High-throughput screening of metal-porphyrin-like graphenes for selective capture of carbon dioxide.

Hyeonhu Bae,Jinwoo Park,Suklyun Hong,Haegeun Chung,Boris I Yakobson,Hoonkyung Lee,Yongkyung Kwon,Minwoo Park,Hosik Lee,Chihye Chung,Byungryul Jang,Yura Kang

doi:10.1038/srep21788

Abstract

Nanostructured materials, such as zeolites and metal-organic frameworks, have been considered to capture CO2. However, their application has been limited largely because they exhibit poor selectivity for flue gases and low capture capacity under low pressures. We perform a high-throughput screening for selective CO2 capture from flue gases by using first principles thermodynamics. We find that elements with empty d orbitals selectively attract CO2 from gaseous mixtures under low CO2 pressures (~10−3 bar) at 300 K and release it at ~450 K. CO2 binding to elements involves hybridization of the metal d orbitals with the CO2 π orbitals and CO2-transition metal complexes were observed in experiments. This result allows us to perform high-throughput screening to discover novel promising CO2 capture materials with empty d orbitals (e.g., Sc– or V–porphyrin-like graphene) and predict their capture performance under various conditions. Moreover, these findings provide physical insights into selective CO2 capture and open a new path to explore CO2 capture materials.

Highlights

Carbon dioxide gas is a greenhouse gas that is a primary cause of global warming, which is known to cause severe climate change[1]
We performed first-principles total energy calculations regarding CO2 adsorption onto metal–porphyrin-like structures to explore the feasibility of achieving room-temperature CO2 capture under low pressures
We found that transition metal–porphyrin-like structures adsorb CO2 molecules with the desirable binding energy range

Summary

Introduction

Carbon dioxide gas is a greenhouse gas that is a primary cause of global warming, which is known to cause severe climate change[1]. The technology involving the capture of CO2 gas from the flue gas is currently not sufficiently developed, in the backdrop of the urgent need to reduce CO2 emission. Nanostructured materials, such as graphene, zeolites, and metal-organic frameworks, have been considered to capture CO2. These materials are potentially useful because of their high capacity, fast CO2 adsorption kinetics, and effective regeneration[2,3,4,5,6,7,8,9,10,11]. We perform first-principles thermodynamics based high-throughput screening for suitable M elements as selective CO2 attractors using M–porphyrin-like graphene

Methods

Results

Conclusion