Noble metal‐catalyzed reductive amination of carbonyl compounds using molecular hydrogen is a promising green route for amine synthesis, but a challenge remains to boost the atomic efficiency of noble metal species. Herein, MFI zeolite encapsulated Pt species with tunable Si/Al ratios were synthesized to allow the formation of Pt nanoparticles (NPs) with almost the same loading amount, particle size, and electronic state. Confining Pt NPs allows the spatial satisfaction for the synergy of metal centers and acid sites, and Pt@ZSM‐5(100) with a moderate Si/Al ratio performed high efficiency in the conversion of carbonyl compounds and boosted high TOF of 23,409 h−1 in reductive amination of benzaldehyde. Combined with structure refinement, x‐ray absorption fine structure (XAFS), in situ Fourier transforms infrared (FTIR) spectroscopy, and theoretical calculation, the study indicated that modulating the Si/Al ratio enables the fine rationalization of the microenvironment. The moderate Si/Al ratio causes suitable acid intensity that significantly contributes to the carbonyl compound activation and product desorption.

中文翻译：

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将 Pt 物质封装到具有可调酸位点的 MFI 分子筛中可促进对叔胺的还原胺化


使用分子氢的贵金属催化羰基化合物的还原胺化是一种很有前途的胺合成绿色途径，但提高贵金属种类的原子效率仍然存在挑战。在此，合成了具有可调 Si/Al 比率的 MFI 沸石封装的 Pt 物种，以允许形成具有几乎相同负载量、粒径和电子状态的 Pt 纳米颗粒 （NP）。限制 Pt NPs 允许金属中心和酸位点协同作用的空间满足，具有适度 Si/Al 比率的 Pt@ZSM-5（100） 在羰基化合物的转化中表现出高效率，并在苯甲醛的还原胺化中提高了 23,409 h-1 的高 TOF。结合结构细化、X 射线吸收精细结构 （XAFS）、原位傅里叶变换红外 （FTIR） 光谱和理论计算，研究表明，调节 Si/Al 比率可实现微环境的精细合理化。适度的 Si/Al 比率会产生合适的酸强度，从而显着促进羰基化合物的活化和产物解吸。