“…35,55 Interestingly, pyridinic N accounts for the highest percentage (38.64 at.%) in the N atomic concentration, followed by C-N-B bonding (27.6 at.%), implying that a large number of ORR active sites exists in our BCN nanosheets. 43,56,57 In agreement with XRD, Raman and FTIR, the XPS results demonstrate the successful synthesis of BCN nanosheets. In addition, the potential complementary effects of B and N atoms as well as adjustable electronic structure of carbon should greatly benefit the electrochemical activity as ORR catalysts.…”
supporting
confidence: 77%
“…47 A typical shift of the G band (1600cm -1 ) in BCN is observed from pure graphene (1580cm -1 ), attributing to the structural distortion of graphitic carbon with different bond lengths of N-B and C-N. 41 Besides, the appearance of relatively weak 2D band indicates the presence of a few layers in BCN nanosheets, 46 conforming to XRD analysis. Noticeably, the relative intensity of I D /I G , which represents the level of defects and heteroatom doping, 52 is 0.945 in this study, less than most of the B,N co-doped graphene (I D /I G >1) [38][39][40][41][42][43][44][45] . On one hand, it suggests that local structures of our BCN nanosheets evolve towards graphitization instead of highly defective and disordered heterojunctions.…”
mentioning
confidence: 91%
“…Although B, N doped CNTs, 36,37 graphene [38][39][40] or BCN nanostructures [41][42][43][44][45] have been reported as effective ORR catalysts in alkaline media, no research has proposed the ORR electrocatalysis by metal-free BCN in acid condition. Hence, it is a challenge to developing a BCN-based nanostructured electrocatalyst performing not only in alkaline, but also in acid environment.…”
Carbon materials have become a hot topic as potential substitutes for Pt/C catalysts for the oxygen reduction reaction (ORR). However, most of them exhibit their catalytic activities only in alkaline solutions, which severely limits their application in polyelectrolyte membrane fuel cells. To address this issue, here porous boron carbon nitride (BCN) nanosheets are fabricated by a facile and efficient polymer sol−gel method, which involves the annealing of polyvinylic akohol (PVA), boric acid, guanidine, and poly(ethylene oxide-co-propylene oxide) (P123) gel mixtures. The as-prepared porous BCN nanosheets possess a high surface area of 817 m 2 /g and display impressive ORR catalytic performance in both alkaline and acidic media, rivalling that of commercial Pt/C and other recently reported carbon materials. Importantly, the resulting metal-free catalysts exhibit much greater durability and higher methanol tolerance in both alkaline and acidic environments. This study provides a new insight into metal-free ORR catalysts that are practicable in industrial fuel cells.
“…35,55 Interestingly, pyridinic N accounts for the highest percentage (38.64 at.%) in the N atomic concentration, followed by C-N-B bonding (27.6 at.%), implying that a large number of ORR active sites exists in our BCN nanosheets. 43,56,57 In agreement with XRD, Raman and FTIR, the XPS results demonstrate the successful synthesis of BCN nanosheets. In addition, the potential complementary effects of B and N atoms as well as adjustable electronic structure of carbon should greatly benefit the electrochemical activity as ORR catalysts.…”
supporting
confidence: 77%
“…47 A typical shift of the G band (1600cm -1 ) in BCN is observed from pure graphene (1580cm -1 ), attributing to the structural distortion of graphitic carbon with different bond lengths of N-B and C-N. 41 Besides, the appearance of relatively weak 2D band indicates the presence of a few layers in BCN nanosheets, 46 conforming to XRD analysis. Noticeably, the relative intensity of I D /I G , which represents the level of defects and heteroatom doping, 52 is 0.945 in this study, less than most of the B,N co-doped graphene (I D /I G >1) [38][39][40][41][42][43][44][45] . On one hand, it suggests that local structures of our BCN nanosheets evolve towards graphitization instead of highly defective and disordered heterojunctions.…”
mentioning
confidence: 91%
“…Although B, N doped CNTs, 36,37 graphene [38][39][40] or BCN nanostructures [41][42][43][44][45] have been reported as effective ORR catalysts in alkaline media, no research has proposed the ORR electrocatalysis by metal-free BCN in acid condition. Hence, it is a challenge to developing a BCN-based nanostructured electrocatalyst performing not only in alkaline, but also in acid environment.…”
Carbon materials have become a hot topic as potential substitutes for Pt/C catalysts for the oxygen reduction reaction (ORR). However, most of them exhibit their catalytic activities only in alkaline solutions, which severely limits their application in polyelectrolyte membrane fuel cells. To address this issue, here porous boron carbon nitride (BCN) nanosheets are fabricated by a facile and efficient polymer sol−gel method, which involves the annealing of polyvinylic akohol (PVA), boric acid, guanidine, and poly(ethylene oxide-co-propylene oxide) (P123) gel mixtures. The as-prepared porous BCN nanosheets possess a high surface area of 817 m 2 /g and display impressive ORR catalytic performance in both alkaline and acidic media, rivalling that of commercial Pt/C and other recently reported carbon materials. Importantly, the resulting metal-free catalysts exhibit much greater durability and higher methanol tolerance in both alkaline and acidic environments. This study provides a new insight into metal-free ORR catalysts that are practicable in industrial fuel cells.
