PdCu alloy anchored defective titania for photocatalytic conversion of carbon dioxide into methane with 100% selectivity  

作　　者：Lina Zhang Sajjad Hussain Qiuye Li Jianjun Yang 

机构地区：[1]National&Local Joint Engineering Research Center for Applied Technology of Hybrid Nanomaterials,Henan University,Kaifeng 475004,Henan,China

出　　处：《Journal of Energy Chemistry》2024年第4期254-265,共12页能源化学（英文版）

基　　金：the financial support from the Program for Innovative Research Team in University of Henan Province(21IRTSTHN009);Science and Technology Fund of Henan Province(225200810051);Natural Science Foundation of Henan Province(222300420406)。

摘　　要：The photoreduction of CO_(2)into CH_(4)with simultaneous high activity and selectivity is a promising strategy to increase energy supply and alleviate global warming.However,the absence of the active sites that is responsible for the adsorption and activation of CO_(2)and the generation of CO and H2via side reactions often lead to poor efficiency and low selectivity of the catalyst.Herein,Cu,Pd,and PdCu metal clusters cocatalyst-anchored defective TiO_(2)nanotubes(Cu/TiO_(2)-SBO,Pd/TiO_(2)-SBO,and Pd1Cu1/TiO_(2)-SBO)were designed via a simple solution impregnation reduction and applied for photocatalytic conversion of CO_(2)to CH_(4).The Pd1Cu1/TiO_(2)-SBO photocatalyst exhibits excellent catalytic performance among the other catalysts for photoreduction of CO_(2)into CH_(4).More interestingly,the product selectivity of CH_(4)reaches up to 100%with a rate of 25μmol g^(-1)h^(-1).In-situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)and density functional theory(DFT)simulations indicate that the main reasons for the high selectivity of CH_(4)are attributed to the PdCu alloy and oxygen vacancies,which jointly enhance the photoinduced carrier separation and lower energy barriers of key intermediates.Moreover,due to the tunable d-band center of the Cu site in the PdCu alloy,the generated intermediates can be well prevented from poisoning and promoted to participate in further reactions.Hopefully,the current study will provide insight into the development of new,highly selective photocatalysts for the visible light-catalytic reduction of CO_(2)into CH_(4).

关 键 词：PdCu alloy Defective TiO_(2) Photoreduction of CO_(2) Photocatalytic mechanism 

分 类 号：O643.36[理学—物理化学] O644.1[理学—化学] TQ221.11[化学工程—有机化工]