We developed nano Pd catalysts, encapsulated within carbon-nitrogen layers at both intra-pore and interfacial levels on SiO, via in-situ thermolysis of metal-organic coordination compounds. The catalysts dehydrogenation efficacy is greatly influenced by thermolysis temperature and ligand-to-metal ratio. The Pd-C-N/SiO-600 catalyst notably achieved complete dehydrogenation of 12 H-NPCZ within 240 minutes, demonstrating exceptional stability over 10 cycles without significant degradation, highlighting its viability for commercial use. Characterizations revealed that the C-N layer integration improves Pd nanoparticle dispersion and reduces strong acid site formation on catalyst surface. This synergy between the C-N layer and Pd nanoparticles promotes the formation and stabilization of Pd species, optimizing them as adsorption sites for dehydrogenation with appropriate acid strength. Moreover, this interaction adjusts the electronic states of Pd active sites, optimizing adsorption dynamics for intermediates. This cooperative action between Pd and Pd significantly boosts the desorption rate of dehydrogenation products, substantially improving the catalysis performance.

中文翻译：

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吡啶N诱导孔内和界面双限域Pd0-Pdδ+协同催化十二氢-N-丙基咔唑超稳定脱氢

我们开发了纳米钯催化剂，通过金属有机配位化合物的原位热解，将其封装在 SiO2 的孔内和界面水平的碳氮层中。催化剂的脱氢效率受热解温度和配体与金属的比例影响很大。 Pd-CN/SiO-600 催化剂在 240 分钟内实现了 12 H-NPCZ 的完全脱氢，在 10 个循环中表现出卓越的稳定性，而没有明显降解，突出了其商业用途的可行性。表征表明，CN 层集成改善了 Pd 纳米粒子的分散性并减少了催化剂表面强酸位点的形成。 CN层和Pd纳米粒子之间的协同作用促进了Pd物质的形成和稳定，优化它们作为具有适当酸强度的脱氢的吸附位点。此外，这种相互作用调节钯活性位点的电子态，优化中间体的吸附动力学。 Pd和Pd之间的这种协同作用显着提高了脱氢产物的解吸速率，从而显着提高了催化性能。