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Schematic diagram for the preparation of N-doped graphene with different N bonding states using different N-containing precursors . Reprinted with permission from ref. 52, Copyright (2012) Royal Society of Chemistry.
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It is of great interest to develop new carbon-based materials as electrodes for supercapacitors because the conventional electrodes of activated carbons in supercapacitors cannot meet the ever-increasing demands for high energy and power densities for electronic devices. Due to their high electronic conductivity and improved hydrophilic properties,...
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... that the choice of precursors has a signicant effect on the bonding congurations and nitrogen content. That is, annealing of GO with ammonia preferentially results in the formation of graphitic N and pyridinic N centers, while annealing of GO with PANI and PPy tends to generate pyridinic and pyrrolic N moie- ties, respectively, as shown in Fig. ...
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... capaci- tance is mainly attributed to the pseudocapacitance arising from high concentrations of N and O functionalities. In another typical example, Jin et al. fabricated novel carbon-based microporous nanoplates with numerous heteroatoms (H- CMNs) and high surface area by using regenerated silk broin and KOH activation during carbonization (Fig. 13). 104 Conse- quently, the obtained H-CMNs possess potential advantages for applications in supercapacitors with high energy and power density. Human hair has become commercially available to crop producers in the past few years because it is a readily available waste generated in barber shops and hair salons. It consists of about 51% ...
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... derived from a gelatin biomolecule also showed a higher specic capacitance in H 2 SO 4 electrolyte than in KOH electrolyte. 273 They suggested that the capacitive properties of the carbons were improved by virtue of the pseudocapacitance effect in the acidic solution, which was demonstrated by the shape of CV curves recorded in the acidic medium (Fig. 30). In addition, the rate capability under acidic conditions was rather moderate, where the capacitance values at 10 A g À1 were 73- 80% of those obtained at 0.1 A g À1 , indicating that faradaic redox reactions were not sufficiently fast during the quick charge/discharge operation. The very high capacitance reten- tion at high rates ...
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... contribution of nitrogen containing functional groups to the specic capacitance (C S,T ) in acidic and alkaline electrolytes. 269 It was found that the additional pseudocapaci- tance provided by pyridinic-N and pyrrolic-N/pyridone-N was clearly observed at a potential negative to 0.6 V vs. the reversible hydrogen electrode (RHE) in 1 M H 2 SO 4 (Fig. 31a), while this contribution to pseudocapacitance diminished in 1 M KOH (Fig. 31b) due to the lack of protons in the electrolyte for the basic functional groups to undergo redox reactions. The double- layer capacitance of N-RGO in 1 M H 2 SO 4 ( Fig. 31c) is higher than that in 1 M KOH (Fig. 31d) owing to the presence of N- containing ...
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... (C S,T ) in acidic and alkaline electrolytes. 269 It was found that the additional pseudocapaci- tance provided by pyridinic-N and pyrrolic-N/pyridone-N was clearly observed at a potential negative to 0.6 V vs. the reversible hydrogen electrode (RHE) in 1 M H 2 SO 4 (Fig. 31a), while this contribution to pseudocapacitance diminished in 1 M KOH (Fig. 31b) due to the lack of protons in the electrolyte for the basic functional groups to undergo redox reactions. The double- layer capacitance of N-RGO in 1 M H 2 SO 4 ( Fig. 31c) is higher than that in 1 M KOH (Fig. 31d) owing to the presence of N- containing functional groups, which increase the electronic charge density of graphene and ...
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... at a potential negative to 0.6 V vs. the reversible hydrogen electrode (RHE) in 1 M H 2 SO 4 (Fig. 31a), while this contribution to pseudocapacitance diminished in 1 M KOH (Fig. 31b) due to the lack of protons in the electrolyte for the basic functional groups to undergo redox reactions. The double- layer capacitance of N-RGO in 1 M H 2 SO 4 ( Fig. 31c) is higher than that in 1 M KOH (Fig. 31d) owing to the presence of N- containing functional groups, which increase the electronic charge density of graphene and favor proton adsorption in the acidic ...
