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Direct conversion of CO and H2O to hydrocarbons at atmospheric pressure using a TiO2−x/Ni photothermal catalyst
Nature Energy ( IF 49.7 ) Pub Date : 2024-01-05 , DOI: 10.1038/s41560-023-01418-1
Xuetao Qin , Ming Xu , Jianxin Guan , Li Feng , Yao Xu , Lirong Zheng , Meng Wang , Jian-Wen Zhao , Jia-Lan Chen , Jie Zhang , Jinglin Xie , Zhihao Yu , Ruiqi Zhang , Xinmao Li , Xi Liu , Jin-Xun Liu , Junrong Zheng , Ding Ma

Hydrocarbon fuels can be synthesized from CO and water via Kölbel–Engelhardt synthesis, a thermocatalytic process in which temperatures of ≥200 °C and elevated pressures are typically needed. While light-driven hydrocarbon production by CO hydrogenation has been demonstrated under milder conditions, for this reaction H2 must first be sourced. Here we report the direct production of hydrocarbons from CO and water at atmospheric pressure via light-driven Kölbel–Engelhardt synthesis without external heating or the addition of H2. Using a TiO2-supported Ni catalyst, we obtain an activity of 8.83 molCH2 molNi−1 h−1 and C2+ selectivity higher than 55%. In situ spectroscopy and density functional theory calculations suggest that the migration of photogenerated electrons from TiO2 to Ni facilitates carbon–carbon coupling at the interface of the TiO2x/Ni catalyst, which accounts for the observed high selectivity towards multi-carbon products.



中文翻译:

使用 TiO2−x/Ni 光热催化剂在大气压下将 CO 和 H2O 直接转化为碳氢化合物

碳氢化合物燃料可以通过柯尔贝尔-恩格尔哈特合成法由二氧化碳和水合成,这是一种热催化过程,通常需要 ≥200 °C 的温度和高压。虽然已经在较温和的条件下证明了通过CO加氢进行光驱动碳氢化合物生产,但对于该反应,必须首先获取H 2 。在这里,我们报告了在大气压下通过光驱动的 Kölbel-Engelhardt 合成直接从 CO 和水生产碳氢化合物,无需外部加热或添加 H 2。使用TiO 2负载的Ni催化剂,我们获得了8.83 mol CH2  mol Ni -1  h -1的活性和高于55%的C 2+选择性。原位光谱和密度泛函理论计算表明,光生电子从 TiO 2迁移到 Ni 促进了 TiO 2 x /Ni 催化剂界面处的碳-碳偶联,这解释了观察到的对多碳产物的高选择性。

更新日期:2024-01-06
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