高稳定片层Ni-Mg-Al催化剂的可控制备及其在干气重整中的性能研究

项目名称： 高稳定片层Ni-Mg-Al催化剂的可控制备及其在干气重整中的性能研究

项目编号： No.21506022

项目类型： 青年科学基金项目

立项/批准年度： 2016

项目学科： 有机化学

项目作者： 贺雷

作者单位： 大连理工大学

项目金额： 21万元

中文摘要： 干气重整能够实现甲烷和二氧化碳两种温室气体的转化，对推动碳资源的高效利用及生态环境的可持续发展具有重要意义。Ni基催化剂在该反应中表现出优异的活性，但是粒子烧结和表面积炭造成的失活是该反应面临的首要难题。本项目提出通过插层作用和原位聚合对Ni-Mg-Al水滑石纳米片进行可控包覆，再经高温处理制备具有高温稳定纳米片层结构的新型干气重整Ni催化剂。具体研究包括：从分子底层设计的角度出发，选择合适的结构导向剂及包覆物（氧化石墨烯、SiO2、炭）对Ni-Mg-Al水滑石纳米片进行可控包覆；研究包覆过程的组装化学，准确调控包覆厚度及孔道结构；考察热处理气氛及温度对催化剂结构的影响，制备具有稳定片层结构的Ni-Mg-Al催化剂；对Ni粒子的微观分布及配位环境进行系统表征，明晰化学键合与物理限域对Ni的稳定机制；利用TPSR-MS等原位谱学跟踪反应历程，理解催化剂微观结构与反应性能的内在联系。

中文关键词： 镍；水滑石；纳米片；可控包覆；干气重整

英文摘要： Two greenhouse gases (CH4 and CO2) could be efficiently converted through dry reforming reaction, which is considerably important for carbon resource utilization and environment protection. Ni-based catalysts showed excellent performance in this reaction. However, the deactivation of Ni catalyst originated from sintering and coking remains the major challenge. This project aims to synthesize a novel Ni catalyst with highly stable nanosheet structure derived from Ni-Mg-Al hydrotalcite nanosheet with a coating layer based on the interlayer reaction and in-situ polymerization principle. The details are: synthesis of nanocoated Ni-Mg-Al hydrotalcite nanosheet based on molecular design using desirable structure-directing agents and coating precursors (GO, SiO2, carbon); studying the assembly mechanism of the nanocoating process to make precise control of the thickness and pore-structure of the coating layer; investigating the influence of heat treatment conditions on the structure of final Ni-Mg-Al catalyst; identifying the dispersion and coordination environment of Ni nanoparticles to clarify the stability mechanism for Ni via chemical bonding and physical confinement; investigating the catalytic performance of the above-mentioned catalyst in dry reforming and revealing the intrinsic relationship between the micro-structure and its catalytic performance using in-situ spectrometry characterization (e.g., TPSR-MS) for tracking the reaction process.

英文关键词： nickel;hydrotalcite;nanosheet;controlled nanocoating;dry reforming