煤焦在甲烷水蒸气重整反应中的构效关系与制氢机理

Blue coke, known as semi-coke from coal pyrolysis (denoted as coal-coke), has been an important industry in several Chinese regions (such as Shanbei and Inner Mongolia). But now the product is suffering from overcapacity and the absence of high-value conversion and utilization. At present, hydrogen is considered as the only clean energy can provide us with a good life without the threat of greenhouse effect or pollutants. To realize high-value utilization of coal-coke and to obtain clean hydrogen energy, this proposal intends to design an integrated process of steam methane reforming and catalytic gasification of coal-coke, with the aim of boosting the coal-coke reactivity and hydrogen yield and developing co-generation of hydrogen and activated carbon system based on the synergistic mechanism. According to the process cleavage and the composition and structure assembly of modified coal-coke products, effects of the compositions and structures of the coal-coke and its modified products will be studied on the catalytic activity, hydrogen producing performance and textural properties of the activated carbon. Then the quantitative structure-activity relationship will be built accordingly. Two processes (steam gasification and catalytic methane conversion) of the coal-coke and its modified products will be systematically studied based on the macroscopic performance and microstructure, to reveal the mechanism of co-generation of hydrogen and activated carbon. It can be expected that this project we propose here will not only make a positive impact on coal-coke conversion and utilization, co-generation of hydrogen and activated carbon by catalytic methane conversion, but also provide theoretical guidance for design and preparation of novel catalysts.

兰炭又称为煤热解半焦（简称为煤焦），已成为我国陕北、内蒙等地区的一项重要产业，目前面临着产能过剩、亟需高值化转化与利用的挑战。氢气是目前唯一能够提供既没有温室效应、也没有污染威胁的高质量生活的清洁能源。为实现煤焦的高值化利用、制取清洁的氢能源，本项目拟构建甲烷水蒸气重整与煤焦催化气化两个工艺的协同作用机制，强化煤焦的气化反应性、实现氢气收率的定向提高并联产活性炭的目的。拟通过对工艺过程的拆解、煤焦改性产品成分与结构的组装两种手段，系统研究煤焦及其改性产品的成分与结构对其催化活性、产氢性能、活性炭产品结构的影响规律，建立定量的构效关系。通过研究煤焦及其改性产品在水蒸气气化与催化甲烷转化两种工艺过程中的宏观反应性能及微观结构特征，解明制氢联产活性炭的机理。本项目的实施不仅对煤焦的转化利用、甲烷转化制氢联产活性炭工艺具有重要的科学意义，还可为新型催化剂的设计制备提供理论指导。

煤焦（局部地区称为兰炭）是煤炭中低温热解后产生的主要固态产物，它已成为我国陕北、内蒙等地区的一项重要产业，目前面临着产能过剩、亟需高值化转化与利用的挑战。氢气是目前为数不多的清洁、高效能源，而甲烷转化制氢是一种重要的制氢路径。为实现煤焦的高值化利用、制取清洁的氢能源，本项目研究中设计制备了煤焦改性产品（包括煤焦负载Ni、K2CO3等单组分或复合组分的催化剂），考察了它们在水蒸气气化反应、甲烷裂解反应、甲烷水蒸气重整反应中催化制氢反应性能；通过设计与构建煤焦改性产品各成分或活性中心之间的协同作用机制，强化了其作为催化剂时的反应活性，实现了氢气收率的定向提高并联产多孔炭（或活性炭）的目的；通过系统研究煤焦及其改性产品的成分与结构对其催化活性、产氢性能、多孔炭产品结构的影响规律，建立了定量的构效关系，解明了制氢联产多孔炭的机理。本项目的实施不仅对煤焦的转化利用、甲烷转化制氢联产多孔炭工艺具有重要的科学意义，还可为新型催化剂的设计制备提供理论指导。相关成果在本领域国际学术期刊上发表SCI论文11篇，申请发明专利9件（现已获得授权7件）。