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91.
Yan Luo Zeming Tang Guiqiang Cao Da Bi David P. Trudgeon Adeline Loh Xiaohong Li Qingxue Lai Yanyu Liang 《International Journal of Hydrogen Energy》2021,46(2):1997-2006
Atomically dispersed transition metals anchored on N-doped carbon have been successfully developed as promising electrocatalysts for acidic oxygen reduction reaction (ORR). Nonetheless, how to introduce and construct single-atomic active sites is still a big challenge. Herein, a novel concave dodecahedron catalyst of N-doped carbon (FeCuNC) with well confined atomically dispersed bivalent Fe sites was facilely developed via a Cu-assisted induced strategy. The obtained catalyst delivered outstanding ORR performance in 0.5 M H2SO4 media with a half-wave potential (E1/2) of 0.82 V (vs reversible hydrogen electrode, RHE), stemming from the highly active bivalent Fe-Nx sites with sufficient exposure and accessibility guaranteed by the high specific surface area and curved surface. This work provides a simple but efficient metal-assisted induced strategy to tune the configurations of atomically dispersed active sites as well as microscopy structures of carbon matrix to develop promising PGM-free catalysts for proton exchange membrane fuel cell (PEMFC) applications. 相似文献
92.
Chunyu Zhang Guozhu Liu Bo Ning Shuairen Qian Danning Zheng Li Wang 《International Journal of Hydrogen Energy》2021,46(27):14277-14287
The electrochemical oxygen reduction reaction (ORR) via two-electron pathway is a sustainable way of producing hydrogen peroxide. Nanostructured carbon materials are proved to be effective catalysts for 2e? ORR. Herein, a series of mesoporous carbon with tunable nitrogen species and oxygen functional groups were synthesized by varying the added amount of dopamine hydrochloride as nitrogen and oxygen source. The modified catalysts exhibited higher content of pyrrolic-N and ether C–O groups which are confirmed by a series of characterization. Raman spectra and correlation analysis revealed that the increased proportion of defect sites in carbon materials are closely related to the introduced pyrrolic-N and ether C–O groups. And the rotating ring-disk electrode (RRDE) measurement carried out in 0.1 M KOH electrolyte showed the H2O2 selectivity increased with the content of defect sites. Among them, the optimized catalyst (NOC-6M) exhibited a selectivity of 95.2% and a potential of 0.71 V vs. RHE at ?1 mA cm?2. Moreover, NOC-6M possessed the high H2O2 production rate of 548.8 mmol gcat?1 h?1 with faradaic efficiency of 92.4% in a two-chamber H-cell. Further mechanistic analysis revealed that the introduction of pyrrolic-N and ether C–O are likely to improve the binding energy of the defect sites toward 1OOH intermediate, resulting in a more favorable 2e? ORR pathway for H2O2 production. 相似文献
93.
《International Journal of Hydrogen Energy》2021,46(58):30061-30078
A uniform solid product layer normally assumed in the shrinking-core model cannot predict the kinetic transition behavior of the H2 adsorption reactions. In this study, the concept of a uniform solid product layer has been replaced by that of the inward growth of solid products on the solid surface. A rate equation is established to calculate the inward growth of the solid product and was implemented into the shrinking-core model to calculate the H2 adsorption kinetics for various shapes of Mg-based materials. The prediction accuracy of the developed model is verified from the detailed experimental data. To account for the external gas diffusion around the particle and the intraparticle gas diffusion, an analytical equation is derived using the Thiele modulus method. This model can be used to analyze various kinetic aspects and to analyze the effect of change in the particle microstructure on intraparticle diffusion. 相似文献
94.
