Oxidation of methane into valuable chemicals, such as C 2+ molecules, has been long sought after but the dilemma between high yield and high selectivity of desired products remains. Herein, methane is upgraded through the photocatalytic oxidative coupling of methane (OCM) over a ternary Ag−AgBr/TiO 2 catalyst in a pressurized flow reactor. The ethane yield of 35.4 μmol/h with a high C 2+ selectivity of 79% has been obtained under 6 bar pressure. These are much better than most of the previous benchmark performance in photocatalytic OCM processes. These results are attributed to the synergy between Ag and AgBr, where Ag serves as an electron acceptor and promotes the charge transfer and AgBr forms a heterostructure with TiO 2 not only to facilitate charge separation but also to avoid the overoxidation process. This work thus demonstrates an efficient strategy for photocatalytic methane conversion by both the rational design of the catalyst for the high selectivity and reactor engineering for the high conversion.
Electronic metal–support interactions (EMSI) describe the electron flow between metal sites and a metal oxide support. It is generally used to follow the mechanism of redox reactions. In this study of CuO‐CeO2 redox, an additional flow of electrons from metallic Cu to surface carbon species is observed via a combination of operando X‐ray absorption spectroscopy, synchrotron X‐ray powder diffraction, near ambient pressure near edge X‐ray absorption fine structure spectroscopy, and diffuse reflectance infrared Fourier transform spectroscopy. An electronic metal–support–carbon interaction (EMSCI) is proposed to explain the reaction pathway of CO oxidation. The EMSCI provides a complete picture of the mass and electron flow, which will help predict and improve the catalytic performance in the selective activation of CO2, carbonate, or carbonyl species in C1 chemistry.
Compared to phase retrieval from single sample-to-detector distance (SDD) image, phase retrieval with multiple SDD images could improve the precision in quantitative X-ray in-line phase contrast imaging (QXIPCI). Among all the related phase retrieval approaches, the two-SDD-image-based one is the simplest and well compromises between precision and dose. However, how to optimize the recording distances for the two images to achieve highest precision, remains unsolved. In this paper, the problem was investigated systematically based on digital simulation and related experiments. Spectral correlation degree (SCD) is introduced to evaluate the pertinence between the two SDD images. The simulation results show that the highest retrieving precision could be obtained while the SDD of the second image is three times that of the first image. The best retrieval could be achieved when SDD of the first image is selected properly, meanwhile the SCD occurs with a typical damping oscillation. Experiments, carried out at the X-ray imaging beamline of SSRF, demonstrated the simulation results.
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