环境影响下Pd基催化双氧水直接合成理论模拟

双氧水直接合成法是极具潜力的化工过程，研究表界面反应机理是设计出高活性和高稳定催化剂的关键。大多数采用密度泛函理论结合微观动力学研究双氧水反应机理是不含环境影响的，进而导致动力学预测结果和实验原位表征结论的不匹配性。针对这一现状，并基于申请人对含覆盖度影响的微观动力学模拟的研究基础，本项目将采用含环境影响的微观动力学模型研究Pd基催化剂双氧水直接合成反应机理，旨在阐明反应环境如覆盖度，溶剂，温度，压力以及催化剂表面和界面空间结构对化学反应过程的影响。此外，本项目将开发从活性位点到纳米粒子的微观动力学模型，预测双氧水合成在纳米粒子表界面反应机制，为催化剂的研发提供理论依据。

The direct synthesis of hydrogen peroxide is a potential chemical process. Studying the reaction mechanism of surface and interface is the key to designing a highly active and stable catalyst. Most of the studies on the reaction mechanism of hydrogen peroxide using density functional theory combined with microkinetic modeling does not contain the environmental impact, which leads to a mismatch between the kinetic results and the experimental in-situ characterization conclusions. In view of this situation and based on applicant's research experience on coverage-dependent kinetic modeling, this project will use microkinetic modeling with environmental effects to study the reaction mechanism of the direct synthesis of hydrogen peroxide in Pd-based catalysts in order to clarify the reaction environment such as coverage, solvent, temperature, pressure and the effect of catalyst surface and interface space structure on the chemical reaction process. In addition, this project will develop microkinetic modeling from active sites to nanoparticles, predict the reaction mechanism of hydrogen peroxide synthesis on the surface and interface of nanoparticles, and provide a theoretical basis for the development of catalysts.