44946 2018 eng 5930 5933 20 57 article Wiley-VCH Weinheim 1 -- -- -- We present an in situ triple coupling of synchrotron X-ray diffraction with Raman spectroscopy, and thermography to study milling reactions in real time. This combination of methods allows a correlation of the structural evolution with temperature information. The temperature information is crucial for understanding both the thermodynamics and reaction kinetics. The reaction mechanisms of three prototypical mechanochemical syntheses, a cocrystal formation, a C@C bond formation (Knoevenagel condensation), and the formation of a manganese-phosphonate, were elucidated. Trends in the temperature development during milling are identified. The heat of reaction and latent heat of crystallization of the product contribute to the overall temperature increase. A decrease in temperature occurs via release of, for example, water as a byproduct. Solid and liquid intermediates are detected. The influence of the mechanical impact could be separated from temperature effects caused by the reaction. Angewandte Chemie International Edition 10.1002/anie.201800147 1433-7851 1521-3773 18.05.2018 Hannes Kulla Sebastian Haferkamp Irina Akhmetova Mathias Röllig Christiane Maierhofer Klaus Rademann Franziska Emmerling eng uncontrolled In situ studies eng uncontrolled Mechanochemistry eng uncontrolled Raman spectroscopy eng uncontrolled Thermography eng uncontrolled X-ray diffraction Analytische Chemie Ingenieurwissenschaften und zugeordnete Tätigkeiten Verlagsliteratur Datei im Netzwerk der BAM verfügbar ("Closed Access")