Supporting Data for the paper : Impurity-driven spontaneous and infrared-activated Fischer–Tropsch chemistry on commercial aluminum

This data accompanies the paper " Impurity-driven spontaneous and infrared-activated Fischer–Tropsch chemistry on commercial aluminum " by Seon Young Hwang, Seungwon Kim, Jihye Lee, Gi Beom Sim, Go Eun Park, Soohaeng Yoo Willow, Chang Woo Myung, and Youngku Sohn Data/ contains initial input data of 1) geometry relaxation and 2) vibrational frequency calculation of nitrate reduction reaction intermediates. Calculated data file FT_on_AlFe.xlsx for Gibbs free energy exists in Data/. Figures/ contains figures of the paper that obtained from Data/. Scripts/ contains Jupyter notebook and Python scripts that can reproduce figures. Zero-point energy, entropy, and enthalpy corrections can be calculated using the Python scripts Scripts/calculate_*.py at the directory Data/geometry_relaxation_and_zpe/.../zpe/ If you want to calculate your own project, please visit our repository of project. (github link: https://github.com/myung-group/Data_FT_on_AlFe ) ## Pseudopotentials The following PAW potentials (PBE) and BEEF-vdW functionals were used in this study. Note: Due to licensing restrictions, the POTCAR files are not included in this repository. | Element | Label | Date (Version) | | :--- | :--- | :--- | | Al | PAW_PBE Al | 04Jan2001 | | Fe | PAW_PBE Fe | 06Sep2000 | | C | PAW_PBE C | 08Apr2002 | | O | PAW_PBE O | 08Apr2002 | | H | PAW_PBE H | 15Jun2001 | Paper abstract Fischer–Tropsch (F–T) synthesis conventionally requires high temperatures, elevated pressures, and externally supplied H2 to convert CO into hydrocarbons. Here, we report a fundamentally distinct ambient-temperature analogue: spontaneous F–T chemistry occurring on commercial aluminum (Al) in aqueous solution. This reaction is driven by Al corrosion, which supplies electrons and surface hydrogen (*H), while trace Fe impurities embedded in the Al matrix act as catalytic microdomains that stabilize *CO and promote C–C coupling. Under CO-saturated alkaline conditions, this self-sustained Al–Fe redox system produces H2, CH4, and long-chain C2–C7 hydrocarbons with product distributions following Anderson–Schulz–Flory kinetics, whereas ultrapure Al yields only H2. Infrared irradiation further enhances hydrocarbons via localized surface restructuring and transient photothermal heating. Density functional theory identifies the Al–Fe interface as the critical site for CO adsorption and *CH2-mediated chain propagation, establishing spontaneous redox interfaces as a platform for low-temperature CO valorization.本数据集配套论文《商业铝表面杂质驱动的自发与红外活化费托合成（Fischer–Tropsch）化学》，作者为Seon Young Hwang、Seungwon Kim、Jihye Lee、Gi Beom Sim、Go Eun Park、Soohaeng Yoo Willow、Chang Woo Myung及Youngku Sohn。 Data/ 文件夹包含初始输入数据，具体包括1）硝酸盐还原反应中间体的几何弛豫计算数据，以及2）其振动频率计算数据。 Data/ 文件夹中还包含用于计算吉布斯自由能的已计算数据文件 FT_on_AlFe.xlsx。 Figures/ 文件夹收录了从Data/ 数据中生成的论文配图。 Scripts/ 文件夹包含可复现论文配图的Jupyter Notebook文件与Python脚本。 可通过路径 Data/geometry_relaxation_and_zpe/.../zpe/ 下的Python脚本 Scripts/calculate_*.py 计算零点能、熵与焓的校正值。 若需开展自有项目的相关计算，请访问本项目的开源代码仓库（GitHub链接：https://github.com/myung-group/Data_FT_on_AlFe）。 ### 赝势 本研究采用了如下投影缀加波（PAW）势（PBE泛函）与BEEF-vdW泛函： 注意：由于授权限制，本仓库未包含POTCAR文件。 | 元素 | 标识 | 日期（版本） | | :--- | :--- | :--- | | 铝（Al） | PAW_PBE Al | 2001年1月4日 | | 铁（Fe） | PAW_PBE Fe | 2000年9月6日 | | 碳（C） | PAW_PBE C | 2002年4月8日 | | 氧（O） | PAW_PBE O | 2002年4月8日 | | 氢（H） | PAW_PBE H | 2001年6月15日 | ### 论文摘要 传统费托合成（Fischer–Tropsch，F-T）工艺需在高温高压条件下进行，并需外部供给氢气以将一氧化碳（CO）转化为烃类化合物。本研究报道了一种本质迥异的室温近似工艺：在水溶液中的商业铝（Al）表面可发生自发费托合成反应。该反应由铝腐蚀过程驱动，可提供电子与表面氢物种（*H）；而嵌入铝基体中的微量铁杂质则充当催化微区，稳定*CO中间体并促进碳-碳偶联反应。在CO饱和的碱性条件下，该自维持铝-铁氧化还原体系可生成氢气、甲烷（CH4）以及长链C2~C7烃类产物，产物分布符合安德森-舒尔茨-弗洛里（Anderson–Schulz–Flory）动力学规律；而超纯铝仅能生成氢气。红外辐照可通过局域表面重构与瞬态光热加热进一步提升烃类产物产率。密度泛函理论（Density Functional Theory）研究表明，铝-铁界面是CO吸附与*CH2介导的链增长的关键位点，证实自发氧化还原界面可作为低温CO资源化利用的平台。