| Reducing carbon emissions and achieving carbon standards is a major climate problem facing mankind at present,and also an important research field in scientific research,among which more efficient technology to achieve carbon dioxide conversion is an important research direction.Electrochemical reduction of carbon dioxide is a relatively efficient means to achieve carbon dioxide conversion.This paper intends to use proton and electron irradiation to modify the surface composition and structure of Cu in Cu/Pi materials,and explore a new way to improve the efficiency of Cu-based CO2 catalytic reduction.In this paper,the nano-Cu thin film/polyimide composite material was used as the research object.With the help of various material analysis techniques,the morphology and structure of Cu/PI material modified by electron/proton irradiation were characterized,and the irradiation modification mechanism was revealed.The catalytic efficiency and catalytic products of Cu/Pi material irradiated by charged particles were analyzed in a three-electrode catalytic reaction apparatus.The influence of irradiation modification on the catalytic behavior of the material and its mechanism were studied.Low-energy proton irradiation is used to modify Cu/PI materials to obtain catalysts modified with different irradiation fluence.It can be seen from the results of X-ray diffraction and X-ray photoelectron spectroscopy that copper nitride compounds are formed on the surface of the catalyst as the proton radiation fluence increases.The electro-catalytic reduction performance test of the catalyst modified by irradiation with different fluence of low energy protons showed that with the increase of the irradiation fluence,the Faraday efficiency of ethylene and methane showed a trend of first increasing and then decreasing.The amount is 7×1015 cm-2,and the maximum value is 9.45%and 2.5%when the potential is-1.1 V.It can be seen that with the increase of proton irradiation fluence,the selectivity to methane and ethylene shows a strengthening trend.When the irradiation fluence reaches2×1016 cm-2,the selectivity of methane and ethylene weakens,which may be due to the reorganization of the surface structure of the catalyst caused by the excessive proton irradiation fluence,which makes it easier to poison in the catalytic reaction.This needs further Theoretical analysis and experimental verification.Using high-energy electrons to modify the Cu/PI material by irradiation,a series of fluence gradient catalysts are obtained.The analysis results of X-ray diffraction and X-ray photoelectron spectroscopy show that as the fluence of high-energy electron irradiation increases,organic copper and basic copper carbonate are formed on the surface of the catalyst.The analysis results of atomic force microscope and scanning electron microscope indicate that high fluence of high-energy electrons can cause the migration of surface copper atoms,resulting in the formation of new structural morphologies on the surface of the catalyst.The electro-catalytic reduction performance test results of the catalyst modified by high-energy electron irradiation with different fluence show that the selectivity of methane and ethylene increases with the increase of the irradiation fluence.High-energy electron irradiation causes new compounds generated on the catalyst surface,thereby generating new active sites and enhancing the selectivity of methane and ethylene.On the other hand,high-energy electron irradiation leads to changes in the surface morphology of the catalyst,which increases the catalytic active surface area,thereby enhancing the selectivity of methane and ethylene. |