过渡金属硫化物催化剂上木质素催化转化反应研究

Transition metal sulfide catalysts have great value in sulfur containing lignin conversion research since they have acid sites, sulfur resistant ability and hydrogenation activity. This project aims at the application of transition metal sulfide catalysts in the catalytic conversion of lignin, using the aromatic model compounds which have similar C-C and C-O bonds with that in lignin structure as the probe molecules, it will focus on the hydrodeoxygenation of several aromatic model compounds using sulfide catalysts. A series of monometallic or bimetallic transition metal sulfide catalysts will be designed and synthesized. Meanwhile, several characterization methods will be introduced to characterize the composition and structure of the as-synthesized catalysts in order to have a deep understanding of the interaction and synergistic effect between the metal and sulfide active sites on the bimetallic catalysts. At last, hydrodeoxygenation of several aromatic model compounds using the as-synthesized transition metal sulfide catalysts will be studied. The catalytic activity, selectivity and stability of the catalysts in the reaction will be examined. More importantly, the effect of the interaction between the active sites and the products will be studied associated with physicochemical properties of the catalyst. Upon the implementation of this proposal, it could provide theoretical and technical guidance for the activation of the different C-C and C-O linkages existing in lignin structure as well as the development of highly efficient catalyst systems in lignin conversion research.

过渡金属硫化物催化剂由于具有良好的酸性、抗硫性及加氢活性，在含硫木质素转化领域具有重要的研究价值。本项目以探索硫化物催化剂在木质素转化反应中的应用为目的，采用具有与木质素结构中不同C-C键及C-O键相似的芳香族模型化合物作为探针反应物，开展硫化物催化木质素加氢脱氧反应研究。设计合成对木质素加氢脱氧反应具有高活性及高选择性的单/双金属硫化物催化剂，并借助物理化学表征手段深入认识催化剂的组成及结构性质，揭示金属助剂与硫化物组分间的相互作用及协同机制；与木质素模型化合物加氢脱氧反应行为进行关联，深入认识催化剂对不同C-C键及C-O键的活化能力，揭示其活性、选择性及稳定性的变化规律，并与催化剂的物化性质进行关联，阐明催化剂活性中心与产物间的应答机制。本项目的实施将为探索活化木质素结构中不同C-C键及C-O键新方法，发展新型木质素高效转化催化剂体系提供重要的科学依据与理论指导。

木质素是自然界唯一含有芳香环结构的化合物，将其催化降解可以得到小分子芳香族化合物。过渡金属硫化物催化剂由于具有良好的酸性、抗硫性及加氢活性，在含硫木质素转化领域具有重要的研究价值。本项目以探索硫化物催化剂在木质素转化反应中的应用为目的，采用具有与木质素结构中不同C-C键及C-O键相似的芳香族模型化合物作为探针反应物，开展了硫化物催化木质素加氢脱氧反应研究。项目首先制备合成了对木质素加氢脱氧反应具有高活性及高选择性的MoS2、Co- MoS2及Ni- MoS2催化剂体系，并借助物理化学表征手段深入认识催化剂的组成及结构性质，揭示了金属助剂与硫化物组分间的相互作用及协同机制；与木质素模型化合物加氢脱氧反应行为进行关联，深入认识催化剂对不同C-C键及C-O键的活化能力，揭示了其活性、选择性及稳定性的变化规律。并深入与催化剂的物化性质进行关联，阐明了催化剂活性中心与产物选择性间的应答机制。本项目研究成果为活化木质素结构中不同C-C键及C-O键提供了新方法，为发展新型木质素高效转化催化剂体系提供了重要的科学依据与理论指导。