TY - JOUR
T1 - Strong bases behave as weak bases in nanoscale chemical environments: implication in humidity-swing CO2air capture
AU - HAN, Y.
AU - ZHU, L.
AU - YAO, Y.
AU - SHI, X.
AU - ZHANG, Y.
AU - XIAO, H.
AU - CHEN, X.
N1 - This work was supported by the National Natural Science Foundation of China (11872302), the R&D Program of Xi’an (2020KJRC0147), the Xi’an Science and Technology Plan Project, China (2019220914SYS024CG046) and the Earth Engineering Center and Center for Advanced Materials for Energy and Environment at Columbia University.
PY - 2021
Y1 - 2021
N2 - Hydration of ions/molecules in nanometer-sized clusters or nanoscopic pores is ubiquitous and plays a key role in many chemical and physical systems. In this work, guanidine-H2O reactions withn= 1-8 water molecules were systematically studied byab initiomethods. The result suggests that the reduced availability of water molecules greatly inhibits the strong base guanidine from producing OH−. That is, guanidine exhibits the behavior of a weak bases in low-humidity nanoscale environments. Intriguingly, this effect is not limited to guanidine but could be applied to other strong bases. Furthermore, we demonstrate that the direction of guanidine-CO2reactions can be controlled by changing the number of water molecules present, which in turn responds to the humidity change in air. These findings not only shed some light on unconventional chemical reactions of strong bases in atmospheric clusters and on solid porous surfaces, but also provide insights into the development of guanidine-based CO2air-capture sorbents. © the Owner Societies 2021.
AB - Hydration of ions/molecules in nanometer-sized clusters or nanoscopic pores is ubiquitous and plays a key role in many chemical and physical systems. In this work, guanidine-H2O reactions withn= 1-8 water molecules were systematically studied byab initiomethods. The result suggests that the reduced availability of water molecules greatly inhibits the strong base guanidine from producing OH−. That is, guanidine exhibits the behavior of a weak bases in low-humidity nanoscale environments. Intriguingly, this effect is not limited to guanidine but could be applied to other strong bases. Furthermore, we demonstrate that the direction of guanidine-CO2reactions can be controlled by changing the number of water molecules present, which in turn responds to the humidity change in air. These findings not only shed some light on unconventional chemical reactions of strong bases in atmospheric clusters and on solid porous surfaces, but also provide insights into the development of guanidine-based CO2air-capture sorbents. © the Owner Societies 2021.
UR - http://www.scopus.com/inward/record.url?scp=85110433514&partnerID=8YFLogxK
U2 - 10.1039/d1cp01121a
DO - 10.1039/d1cp01121a
M3 - Journal Article (refereed)
SN - 1463-9076
VL - 23
SP - 14811
EP - 14817
JO - Physical Chemistry Chemical Physics
JF - Physical Chemistry Chemical Physics
IS - 27
ER -