具有协同作用的铜基石墨烯-氧化锌膜催化剂的制备及其在催化二氧化碳加氢合成甲醇中的应用

Cyclic utilization of carbon dioxide from industrial waste gas is a chanllenging research topic in the field of chemical engineering and enviromental protection. Carbon dioxide hydrogenation to synthesize methanol is considered as one of ideal way to utilize of carbon dioxide effectively. However,the conversion of carbon dioxde and the selectivity of methanol are very low in this catalytic process,which restrict the industrial application of this catalytic technology.In this project, Cu-based graphene/zinc oxide film catalysts with layered structure will be designed and prepared based on our initial research using chemical reduction and sputtering techniques; the effect of preparation methods on catalysts'structure and catalytic performance for synthesis methanol via carbon dioxid hydrogenation will be investigated; the inherent relations between structure of Cu-based graphene-zinc oxide film catalysts and catalytic activity, methanol selectivtiy will also be studied to reveal the synergistic effect of support and active component.The purpose of this project was to get a new catalyst with high catalytic activity and high methanol selectivity for synthesis methanol from carbon dioxide hydrogenation and provide theoretical basis and technological support to utilize efficiently in the industry.

工业废气二氧化碳的高效循环利用是化学化工和环境保护领域极具挑战性的研究课题。二氧化碳催化加氢合成甲醇是实现二氧化碳有效利用的理想途径之一。然而，目前此催化反应过程二氧化碳的转化率和生成甲醇的选择性均很低，无疑制约了这一催化转化技术的工业化应用。本项目在前期研究基础上，采用化学还原和溅射技术，设计制备具有层状结构的铜基石墨烯-氧化锌膜催化剂；考察制备方法对催化剂结构以及二氧化碳加氢合成甲醇的催化性能的影响；研究铜基石墨烯-氧化锌膜催化剂的结构因素与催化活性和甲醇选择性间的内在联系，揭示催化剂复合载体与活性组分间协同作用机理，最终获得高活性和高选择性的二氧化碳加氢新型催化剂，为实现工业上二氧化碳的高效利用提供理论基础和技术支撑。

二氧化碳催化加氢合成甲醇是实现二氧化碳有效利用的理想途径之一。本项目采用共沉淀法，制备了具有层状结构的铜基石墨烯-ZnO-Al2O3等系列催化剂；考察了原料添加顺序，石墨烯及其衍生物类型，石墨烯添加量以及金属氧化物类型等对石墨烯复合材料结构和对二氧化碳加氢催化性能的影响。同时，对反应温度等不同反应工艺条件对合成甲醇结果的影响规律。研究结果表明，石墨烯的加入利于铜锌铝双电层结构的形成，有效增加了铜的分散度，提高了其对氢气的吸附性能，改善了其对二氧化碳合成甲醇的催化活性。相比与单纯铜锌铝催化剂，二氧化碳的转化率提高了5%,甲醇选择性提高了10%。此项目的实施，为二氧化碳的高效利用提供理论基础和技术支撑。