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... reversible hydrogen electrode (RHE) in 1 M H 2 SO 4 (Fig. 31a), while this contribution to pseudocapacitance diminished in 1 M KOH (Fig. 31b) due to the lack of protons in the electrolyte for the basic functional groups to undergo redox reactions. The double- layer capacitance of N-RGO in 1 M H 2 SO 4 ( Fig. 31c) is higher than that in 1 M KOH (Fig. 31d) owing to the presence of N- containing functional groups, which increase the electronic charge density of graphene and favor proton adsorption in the acidic ...
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... CV curve of NC-TEG in pure 2 M KOH elec- trolyte, it should be noted that prominent redox peaks appeared in the CV curves at $0.2 and $0.5 V of NC-TEG in the mixed electrolytes (2 M KOH electrolyte with different amounts of PD), which reects pseudo-capacitive behavior due to the reversible electron transfer between the electrolyte and electrodes (Fig. 33a). The proposed electron transfer mechanism during the redox reaction is illustrated in Fig. ...
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... to increase continuously upon the gradual addition of PD and reached a maximum (635 F g À1 ) in PK23 (2 M KOH with 0.025 M PD). Beyond this concentration, the specic capacitance values decreased to 604 and 483 F g À1 for PK24 (2 M KOH with 0.05 M PD) and PK25 (2 M KOH with 0.10 M PD) electrolytes, respec- tively. The charge-discharge curves (Fig. 33b) display a plateau in the mixed electrolytes due to the pseudocapacitance, which results from the electron transfer between the aromatic di- amine and quinine-imine. The specic capacitance of the NC- TEG electrode in the mixed electrolytes was calculated from the CV experiment, as shown in Fig. 33c, which showed that the highest ...
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... respec- tively. The charge-discharge curves (Fig. 33b) display a plateau in the mixed electrolytes due to the pseudocapacitance, which results from the electron transfer between the aromatic di- amine and quinine-imine. The specic capacitance of the NC- TEG electrode in the mixed electrolytes was calculated from the CV experiment, as shown in Fig. 33c, which showed that the highest specic capacitance was achieved in PK23 electrolyte. The over-concentrated mediator (PD) restrained the capacitive behavior, which was reected by the decreased capacitance when using 0.05 and 0.1 M PD mediator in the electrolyte. With the increase of PD, the charge transfer resistance (R ct ) between ...
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... transfer resistance (R ct ) between the electrolyte and electrode surfaces in PK21, PK22, PK23, PK24 and PK25 electrolytes was found to be 0.23, 0.26, 1.21, 3.15, and 5.32 U, respectively. In addition, the solution resis- tance (R L ) values in PK21, PK22, PK23, PK24, and PK25 were found to be 0.74, 0.95, 1.21, 1.43, and 1.47 U, respectively (Fig. 33d). These results indicate that PD ameliorates the contact between the electrolyte and electrode ...
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Citations
... 1,2 In particular, the nitrogen doping (N-doping) of various carbon materials, including graphene, graphite, and nanodiamonds, has been extensively studied to develop promising material candidates for diverse applications, such as battery electrodes, supercapacitors, and sensors. [3][4][5][6][7][8][9] Furthermore, N-doped carbon materials catalyze the oxygen reduction reaction, a cathode electrode reaction in fuel cells, 10,11 stimulating the development of multiple new catalysts over the past decade 1,2 and exhibiting advantages for methane storage. 12,13 Despite the intense research on catalytic active sites and reaction mechanisms, N-doped carbon materials remain controversial, [14][15][16][17][18] mainly owing to the incompleteness of analytical methods for the chemical speciation of N. Conventionally, CHN elemental analysis and X-ray photoelectron spectroscopy (XPS) are considered as the primary analytical techniques. ...
... Incorporating polar atoms into the as-prepared carbon-based materials is generally done by a post-treatment ( Figure 3A). 63,64 According to specific operation process, the posttreatment approach commonly includes direct heattreatment under a precursor containing polar atoms ( Figure 3B) 56 and wet chemical treatment with a precursor containing polar atoms followed by hydrothermal carbonization 63,65 and/or high-temperature annealing ( Figure 3C). 66,67 The precursors containing polar atoms applied in post-treatment process generally comprise of ammonia (NH 3 ), 56 chitosan, 60 ionic liquids, 16 melamine, 68 urea, 69 phytic acid, 60 N-allylthiourea, 11 NaH 2 PO 4 , 70 diammonium hydrogen phosphate (DHP), 71 MgSO 4 , 58 H 3 BO 3 , 61 BCl 3 , 72 fluorine gas (F 2 ), 55 hydrofluoric acid (HF), 73 and so on. ...
