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This work brings deeper insights into the atomistic OR mechanism and also paves the way for real-time monitoring of catalyst sintering at the atomic scale.A newly synthesized microporous zincosilicate THK-2 (estimated structural composition |(H2O)6.7(C6H13N)0.9|[Li0.5Zn3.1Si32O62.7(OH)9.3]) was characterized by single-crystal electron diffraction using the automated electron diffraction tomography (ADT) approach in combination with powder X-ray diffraction. The lattice constants and space group of as-synthesized THK-2 were a = 2.50377(7