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- CO2 electrolysis (1)
- Electrochemical CO2 conversion (1)
- Explosion overpressures (1)
- Explosion pressure (1)
- Flame propagation (1)
- Free radicals (1)
- Gas concentration (1)
- Hydrocarbon fuel-air explosion (1)
- Hydrogen (1)
- Obstacle location (1)
Organisationseinheit der BAM
Experiments were conducted in a semi-confined pipe to investigate the effects of obstacle location and gasoline vapor concentration on gasoline-air fuel explosions. The variations of internal overpressure, external overpressure, flame propagation and flame-overpressure coupling relationship were analyzed. The results showed thatthe internal overpressure histories existed three obvious peaks, and when the obstacle location was set at 0.4 m, the maximum absolute values of overpressure (pmax and pneg), overpressure rise rates ((dp/dt)ave and (dp/dt)max) and the deflagration index (KG) were obtained. Additionally, more than two positive overpressure peaks were observed in the external overpressure histories. The maximum values of external overpressures and overpressure rise rates were obtained at the obstacle location of 0.4 m. For the fuel concentrations of 1.3%,.1.7% and 2.1%, the shortest time to reach pmax appeared at the obstacle location of 0.4 m, 0.2 m and 0.6 m, respectively, while the shortest time to reach (dp/dt)max and the maximum flame propagation speed were obtained for all the fuel concentrations at the obstacle location of 0.2 m. Moreover, a coupling relationship between overpressure and flame propagation was found. lt could be tleduced that the formation of the positive overpressure peak ofthe external overpressure might be directly related to the gas explosion inside the pipe and the flow jet caused by the high-speed flame propagation. rat her than the external explosion (or secondary explosion) out of the pipe. These results improve our understanding on gas explosion dynamics in a semi- confined space.
The combustion characteristics and explosive hazard of syngas (H2/CO)/air mixtures are affected by its exact composition and equivalence ratios. In this paper, the explosion pressure and spectral radiant intensity of free radicals were quantitatively examined for syngas with different H2 proportions ([H2 in syngas] = 0, 30, 50, 70, 100 vol%) and equivalence ratios (φ = 0.8, 1.0, 1.2, 1.4, 1.6, 2.0, 2.5). The results show that the explosion process of syngas/air mixtures can be separated into the initial slow combustion stage, the violent deflagration stage and the deflagration ending stage. The peaks of explosion pressure, pressure rise rate, OH*spectral intensity and rise rate of spectral intensity first increase and then decrease with increasing the equivalence ratio, and they reduce gradually with the decrease of H2 proportion in syngas. The H2 content in syngas greatly affects the heat release and the concentration of excited state OH*, especially for the syngas/air mixtures with smaller proportion of H2. Additionally, the presence of H2 greatly increases the deflagration index and spectral radiant index of OH* for syngas/air mixtures. The average rise rates of explosion pressure and spectral intensity of free radicals are introduced and the coupling model between them is established based on the first law of thermodynamics and the principle of chain reaction. The established model is furthermore verified by the experimental results. It is indicated that there is a linear relationship between average rise rates of explosion pressure and spectral intensity (OH*). The results can be used to improve the combustion efficiency of syngas and to guide theoretically the prevention, mitigation and control of syngas explosions.
Unsaturated Ni single-atom catalysts (SACs), Ni-Nx (x=1,2,3), have been investigated to break the conventional Ni-N4 structural limitation and provide more unoccupied 3d orbitals for CO2 reduction reaction (CO2RR) intermediates adsorption, but their intrinsically low structural stability has seriously hindered their applications. Here, we developed a strategy by integrating Ni nanoclusters to stabilize unsaturated Ni-N3 atomic sites for efficient CO2 electroreduction to CO at industrial-level current. Density Functional Theory (DFT) calculations revealed that the incorporation of Ni nanocluster effectively stabilizes the unsaturated Ni-N3 atomic sites and modulates their electronic structure to enhance the adsorption of the key intermediate *COOH during CO2RR. Guided by these insights, we prepared an optimal composite catalyst, Ni6@Ni-N3, which features a Ni6N6 nanocluster surrounded by six Ni-N3 single atoms sites, through low-temperature pyrolysis. The morphology and coordinative structure of Ni6@Ni-N3 were confirmed by an aberration-corrected transmission electron microscope (AC-TEM) and X-ray absorption spectroscopy (XAS). As a result, Ni6@Ni-N3 demonstrated a remarkably high CO Faradaic efficiency (FECO) of 99.7 % and a turnover frequency (TOF) of 83984.2 h−1 at 500 mA cm−2 under −1.15 VRHE, much better than those of Ni-N4 with a lower FECO of 86 % at 100 mA cm−2 and a TOF of 39309.9 h−1under identical potential. XAS analyses of Ni6@Ni-N3 before and after long-term CO2RR testing confirmed the excellent stability of its coordinative environment. This work highlights a generalizable approach for stabilizing unsaturated single-atom catalysts, paving the way for their application in high-performance CO2RR.