“…Generally, two major methods have been adopted for preparing electrospun porous carbon nanofibers i. e., sacrificial component methods and activation methods. Thermally induced selective phase separation method is widely recognized as a suitable method for preparing porous structure and the commonly used porogens are hard template, soluble salts or, sacrificial polymers ,,,. Therefore, it is highly desirable to design and fabricate hollow carbon nanofibers tailored with numerous regular mesopores for achieving high‐performance electrodes to be used in fuel cells.…”
An electrocatalyst support material based on hierarchical mesoporous hollow carbon nanofibers (mPHCNFs) has been developed by co-axial electrospinning and has been deployed for the fabrication of polymer electrolyte membrane fuel cells (PEMFCs). The synergistic effect of a high specific surface area (780 m 2 /g), homogeneous formation of mesopores (20-50 nm), and hollow nanochannels in the carbon nanofiber matrix lead to the uniform distribution of Pt electrocatalysts. XPS analysis revealed that the presence of nitrogen species in the mesoporous hollow carbon nanofibers in the form of pyridinic, pyrrolic, and quaternary nitrogen atoms played a crucial role in the augmentation of triple-phase boundaries. Pt/mPHCNFs exhibited superior electrocatalytic activity towards the oxygen reduction reaction with a positively shifted onset potential (62 mV) and half-wave potential (86 mV) as well as a high limiting current density (4.76 mA/cm 2 ) compared to commercial electrocatalysts. The Pt/mPHCNFs catalyst exhibited excellent stability in acidic medium and showed only 23 mV loss in the half-wave potential; whereas, Pt/CNFs (35 mV) and Pt/C (77 mV) exhibited a much higher shift in half-wave potential. The PEMFC testing of the membrane electrode assembly based on Pt/ mPHCNFs (411 mW/cm 2 ) revealed a superior performance compared to Pt/CNFs (297.4 mW/cm 2 ) and Pt/C (212.8 mW/cm 2 ). This method can offer an effective strategy for the development of durable, low-cost, and high-performance PEMFCs.
“…Being the most promising alternative, carbon-based metal-free catalysts not only possess the advantages of low cost, abundance, and easy accessibility, but also have an easily tailored composition and a tunable pore structure [7][8][9][10][11][12][13]. To improve electrocatalytic activity, heteroatoms like N, B, P, O, and S are often used to dope carbon materials, facilitating the chemical adsorption of oxygen and providing more effective active sites [14][15][16]. However, the incorporated heteroatoms may decrease conductivity and thus hinder charge transport to some extent [17,18].…”
Carbon-based metal-free catalysts are a promising substitute for the rare and expensive platinum (Pt) used in the oxygen reduction reaction. We herein report N-doped graphene (NG) that is exquisitely integrated into highly conductive frameworks, simultaneously providing more active sites and higher conductivity. The NG was in situ grown on carbon fibers derived from silk cocoon (SCC f ) using a simple one-step thermal treatment. The resulting product (NG-SCC f ), possessing a meso-/macroporous structure with three-dimensional (3D) interconnected networks, exhibits an onset potential that is only 0.1 V less negative than that of Pt/C and shows stability and methanol tolerance superior to those of Pt/C in alkaline media. Moreover, in the absence of Pt as co-catalyst, NG-SCC f shows a photocatalytic H 2 production rate of 66.0 μmol·h -1 ·g -1 , 4.4-fold higher than that of SCC f . This outstanding activity is intimately related to the in situ grown NG, hierarchically porous structure, and 3D interconnected networks, which not only introduce more active sites but also enable smooth electron transfer, mass transport, and effective separation of electron-hole pairs. Considering the abundance of the green raw material in combination with easy and low-cost preparation, this work contributes to the development of advanced sustainable catalysts in energy storage/conversion fields, such as electro-and photocatalysis.
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