o2 reduction
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Membranes ◽  
2022 ◽  
Vol 12 (1) ◽  
pp. 74
Author(s):  
Tar-Hwa Hsieh ◽  
Sin-Nan Chen ◽  
Yen-Zen Wang ◽  
Ko-Shan Ho ◽  
Jung-Kuan Chuang ◽  
...  

Cobalt-doped carbon nitride frameworks (CoNC) were prepared from the calcination of Co-chelated aromatic polyimines (APIM) synthesized from stepwise polymerization of p-phenylene diamine (PDA) and o-phthalaldehyde (OPAl) via Schiff base reactions in the presence of cobalt (II) chloride. The Co-chelated APIM (Co-APIM) precursor converted to CoNC after calcination in two-step heating with the second step performed at 100 °C lower than the first one. The CoNCs demonstrated that its Co, N-co-doped carbonaceous framework contained both graphene and carbon nanotube, as characterized by X-ray diffraction pattern, Raman spectra, and TEM micropictures. CoNCs also revealed a significant ORR peak in the current–voltage polarization cycle and a higher O2 reduction current than that of commercial Pt/C in a linear scanning voltage test in O2-saturated KOH(aq). The calculated e-transferred number even reaches 3.94 in KOH(aq) for the CoNC1000A900 cathode catalyst, which has the highest BET surface area of 393.94 m2 g−1. Single cells of anion exchange membrane fuel cells (AEMFCs) are fabricated using different CoNCs as the cathode catalysts, and CoNC1000A900 demonstrates a peak power density of 374.3 compared to the 334.7 mW cm−2 obtained from the single cell using Pt/C as the cathode catalyst.


Author(s):  
Jason S. Bates ◽  
Sourav Biswas ◽  
Sung-Eun Suh ◽  
Mathew R. Johnson ◽  
Biswajit Mondal ◽  
...  
Keyword(s):  

2022 ◽  
Author(s):  
Yong Cao ◽  
Qi zhang ◽  
Mi Peng ◽  
Zirui Gao ◽  
Wendi Guo ◽  
...  

Abstract Development of biomimetic catalytic systems that can imitate or even surpass natural enzymes remains an ongoing challenge 1–3. This is particularly true in the context of accessing non-natural reactions by bioinspired approaches, which offer intriguing possibilities for benign and affordable chemical synthesis 4. Exploiting the untapped potential of inorganic solids by translating complex knowledge in (bio)molecular-based systems may constitute a potentially useful strategy for such purpose 5, but efforts to capitalize on the minimum catalytic unit of a versatile solid matrix have been largely unsuccessful. Here, we show how an all-inorganic biomimetic system bearing robust nitrogen-neighboured single cobalt site/pyridinic-N site (Co-N4/Py-N) pairs can act cooperatively as an oxidase mimic, which renders an engaged coupling of oxygen (O2) reduction with synthetically beneficial chemical transformations. By developing this broadly applicable platform, the scalable synthesis of greater than 100 industrially and pharmaceutically appealing O-silylated compounds via the unprecedented aerobic oxidation of hydrosilane under ambient conditions is demonstrated. Moreover, this heterogeneous oxidase mimic also offers potential for expanding the catalytic scope of enzymatic synthesis. We anticipate that the strategy demonstrated here will pave a new avenue for understanding the underlying nature of redox enzymes and open up a new class of material systems for artificial biomimetics.


2021 ◽  
Author(s):  
Behnaz Rahmani Didar ◽  
Axel Gross

Density functional theory calculations together with ab initio molecular dynamics (AIMD) simulations have been used to study the solvation, diffusion and transformation of Li+ and LiO2 upon O2 reduction in three organic electrolytes. These processes are critical for the performance of Li-air batteries. Apart from studying the structure of the solvation shells in detail, AIMD simulations have been used to derive the diffusivity and together with the Blue Moon ensemble approach to explore LiO2 formation from Li+ and O2- and the subsequent disproportionation of 2LiO2 into Li2O2 + O2. By comparing the results of the simulations to gas phase calculations the impact of electrolytes on these reactions is assessed which turns out to be more pronounced for the ionic species involved in these reactions.


