南京大学祝艳团队报道了分子样Au8M(PPh3)8n+簇在介孔SBA-15中培养的非均相催化。相关研究成果发表在2024年12月2日出版的国际知名学术期刊《德国应用化学》。

研究人员的梦想是能够通过在原子水平上，调节非均相催化剂来定制催化性能。原子精确的金属团簇为研究人员提供了实现这一挑战的可能性。

该文中，研究人员设计了一种推拉合成策略，通过在介孔分子筛中培养原子精确的Au8M(PPh3)8n+（M=Pd、Pt或Au；Pd/Pt n=2，Au n=3）团簇，结合TiOx涂层来制备表示为TiOx/Au8M@SBA的非均相催化剂。

催化剂由三个功能单元组成，其中包括可以充当活性位点的Au8M（PPh3）8n+簇、可以在化学反应过程中保持精确原子数的SBA-15的孔环境，以及可以进一步抑制簇在反应条件下迁移的TiOx涂层。以在固定床反应器中进行的乙炔选择性氢化为例，研究人员揭示了非均相催化剂的逐个原子定制，如何通过簇催化开启难以捉摸的非均相机制。

该项工作揭示了非均相催化剂催化起源的重要见解，并为簇催化提供了卓越的细节水平。

附：英文原文

Title: Heterogeneous Catalysis of Molecular-Like Au8M(PPh3)8n+ Clusters Cultivated in Mesoporous SBA-15

Author: Tianqi Sun, Bingqing Ge, Shuangshuang Huang, Xiuwen Wang, Yiqi Tian, Xiao Cai, Weiping Ding, Yan Zhu

Issue&Volume: 2024-12-02

Abstract: It is a dream of researchers to be able to tailor the catalytic performances by adjusting heterogeneous catalysts at the atomic level. Atomically precise metal clusters provide us with the possibility to achieve this challenge. Here, we design a push-and-pull synthesis strategy coupled with TiOx coating to prepare the heterogeneous catalysts denoted as TiOx/Au8M@SBA via cultivating atomically precise Au8M(PPh3)8n+ (M = Pd, Pt or Au; n = 2 for Pd/Pt and 3 for Au) clusters in mesoporous molecular sieve. The catalysts are made up of the three functional units, which include Au8M(PPh3)8n+ clusters that can act as the active sites, the pore environment of the SBA-15 that can announce a catalysis show for the clusters with precise number of atoms maintained during the chemical reactions, and the TiOx coating that can further inhibit the migration of the clusters under reaction conditions. The selective hydrogenation of acetylene performed in the fixed-bed reactor taken, for example, we learn how the atom-by-atom tailoring of a heterogeneous catalyst can switch on elusive heterogeneous mechanisms with cluster catalysis. This work sheds light on the fundamental insight into catalysis origin of heterogeneous catalysts and achieves a distinguished level of detail for cluster catalysis.

DOI: 10.1002/anie.202420274

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202420274