| Converting CO2 into high value-added chemicals and fuels via solar semiconductor photocatalysis technology can not only reduce CO2 emissions and solve greenhouse effect in environmental issue,but also realize the cyclic utilization of carbon resource on the basis of renewable energy,which has become one of important research orientations for the development of new energy in the future.However,it is difficult for a single photocatalyst to take into account good light response,CO2 adsorption and carrier separation capability.Therefore,it will be significant scientifically for the design and development of an efficient photocatalyst system to achieve CO2photoreduction and improve the directional conversion and yield of CO2photoreduction products.In the thesis,based on the intrinsic material properties and CO2photoreduction reaction principle,the Bi2MO6(M=Mo,W)photocatalysts with reasonable band gap structures are firstly selected,and satisfy with the scientific utilization of sunlight and the coordination between valence-conduction band potentials and reactant potentials.Secondly,the activated carbon spheres(ACSs),with high CO2 adsorption capacity and large specific surface area,are chosen to support high-efficiency Bi2MO6photocatalysts and optimize the separation efficiency of photogenerated electron-hole pairs,constructing the Bi2MO6/ACSs photocatalyst system with highly efficient solar light response,CO2 adsorption and CO2 reduction performances.The main research contents are as follows:(1)Preparation and CO2 photoreduction performances of Bi2WO6/ACSs.Firstly,the phenolic resin spheres are prepared by suspension polymerization and further carbonized and activated to obtain ACSs supporter with good sphericity.In the process of hydrothermal synthesis of Bi2WO6,the customized carrier ACSs is introduced to prepare Bi2WO6/ACSs composite photocatalyst.Secondly,XRD,SEM,UV-Vis DRS,PL,BET and CO2adsorption isotherms are used to investigated contrastly the phase structures,chemical compositions,structural morphologies,optical absorption capacities,photoelectric properties and CO2 adsorption activities of pure Bi2WO6 and Bi2WO6/ACSs samples.Thirdly,the photocatalytic CO2 reduction performances and cyclic stability of Bi2WO6 and Bi2WO6/ACSs are studied for comparations under the simulated sunlight irradiation.Lastly,the enhanced mechanism of photocatalytic CO2 reduction activity for Bi2WO6/ACSs is prop,which is should be the synergistic effects between Bi2WO6,with the energy band structure and excellent redox potentials of,and ACSs,with good CO2 absorption capacity and electrical conductivity.Our findings indicate that ACSs can be used as an excellent support for the construction of high efficiency CO2 photoreduction catalyst system.(2)CO2 photoreduction performances of ACSs assisting 3D Bi2MoO6microspheres.Accorrding to excellent CO2 adsorption and electronic conductivity of ACSs,the photocatalyst system of ACSs assisted 3D Bi2MoO6 microspheres is designed.First of all,3D Bi2MoO6 microspheres are loaded on the surface of ACSs via simple and mild impregnation method so as to obtain Bi2MoO6/ACSs samples.In addition,the analysis results of XRD and SEM show that Bi2MoO6 crystal phase is good and uniformly loaded on the surface of ACSs.The structure and particle size of Bi2MoO6 have no obvious change before and after loading ACSs.Then,the XPS,EDX,DRS,BET,CO2adsorption isotherms,EIS and transient photocurrent of the samples are analyzed and compared in detail.Finally,the photocatalytic CO2 reduction performances of samples are evaluated under the simulated sunlight irradiation,and the Bi2MoO6/ACSs reveal excellent activity,selectivity and stability of CO2 photoreduction.The CO yield of Bi2MoO6/ACSs is 1.8 times than that of pure Bi2MoO6,and after four cycles,one of less than 10%only reduces.The photocatalytic CO2 reduction mechanism of Bi2MoO6/ACSs is proposed.Our findings reveal that millimeter grade ACSs can effectively improve the CO2 reduction activity and stability of Bi2MO6 catalyst,which should be expanded to support other Bi-based semiconductor materials and the construction of other powder catalyst systems,providing good basic scientific data for promoting the engineering research of solar photocatalytic CO2 green conversion. |