Tang Huarong, Lu Dongmei, Wu Chao
School of Materials Science and Engineering, Center for Advancing Materials Performance from the Nanoscale (CAMP-Nano), State Key Laboratory for Mechanical Behavior of Materials, Xi'an Jiaotong University (China).
Department of Applied chemistry, School of Science, Xi'an Jiaotong University (China).
Chemphyschem. 2015 Jun 22;16(9):1926-32. doi: 10.1002/cphc.201500164. Epub 2015 Apr 23.
Reducing the emission of greenhouse gases, such as CO2 , requires efficient and reusable capture materials. The energy for regenerating sorbents is critical to the cost of CO2 capture. Here, we design a series of photoswitchable CO2 capture molecules by grafting Lewis bases, which can covalently bond CO2 , to azo-based backbones that can switch configurations upon light stimulation. The first-principles calculations demonstrate that intramolecular hydrogen bonds are crucial for enlarging the difference of CO2 binding strengths to the cis and trans isomers. As a result, the CO2 -sorbent interaction can be light-adjusted from strong chemical bonding in one configuration to weak bonding in the other, which may lead to a great energy reduction in sorbent regeneration.
减少二氧化碳等温室气体的排放需要高效且可重复使用的捕获材料。吸附剂再生所需的能量对于二氧化碳捕获成本至关重要。在此，我们通过将能与二氧化碳共价结合的路易斯碱接枝到基于偶氮的主链上，设计了一系列可光开关的二氧化碳捕获分子，该主链在光刺激下可改变构型。第一性原理计算表明，分子内氢键对于扩大二氧化碳与顺式和反式异构体结合强度的差异至关重要。因此，二氧化碳与吸附剂的相互作用可以通过光从一种构型下的强化学键调整为另一种构型下的弱化学键，这可能会大幅降低吸附剂再生所需的能量。
