Disclosed are zeolitic materials that include a microporous crystalline framework substituted with one or more paired Lewis acid sites. Each of the one or more paired Lewis acid sites within the zeolitic material can comprise a first Lewis acid metal center and a second Lewis acid metal center. The first Lewis acid metal center and the second Lewis acid metal center can be separated by three or fewer atoms within the crystalline framework. Also provided herein are methods of making these zeolitic materials as well as methods of using these zeolitic materials as catalysts.