... The content of polar atoms doped on the electrode active materials or current collectors could be regulated by the heat-treatment time and temperature. 65,74 The N-doping process of macroporous carbon films as electrode active materials is performed under a mixture of 60 sccm NH 3 and 40 sccm H 2 at 1000 C for 5 min in a tube furnace. A strong signal is detected in the N 1s x-ray Photoelectron Spectra (XPS) in the sample that is treated with NH 3 , which is, in contrast with the sample obtained after pyrolysis or heated under H 2 (no NH 3 ) ( Figure 4A), confirming that N is successfully incorporated into the sample. ...
... Apart from direct heat-treatment, wet chemical treatment is proposed to pre-introduce the precursors containing polar atoms onto the surface of carbon materials, and then followed by high-temperature annealing 65 F I G U R E 3 (A) Schematic illustration of polar atom doping by post treatment; the post-treatment approach includes (B) direct heattreatment and (C) wet chemical treatment followed by heat-treatment. and/or hydrothermal carbonization 77 to prepare the carbon-based materials doped by polar atoms. ...
The electrolyte‐wettability at electrode material/electrolyte interface is a critical factor that governs the fundamental mechanisms of electrochemical reaction efficiency and kinetics of electrode materials in practical electrochemical energy storage. Therefore, the design and construction of electrode material surfaces with improved electrolyte‐wettability has been demonstrated to be important to optimize electrochemical energy storage performance of electrode material. Here, we comprehensively summarize advanced strategies and key progresses in surface chemical modification for enhancing electrolyte‐wettability of electrode materials, including polar atom doping by post treatment, introducing functional groups, grafting molecular brushes, and surface coating by in situ reaction. Specifically, the basic principles, characteristics, and challenges of these surface chemical strategies for improving electrolyte‐wettability of electrode materials are discussed in detail. Finally, the potential research directions regarding the surface chemical strategies and advanced characterization techniques for electrolyte‐wettability in the future are provided. This review not only insights into the surface chemical strategies for improving electrolyte‐wettability of electrode materials, but also provides strategic guidance for the electrolyte‐wettability modification and optimization of electrode materials in pursuing high‐performance electrochemical energy storage devices.
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... The primary agents used for nitrogen doping include ammonia, urea, ammonium bicarbonate, and other nitrogen-containing organic compounds. NH 3 is typically used as an external source of nitrogen to facilitate its introduction into biosorbents, and its content can reach approximately 10 wt% (Chen et al., 2016;Deng et al., 2015). The main nitrogen-containing functional groups in biosorbents are pyridinic N, pyrrolic N, quaternary N, and pyridone N-oxide. ...
... The main nitrogen-containing functional groups in biosorbents are pyridinic N, pyrrolic N, quaternary N, and pyridone N-oxide. These are formed as follows: ammonia initially reacts with -OH and -C=O in biosorbents to produce pyridinic-N and pyrrolic-N, after which pyridinic-N is transformed into quaternary-N through a polymerization reaction (Deng et al., 2015). The modification of nitrogen-based chemicals with functional groups can significantly enhance the adsorption capacity of biosorbents. ...
... Nitrogen (N) is adjacent to carbon (C) in the periodic table and has similar atomic radii, making it easier to displace carbon atoms in the carbon skeleton to achieve doping, in addition, N(3.04) has a higher electronegativity compared to carbon (2.55) [16]. N introduced into the carbon skeleton can generally be classified into four types, depending on where they are present: pyridine nitrogen (N-6), pyrrole nitrogen (N-5), graphitic nitrogen (N-Q) and oxidized nitrogen (N-X) [17]. Both the N-6 and the N-5 are located at the edge positions of the carbon skeleton, therefore, both the N-6 and the N-5 can provide active sites, in addition they can contribute additional pseudo-capacitance, where the N-6 is attached to five carbon atoms to form a six-membered ring, while the N-5 is attached to four carbon atoms to form a five-membered ring. ...
