Regulating contents evolution of valence bonds on carbon surface to inhibit dissolution of polysulfides during production

Carbon ◽  
2020 ◽  
Vol 169 ◽  
pp. 142-154
Author(s):  
Caiwei Wang ◽  
Jianfeng Huang ◽  
Yixuan Huang ◽  
Chaozheng He ◽  
Jiayin Li ◽  
...  
Keyword(s):  
2020 ◽  
Author(s):  
Weihong Lai ◽  
Heng Wang ◽  
Quan jiang ◽  
Zichao Yan ◽  
Hanwen Liu ◽  
...  

<p>Herein, we develop a non-selective charge compensation strategy to prepare multi-single-atom doped carbon (MSAC) in which a sodium p-toluenesulfonate (PTS-Na) doped polypyrrole (S-PPy) polymer is designed to anchor discretionary mixtures of multiple metal cations, including iron (Fe<sup>3+</sup>), cobalt (Co<sup>3+</sup>), ruthenium (Ru<sup>3+</sup>), palladium (Pd<sup>2+</sup>), indium (In<sup>3+</sup>), iridium (Ir<sup>2+</sup>), and platinum (Pt<sup>2+</sup>) . As illustrated in Figure 1, the carbon surface can be tuned with different level of compositional complexities, including unary Pt<sub>1</sub>@NC, binary (MSAC-2, (PtFe)<sub>1</sub>@NC), ternary (MSAC-3, (PtFeIr)<sub>1</sub>@NC), quaternary (MSAC-4, (PtFeIrRu)<sub>1</sub>@NC), quinary (MSAC-5, (PtFeIrRuCo)<sub>1</sub>@NC), senary (MSAC-6, (PtFeIrRuCoPd)<sub>1</sub>@NC), and septenary (MSAC-7, (PtFeIrRuCoPdIn)<sub>1</sub>@NC) samples. The structural evolution of carbon surface dictates the activities of both ORR and HER. The senary MSAC-6 achieves the ORR mass activity of 18.1 A·mg<sub>metal</sub><sup>-1</sup> at 0.9 V (Vs reversible hydrogen electrode (RHE)) over 30K cycles, which is 164 times higher than that of commercial Pt/C. The quaternary MSAC-4 presented a comparable HER catalytic capability with that of Pt/C. These results indicate that the highly complexed carbon surface can enhance its ability over general electrochemical catalytic reactions. The mechanisms regarding of the ORR and HER activities of the alternated carbon surface are also theoretically and experimentally investigated in this work, showing that the synergistic effects amongst the co-doped atoms can activate or inactivate certain single-atom sites.</p>


Author(s):  
Xi Yin ◽  
Ling Lin ◽  
Hoon T. Chung ◽  
Ulises Martinez ◽  
Andrew M. Baker ◽  
...  

Finding a low-cost and stable electrocatalyst for hydrogen evolution reaction (HER) as a replacement for scarce and expensive precious metal catalysts has attracted significant interest from chemical and materials research communities. Here, we demonstrate an organic catalyst based on 2,2’-dipyridylamine (dpa) molecules adsorbed on carbon surface, which shows remarkable hydrogen evolution activity and performance durability in strongly acidic polymer electrolytes without involving any metal. The HER onset potential at dpa adsorbed on carbon has been found to be less than 50 mV in sulfuric acid and in a Nafion-based membrane electrode assembly (MEA). At the same time, this catalyst has shown no performance loss in a 60-hour durability test. The HER reaction mechanisms and the low onset overpotential in this system are revealed based on electrochemical study. Density functional theory (DFT) calculations suggest that the pyridyl-N functions as the active site for H adsorption with a free energy of -0.13 eV, in agreement with the unusually low onset overpotential for an organic molecular catalyst.<br>


2019 ◽  
Author(s):  
Xi Yin ◽  
Ling Lin ◽  
Hoon T. Chung ◽  
Ulises Martinez ◽  
Andrew M. Baker ◽  
...  

