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21.
《International Journal of Hydrogen Energy》2022,47(43):18663-18674
Developing non-precious metal-based catalysts as the substitution of precious catalysts (Pt/C) in oxygen reduction reaction (ORR) is crucial for energy devices. Herein, a template and organic solvent-free method was adopted to synthesize Fe, B, and N doped nanoflake-like carbon materials (Fe/B/N–C) by pyrolysis of monoclinic ZIF-8 coated with iron precursors and boric acid. Benefiting from introducing B into Fe–N–C, the regulated electron cloud density of Fe-Nx sites enhance the charge transfer and promotes the ORR process. The as-synthesized Fe/B/N–C electrocatalyst shows excellent ORR activity of a half-wave potential (0.90 V vs 0.87 V of Pt/C), together with superior long-term stability (95.5% current density retention after 27 h) in alkaline media and is even comparable to the commercial Pt/C catalyst (with a half-wave potential of 0.74 V vs 0.82 V of Pt/C) in an acidic electrolyte. A Zn-air battery assembled with Fe/B/N–C as ORR catalyst delivers a higher open-circuit potential (1.47 V), specific capacity (759.9 mA h g?1Zn at 10 mA cm?2), peak power density (62 mW cm?2), as well as excellent durability (5 mA cm?2 for more than 160 h) compared to those with commercial Pt/C. This work provides an effective strategy to construct B doped Fe–N–C materials as nonprecious ORR catalyst. Theoretical calculations indicate that introduction of B could induce Fe-Nx species electronic configuration and is favorable for activation of OH1 intermediates to promote ORR process. 相似文献
22.
《International Journal of Hydrogen Energy》2022,47(47):20494-20506
Proton exchange membrane fuel cells (PEMFCs) durability has been severely hindered by carbon support poor stability in the cathodic Pt-based catalyst. Herein, a high-surface-area nitrogen-doped graphitic nanocarbon (N-G-CA) with mesopores is developed as Pt support to address PEMFCs durability challenge. Resorcinol-formaldehyde aerogel pyrolyzed carbon aerogel is selected as N-G-CA raw material. Nitrogen atoms are introduced into carbon aerogel via NH3 heat treatment. Then, nitrogen-doped carbon aerogel is transferred into N-G-CA via heating together with transition-metal salts (one of FeCl3, FeCl2, CoCl2, or MnCl2, etc.) at 1200 °C. As ORR catalyst, Pt/N-G-CA half-wave potential only lost 10 mV, after 30, 000 cycles accelerated aging test in the rotating-desk-electrode. Only 12 mV voltage loss at 1.5 A/cm2 is observed, after 5, 000 cycles for membrane electrode. Pt/N-G-CA exhibits superior durability and activity than commercial Pt/C. High durability of Pt/N-G-CA is due to N-G-CA high graphitization extent, as well as the interactions between doping nitrogen and Pt. N-G-CA is promising as stable support for durable Pt-based catalysts in PEMFCs, thanks to enhanced carbon corrosion resistance, uniformly dispersed Pt, and strong support-metals interaction. 相似文献
23.
《International Journal of Hydrogen Energy》2022,47(95):40340-40348
The enhancement in intrinsic catalytic activity and material conductivity of an electrocatalyst can leads to promoting HER activity. Herein, a successful nitrogenation of CoS2 (N–CoS2) catalyst has been investigated through the facile hydrothermal process followed by N2 annealing treatment. An optimized N–CoS2 catalyst reveals an outstanding hydrogen evolution reaction (HER) performance in alkaline as well as acidic electrolyte media, exhibiting an infinitesimal overpotential of ?0.137 and ?0.097 V at a current density of ?10 mA/cm2 (?0.309 and ?0.275 V at ?300 mA/cm2), corresponding respectively, with a modest Tafel slope of 117 and 101 mV/dec. Moreover, a static voltage response was observed at low and high current rates (?10 to ?100 mA/cm2) along with an excellent endurance up to 50 h even at ?100 mA/cm2. The excellent catalytic HER performance is ascribed to improved electronic conductivity and enhanced electrochemically active sites, which is aroused from the synergy and mutual interaction between heteroatoms that might have varied the surface chemistry of an active catalyst. 相似文献
24.
Borazine rings act as a pivotal part in siliconboroncarbonitride ceramics (SiBCN) for high-temperature stability and great resistance to crystallization. A detailed investigation of the ring formation mechanism will guide the design and synthesis of SiBCN to meet application requirements under extreme conditions. Boron trichloride (BCl3) and hexamethyldisilazane (HN(SiMe3)2) are common raw materials for the synthesis of precursors for SiBCN. In this paper, quantum chemical calculation was used to study the cyclization reaction mechanism between BCl3 and HN(SiMe3)2 to form trichloroborazine (TCBZ) at the MP2/6-31G (d,p) level of theory. We discussed the structure properties, reaction pathways, energy barriers, reaction rates, and other aspects in detail. The results show that BCl3 and HN(SiMe3)2 alternately participate in the reaction process, accompanied by the release of trimethylchlorosilane (TMCS), and that the entire reaction shows an absolute advantage in terms of energy. In the Step by step reaction, lower reaction barriers are formed due to the introduction of BCl3 with more heat released compared to that for the introduction of HN(SiMe3)2. The final single-molecule cyclization and TMCS elimination steps are found to be faster compared to all previous bimolecular reactions. 相似文献
25.
