Keturakis Christopher J, Ni Fan, Spicer Michelle, Beaver Michael G, Caram Hugo S, Wachs Israel E
Operando Molecular Spectroscopy and Catalysis Laboratory, Department of Chemical Engineering, Lehigh University, Bethlehem, PA 18015 (USA).
ChemSusChem. 2014 Dec;7(12):3459-66. doi: 10.1002/cssc.201402474. Epub 2014 Oct 21.
The separation, capture, and storage of CO2 , the major greenhouse gas, from industrial gas streams has received considerable attention in recent years because of concerns about environmental effects of increasing CO2 concentration in the atmosphere. An emerging area of research utilizes reversible CO2 sorbents to increase conversion and rate of forward reactions for equilibrium-controlled reactions (sorption-enhanced reactions). Little fundamental information, however, is known about the nature of the sorbent surface sites, sorbent surface-CO2 complexes, and the CO2 adsorption/desorption mechanisms. The present study directly spectroscopically monitors Na2 O/Al2 O3 sorbent-CO2 surface complexes during adsorption/desorption with simultaneous analysis of desorbed CO2 gas, allowing establishment of molecular level structure-sorption relationships between individual surface carbonate complexes and the CO2 working capacity of sorbents at different temperatures.
由于担心大气中二氧化碳浓度增加对环境产生影响，近年来，从工业气流中分离、捕获和储存主要温室气体二氧化碳受到了广泛关注。一个新兴的研究领域利用可逆二氧化碳吸附剂来提高平衡控制反应（吸附增强反应）的转化率和正向反应速率。然而，关于吸附剂表面位点的性质、吸附剂表面 - 二氧化碳络合物以及二氧化碳吸附/解吸机制，人们所知的基础信息很少。本研究通过光谱直接监测Na2O/Al2O3吸附剂 - 二氧化碳表面络合物在吸附/解吸过程中的情况，同时对解吸的二氧化碳气体进行分析，从而能够建立不同温度下单个表面碳酸盐络合物与吸附剂二氧化碳工作容量之间的分子水平结构 - 吸附关系。
