光催化
可见光谱
异质结
X射线光电子能谱
光化学
解吸
材料科学
吸附
电子顺磁共振
拉曼光谱
电子转移
选择性
热液循环
水热合成
化学
紫外线
乙醇
半导体
载流子
动力学
超快激光光谱学
傅里叶变换红外光谱
催化作用
量子效率
同位素标记
化学工程
作者
Rajashree P. Mishra,Niharika Kumar,Sweta Bastia,Asish K. Dehury,Urmila Baral,Yatendra S. Chaudhary
标识
DOI:10.1021/acssuschemeng.5c09725
摘要
The efficient photocatalytic CO 2 reduction to C 2 products remains a significant challenge due to sluggish multielectron transfer kinetics and C–C coupling. In this study, MoS 2 nanocrystal-decorated Ti 3 C 2 MXene heterostructured photocatalysts with varied loading concentrations have been synthesized using a facile hydrothermal method to enhance selective CO 2 reduction to ethanol under visible light. The optimized MS-TC-10 heterostructure exhibits enhanced ethanol production (1633.8 μmol/g), 1.8 times higher than that of bare MoS 2, along with improved selectivity (58.12%) and quantum efficiency (1.5%). The broadening of Raman peaks, shifts in Ti 2p, Mo 3d, and S 2p binding energies in the XPS spectrum and a hybrid magnetic signature (sharp and broad peaks at g = 2.013 and 1.94, respectively) in EPR suggest intimate interfacial coupling and electronic interaction between the MoS 2 and Ti 3 C 2 MXene. Further, CO 2 -TPD and FTIR studies provided insights into the CO 2 reduction pathway involving the formation of intermediates HCOO –, HCO 3 –, and carbonate species. CO 2 -TPD analysis of the MS-TC-10 heterostructure reveals two broad desorption peaks, corresponding to the weak and strong CO 2 adsorption sites. The prominent high-temperature desorption peak indicates strong CO 2 binding and thereby predominating C 2 H 5 OH formation. The overall improved activity is attributed to increased surface-active sites, broadened light harvesting, optimal band structure alignment, and efficient charge transfer across the MoS 2 –MXene interface. These factors collectively prolong charge carriers’ lifetime, eventually suppressing their recombinations and facilitating a multielectron pathway for C 2 product formation. In brief, these results suggest strong CO 2 adsorption, efficient photoinduced electron transfer from MoS 2 to Ti 3 C 2, and enhanced C–C coupling, enabling selective C 2 product formation. This work highlights electron-rich MXene–MoS 2 architectures as a promising photocatalyst platform for solar-driven CO 2 conversion to value-added chemicals.
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