Smith Louise R, Kohlrausch Emerson C, Aggett Kieran J, Chen Yifan, Gow Isla E, Weilhard Andreas, Norman Luke T, Theis Wolfgang, Morgan David J, Bailey Liam, Khlobystov Andrei N, Alves Fernandes Jesum, Hutchings Graham J
Max Planck-Cardiff Centre on the Fundamentals of Heterogeneous Catalysis FUNCAT, Translational Research Hub, Cardiff University, Maindy Road, Cardiff CF24 4HQ, U.K.
School of Chemistry, University of Nottingham, University Park, Nottingham NG7 2RD, U.K.
ACS Catal. 2025 Aug 22;15(17):15502-15508. doi: 10.1021/acscatal.5c04822. eCollection 2025 Sep 5.
Carbon dioxide is not only a greenhouse gas but also a valuable feedstock for producing chemicals and fuels, especially methanol, which serves as an energy storage medium and a precursor for olefins and gasoline. Herein, we show that a clean, atomically defined interface between a Pd catalyst and a ZnO support allows for the direct production of methanol from CO without any catalyst activation or induction period. Using magnetron sputtering, Pd atoms are directly deposited onto the ZnO surface, self-assembling into Pd nanoclusters with a high fraction of surface atoms, driven solely by the surface chemistry of ZnO, eliminating the need for solvents, reagents, or ligands. This atomically defined Pd/ZnO interface facilitates Pd-Zn alloying in situ during the reaction, achieving an impressive methanol production rate of 16.4 mol h mol , outperforming catalysts prepared by other methods. By eliminating interfacial impurities and the consequent need for pretreatment, our work establishes magnetron sputtering as a transformative method for fabricating high-performance catalysts.
二氧化碳不仅是一种温室气体，也是生产化学品和燃料的宝贵原料，尤其是甲醇，甲醇可作为能量存储介质以及烯烃和汽油的前体。在此，我们表明，钯催化剂与氧化锌载体之间清洁、原子级明确的界面能够在无需任何催化剂活化或诱导期的情况下，直接由一氧化碳生产甲醇。利用磁控溅射，钯原子直接沉积在氧化锌表面，仅在氧化锌表面化学作用的驱动下，自组装成具有高比例表面原子的钯纳米团簇，无需溶剂、试剂或配体。这种原子级明确的钯/氧化锌界面在反应过程中促进了钯 - 锌的原位合金化，实现了令人印象深刻的16.4 mol h⁻¹ mol⁻¹的甲醇生产率，优于通过其他方法制备的催化剂。通过消除界面杂质以及随之而来的预处理需求，我们的工作确立了磁控溅射作为一种制造高性能催化剂的变革性方法。