Catalysts ◽  
2021 ◽  
Vol 11 (11) ◽  
pp. 1404
Author(s):  
Javier Hernández-Ferrer ◽  
Ana M. Benito ◽  
Wolfgang K. Maser ◽  
Enrique García-Bordejé

Carbon nanotubes (CNTs), graphene aerogels (GAs), and their hybrid (CNT-GA) prepared by hydrothermal treatment were tested in the electrocatalytic oxygen reduction reaction (ORR). The importance of porous structure derived from the combination of mesoporosity coming from CNTs with macroporosity stemming from GAs was evidenced because the hybrid carbon material exhibited synergistic performance in terms of kinetic current and onset potential. Different electrocatalysts were prepared based on these hybrids doped with nitrogen using different precursors and also supporting Fe nanoparticles. N-doped carbon hybrids showed higher electrocatalytic activity than their undoped counterparts. Nevertheless, both doped and undoped materials provided a mixed two and four electron reduction. On the other hand, the addition of a Fe precursor and phenanthroline to the CNT-GA allowed preparing an N-doped hybrid containing Fe nanoparticles which favored the 4-electron oxygen reduction to water, thus being an excellent candidate as a structured cathode in fuel cells.


2021 ◽  
Vol 8 (4) ◽  
pp. 267-276
Author(s):  
Fatma Deniz ◽  
Mehmet Ali Mazmancı

Background: Formaldehyde (FA) is a carcinogen compound, which is soluble in water. FA can be removed from aqueous solution using advanced oxidation methods. Methods: In this study, the oxidation of FA was studied under fluorescent and UV light. Hydrogen peroxide (H2 O2 ) was used as an oxidant. The pH value and H2 O2 amount of samples were optimized. The chemical oxygen demand (COD), FA concentration, and H2 O2 consumption were followed. Results: It was observed that the pH value of the sample was more significant under fluorescent light than UV light at oxidation of FA. The highest COD removal and H2 O2 reduction were 18.57 and 30.90%, respectively, at pH 12.00, with a 1:1 ratio of FA:H2 O2 under fluorescent light. 86.41% FA and 62.12% COD removal were achieved at pH 7.00, with a 1:2 ratio of FA:H2 O2 , under UV light. It was observed that H2 O2 was consumed at all pH values under UV light. On the other hand, under fluorescent light, the concentration of H2 O2 decreased only at pH 12. In control samples containing only H2 O2 , the H2 O2 reduction was 92.09% at pH 11.91, while it was 2-6% at other pH levels under fluorescent light. The H2 O2 reduction changed between 33 and 44% at different pH values under UV light. The oxidation of FA was found to be suitable for the pseudo-first-order kinetic model and Langmuir isotherm model. Conclusion: The most effective oxidation was obtained at the original pH value (7.00) and 1:2 ratio of FA:H2 O2 under UV light.


Author(s):  
Pongkarn Chakthranont ◽  
Sakvarit Nitrathorn ◽  
Sutarat Thongratkaew ◽  
Pongtanawat Khemthong ◽  
Hideki Nakajima ◽  
...  

Polymers ◽  
2021 ◽  
Vol 13 (21) ◽  
pp. 3850
Author(s):  
Yu-Wei Cheng ◽  
Wen-Yao Huang ◽  
Ko-Shan Ho ◽  
Tar-Hwa Hsieh ◽  
Li-Cheng Jheng ◽  
...  

Aromatic polyimine (PIM) was prepared through condensation polymerization between p-phenylene diamine and terephthalaldehyde via Schiff reactions. PIM can be physically crosslinked with ferrous ions into gel. The gel-composites, calcined at two consecutive stages, with temperatures ranging from 600 to 1000 °C, became Fe- and N-doped carbonaceous organic frameworks (FeNC), which demonstrated both graphene- and carbon nanotube-like morphologies and behaved as an electron-conducting medium. After the two-stage calcination, one at 1000 °C in N2 and the other at 900 °C in a mixture of N2 and NH3, an FeNC composite (FeNC-1000A900) was obtained, which demonstrated a significant O2 reduction peak in its current–voltage curve in the O2 atmosphere, and thus, qualified as a catalyst for the oxygen reduction reaction. It also produced a higher reduction current than that of commercial Pt/C in a linear scanning voltage test, and the calculated e-transferred number reached 3.85. The max. power density reached 400 mW·cm−2 for the single cell using FeNC-1000A900 as the cathode catalyst, which was superior to other FeNC catalysts that were calcined at lower temperatures. The FeNC demonstrated only 10% loss of the reduction current at 1600 rpm after 1000 redox cycles, as compared to be 25% loss for the commercial Pt/C catalyst in the durability test.


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