中文摘要：

纳米Au催化剂被认为是具有商业价值的用于醇选择氧化的第二代催化剂.这是因为Au氧化还原电势高,化学稳定性好,可抑制易使Pt族元素中毒的胺等的毒化;其次,对于一些特定选择氧化和还原反应而言,具有较优的反应选择性.目前较多的研究集中在调变Au纳米颗粒与氧化物载体的相互作用,获得协同效应.例如,利用CeO2纳米晶为载体,沉积Au纳米颗粒（约3 nm）,使CeO2部分还原为非计量比的催化材料,活化氧并获得高选择氧化性能.碳是相对惰性的载体,与Au相互作用力弱,因此可被用于研究Au纳米颗粒本征催化性能.但负载碳金催化剂在焙烧甚至还原过程中易团聚,且在反应中易流失,可能导致活性下降.利用胶体沉积法可获得介孔碳担载纳米Au催化剂,对葡萄糖选择氧化具有很高的催化活性和选择性.但是,制备中使用的保护剂残留经常被忽略.由于立体效应或电子结构调变作用,保护剂可能影响Au催化剂活性或稳定性.我们前期建立了反应单体参与的自组装技术合成功能化介孔碳路线,一步在介孔碳骨架中掺杂氧化物纳米催化剂.本文从介孔催化材料的结构出发,设计＂镶嵌＂在碳骨架中的纳米Au颗粒.采用配位作用辅助表面活性剂自组装技术,以苯酚和甲醛为碳前体,引入含巯基硅烷偶联剂,通过配位作用稳定金离子,获得尺寸可控介孔碳限域纳米Au催化剂.低温炭化中,由于巯基-金的配位作用阻抑金属移动或团聚,高温下聚合物炭化为相对刚性的碳骨架.此时,Au纳米颗粒被相邻介孔孔墙限制.硅烷偶联剂可除去,不影响碳载体,并可产生丰富二级孔道,获得多级孔道介孔碳材料.X射线衍射和透射电镜结果显示,所合成的催化剂中Au颗粒的尺寸可控,为3-18nm,且具有单分散性,均匀地分散在整个介孔碳骨架中,其含量为1.1-9.0wt%.金碳催化剂具有有序的二维六方介孔结构.能量散射谱（EDX）

英文摘要：

Simultaneously controlling the size of Au nanoparticles and immobilizing their location to specific active sites while hindering migration and sintering at elevated temperatures is a current challenge within materials chemistry.Typical methods require the use of protecting agents to control the properties of Au nanoparticles and therefore it is difficult to decouple the influence of the protecting agent and the support material.By functionalizing the internal surface area of mesoporous carbon supports with thiol groups and implementing a simple acid extraction step,we are able to design the resulting materials with precise control over the Au nanoparticle size without the need for the presence of any protecting group,whilst simultaneously confining the nanoparticles to within the internal porous network.Monodispersed Au nanoparticles in the absence of protecting agents were encapsulated into ordered mesoporous carbon at various loading levels via a coordination-assisted self-assembly approach.The X-ray diffractograms and transmission electron microscopy micrographs show that the particles have controlled and well-defined diameters between 3 and 18 nm at concentrations between 1.1 and 9.0 wt%.The Au nanoparticles are intercalated into the pore matrix to different degrees depending on the synthesis conditions and are stable after high temperature treatment at 600 °C.N2 adsorption-desorption isotherms show that the Au functionalized mesoporous carbon catalysts possess high surface areas（1269–1743 m~2/g）,large pore volumes（0.78–1.38 cm~3/g）and interpenetrated,uniform bimodal mesopores with the primary larger mesopore lying in the range of 3.4–5.7 nm and the smaller secondary mesopore having a diameter close to 2 nm.X-ray absorption near extended spectroscopy analysis reveals changes to the electronic properties of the Au nanoparticles as a function of reduced particle size.The predominant factors that significantly determine the end Au nanoparticle size is both the thiol group concentration and subject