TS-1 zeotype with one dimension in the nanoscale leads to shorter diffusion channels, conferring reduced diffusion resistance, enhanced accessibility of active sites, and thus improved catalytic performance, especially for bulky molecular substrates. Herein, TS-1 macro-nanosheets, with b-axis thickness in the nanoscale and sizes of a- and c-axis in the micron level, have been successfully synthesized via a direct hydrothermal route with the combination of pre-aging and pH regulation by (NH₄)₂SO₄. Synthesis parameters like the pH value of gel, the type of ammonium salt and the content of structure-directing agent show significant impacts on the morphology of obtained TS-1 zeotypes and the state of Ti sites. The crystallization process of TS-1 macro-nanosheets manifests assembly followed by oriented growth, namely the nonclassical crystallization mechanism. In the epoxidation of alkenes, TS-1 macro-nanosheets exhibit improved catalytic performance in comparison with small-crystals and microcrystals, especially in the epoxidation of long-chain alkenes and bulky molecular substrates. This work offers a straightforward approach to synthesizing high-quality TS-1 macro-nanosheets, providing new insights into developing titanosilicate zeotypes for sustainable catalysis and synthesizing other heteroatom-containing zeolites with morphology control.

在纳米尺度中具有一维的 TS-1 zeotype 导致更短的扩散通道，从而降低了扩散阻力，增强了活性位点的可及性，从而提高了催化性能，特别是对于大体积的分子底物。在此，TS-1 大纳米片材，其 b 轴厚度为纳米级，a 轴和 c 轴尺寸为微米级，通过直接水热路线成功合成，结合 （NH₄）₂SO₄ 的 pH 调节。凝胶的 pH 值、铵盐的类型和结构导向剂的含量等合成参数对获得的 TS-1 沸型的形态和 Ti 位点的状态有显著影响。TS-1 大纳米片的结晶过程表现为组装后定向生长，即非经典结晶机制。在烯烃的环氧化中，与小晶体和微晶相比，TS-1 大纳米片表现出更好的催化性能，尤其是在长链烯烃和大体积分子底物的环氧化中。这项工作提供了一种合成高质量 TS-1 大纳米片的简单方法，为开发用于可持续催化的钛硅酸盐分子筛和通过形态控制合成其他含杂原子分子筛提供了新的见解。