W0269
Structure Determination from Powder Diffraction Data
– Challenging Open Framework Materials. Peter Y. Zavalij and M.
Stanley Whittingham, Institute for Materials Research and Dept. of Chemistry,
SUNY-Binghamton, Binghamton, NY 13902-6000.
Crystal structure determination from powder data (SDPD) is not
a straightforward process because of the accuracy in integrated intensity that
is due to the peaks overlapping, preferred orientation and other factors. It is
even more challenging in case of open framework materials, where those factors
are intensified and often unavoidable.
In recent years, we have been involved in developing new
materials that can be used as a cathode in rechargeable lithium batteries. These
materials have usually open framework structure, mostly layered, which along
with often relatively low crystallinity and inability to grow crystals provide
additional challenges for SDPD. Nevertheless, ab-initio crystal structure
solution was successfully used to determine the crystal structure of over 15
compounds.
This presentation summarizes the results of solving structures
from powder data and discusses problematic cases. Most of the structures were
challenging in many different ways: ab-initio indexing in the presence of
other phases; powder pattern decomposition with substantial peak broadening at
elevated angles; preferred orientation correction (prior to solving structure)
and refinement (several different axes). Of course the main challenge was
solving the structure that was done using different methods: direct (automatic)
or heavy atom (manual), geometry optimization (DLS) or energy minimization
(DMol), but always involving de facto or a priori chemical and structural
knowledge as well as any available analytical data.