Regulated reaction pathway of CO_(2)photoreduction into CH_(4)by metal atom pair sites  

作　　者：Dong-Po He Guang-Bing Huang Jun Hu Yang Wu Xiao-Dong Li Qing-Xia Chen Shan Zhu Wen-Sheng Yan Jun-Fa Zhu Yang Pan Xing-Chen Jiao 

机构地区：[1]Key Laboratory of Synthetic and Biological Colloids,Ministry of Education,School of Chemical and Material Engineering,Jiangnan University,Wuxi 214122,China [2]Hefei National Research Center for Physical Sciences at Microscale,National Synchrotron Radiation Laboratory,University of Science and Technology of China,Hefei 230026,China [3]Max Planck Institute of Microstructure Physics,Weinberg 2,06120 Halle,Germany [4]State Grid Anhui Electric Power Research Institute,Hefei 230601,China

出　　处：《Rare Metals》2024年第9期4620-4627,共8页稀有金属（英文版）

基　　金：supported by the National Key R&D Program of China(No.2022YFA1502904);the National Natural Science Foundation of China(Nos.22275178 and 22002148);the Fundamental Research Funds for the Central Universities(Nos.JUSRP123013 and JUSRP123015)。

摘　　要：The carbon dioxide(CO_(2))reduction process involves complex protonation,making the resulting product often unpredictable.To achieve the desired product,it is crucial to manipulate the reaction steps.Herein,we build the metal atom pair sites for selective CO_(2)photoreduction into methane.As a prototype,Ni atom pair sites loaded on the Mo S_(2)nanosheets were synthesized and verified by highresolution transmission electron microscopy(HRTEM),X-ray photoelectron spectroscopy(XPS)and X-rayabsorption near edge structure spectra(XANES).In-situ Fourier transform infrared spectroscopy(FTIR)monitors the*CHO group,a crucial intermediate in CH_(4)production,during CO_(2)photoreduction on the Ni-Mo S_(2)nanosheets,whereas this monitoring is not observed for the Mo S_(2)nanosheets.Also,theoretical calculations disclose that over the Ni-Mo S_(2)nanosheet slab,the formation energy of*CHO intermediates is determined to be lower(0.585 e V)than the desorption energy of*CO intermediates for CO production(0.64 e V),implying the higher selectivity of CH_(4)production.

关 键 词：STEPS dioxide DESIRED 

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]