锰基尖晶石协同脱除煤气中Hg0/AsH3/H2Se的性能与机理研究

吸附法协同脱除煤气中的Hg0/AsH3/H2Se是一种极具潜力的挥发性有毒痕量元素控制技术，高性能吸附剂的开发是该技术的关键。锰基尖晶石具有灵活的可调性、独特的形貌结构和氧化还原特性，是很有发展前景的痕量元素吸附剂。关键科学问题在于深刻理解多污染物协同脱除的反应机理和动力学。现有研究局限于实验现象观测和数据积累，缺乏微观层面上相互作用机理的深入理解。本项目将量子化学和过渡态理论交叉融入到燃烧学中，从原子水平上剖析相互作用的本质和微观反应机理。探究吸附剂微观结构与吸附性能之间的构效关系；揭示吸附剂表面上Hg0/AsH3/H2Se脱除的竞争机制和协同反应机理；阐释煤气组分对锰基尖晶石协同脱除性能的影响机理。通过大气污染控制化学、量子化学、催化化学等交叉研究，为高性能Hg0/AsH3/H2Se协同脱除吸附剂的分子设计和定向调控奠定基础。

Adsorption is a promising method for the simultaneous removal of Hg0/AsH3/H2Se from syngas. Highly efficient sorbents are crucial to the simultaneous removal of multi-pollutants. Mn-based spinels are regarded as the potential sorbents due to its inherent structural and physicochemical properties. The key factor for the successful application of Mn-based spinels is to uncover the reaction mechanisms and kinetics of multi-pollutants simultaneous removal. However, the current studies mainly focus on experimental observation and data accumulation, and cannot provide a deeper understanding of interaction mechanism at the microscopic level. This project integrates quantum chemistry and transition state theory into combustion science to understand the nature and microscopic mechanism of interaction at the molecular level. The structure-activity relationship of sorbents will be explored. The competition and reaction mechanisms of Hg0/AsH3/H2Se removal on sorbent surface will be revealed. The effects of syngas compositions on the simultaneous removal performance of sorbents will be systematically studied to clarify the anti-poisoning mechanism of Mn-based spinels. Based on the multi-disciplinary studies of air pollution control chemistry, quantum chemistry, and catalytic chemistry, this project will provide the basis for the molecular design and performance manipulation of highly efficient sorbents.