Cu-Pd合金团簇可控制备及其CO2电催化还原机制的研究

The design and preparation of highly efficient catalyst are the key to the realization of CO2 electrocatalytic reduction. In this project, we focus on two key issues: the preparation of Cu-Pd alloy clusters with controllable size, and how the size of clusters and the phase structure of alloy clusters affect the process of CO2 electrocatalytic reduction. Both experimental and theoretical research will be carried out on these two aspects simultaneously. Multiple target magnetron plasma gas source and low energy cluster beam deposition technique will be used to obtain highly mono-dispersed surface supported Cu-Pd alloy clusters by controlling the gas phase growth conditions. The influence of preparation conditions on the composition, size and structure of Cu-Pd alloy clusters will be studied. The evolution of phase structure of Cu-Pd alloy clusters with composition and size will be investigated. Further, the effect of composition, size and structure of Cu-Pd alloy clusters on CO2 electrocatalytic reduction will be explored by combing the in-situ monitoring system of electrocatalysis-mass spectrometry. The final goals are to establish a stable and controllable method for the preparation of Cu-Pd alloy clusters and to obtain Cu-Pd alloy clusters with excellent CO2 electrocatalytic reduction performance, which is expected to promote the research and development of CO2 electrocatalysts.

高效催化剂的设计和制备是实现CO2电催化还原的关键。本项目针对尺寸、结构可控的Cu-Pd合金团簇的制备以及团簇尺寸与合金相结构如何影响CO2电催化还原过程这两个关键问题，开展实验和理论研究。采用多靶磁控等离子体气体聚集源和低能团簇束流沉积技术，通过控制气相生长条件获得高度单分散的表面担载Cu-Pd合金团簇。研究制备条件对Cu-Pd合金团簇的组分、尺寸及结构的影响，探讨Cu-Pd合金团簇的相结构随组分、尺寸的演变规律。结合电催化-质谱原位监测系统，阐明不同组分、尺寸及结构的Cu-Pd合金团簇对CO2电催化还原的影响机制。建立稳定、可控制备Cu-Pd合金团簇的方法，获得具有优良CO2电催化还原性能的Cu-Pd合金团簇，推动CO2电催化剂的研究开发。

设计和制备高效催化剂是实现CO2电催化还原的关键。金属原子团簇因其具有超高的表面能和极强的催化活性，有望得到广泛应用。本项目采用低能团簇束流沉积技术，设计并可控制备了Cu-Pd合金团簇，同时对其相结构、催化性能与组分、尺寸的关联进行了系统深入的研究。针对合金团簇结构难以控制的问题，本项目以双靶材或复合单靶为靶源，获得不同结构的合金团簇，探究了靶材结构对团簇结构的影响。其中，通过采用特殊的复合靶材结构获得核-壳结构的Cu-Pd合金团簇，其具有结构统一，尺寸均匀等特性，结果表明该方法可有效制备合金团簇且具有通用性。在此基础上，结合团队自行设计的CO2电催化还原反应流动池，并通过气相色谱证明Cu-Pd合金团簇有效促进了乙烯的生成。针对CO2电催化还原反应能耗大的问题，本项目创新性提出将气相沉积技术和电化学剥离技术相结合，获得具有超高稳定性和活性的对电极，有效降低CO2电催化还原的能量损耗。本项目为可控制备新型合金原子团簇及其在电催化领域的应用提供了充分的理论指导和详实的数据支撑，为原子团簇在新能源领域的应用提供了宝贵经验。