If you want to find the word you can use
var word = words.Where(item => item.IsKey).First();
This gives you the first item for which IsKey is true (if there might be non you might want to use .FirstOrDefault()
To get both the item and the index you can use
KeyValuePair<WordType, int> word = words.Select((item, index) => new KeyValuePair<WordType, int>(item, index)).Where(item => item.Key.IsKey).First();