The recently reported interesting behavior of the EPR spin intensity a
s freshly prepared CuZSM-5 is dehydrated has been confirmed, and the i
nterpretation offered in explanation has been tested by extending the
data. Magnetic susceptibility and optical diffuse reflection spectrosc
opy have been used to show that the anomalous EPR data correspond to c
hanges in symmetry rather than disproportionation of [CuOH](+) into Cu
+ and Cu2+O- as H2O is removed, as previously suggested. Moreover, the
relatively small negative Weiss constants suggest that antiferromagne
tic coupling through the supposedly EPR silent conventional bridge spe
cies, [Cu2+-O2--Cu2+](2+), cannot be responsible for the relatively la
rge changes in observed EPR spin intensity on dehydration. EPR measure
s selectively individual paramagnetic species and ignores those of low
symmetry, while magnetic susceptibility integrates over all magnetic
species in the sample. The changes in the EPR intensities were much la
rger than those observed by magnetic susceptibility. Furthermore, thos
e from EPR occurred as the first H2O was removed, before any significa
nt change in susceptibility occurred. The EPR data reflected those exp
ected for the decrease in symmetry accompanying dehydration. Support f
or these views was found in the magnetic susceptibility and optical re
flectance data. Evidence for CuO formation concomitant with dehydratio
n was obtained.