Insights into the Correlation of Aluminum Distribution and Brönsted Acidity in H-Beta Zeolites from Solid-State NMR Spectroscopy and DFT Calculations.

Here we utilized 27Al MAS/MQMAS and 31P MAS NMR of quantitative adsorption of trimethylphosphine oxide (TMPO) and DFT calculations to elucidate the relationship between Al distribution and Brönsted acidity of series H-Beta zeolites derived from dealumination of Al-rich H-Beta zeolite. Three types of Brönsted acid strengths corresponding to different specific Al T-sites were demonstrated. The removal of one framework Al in 5MR2--2Al and 6MR-2Al sites led to increasing the Brönsted acid strength of dealuminated H-Beta. Our findings on such exact correlation between specific Al distributions and corresponding Brönsted acid sites may guide the controlling Al distribution to get desired acid properties through zeolite synthesis or finely tuned dealumination, which has a great impact on the catalytic activity and selectivity of zeolite catalysts.