Dopant species and strategies for the preparation of N/P-C are systematically summarized. • N/P-C for versatile applications were carefully analyzed. • The heteroatom doping enhancement mechanisms were discussed. • The challenges and the future outlook were proposed. A R T I C L E I N F O Keywords: N/P co-doped porous carbon Supercapacitor Battery Metal-ion hybrid capacitors Fuel cells A B S T R A C T Porous carbon is widely used in energy storage and environmental protection due to its well-developed pore structure, large specific surface area, low cost and excellent chemical/thermal stability. However, the hydro-phobic surface of pure carbon materials can limit the performance of carbon materials. Non-metallic heteroatom doping is an effective strategy to improve the performance of carbon materials efficiently. In particular, nitrogen-phosphorus co-doped porous carbon (N/P-C) has received much attention in the past few years. When N/P-C is applied in the field of energy storage and adsorption, its internal micropores are the main part contributing to the active sites, mesopores and macropores mainly play the role of transport channels and storage reservoirs, respectively; therefore, the hierarchical pore structure combining both micropores, mesopores and macropores can significantly enhance the electrochemical and adsorption properties of N/P-C. In addition, the hydrophobic surface of pure carbon materials can limit the performance of carbon materials. In contrast, the doping of N and P heteroatoms introduces a large number of functional groups on the surface of the carbon material and improves 2 the surface wettability of the carbon material, in addition to enhancing the electrical conductivity and providing more active sites, thus further improving the performance of the N/P-C. In this review, dopants and preparation methods for synthesis N/P-C are summarized in recent years. And the mechanism of nitrogen (N)-phosphorus (P) co-doping for performance enhancement is also discussed. Then, we discuss in detail the applications of N/P-C in the fields of supercapacitors (SCs), metal-ion hybrid capacitors (HC), metal-ion batteries, fuel cells, adsorption, etc. Finally, the potential and challenges of N/P-C for applications in energy storage/conversion and adsorption are discussed.
... The above results indicated that doped chlorella as a nitrogen source can indeed produce abundant nitrogen-containing functional groups on the porous carbon surface. It has been suggested that pyridine-N and pyrrole-N are considered active sites that can effectively improve pseudocapacitor (Czerw et al. 2001;Deng et al. 2015), and graphite nitrogen can promote Environmental Science and Pollution Research rapid electron transfer and enhance electrical conductivity (Hao et al. 2013). Figure 5c analyzes the composition and content of nitrogen in different samples, and it can be seen that the nitrogen contents of ZBC@C-5 and ZBC@M were very close to each other, which further confirmed that chlorella was an effective nitrogen source. ...
Porous carbon generated from biomass has a rich pore structure, is inexpensive, and has a lot of promise for use as a carbon material for energy storage devices. In this work, nitrogen-doped porous carbon was prepared by co-pyrolysis using bagasse as the precursor and chlorella as the nitrogen source. ZnCl2 acts as both an activator and a nitrogen fixer during activation to generate pores and reduce nitrogen loss. The thermal weight loss experiments showed that the pyrolysis temperatures of bagasse and chlorella overlap, which created the possibility for the synthesis of nitrogen-rich biochar. The optimum sample (ZBC@C-5) possessed a surface area of 1508 m²g⁻¹ with abundant nitrogen-containing functional groups. ZBC@C-5 in the three-electrode system exhibited 244.1F/g at 0.5A/g, which was extremely close to ZBC@M made with melamine as the nitrogen source. This provides new opportunities for the use of low-cost nitrogen sources. Furthermore, the devices exhibit better voltage retention (39%) and capacitance retention (96.3%). The goal of this research is to find a low cost, and effective method for creating nitrogen-doped porous carbon materials with better electrochemical performance for highly valuable applications using bagasse and chlorella.
Graphical Abstract
... Such a combination will facilitate unlocking the Helmholtz capacitance through the capacitance of the spatial charge region in a solid. For this purpose, carbon materials are modified by introducing ions of various impurities (atoms of O, N, B, S, P, Si, etc.) into their structures [3][4][5][6][7]. Nitrogen and oxygen are the most widely used. ...
