BCN负载Ru纳米颗粒的合成及HER性能研究

Synthesis and HER Properties of Ru Nanoparticles Loaded with BCN

在碳载体上负载金属纳米颗粒是提高金属利用率和电催化活性的有效途径。强金属–载体相互作用可以有效调节金属纳米粒子的表面结构与电子状态,提升其活性。B、N和C原子因其具有不同电负性,可以诱导BCN结构出现离子化特征,增强金属颗粒与基底的相互作用,优化析氢中间体结合能。采用4,4’-联吡啶与Cs2 [closo-B12H12]组装的新型硼有机聚合物BOPs作为还原剂和载体,一方面原位还原Ru盐生成金属Ru颗粒,另一方面作为B源和N源,构建了BCN材料。热解后,由于双掺杂B和N的协同耦合作用,增加了金属纳米颗粒与载体之间的电子传递,使得Ru/BCN展现出优异析氢性能,尤其是Ru/BCN-700在碱性介质中,只需要17 mV的过电位就能达到10 mA∙cm−2的电流密度,因此,B,N双掺杂碳基底促进了Ru金属颗粒的分散,调控了Ru的电子结构,为制备高性能催化剂提供了简便的策略。

Loading metal nanoparticles on carbon carriers is an effective way to improve metal utilization and electrocatalytic activity. Strong metal-support interactions can effectively modulate metal nanoparticles’ surface structure and electronic state to enhance their activity. Due to their different electronegativity, B, N, and C atoms can induce ionization features in BCN structures, enhance the interaction between metal particles and substrates, and optimize the binding energy of hydrogen precipitation intermediates. The new boron organic polymer BOPs assembled with 4,4’-bipyridine and Cs2 [closo-B12H12] were used as reducing agents and carriers to generate metal Ru particles by in situ reduction of Ru salts on the one hand, and as B and N sources on the other hand to construct BCN materials. After pyrolysis, due to the synergistic coupling effect of the double-doped B and N, the electron transfer between the metal nanoparticles and the carriers was increased, which made Ru/BCN exhibit excellent hydrogen precipitation performance, especially Ru/BCN-700 could reach a current density of 10 mA cm−2 with only 17 mV overpotential in alkaline medium, thus, the B, N double-doped carbon substrate promoted the Ru metal particle dispersion, modulates the electronic structure of Ru, and provides a facile strategy for the preparation of high-performance catalysts.