Hwang Chih-Chau, Tour Josiah J, Kittrell Carter, Espinal Laura, Alemany Lawrence B, Tour James M
Department of Chemistry, Rice University, 6100 Main Street, Houston, Texas 77005, USA.
The Richard E. Smalley Institute for Nanoscale Science and Technology, Rice University, 6100 Main Street, Houston, Texas 77005, USA.
Nat Commun. 2014 Jun 3;5:3961. doi: 10.1038/ncomms4961.
Natural gas is considered the cleanest and recently the most abundant fossil fuel source, yet when it is extracted from wells, it often contains 10-20 mol% carbon dioxide (20-40 wt%), which is generally vented to the atmosphere. Efforts are underway to contain this carbon dioxide at the well-head using inexpensive and non-corrosive methods. Here we report nucleophilic porous carbons are synthesized from simple and inexpensive carbon-sulphur and carbon-nitrogen precursors. Infrared, Raman and (13)C nuclear magnetic resonance signatures substantiate carbon dioxide fixation by polymerization in the carbon channels to form poly(CO2) under much lower pressures than previously required. This growing chemisorbed sulphur- or nitrogen-atom-initiated poly(CO2) chain further displaces physisorbed hydrocarbon, providing a continuous carbon dioxide selectivity. Once returned to ambient conditions, the poly(CO2) spontaneously depolymerizes, leading to a sorbent that can be easily regenerated without the thermal energy input that is required for traditional sorbents.
天然气被认为是最清洁且近期储量最为丰富的化石燃料来源，然而，当它从油井中开采出来时，通常含有10 - 20摩尔%的二氧化碳（20 - 40重量%），这些二氧化碳一般会排放到大气中。目前正在努力采用廉价且无腐蚀性的方法在井口捕获这些二氧化碳。在此，我们报道了通过简单且廉价的碳 - 硫和碳 - 氮前驱体合成亲核多孔碳。红外、拉曼和（13）C核磁共振特征证实，在比先前所需压力低得多的情况下，二氧化碳通过在碳通道中聚合形成聚（二氧化碳）而被固定。这种不断增长的由化学吸附的硫或氮原子引发的聚（二氧化碳）链进一步取代物理吸附的碳氢化合物，从而提供持续的二氧化碳选择性。一旦恢复到环境条件，聚（二氧化碳）会自发解聚，形成一种无需传统吸附剂所需热能输入就能轻松再生的吸附剂。
