Yun Yapei, Shen Honglei, Shi Yanan, Zhu Yanan, Wang Sicong, Li Kaikai, Zhang Bei, Yao Tao, Sheng Hongting, Yu Haizhu, Zhu Manzhou
School of Chemistry & Chemical Engineering, School of Materials Science and Engineering and Anhui Province Key Laboratory of Chemistry for Inorganic/Organic Hybrid Functionalized Materials, Institutes of Physical Science and Information Technology, Department of Chemistry and Center for Atomic Engineering of Materials, Key Laboratory of Structure and Functional Regulation of Hybrid Materials of the Ministry of Education, Anhui University, Hefei, 230601, P. R. China.
National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, 230026, P. R. China.
Adv Mater. 2024 Sep;36(39):e2409436. doi: 10.1002/adma.202409436. Epub 2024 Aug 9.
Dual-atom catalysts (DACs) originate unprecedented reactivity and maximize resource efficiency. The fundamental difficulty lies in the high complexity and instability of DACs, making the rational design and targeted performance optimization a grand challenge. Here, an atomically dispersed Pd DAC with an in situ generated Pd─Pd bond is constructed by a dynamic strategy, which achieves high activity and selectivity for semi-hydrogenation of alkynes and functional internal acetylene, twice higher than commercial Lindlar catalyst. Density functional theory calculations and systematic experiments confirms the ultrahigh properties of Pd DAC originates from the synergistic effect of the dynamically generated Pd─Pd bonds. This discovery highlights the potential for dynamic strategies and opens unprecedented possibilities for the preparation of robust DACs on an industrial scale.
双原子催化剂（DACs）展现出前所未有的反应活性，并使资源利用效率最大化。其根本难点在于DACs具有高度的复杂性和不稳定性，这使得合理设计和有针对性的性能优化成为一项巨大挑战。在此，通过一种动态策略构建了一种具有原位生成的Pd─Pd键的原子分散Pd双原子催化剂，该催化剂在炔烃和官能化内乙炔半加氢反应中实现了高活性和高选择性，比商业林德拉催化剂高出两倍。密度泛函理论计算和系统实验证实，Pd双原子催化剂的超高性能源于动态生成的Pd─Pd键的协同效应。这一发现凸显了动态策略的潜力，并为在工业规模上制备稳定的双原子催化剂开辟了前所未有的可能性。
