized using Ca3(PO4)2 to achieve homogeneous phosphorus doping and inhibit carbon microcrystal development during high-temperature carbonization. This involved a carbon dissolution reaction where Ca3(PO4)2 reacted with SiO2 and carbon in coal to form phosphorus and CO. The resulting hierarchical porous structure allowed for rapid diffusion of Na+ and resulted in a high reversible capacity of 200 mAh g−1 when used as an anode material for Na+ storage. Compared to unpretreated coal-based hard carbon, the P-doped hard carbon displayed a larger initial coulombic efficiency (64%) and proportion of plateau capacity (47%), whereas the unpretreated carbon only exhibited an initial coulombic efficiency of 43.1% and a proportion of plateau capacity of 29.8%. This work provides a green, scalable approach for effective microcrystalline regulation of hard carbon from low-cost and highly aromatic precursors.
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