Finding a low-cost and stable electrocatalyst for hydrogen evolution reaction (HER) as a replacement for scarce and expensive precious metal catalysts has attracted significant interest from chemical and materials research communities. Here, we demonstrate an organic catalyst based on 2,2’-dipyridylamine (dpa) molecules adsorbed on carbon surface, which shows remarkable hydrogen evolution activity and performance durability in strongly acidic polymer electrolytes without involving any metal. The HER onset potential at dpa adsorbed on carbon has been found to be less than 50 mV in sulfuric acid and in a Nafion-based membrane electrode assembly (MEA). At the same time, this catalyst has shown no performance loss in a 60-hour durability test. The HER reaction mechanisms and the low onset overpotential in this system are revealed based on electrochemical study. Density functional theory (DFT) calculations suggest that the pyridyl-N functions as the active site for H adsorption with a free energy of -0.13 eV, in agreement with the unusually low onset overpotential for an organic molecular catalyst.<br>


2008 ◽  
Author(s):  
P. M. Natishan ◽  
F. J. Martin ◽  
E. J. Lemieux ◽  
T. M. Newbauer ◽  
R. Rayne ◽  
...  

2008 ◽  
Vol 73 (6-7) ◽  
pp. 755-770 ◽  
Author(s):  
Andriy Pysanenko ◽  
Ján Žabka ◽  
Zdeněk Herman

The scattering of the hydrocarbon radical cation C2D4•+ from room-temperature carbon (highly oriented pyrolytic graphite, HOPG) surface was investigated at low incident energies of 6-12 eV. Mass spectra, angular and translational energy distributions of product ions were measured. From these data, information on processes at surfaces, absolute ion survival probability, and kinematics of the collision was obtained. The projectile ion showed both inelastic, dissociative and reactive scattering, namely the occurrence of H-atom transfer reaction with hydrocarbons present on the room-temperature carbon surface. The absolute survival probability of the ions for the incident angle of 30° (with respect to the surface) decreased from about 1.0% (16 eV) towards zero at incident energies below 10 eV. Estimation of the effective surface mass involved in the collision process led to m(S)eff of about 57 a.m.u. for inelastic non-dissociative collisions of C2D4•+ and of about 115 a.m.u. for fragment ions (C2D3+, C2D2•+) and ions formed in reactive surface collisions (C2D4H+, C2D2H+, contributions to C2D3+ and C2D2•+). This suggested a rather complex interaction between the projectile ion and the hydrocarbon-covered surface during the collision.


2021 ◽  
Vol 11 (1) ◽  
Author(s):  
Lilla Fijołek ◽  
Joanna Świetlik ◽  
Marcin Frankowski

AbstractIn water treatment technology, activated carbons are used primarily as sorbents to remove organic impurities, mainly natural organic matter, but also as catalysts in the ozonation process. Commercially available activated carbons are usually contaminated with mineral substances, classified into two main groups: alkali metals (Ca, Na, K, Li, Mg) and multivalent metals (Al, Fe, Ti, Si). The presence of impurities on the carbon surface significantly affects the pHpzc values determined for raw and ozonated carbon as well as their acidity and alkalinity. The scale of the observed changes strongly depends on the pH of the ozonated system, which is related to the diffusion of impurities from the carbon to the solution. In an acidic environment (pH 2.5 in this work), the ozone molecule is relatively stable, yet active carbon causes its decomposition. This is the first report that indirectly indicates that contaminants on the surface of activated carbon (multivalent elements) contribute to the breakdown of ozone towards radicals, while the process of ozone decomposition by purified carbons does not follow the radical path in bulk solution. Carbon impurities also change the distribution of the reaction products formed by organic pollutants ozonation, which additionally confirms the radical process. The study showed that the use of unpurified activated carbon in the ozonation of succinic acid (SA) leads to the formation of a relatively large amount of oxalic acid (OA), which is a product of radical SA degradation. On the other hand, in solutions with purified carbon, the amount of OA generated is negligible.


Materials ◽  
2021 ◽  
Vol 14 (11) ◽  
pp. 3114
Author(s):  
Bartosz Hekner ◽  
Jerzy Myalski ◽  
Patryk Wrześniowski ◽  
Tomasz Maciąg

In this paper, the applicability of aluminium matrix composites to high-temperature working conditions (not exceeding the Al melting point) was evaluated. The behaviour of Al-Ti-C composites at elevated temperatures was described based on microstructural and phase composition observations for composites heated at temperatures of 540 and 600 °C over differing time intervals from 2 to 72 h. The materials investigated were aluminium matrix composites (AMC) reinforced with a spatial carbon (C) structure covered by a titanium (Ti) layer. This layer protected the carbon surface against contact with the aluminium during processing, protection which was maintained for the material’s lifetime and ensured the required phase compositions of Al4C3 phase limitation and AlTi3 phase creation. It was also proved that heat treatment influenced not only phase compositions but also the microstructure of the material, and, as a consequence, the properties of the composite.


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