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中文摘要：
本项目充分利用近年来不断涌现的纳米新材料和纳米催化材料的新制备方法，紧密结合基于超高真空的表面科学技术的模型体系研究、原位谱学表征和理论计算研究，开展与轻质烷烃、合成气和纤维素高选择性催化转化、电动汽车用高效蓄电体系和燃料电池以及与太阳能转化相关的功能材料的设计、研制和相关的基础研究，在分子和原子水平上认识相关过程的机理，为设计和研制具有优异性能的功能材料提供科学基础，以期解决国家在能源领域的关键科学与技术瓶颈问题。
英文摘要：
synthesis gas；selectivity control；liquid fuel；olefin；oxygenate
结论摘要：
本项目遴选合成气催化转化制碳氢化合物燃料、烯烃和醇醚以及合成气间接法制乙二醇路线的草酸酯加氢为主要目标反应，围绕选择性调控这一关键科学问题，从催化剂和催化体系的设计和构筑、催化剂活性中心及其作用机理和反应机理的表征等方面开展了系统的基础和应用研究。针对费托合成制备汽、柴油等液体燃料反应，提出了使用新型固体酸材料，通过控制载体的二次裂解反应以及调节载体孔结构提高燃料烃选择性的新策略。使用该方法，我们在碳纳米管和介孔分子筛载体负载金属催化剂上实现了高选择性合成气直接转化生成柴油(C10？C20, 60%)和汽油(C5？C11, 80%)烃的目标。针对CO加氢制低碳烯烃反应，制备并研究了纳米碳化铁在合成气制烯烃反应中的催化性能。针对CO2加氢制烯烃反应，研究了K，B修饰对体相铁催化剂催化性能的促进作用；构建了碳纳米管负载的粒径分布均匀、助剂与活性组分紧密接触的Fe3-xMnxO4/CNT模型催化剂，在排除了金属的粒径以及助剂与载体之间的强相互作用的情况下考察了Mn对Fe基催化剂上费托合成制低碳烯烃的促进作用。针对合成气加氢制乙醇、低碳醇反应，研发出具工业应用前景的碳纳米管促进Ni-Mo-K硫化物基催化剂和Ni-M′-Mo-K氧化物基催化剂。前者的主要产物为乙醇，其C-基选择性达33.1%；后者的主要产物为C2~4-醇，其C-基选择性达50.6%。催化剂的表征研究揭示CNT促进剂系通过其sp2-C表面吸附活化H2，产生sp2-C–H形式的氢吸附物种; 适当降低CNT 的颗粒度（相应地增大sp2-C表面积）能提高CNT的促进效应。针对合成气间接法制乙二醇路线的草酸酯加氢反应，研制出具优异催化活性和极高的稳定性的少量币（饰）族金属Au，Ag和Pt等修饰以及碳纳米管，La2O3，B2O3和MFI分子筛等促进的负载铜催化剂。对催化剂作用机理的研究表明，铜与币（饰）族的合金作用或促进剂与铜物种之间的相互作用，有利于催化剂表面形成比例合适的Cu+和Cu0物种，并可促进铜纳米粒子的分散、提高活性铜物种的表面积和对氢分子活化能力。
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期刊论文
Supported monodisperse Pt nanoparticles from Pt-3(CO)(3)(mu(2)-CO)(3) (5)(2-) clusters for investiga
Cu24O24Si8R8: Organic Soluble 56-Membered Copper(I) Siloxane Cage and Its Use in Homogeneous Catalys
Probing Stepwise Reaction of NNP-Ligand Copper(I) Complex with Elemental Sulfur by Using N-Heterocyc
Structure and catalytic performance of alumina-supported copper-cobalt catalysts for carbon monoxide
Highly efficient mesostructured Ag/SBA-15 catalysts for the chemoselective synthesis of methyl glyco
Bronsted acidic ionic liquid as an efficient and recyclable promoter for hydroesterification of olef
Copper-catalyzed propylene epoxidation by oxygen Significant promoting effect of vanadium on unsuppo
Iron-Catalyzed Highly Enantioselective Reduction of Aromatic Ketones with Chiral P2N4-Type Macrocycl
Spectroscopic and DFT Study on the Interaction System of Vanadium with L-Proline in Aqueous Solution
Trends in R-X Bond Dissociation Energies (R-center dot = Me, Et, i-Pr, t-Bu, X-center dot = H, Me, C
Theoretical studies of Na+ location in ZSM-5: Model selection for accurate coordination structure an
Acid-catalysed direct transformation of cellulose into methyl glucosides in methanol at moderate tem
Exploring the Sodium Cation Location and Aluminum Distribution in ZSM-5: A Systematic Study by the E
Conversion of cellobiose into sorbitol in neutral water medium over carbon nanotube-supported ruthen
Production of ethanol by gas phase hydrogenation of acetic acid over carbon nanotube-supported Pt-Sn
PVP-stabilized heteropolyacids as reusable self-assembling catalysts for alcoholysis of cellulosic s
DCMB that Combines Divide-and-Conquer and Mixed-Basis Set Methods for Accurate Geometry Optimization
Cu/SiO2 hybrid catalysts containing HZSM-5 with enhanced activity and stability for selective hydrog
An efficient Ni-Mo-K sulfide catalyst doped with CNTs for conversion of syngas to ethanol and higher
Improved performance of magnetically recoverable Ce-promoted Ni/Al2O3 catalysts for aqueous-phase hy
Electronic Properties and Desolvation Penalties of Metal Ions Plus Protein Electrostatics Dictate th
Influence of the support and promotion on the structure and catalytic performance of copper-cobalt c
Vapor-phase hydrogenation of dimethyl oxalate over a CNTs-Cu-SiO2 hybrid catalyst with enhanced acti
Synthesis of novel chiral tetraaza ligands and their application in enantioselective transfer hydrog
A boracite metal-organic framework displaying selective gas sorption and guest-dependent spin-crosso
Na+-intercalated carbon nanotubes-supported platinum nanoparticles as new highly effective catalysts
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