Abstract:Exploring efficient and low‐cost catalysts for the oxygen reduction reaction (ORR) is a key issue in the development of renewable energy devices such as fuel cells and metal−air batteries. The design and construct of advanced catalysts can be guided by identifying the sites with high activity. In this study, an indicative research study on the ORR of yam‐derived N and S self‐doped porous carbons (NSDCs) is presented. The NSDC optimized at 800 °C (NSDC800) with more exposed intrinsic N and S active sites shows … Show more
“…It implies that the graphitic N and pyridinic N groups account for the majority. The S2p XPS spectra reveals that S atoms are in the form of oxidic‐S (‐C‐SO 4 ‐ (169.8 eV), ‐C‐SO 3 ‐ (168.3 eV), ‐C‐SO 2 ‐ (166.2 eV)), thiophenic‐S (S2p 1/2 (165.1 eV)and S2p 3/2 (163.9 eV)) and H 2 S (170.7 eV), as shown in Figure c and Figure S1e, and the thiophenic‐S is dominated in the sulfur species . Figure d shows that the percentages of the four types of N and thiophenic‐S, and it is easy to observe that the contents both of graphitic N and thiophenic‐S of S3/N‐CNS800 are more than those of S3/N‐CN800.…”
Developing eco-friendly, high-efficiency and cost-effective catalysts for oxygen reduction reaction are significantly crucial for the application of direct-methanol fuel cells. The metal-free sulfur/nitrogen in-situ co-doped carbon nanosheets are prepared through polymerization process and carbonization process using aniline as a nitrogen source, 4-aminobenzenesulfonamide as a sulfur source and NaCl as a template and protective layer. The obtained catalysts show the obvious two dimensional nanosheet structure with successful doping of S and N. Benefiting from high contents of S atoms and N atom, high special surface area and graphitic degree, well-ordered micropores and synergetic interaction between thiophenic-S, pyridinic N and graphitic N, the optimal catalyst S3/N-CNS800 shows excellent oxygen reduction performance with 13.2 mV more positive half-wave potential than that of 20% Pt/C, superior long-term durability and tolerance to methanol crossover.
Results and DiscussionThe synthesis of the carbon nanosheets is described in the Experimental Section, as shown in Scheme 1, which contains [a] C.
“…It implies that the graphitic N and pyridinic N groups account for the majority. The S2p XPS spectra reveals that S atoms are in the form of oxidic‐S (‐C‐SO 4 ‐ (169.8 eV), ‐C‐SO 3 ‐ (168.3 eV), ‐C‐SO 2 ‐ (166.2 eV)), thiophenic‐S (S2p 1/2 (165.1 eV)and S2p 3/2 (163.9 eV)) and H 2 S (170.7 eV), as shown in Figure c and Figure S1e, and the thiophenic‐S is dominated in the sulfur species . Figure d shows that the percentages of the four types of N and thiophenic‐S, and it is easy to observe that the contents both of graphitic N and thiophenic‐S of S3/N‐CNS800 are more than those of S3/N‐CN800.…”
Developing eco-friendly, high-efficiency and cost-effective catalysts for oxygen reduction reaction are significantly crucial for the application of direct-methanol fuel cells. The metal-free sulfur/nitrogen in-situ co-doped carbon nanosheets are prepared through polymerization process and carbonization process using aniline as a nitrogen source, 4-aminobenzenesulfonamide as a sulfur source and NaCl as a template and protective layer. The obtained catalysts show the obvious two dimensional nanosheet structure with successful doping of S and N. Benefiting from high contents of S atoms and N atom, high special surface area and graphitic degree, well-ordered micropores and synergetic interaction between thiophenic-S, pyridinic N and graphitic N, the optimal catalyst S3/N-CNS800 shows excellent oxygen reduction performance with 13.2 mV more positive half-wave potential than that of 20% Pt/C, superior long-term durability and tolerance to methanol crossover.
Results and DiscussionThe synthesis of the carbon nanosheets is described in the Experimental Section, as shown in Scheme 1, which contains [a] C.