《International Journal of Hydrogen Energy》2022,47(70):30172-30177
Sulfured doped carbon electrocatalysts is synthesized from the waste biomass Sargassum spp. Two doping procedures are examined to determine which is better for Oxygen Reduction Reaction (ORR); one by doping biocarbon obtained from the pyrolysis of the biomass and the second through a process of in situ doping in autoclave. The electrocatalyst are obtained from pyrolysis of the sample at 700 °C, which is finally characterized as a metal free electrocatalyst for the ORR. The electrocatalyst are characterized by BET surface area analysis, Raman spectroscopy, X-ray Photoelectron Spectroscopy (XPS) and the electrochemical characterization is determined in 0.1 M KOH. The sample SSKPT-1 exhibits a promising electrocatalytic activity with an onset potential of 0.896 V vs RHE and a current density of 5 mA cm?2 (at 0.2 V vs. RHE) which could be partly attributed to its high BET surface area of 2755 m2 g?1. 相似文献
26.
《International Journal of Hydrogen Energy》2022,47(49):21033-21043
Magnetron sputtered low-loading iridium-ruthenium thin films are investigated as catalysts for the Oxygen Evolution Reaction at the anode of the Proton Exchange Membrane Water Electrolyzer. Electrochemical performance of 50 nm thin catalysts (Ir pure, Ir–Ru 1:1, Ir–Ru 1:3, Ru pure) is tested in a Rotating Disk Electrode. Corresponding Tafel slopes are measured before and after the CV-based procedure to compare the activity and stability of prepared compounds. Calculated activities prior to the procedure confirm higher activity of ruthenium-containing catalysts (Ru pure > Ir–Ru 1:3 > Ir–Ru 1:1 > Ir pure). However, after the procedure a higher activity and less degradation of Ir–Ru 1:3 is observed, compared to Ir–Ru 1:1, i.e. the sample with a higher amount of unstable ruthenium performs better. This contradicts the expected behavior of the catalyst. The comprehensive chemical and structural analysis unravels that the stability of Ir–Ru 1:3 sample is connected to RuO2 chemical state and hcp structure. Obtained results are confirmed by measuring current densities in a single cell. 相似文献
27.
We report a simple processing method to simultaneously improve the efficiency and stability of organic solar cells (OSCs). Poly(4-styrene sulfonate)-doped poly(3,4-ethylenedioxy-thiophene (PEDOT:PSS), widely used as hole transport layer (HTL) in OSCs, tends to accelerate the degradation of devices because of its hygroscopic and acidic properties. In this regard, we have modified PEDOT:PSS to reduce its hygroscopic and acidic properties through a condensation reaction between PEDOT:PSS and poly(ethylene glycol) methyl ether (PEGME) in order to improve the efficiency and stability of OSCs. As a result, the power conversion efficiency (PCE) increased by 21%, from 2.57% up to 3.11%. A better energy level alignment by the reduced work function of the modified PEDOT:PSS with a highest occupied molecular orbital (HOMO) level of poly(3-hexylthiophene-2,5-diyl) (P3HT) is considered the origin of the improved the efficiency. The half-life of OSCs with PEDOT:PSS modified with PEGME buffer layer also increased up to 3.5 times compared to that of devices with pristine PEDOT:PSS buffer layer. 相似文献
28.
Amir Abdolmaleki Mohammad Reza Molavian 《Polymer-Plastics Technology and Engineering》2015,54(12):1241-1250
2,6-Bis(5-amino-1H-benzimidazol-2-yl)pyridine was prepared and characterized by Fourier transform infrared spectroscopy, elemental analysis, 1H-NMR, and 13C-NMR spectroscopic methods. Then a new poly(benzimidazole-amide) was synthesized by polymerization of the corresponding diamine and isophthalic acid. The obtained poly(benzimidazole-amide) exhibited good yield and high thermal stability. Due to the existence of benzimidazole moieties in polymer’s structure, it has the tendency to form complexes with metal ions. So, a new poly(benzimidazole-amide)/Co nanocomposite was prepared. Morphological studies revealed that metal nanoparticles were dispersed in the polymer matrix without any aggregation. poly(benzimidazole-amide)/Co nanocomposite was used as a catalyst in the oxidation of ethyl benzene to acetophenone with tert-butyl hydroperoxide. 相似文献
29.
Gel state reactions offer new direction for the reactivity of the organic molecules or metal‐organic materials upon photoirradiation with shorter reaction times and high yields compared to solid and solution states. The restricted molecular movement among the molecules in the soft solids control the stereoselectivity of the photoproducts in the gel state reactions. To date, most of the strategies based on self‐assembly have been demonstrated in the solid state, in particular for [2+2] reactions of olefins and polymerization reactions of diacetylenes via 1,4 addition. The soft materials are of emerging materials in recent days given their many applicative day‐to‐day aspects. This review gives a glimpse of recent reports on pericyclic reactions in the gel state that are designed based on the self‐assembly concept. Also it highlights how such reactions accompany the physical changes in the structure of the gels and stereo controlled products with high yields. 相似文献
30.