| Modern industry relies heavily on the consumption of fossil energy,which has produced huge carbon emission.There are a series of environmental problems such as the greenhouse effect caused by the excessive atmospheric CO2 concentration,which will seriously threaten the survival human society.The development of renewable energy technology has gradually reduced the cost of new energy power.However,the intermittent nature of wind and solar energy is an inevitable problem that restricts its efficient utilization.It’s necessary to design corresponding energy storage or energy conversion devices.Electroreduction CO2(CO2RR)into hydrocarbon fuels provides a promising route for the“renewable power-energy storage”structure transformation and closing anthropogenic carbon cycle.Copper is the only catalyst that can effectively reduce CO2 to hydrocarbons.Rational design of electrocatalysts and reactors to improve the selectivity and activity of Cu-based materials is a key scientific issue.This paper focuses on engineering the high efficiency reactor and the medication of Cu with molecular ligands to promote the production of methane.Combine with material characterization and theoretical analysis,the mechanism of surface ligands and reaction route are initially revealed.The results are summarized as follows:(1)We design a Flow-cell system for CO2RR to multi-carbon products.Through adjusting related parameters and optimizing electrode preparation methods,the stability and durable of reactor is improved.The gas diffusion electrode is used in Flow-cell to improve the mass transformation of CO2,and a three-phase reaction react interface is formed in catalytic layer,which increase current by dozens of times.Compared with neutral electrolyte,the alkaline environment has significantly improved the ethylene selectivity,the faradaic efficiency of C2H4 maintained above45%in over 5 h test.(2)We design and fabricate Cu nanoparticles modified with specific functional-groups,The microscopic morphology,phase composition of nanoparticles and the anchoring of ligands on the surface of catalyst are analyzed.The functional groups hanging at the end of ligands stabilize intermediates through hydrogen bonding.In suit Raman spectrum indicates the changes in the adsorption state of*CO by ligands,which promotes hydrogenation process to produce methane.Finally,the Cu modified by glutathione was fabricated and the FE of CH4 reached 63.70%at 250 m A cm-2,partial current density exceeded 150 m A cm-2,together with a high cathode energy efficiency of 28%. |