Photothermal catalytic C-C coupling to ethylene from CO_(2) with high efficiency by synergistic cooperation of oxygen vacancy and half-metallic WTe_(2)  

作　　者：Xiaoyue Zhang Yong Yang Yingjie Hu Lijun Xiong Tianyu Wang Panjie Li Jinyou Shen 

机构地区：[1]Key Laboratory of Environmental Remediation and Ecological Health,Ministry of Industry and Information Technology,School of Environmental and Biological Engineering,Nanjing University of Science and Technology,Nanjing 210094,Jiangsu,China [2]School of Chemistry and Chemical Engineering,Nanjing University of Science and Technology,Nanjing 210094,Jiangsu,China [3]Nanjing Key Laboratory of Advanced Functional Materials,Nanjing Xiaozhuang University,Nanjing 210094,Jiangsu,China [4]Jiangsu Environmental Engineering Technology Co.Ltd,Nanjing 210019,Jiangsu,China

出　　处：《Journal of Energy Chemistry》2024年第6期547-556,I0014,共11页能源化学（英文版）

基　　金：the National Natural Science Foundation of China(51303083);the National Natural Science Foundation of China for Excellent Young Scholars(51922050);the Natural Science Foundation of Jiangsu Province(BK20191293);the Fundamental Research Funds for the Central Universities(30920021123)。

摘　　要：Photothermal catalytic CO_(2) conversion provides an effective solution targeting carbon neutrality by synergistic utilization of photon and heat.However,the C-C coupling initiated by photothermal catalysis is still a big challenge.Herein,a three-dimensional(3D)hierarchical W_(18)O_(49)/WTe_(2) hollow nanosphere is constructed through in-situ embodying of oxygen vacancy and tellurium on the scaffold of WO_(3).The light absorption towards near-infrared spectral region and CO_(2) adsorption are enhanced by the formation of half-metal WTe_(2) and the unique hierarchical hollow architecture.Combining with the generation of oxygen vacancy with strengthened CO_(2) capture,the photothermal effect on the samples can be sufficiently exploited for activating the CO_(2) molecules.In particular,the close contact between W_(18)O_(49)and WTe_(2) largely promotes the photoinduced charge separation and mass transfer,and thus the~*CHO intermediate formation and fixedness are facilitated.As a result,the C-C coupling can be evoked between tungsten and tellurium atoms on WTe_(2).The ethylene production by optimized W_(18)O_(49)/WTe_(2) reaches 147.6μmol g^(-1)with the selectivity of 80%.The in-situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)and density functional theory(DFT)calculations are performed to unveil the presence and significance of aldehyde intermediate groups in C-C coupling.The half-metallic WTe_(2) cocatalyst proposes a new approach for efficient CO_(2) conversion with solar energy,and may especially create a new platform for the generation of multi-carbon products.

关 键 词：Photothermal catalysis HALF-METAL WTe_(2) C–C coupling Carbon neutrality 

分 类 号：O643.36[理学—物理化学] O644.1[理学—化学] TQ221.211[化学工程—有机化工]