Abstract Artificial photosynthesis can convert CO 2 and H 2 O into hydrocarbons via solar energy. However, the extremely low process efficiency is a major obstacle to this application. The photocatalyst is considered to be the key factor to raise the overall solar energy conversion efficiency. Much research focused on co‐catalysts, but less attention has been paid on the high‐temperature semiconductor. Herein, a strategy is proposed involving high‐temperature semiconductor to design target photocatalyst dealing with the artificial photosynthesis at high temperature. Based upon this strategy, a CuO/SiC catalyst with single atom characteristic was designed, prepared and the activity of CO 2 photoreduction with H 2 O was tested in a high temperature environment. Above 150 °C, the catalyst activity was boosted and unprecedented performance values were attained. Under the irradiation condition delivered by a 1000 W Xe light and at 350 °C, the obtained yields of CH 4 , C 2 H 4 , and C 2 H 6 were 2041.4 μmol ⋅ g −1 , 15.2 μmol ⋅ g −1 , and 63.6 μmol ⋅ g −1 , respectively. The overall CO 2 conversion reached 24.6 % and the maximum solar energy conversion efficiency was 2.3 % without any sacrificed agents. This strategy will be helpful to overcome the current limitations for the industrialization of artificial photosynthesis and accelerate the related research on photothermal catalysis.
Converting sunlight into chemical fuels and metal commodities, via solar thermochemical conversion processes, is an attractive prospect for the long-term storage of renewable energy. In this study, the combined methane reforming and ZnO reduction in a single reaction for co-production of hydrogen-rich syngas and metallic Zn was demonstrated in a flexible solar thermochemical reactor prototype, driven by highly concentrated sunlight. Using solar energy as the process heat source in chemical-looping methane reforming with the ZnO/Zn oxygen carrier is a means to reduce the dependence on conventional energy resources and to reduce emissions of CO2 and other pollutants, while upgrading the calorific value of the feedstock for the production of energy-intensive and high-value chemical fuels and materials. On-sun experiments were carried out with different operating parameters including operating temperatures (800–1000 °C), inlet methane flow-rates (0.1–0.4 NL/min), and inlet ZnO feeding-rates (0.5–1.0 g/min) both in batch and continuous modes under reduced (0.15 and 0.45 bar) and atmospheric pressures (0.90 bar), thereby demonstrating solar reactor flexibility and reliability. As a result, increasing the temperature promoted net ZnO conversion at the expense of favored methane cracking reaction, which can be lowered by decreasing pressure to vacuum conditions. Diminishing total pressure improved the net ZnO conversion but favored CO2 yield due to insufficient gas residence time. Rising ZnO feeding rate under a constant over-stoichiometric CH4/ZnO molar ratio of 1.5 enhanced ZnO and methane consumption rates, which promoted Zn and syngas yields. However, an excessively high ZnO feeding rate may be detrimental, as ZnO could accumulate when the ZnO feeding rate is higher than the ZnO consumption rate. In comparison, continuous operation demonstrated greater performance regarding higher ZnO conversion (XZnO) and lower methane cracking than batch operation. High-purity metallic Zn with a well-crystallized structure and of micrometric size was produced from both batch and continuous tests under vacuum and atmospheric pressures, demonstrating suitable reactor performance for the solar thermochemical methane-driven ZnO reduction process. The produced Zn metal can be further re-oxidized with H2O or CO2 in an exothermic reaction to produce pure H2 or CO by chemical-looping.
A method was developed for online analysis of vaporized cadmium in any exhaust gas by coupling an inductively coupled plasma spectrometer to the gas outlet of a laboratory fluidized bed reactor. A calibration device was set up and implemented, and a standard gas synthesis protocol was developed to obtain quantitative data. The calibration method was validated by heating Cd-spiked porous alumina particles in the fluid bed. Mass losses in the solid phase were measured and compared to the amount of cadmium detected by the online gas monitoring system. The mass balance was satisfying, thus validating the method, which was finally applied satisfactorily in the case of combustion of Cd-spiked realistic artificial waste.
La comprehension des processus physico-chimiques controlant l'evolution des metaux lourds (ML) et du role des conditions de fonctionnement des incinerateurs sur la genese des vapeurs metalliques a partir du lit de dechets constituent les principaux objectifs de cette these.
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