多功能载氧体生物质原料CO2原位吸附强化连续化学链制氢机理研究

Because of strongly endothermic reactions and chemical equilibrium limit in the hydrogen production from conventional steam reforming, energy consumption is very high, the hydrogen purity is not high, and CO2 emission is not evitable. In this study, the porous montmorillonite was first synthesized by molecular layer column space template method. The catalyst component of MgO-NiO-Al2O3 is supported on montmorillonite by the chemical doping induced under the ultrasound, and the multifunctional heterostructure oxygen carrier having fine modulation of surface active center was developed. A new technology of the partial oxidation and continuous catalytic sorption-enhanced chemical-looping reforming for hydrogen production from biomass will be constructed based on the structure and surface effect of oxygen carrier by combining the partial oxidation, reforming, water gas shift (WGS), and in-situ CO2 removal. The reforming reactor was continuously operated at auto-thermal state and the process produced an enriched hydrogen product at low temperatures. The process is characterized using slow moving-bed reactors by continuously moving, reaction and regeneration of oxygen carrier always in their fresh states for the production of high purity hydrogen at low temperatures, and CO2 is recovered. The project will focus on the heat-mass transfer, chenmical reaction and variable window regulation of coupling enhanced process by equilibrium shrift, and determine the quantitative relation between structure and performance of oxygen carrier. The factors on long-term stability of continuous reactions will be revealed. The active site types, distribution and quality of oxygen carrier related to some specific reactions will be determined by In-situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS). The mechanisms on improving hydrogen purity, selectivity and conversion of biomass will be studied.

常规水蒸气重整制氢，受强吸热和反应平衡限制，能耗很高，氢气纯度不高，过程排放CO2；本项目以分子层柱空间模板法合成多孔蒙脱石，以超声诱导化学掺杂技术，将化学链制氢载氧催化成份MgO-NiO-Al2O3负载，精细调变表面活性中心，构建多功能多相异质结构载氧体，以显著的结构、表面效应，研究在一个反应器内实现生物质原料部分氧化、重整、水汽变换与CO2原位吸附，建立部分氧化连续吸附强化化学链蒸汽重整制氢新技术，以慢速移动床实现载氧体连续移动、反应和再生，使其始终处于近新鲜状态，自热、低温连续制取高纯度氢气并回收CO2；项目重点研究过程热质传递、反应及引起制氢平衡移动耦合强化作用理论与连续化学链变量调控规律，确定载氧体结构、性能的关系及变化，揭示影响其连续长周期制氢稳定性的因素，利用原位漫反射红外光谱研究表面活性位类型和性质，并与特定反应关联，弄清大幅提高工艺产氢纯度、选择性和原料转化率的机理途径。

具有强化催化、热质传递等多重功能的载氧体的制备是多相反应体系关键问题，是促进新类型重整制氢反应器不断提高的基础。本项目针对传统水蒸气重整制氢，受强吸热和反应平衡的限制，反应温度高，氢气纯度低，CO2捕集耗能等问题，开展多功能载氧体连续吸附强化化学链制氢的研究，应用具有不同结构的载氧体，高效率原位吸附分离CO2，使得制氢平衡移动，持续不断的向生成氢气的方向进行，在低温下，一个反应器内，内实现生物质原料部分氧化、重整、水汽变换与CO2原位吸附。并以慢速移动床实现载氧体的连续反应和再生。项目重点研究探索了超声诱导化学掺杂技术，将催化、吸附成分负载于多孔载体上，形成具有较大孔隙率和比表面积的载氧体。项目重点研究揭示了CO2原位吸附对连续催化化学链重整过程的强化机理及影响规律，确定了载氧体结构和性能变化的关系；解释了影响载氧体长周期制氢的影响因素。利用原位漫反射光谱研究了载氧体表面活性中心类型、分布，及其与特定反应的关系。研究成果相对于常规水蒸气重整制氢，具有工序简化、节约能耗和用水，氢气纯度和原料转化率高等优势。.本项目研究结果以：“可再生原料CO2原位吸附强化制氢理论与方法”，获2016年度辽宁省自然科学奖二等奖（本项目负责人排序第一）；“煤气化联合吸附强化制氢关键技术与应用”，获2017年中国机械工业科学技术奖二等奖 和上海市科技进步三等奖（本项目负责人排序第一）。发表国际SCI收录论文19篇，其中SCI影响因子IF:5.0以上5篇，9篇SCI论文标注了本基金号码第一，ESI高被引论文累计7篇次。授权专利2项。

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