Deok-Hye Park Yo-Seob Kim Sang-Beom Han Woo-Jun Lee Hak-Joo Lee Yong-Soo Lee Sang-Hyun Moon Kyung-Won Park 《International Journal of Hydrogen Energy》2021,46(43):22499-22507
Electrochemical reactions such as the oxygen evolution reaction (OER), oxygen reduction reaction (ORR), and methanol oxidation reaction (MOR) are essential for energy conversion applications such as water electrolysis and fuel cells. Furthermore, Pt or Ir-related materials have been extensively utilized as electrocatalysts for the OER, ORR, and MOR. To reduce the utilization of precious metals, innovative catalyst structures should be proposed. Herein, we report a bi-metallic phosphide (Ni2P and PdP2) structure surrounded by graphitic carbon (Ni–Pd–P/C) with an enhanced electrochemical activity as compared to conventional electrocatalysts. Despite the low Pd content of 3 at%, Ni–Pd–P/C exhibits a low overpotential of 330 mV at 10 mA cm?2 in the OER, high specific activity (2.82 mA cm?2 at 0.8 V) for the ORR, and a high current density of 1.101 A mg?1 for the MOR. The superior electrochemical performance of Ni–Pd–P/C may be attributed to the synergistic effect of the bi-metallic phosphide structure and core-shell structure formed by graphitic carbon. 相似文献
95.
Dinabandhu Patra Ramakrishnan Ganesan Balaji Gopalan 《International Journal of Hydrogen Energy》2021,46(50):25486-25499
We report the catalytic enhancement of hydrogen generation by 1) in situ Fe (0) formed and 2) nitroarenes substrates during Fe3O4@Pd core-shell nanoparticles catalyzed tandem reaction. The active hydrogen species are generated in Pd shell, which either combine to form H2 gas or take part in relatively faster nitroarene reduction reaction. The rate of hydrogen generation from ammonia borane is dependent on the nitroarene substrate and is higher when 4-nitrophenol is used. This is due to the difference in ammonia borane adsorption on the surface of the catalyst. During recyclability, the H2 generation rate of 2 wt% Pd loaded samples is higher than other compositions. Such an enhancement has been attributed to the formation of Fe (0) via γ-FeOOH mediated by Pd species, presumably through Pd(OH)2. The electronic connection between Fe and Pd interface is thus shown to play an important role in the catalytic enhancement of the tandem reaction. 相似文献
96.
《International Journal of Hydrogen Energy》2021,46(70):34565-34573
Water electrolysis is an energy conversion technology to provide green and clean hydrogen energy. Developing a high-efficient and durable electrocatalyst is a critical material for water electrolysis. Therefore, we synthesize a series of iron-doped metal-organic frameworks (MOFs) by a facile one-pot hydrothermal method. In the conventional three-electrode-cell, the Co/Fe (1:1)-MOF catalyst exhibits an overpotential of 317 mV at a current density of 10 mA cm−2 in the oxygen evolution reaction (OER). Furthermore, the electrolysis performance of Co/Fe (1:1)-MOF catalyst is further evaluated in a home-made anion-exchange-membrane water electrolysis cell. With the Co/Fe (1:1)-MOF as the OER catalyst and commercial Pt/C as the hydrogen-evolution-reaction catalyst, the cell presents an overpotential of 490 mV at a large current density of 500 mA cm−2, which is superior to the benchmark cell with commercial IrO2 as the OER catalyst in the alkaline media. Theoretical calculation demonstrates that the introduction of Fe dopant into MOFs significantly reduces the binding energy of 1O and 1OOH intermedium during the OER progress. Consequently, the electrocatalytic activity is increased, which is perfectly consistent with the experimental results. This work suggests that the iron-doped MOFs structure significantly improves the electrocatalytic activity and provides a facile strategy to produce hydrogen at a large current density for industrial water electrolysis. 相似文献
97.
Liqian Wu Dongdong Shi Shiming Yan Wen Qiao Wei Zhong Youwei Du 《International Journal of Hydrogen Energy》2021,46(2):2086-2094
The exploration of efficient, low-cost and earth-abundant oxygen-evolution reaction (OER) electrocatalysts and the understanding of the intrinsic mechanism are important to advance the clean energy conversion technique based on electrochemical water oxidation. In this work, Fe-doping Co3N catalysts were successfully synthesized by a simple nitridation reaction of the Co3-xFexO4 precursor. This material exhibited a low overpotential of 294 mV at a current density of 10 mA cm?2, and a small Tafel slope of 49 mV dec?1 in 1 M KOH solution, superior to the performance of Co3N and IrO2. As revealed by the spectroscopic and electrochemical analyses, the enhanced OER performance mainly originates from the electronic modulation induced by the incorporation of Fe into Co3N, benefitting the formation of CoOOH as active surface species and thus facilitating the OER process. These findings also demonstrate the introduction of heterogeneous element is a simple and effective strategy to regulate the OER property of the cobalt nitrides (Co3N) catalysts. 相似文献
98.
