You can’t modify Hashtable while enumerating it. This is what you can do:
$myHash = @{}
$myHash["a"] = 1
$myHash["b"] = 2
$myHash["c"] = 3
$myHash = $myHash.keys | foreach{$r=@{}}{$r[$_] = 5}{$r}
Edit 1
Is this any simpler for you:
$myHash = @{}
$myHash["a"] = 1
$myHash["b"] = 2
$myHash["c"] = 3
foreach($key in $($myHash.keys)){
$myHash[$key] = 5
}