Zeolite-confined Fe-site catalysts(ZFCs)have emerged as superior materials for sustainably producing high-value chemicals through CO_(2) hydrogenation,owing to their adaptable framework,customizable composition,and th...Zeolite-confined Fe-site catalysts(ZFCs)have emerged as superior materials for sustainably producing high-value chemicals through CO_(2) hydrogenation,owing to their adaptable framework,customizable composition,and thermal robustness.They excel in activating,adsorbing,and converting CO_(2) with remarkable efficiency and consistency in performance.This has sparked a surge in research interest in recent years.The review delves into the latest advancements in CO_(2) catalytic hydrogenation to olefins,alcohols,aromatics,and other liquid hydrocarbons,examining the synthesis,modification tactics,and the correlation between structure and performance across various ZFCs.Additionally,it underscores the pivotal factors affecting performance and sheds light on the mechanisms behind selectivity control in the CO_(2) hydrogenation process facilitated by ZFCs.To conclude,it presents pressing challenges and strategic recommendations to inspire the development of high-performance,durable ZFCs for CO_(2) hydrogenation applications.展开更多
基金the National Natural Science Foundation of China(Nos.U22A20107,U1967215,22078307,22208314,22278379,22238003,and 22002008)the Science and Technology R&D Program Joint Fund Project of Henan Provincial,China(No.222301420001)+3 种基金the Distinguished Young Scholars Innovation Team of Zhengzhou University,China(No.32320275)the Postgraduate Education Reform Project of Henan Province,China(No.2021SJGLX093Y)the National Funded Postdoctoral Researcher Program,China(No.GZC20232382)the Key Research Projects of University in Henan Province,China(No.24A150041).
文摘Zeolite-confined Fe-site catalysts(ZFCs)have emerged as superior materials for sustainably producing high-value chemicals through CO_(2) hydrogenation,owing to their adaptable framework,customizable composition,and thermal robustness.They excel in activating,adsorbing,and converting CO_(2) with remarkable efficiency and consistency in performance.This has sparked a surge in research interest in recent years.The review delves into the latest advancements in CO_(2) catalytic hydrogenation to olefins,alcohols,aromatics,and other liquid hydrocarbons,examining the synthesis,modification tactics,and the correlation between structure and performance across various ZFCs.Additionally,it underscores the pivotal factors affecting performance and sheds light on the mechanisms behind selectivity control in the CO_(2) hydrogenation process facilitated by ZFCs.To conclude,it presents pressing challenges and strategic recommendations to inspire the development of high-performance,durable ZFCs for CO_(2) hydrogenation applications.
基金supported by National Natural Science Foundation of China(22108306)Taishan Scholars Program of Shandong Province(tsqn201909065)Shandong Provincial Natural Science Foundation(ZR2021YQ15,ZR2020QB174)。
基金Project (51002128) supported by the National Natural Science Foundation of ChinaProject (2012M511737) supported by the National Science Foundation for Post-Doctor of China
文摘研制高活性的Fe/N/C氧还原催化剂对于降低燃料电池成本、实现商业化应用有重要意义.为实现Fe/N/C催化剂的理性设计,需要深入研究其活性位结构.本文发展一种研究活性位结构的新策略,以预先合成好的聚间苯二胺基Fe/N/C催化剂(Pm PDA-Fe Nx/C)为起始物,对其在1000~1500 o C高温下再次进行热处理并使其失活,通过关联催化剂热处理前后的结构变化与氧还原催化性能来揭示活性位结构.实验结果表明,随着热处理温度升高,活性中心结构被破坏,铁原子析出团聚并形成纳米颗粒,氮元素挥发损失,导致催化剂失活.XPS分析显示,低结合能含氮物种的含量与催化剂的ORR活性呈良好的正相关性,表明活性中心很可能是由吡啶N和Fe-N物种构成的.
