The shale gas revolution and the carbon-neutrality goal are motivating the landscape toward the synthesis of value-added chemicals or fuels from underutilized ethane with the assistance of greenhouse gas CO₂. Combining ethane aromatization with CO₂ reduction offers an opportunity to directly produce liquid products for facile separation, storage, and transportation. In the present work, Fe/ZSM-5 catalysts showed promise in the simultaneous CO₂ reduction and ethane aromatization at atmospheric pressure and 873 K. The catalysts were further investigated using X-ray diffraction (XRD) and X-ray absorption fine structure (XAFS) measurements under in-situ conditions, indicating that most of Fe species existed in the form of Fe oxides and a portion of Fe was incorporated into the ZSM-5 framework generating Lewis acid sites. Both types of Fe species remained almost unchanged under reaction conditions, contributing to an enhanced aromatization activity of Fe/ZSM-5. The effects of CO₂ and steam on the acid sites and in turn aromatization activity were also investigated by transient studies, which exhibited a reversible modification behavior. Moreover, CO₂ was identified to be critical to enhance coke resistance and in turn catalyst stability. This work highlights the feasibility of using CO₂ to assist the upgrading of abundant ethane from shale gas to aromatics over non-precious Fe-based zeolite catalysts.

页岩气革命和碳中和目标正在推动景观朝着在温室气体 CO ₂的帮助下从未充分利用的乙烷合成增值化学品或燃料的方向发展。将乙烷芳构化与 CO ₂还原相结合，提供了直接生产液体产品以便于分离、储存和运输的机会。在目前的工作中，Fe/ZSM-5 催化剂在大气压和 873 K 下同时进行 CO ₂还原和乙烷芳构化显示出前景。使用 X 射线衍射（XRD）和 X 射线吸收精细结构进一步研究了催化剂（ XAFS)原位测量条件下，表明大多数 Fe 物种以 Fe 氧化物的形式存在，一部分 Fe 结合到 ZSM-5 骨架中，产生路易斯酸位点。两种类型的 Fe 物质在反应条件下几乎保持不变，有助于增强 Fe/ZSM-5 的芳构化活性。还通过瞬态研究研究了 CO ₂和蒸汽对酸性位点和芳构化活性的影响，其表现出可逆的改性行为。此外，CO ₂被确定为提高抗焦炭性并进而提高催化剂稳定性的关键。这项工作强调了使用 CO ₂协助通过非贵重的 Fe 基沸石催化剂将丰富的乙烷从页岩气升级为芳烃的可行性。