NTP耦合Ni/HAP-Fe单原子催化剂强化焦油重整及协同抑制积碳机理研究

焦油是制约生物质气化技术进一步发展的最主要瓶颈。低温等离子体（NTP）和催化是焦油重整的有效手段，针对两者单独作用对焦油中难转化的无支链芳香环结构化合物（苯、萘、菲等）裂解率低、副产物多及催化剂易积碳等问题，本申请提出NTP耦合催化反应体系，通过NTP产生的高活性粒子撞击苯环C-C键使其断裂，利用催化剂的活性位定向转化裂解中间产物。依据该机制设计一系列结构可控的Fe掺杂Ni/HAP-Fe单原子催化剂，系统考察催化剂的构筑方法与其酸（碱）位分布、金属离子尺寸、落位配位结构等在NTP耦合催化过程中对焦油重整反应历程及产物分布的调控规律，建立NTP与催化剂活性位对焦油转化的耦合/解耦机制。结合催化剂积碳的多维度表征，探讨NTP、催化剂及反应气氛（CO2、H2O等）对积碳形成/演化的作用规律及NTP耦合催化剂对积碳抑制/消除的协同作用。为NTP耦合催化转化生物质气化焦油提供理论基础和技术支撑。

Biomass tar is the most important bottleneck restricting the further development of biomass gasification. Non-thermal plasma (NTP) and catalysis are effective means of tar cracking/reforming. Aiming at the problem of the most difficult to convert unbranched aromatic ring compounds (benzene, naphthalene, phenanthrene, etc.) in tar have low cracking rate, many by-products and the catalysts are easily deactivated by carbon deposition when NTP and catalysis are used separately. The present application proposes an NTP coupled catalytic reaction system, in which the high-activity particles generated by NTP collied with the benzene ring to break the C-C bond, and the intermediate products are directionally converted by using the active sites of the catalyst. Then, a series of Fe doped Ni/HAP-Fe single-atom catalysts with controllable structure are constructed according to this mechanism. The effects of the method of constructing the catalyst and its acid (base) position distribution, metal ion size and coordination structure are investigated systematically on tar reforming and its product distribution during NTP coupled catalysis. The coupling/decoupling mechanism between NTP and catalyst surface characteristics for tar conversion are established. Combined with the multi-dimensional and multi-scale characterization of catalyst carbon deposition, the mechanism of NTP, catalyst and reaction atmosphere (CO2, H2O, etc.) in the formation and evolution of carbon deposition and the synergistic effect of NTP coupling catalyst on the inhibition /elimination of carbon deposition are discussed. The completion of this project will provide theoretical basis and technical support for the NTP coupled catalytic cracking of biomass gasification tar.