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In modern Portland cement, calcium aluminum silicate hydrates (C‐A‐S‐H) do not generally form crystalline Al‐tobermorite. In this study, to identify the mechanism of Al‐tobermorite formation, synchrotron micro X‐ray diffraction and field‐emission scanning electron microscopy‐based energy‐dispersive X‐ray spectroscopy (EDS) investigations were performed on a slice of a thick concrete wall in a nuclear...