Unveiling anomalous CO2-to-N2 selectivity of graphene oxide

文献信息

发布日期 2017-08-08

DOI 10.1039/C7CP04318J

影响因子 3.676

作者

Ji Hoon Lee, Hyeon Jeong Lee, Jang Wook Choi

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摘要

When dry sorbents are considered for CO2 capture, selective uptake of CO2 over other gases is highly desirable. However, most dry sorbents suffer from selectivity drop upon temperature increase. Here, we report that graphene oxide (GO) exhibits high CO2-to-N2 selectivity, and the selectivity rises anomalously with temperature increase; CO2-to-N2 selectivity that starts at 192 at 273 K increases to an extraordinarily high value of 607 at 323 K. These high values and unusual trends in selectivity are attributed to a combined effect of CO2-philicity from the functional groups of GO and its relatively large macropores that are efficient at releasing N2. In-depth analysis using FT-IR reveals CO2-philic electrostatic interactions where CO2 serves as an electron donor and acceptor simultaneously; while CO2 can bind with electron-rich oxygen-containing groups of GO, the oxygen of CO2 can also bind with hydrogen-containing groups at the edges of GO. The current study with GO highlights a design principle for highly selective CO2 capture represented by CO2-philic electrostatic sites coupled with relatively large pores for efficient N2 release.

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来源期刊

Physical Chemistry Chemical Physics

CiteScore: 5.5

自引率: 10.3%

年发文量: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.