This article presents the technology for the preparation of a nitrogen-containing nanoporous bio-carbon and investigates its properties. It has been shown that the synthesised bio-carbon is characterised by a high degree of homogeneity, which has been confirmed by energy dispersive spectroscopy. The obtained bio-carbon has a micromesoporous structure, which has been confirmed by the results of studies using the method of low-temperature nitrogen adsorption and desorption. It was found that the specific surface area of biochar is 1247 m2/g. The data on nitrogen adsorption and desorption were compared with the data on small-angle X-ray scattering, and it was found that the micropores in the synthesised bio-carbon are open pores, while mesopores remain closed. The energy dispersion analysis showed that the structure of the bio-carbon does not contain ferromagnetic atoms, but due to the addition of nitrogen, the synthesised bio-carbon in a magnetic field has the properties of a ferromagnet with a characteristic hysteresis of the specific magnetisation. It was found that this material has a saturation magnetisation σs of 1.4 A∙m2∙kg−1 and a coercive force Hc of 10 kA/m. Symmetric supercapacitors were fabricated from the synthesised bio-carbon material with 30% aqueous KOH and 1 M Na2SO4 as electrolytes. It was found that for bio-carbon synthesised at 800 °C, the specific capacitance in a 30% aqueous solution of KOH is 180 F/g, and in a 1 M aqueous solution of Na2SO4, it is 124 F/g. The cyclic voltammetry of the fabricated supercapacitors at different rates of potential expansion was investigated and analysed. Impedance studies on these supercapacitors were carried out. The equivalent electrical circuits describing the electrochemical processes in the studied supercapacitors were constructed and characterised.
... In contrast, the carbon electrode's capacitance and Faradaic electrode's conductivity can be improved. [6,7,20,21] Based on the above idea, it decided to develop a hybrid supercapacitor that consists of battery-type materials combined with EDLC electrodes to serve as a positive electrode. ...
Synthesising and designing pseudocapacitive material with good electrochemical and electrocatalytic behaviour is essential to use as supercapacitor as well as non‐enzymatic glucose sensor electrode. In this work, NiCo2S4 nanoparticles decorated onto the 2D‐Carbyne nanosheets are achieved by the solvothermal process. The as‐prepared NiCo2S4@2D‐Carbyne provides rich reaction sites and better diffusion pathways. On usage as an electrode for supercapacitor application, the NiCo2S4@2D‐Carbyne exhibits the specific capacitance of about 2507 F g⁻¹ at 1 A g⁻¹. In addition, the fabricated hybrid device generates an energy density of 52.2 Wh kg⁻¹ at a power density of 1.01 kW kg⁻¹. Besides, the glucose oxidation behaviour of NiCo2S4@2D‐Carbyne modified GCE has also been performed. The diffusion of glucose from the electrolyte to the electrode obeys the kinetic control process. Furthermore, the fabricated NiCo2S4@2D‐Carbyne non‐enzymatic glucose sensor exhibits a limit of detection of about 34.5 μM with a sensitivity of about 135 μA mM⁻¹ cm⁻². These findings highlight the need to design and synthesis electrode materials with adequate electrolyte‐electrode contact, strong structural integrity, and rapid ion/electron transport.
... 2 Therefore, extensive research in nanomaterial-based electrochemical capacitors of low-cost and abundant monometallic/ bimetallic transition metal oxides has been reported because they offer great capacities for the improvement of future energy storage systems, and lower resistance properties. [3][4][5][6][7][8] Moreover, various combinations of carbon nanomaterials modified with transition metal oxides, hydroxides, phosphates and sulfides are reported that exhibit tremendous adsorption capacity, excellent catalytic performance, and specific capacitance. 9 Mainly the Ni and Co-based compounds are widely recognized as important battery and supercapacitor materials due to their desirable electrochemical properties. ...