Yingying Xing Di Li Longhua Li Huamei Tong Deli Jiang Weidong Shi 《International Journal of Hydrogen Energy》2021,46(11):7989-8001
Electrocatalytic hydrogen evolution under alkaline media holds great promising in hydrogen energy production. Transition-metal sulfides (TMSs) are attractive for electrocatalytic alkaline hydrogen evolution, yet their catalytic performance is unsatisfactory owing to the sluggish water dissociation kinetics. Herein, a Mn/N co-doping strategy is proposed to regulate the water dissociation kinetics of Co9S8 nanowires array grown on nickel foam thus improve the activity of hydrogen evolution reaction (HER). The optimal Mn/N co-doping Co9S8 (Mn–N–Co9S8) catalyst achieves low overpotentials of 102 and 238 mV at 10 and 100 mA cm?2 in the 1 M KOH solution, respectively, remarkably higher than the single-doping Mn–Co9S8 and N–Co9S8 as well as superior to many reported Co9S8-based HER electrocatalysts. Density functional theory (DFT) calculation results confirm that the water dissociation barrier of the Mn–N–Co9S8 is reduced significantly owing to the synergistic co-doping of Mn and N, which accounts for the enhanced alkaline HER performance. This study offers an effective strategy to enhance the alkaline HER activity of TMSs by accelerating water dissociation kinetic via the cation and anion co-doping strategy. 相似文献
99.
Xiaobing Yang Weisen Yang Xingping Fu Jiapeng Hu Juan Chen 《International Journal of Hydrogen Energy》2021,46(35):18318-18325
Splitting water for hydrogen production is still a promising technique to meet the energy requirements of society and overcome many environmental problems. However, the development of carbon-based transition electrocatalysts with superior activity for hydrogen evolution reaction (HER) is still challenging. In this study, a CoNiMo/NPC electrocatalyst was successfully fabricated using ZIF-67 as a precursor via facile absorption, pyrolysis and annealing processes. The fabricated CoNiMo/NPC was used as an electrocatalyst for hydrogen production. The results revealed that the doping of Ni and Mo increase the number of active sites and enhance the conductivity of electrocatalysts. CoNiMo/NPC exhibits excellent HER activity in alkaline solutions and only requires an overpotential of 182 mV to reach a current density of 10 mA/cm2. Furthermore, long-term measurements demonstrated that CoNiMo/NPC has superior durability in alkaline solutions. The excellent HER performance of CoNiMo/NPC can be attributed to the doping of Co, Ni, and Mo on porous carbon. In addition, the high specific surface area and high graphitisation degree of the electrocatalyst are beneficial for rapid charge transport and collection. 相似文献
100.
Yanyan Wu Zijuan Xie Ying Li Zhe Lv Lingling Xu Bo Wei 《International Journal of Hydrogen Energy》2021,46(49):25070-25080
Developing efficient oxygen evolution reaction (OER) electrocatalysts with earth-abundant elements is very important for sustainable H2 generation via electrochemical water splitting. Here we design a crystalline-amorphous Ni–Fe–Al hybrid phosphides nanosheet arrays grown on NiFe foam for efficient OER application. Dynamic surface reorganization of phosphides at anodic/cathodic polarizations is probed by in situ Raman spectroscopy. The reconstructed amorphous Ni(Fe)OOH species are determined as the active phases that facilitate the OER process. This unique electrode shows highly catalytic activity toward water oxidation, achieving the current densities of 10 and 100 mA cm?2 at 181 and 214 mV in 1 M KOH, respectively. Meanwhile, it also exhibits excellent stability at a large current density of 100 mA cm?2 for over 60 h. This work reveals the dynamic structural transformation of pre-catalyst in realistic conditions and highlights the important role of oxyhydroxides as real reactive species in OER process with high activity. 相似文献