Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 59, Issue 42, Pages 18468-18472Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202007766
Keywords
ab initio calculations; adsorption; IR spectroscopy; metal-organic frameworks; surface analysis
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Funding
- US Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-FG02-08ER46491, DE-SC0019902]
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Modification of the external surfaces of metal-organic frameworks offers a new level of control over their adsorption behavior. It was previously shown that capping of MOFs with ethylenediamine (EDA) can effectively retain small gaseous molecules at room temperature. Reported here is a temperature-induced variation in the capping-layer gate-opening mechanism through a combination of in situ infared experiments and ab initio simulations of the capping layer. An atypical acceleration and increase in the loading of weakly adsorbed molecules upon raising the temperature above room temperature is observed. These findings show the discovery of novel temperature-dependent kinetics that goes beyond standard kinetics and suggest a new avenue for tailoring selective adsorption by thermally tuning the surface barrier.
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