Mesoporous 2D nanoflakes architectures of mono- and bi-metallic cobalt and nickel hydroxide (meso-Co-Ni(OH)2) hybrids were synthesized using novel chemical precipitation of foam-surfactant liquid crystal dual template (FSDT). The dissolved cobalt and nickel ions within the aqueous region of the Brij®78 surfactant template was reduced by the excess of sodium borohydride reducing agent that simultaneously generates excessive hydrogen foam as a double template. The physicochemical characterizations of the mono- and bi-metallic nanostructured Co-Ni(OH)2 hybrids performed using X-ray diffraction, surface area analyzer, scanning and transmission electrons microscopic techniques showed the formation of highly mesoporous hydroxides 2D nanoflakes architectures having an amorphous structure and surface area up to 253.50 m2/g. The electrochemical and supercapacitance evaluation of the mono-, and bi-metallic mesoporous hydroxides showed excellent Faradaic supercapacitance performance within a wider potential window and a higher charge and discharge rate. In particular the mesoporous monometallic of Co(OH)2, Ni(OH)2, bimetallic Co-Ni(OH)2 with Co/Ni ratios of (1:1), and (1:3), hydroxides showed total capacitances of 204, 869, 943, and 1384, F/g at charging current density of 5.0 A/g respectively and capacity retention rate of approximately 99.4% after 300 cycles. This suggests that these materials hold promise as electrode materials for energy storage applications.
... These advantages make these compounds well-suited for diverse applications such as gas adsorption, solar cells, supercapacitors, Li-ion batteries, fuel cells, electrochemical, and environmental analysis [30]. Over the recent years, two main methods have been employed for the synthesis of nitrogen-doped carbon-based materials, encompassing post-treatment of carbon and in-situ synthesis [31]. Post-treatment of carbon based methods include (i) direct heat treatment using nitrogen-containing precursors, (ii) wet chemical functionalization involving nitrogen-containing compounds followed by hydrothermal carbonization, (iii) plasma, and (iv) arcdischarge techniques. ...
Fe3O4@nitrogen-doped carbon core-double shell nanotubes (Fe3O4@N-C C-DSNTs) were successfully synthesized and applied as a novel nanosorbent in ultrasonic assisted dispersive magnetic solid phase extraction (UA-DMSPE) of tribenuron-methyl, fenpyroximate, and iprodione. Subsequently, corona discharge ion mobility spectrometry (CD-IMS) was employed for the detection of the extracted analytes. Effective parameters on the extraction recovery percentage (ER%) were systematically investigated and optimized. Under optimal conditions, UA-DMSPE-CD-IMS demonstrated remarkable linearity in different ranges within 1.0 – 700 ng mL⁻¹ with correlation coefficients exceeding 0.993, repeatability values below 6.9%, limits of detection ranging from 0.30 to 0.90 ng mL⁻¹, high preconcentration factors (418 - 435), and ER% values (83 – 87%). The potential of the proposed method was further demonstrated by effectively determining the targeted pesticides in various environmental soil and water samples, exhibiting relative recoveries in the range 92.1 – 102%.
Graphical Abstract
... The above results indicated that doped chlorella as a nitrogen source can indeed produce abundant nitrogen-containing functional groups on the porous carbon surface. It has been suggested that pyridine-N and pyrrole-N are considered active sites that can effectively improve pseudocapacitor(Czerw et al., 2001;Deng et al., 2015), and graphite nitrogen can promote rapid electron transfer and enhance electrical conductivity(Hao et al., 2013).Figure 5(c) analyzed the composition and content of nitrogen in different samples, and it can be seen that the nitrogen content of ZBC@C-5 and ZBC@M were very close to each other, which further con rmed that chlorella was an effective nitrogen source. of electrochemical properties of materials in three electrode systems ...
Porous carbon generated from biomass has a rich pore structure, is inexpensive, and has a lot of promise for use as a carbon material for energy storage devices. In this work, nitrogen-doped porous carbon was prepared by co-pyrolysis using bagasse as the precursor and chlorella as the nitrogen source. The thermal weight loss experiments showed that the pyrolysis temperatures of bagasse and chlorella overlap, which created the possibility for the synthesis of nitrogen-rich biochar. The optimum sample (ZBC@C-5) possessed a surface area of 1508 m ² g ⁻¹ with abundant nitrogen-containing functional groups. ZBC@C-5 in the three-electrode system exhibited 244.1F/g at 0.5A/g, which was extremely close to ZBC@M made with melamine as the nitrogen source. This provides new opportunities for the use of low-cost nitrogen sources. Furthermore, the devices exhibit better voltage retention (39%) and capacitance retention (96.3%). The goal of this research is to find a low cost, and effective method for creating nitrogen-doped porous carbon materials with better electrochemical performance for highly valuable applications using bagasse and chlorella.
