In situ environmental TEM analysis reveals the hydrogen insertion initiated at the GB sites, further supported by DFT results. Great teamwork @utahchemistry.bsky.social PNNL and Argonne! Congrats to all the authors! Thanks, Department of Energy, for funding support!

We addressed this issue by continuously regenerating defective Ag under AC electrolysis to prevent catalyst deactivation and control the formation of reactive chemical species, achieving the selective and continuous electrosynthesis of aminopyralid for over 50 days.

The loss of selectivity is caused by both the structural evolution of the Ag catalyst, as characterized by #4D-STEM, and the in situ formation of reactive species (ClO–, NH3, and NO2–).

Dehalogenation is a critical process in the chemical industry but still faces challenges, including catalyst deactivation, low product selectivity, and limited operational stability. An example is the synthesis of aminopyralid (2) via #echem dechlorination of picloram (1).

Great collaboration with the White Group @utahchemistry.bsky.social @nsf-csoe.bsky.social ! Thanks the funding support from @NIH and @NSF!

The selectivicty arises from binning the products by time duration during AC electrolysis. At short times, the 1st step is fast than the 2nd step due to fast kinetics and sufficient supply of reactant. At long times, the 2nd catches up with the 1st due to concentration change.

The key take-home message is when the potential difference at the foot of the wave between 1-->2 and 2--->3 is larger than 80 mV, AC electrolysis can achieve selectivity toward 2.

And having dinner the legendary Profs. Joel Harris and Henry White @utahchemistry.bsky.social !