“…The porous features of Fe-PIPhen/C were further characterized by N 2 adsorption-desorption measurements. The N 2 adsorption-desorption isotherm of Fe-PIPhen/C is shown in Figure 3, it represents the type-III of N 2 adsorption/desorption isotherms with large specific surface areas and pore volumes (Fan et al, 2017). As summarized in Table 1, the BET surface area and the pore volume of the Vulcan XC-72 carbon and Fe-PIPhen/C are 108.665 m 2 /g, 1.338 cm 3 /g, and 77.849 m 2 /g, 0.90 cm 3 /g, respectively.…”
In this work, the synthesis and evaluation of a new type non-noble metal oxygen reduction reaction (ORR) catalyst is reported. The catalyst is a complex containing iron ions and multiple N active sites, which displayed excellent oxygen reduction activity in alkaline medium. 2-(2-(4-(1H-imidazo[4,5-f][1,10]phenanthrolin-2-yl)pyridin-2-yl)pyridin-4-yl)-1H-imidazo[4,5-f][1,10]phenanthroline (PIPhen) was synthesized and used as a ligand to form a rich nitrogen iron coordination complex (Fe-PIPhen), and the complex was then loaded onto the carbon powder to form the target catalyst of Fe-PIPhen/C. The physical characterization of the catalyst was conducted by using Scanning Electron Microscopy (SEM), nitrogen adsorption-desorption and X-ray photoelectron spectroscopy (XPS), Brunauer-Emmett-Teller analysis etc. Electrochemical characterizations were realized by taking cyclic voltammetry (CV), linear sweep voltammetry (LSV) and rotating ring disk electrode (RRDE). The results show that Fe-PIPhen/C possesses the good performance; it exhibits a high electrocatalytic activity, which is mainly via a four electron ORR pathway, with a low hydrogen peroxide yield of 2.58%. And, the average electron transfer number of 3.93 was obtained in alkaline electrolyte. In summary, Fe-PIPhen/C will likely become a promising alternative to Pt catalyst in fuel cell.
“…As one of the widely distributed and resource-rich green crop, yam has richened starch, protein, and other components, which has attracted great attention in catalysis . Yao et al developed nanoporous carbon microspheres obtained by hydrothermal carbonization and annealing of starch, featuring a high surface area and pore volume and performing good catalytic activities . However, owing to high-temperature pyrolysis during carbonization, the starch-derived carbons partially lose the typical spherical morphology of starch in nature.…”
Section: Introductionmentioning
confidence: 99%
“…28 Yao et al 29 developed nanoporous carbon microspheres obtained by hydrothermal carbonization and annealing of starch, featuring a high surface area and pore volume and performing good catalytic activities. 30 However, owing to high-temperature pyrolysis during carbonization, the starch-derived carbons partially lose the typical spherical morphology of starch in nature. It is believed that the spherical structure of carbons features a curved surface structure and good surface accessibility, which can substantially boost ORR performance.…”
Plant-derived
nonprecious metal catalysts are considered one of
the promising candidates of platinum for oxygen reduction reaction
(ORR). In this work, the typical microscopic morphology of fresh green
crop yam is first detected by cryoscanning electronic microscopy.
Using the green and widely sourced yam with spherical starch in nature
as a precursor, well-defined spherical carbons are prepared via hypersaline-assisted
hydrothermal carbonization and NH3activation, featuring
a high heteroatom doping level and a hierarchical porous structure.
Experimental results and density functional theory (DFT) calculations
reveal that diverse off-plane Fe–N
x
–C
y
ensembles on the spherical
carbons trigger the high performance that exceeds state-of-art Pt/C
and most reported carbon catalysts toward ORR in a KOH solution. The
increased charge density and the bond length of Fe coordinated in
the sites should be responsible for the significantly improved property.
The easily editing of off-plane active sites from the simple carbon
morphology may shed light on optimizing nonprecious carbons as next-generation
catalysts for ORR.
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