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Zusammenfassung:
Natural diamonds that have been partially replaced by graphite have been observed to occur in natural rocks. While the graphite-to-diamond phase transition has been extensively studied the opposite of this (diamond to graphite) remains poorly understood. We performed high-pressure and temperature hydrous and anhydrous experiments up to 1.0 GPa and 1300 °C using Amplex premium virgin synthetic diamonds (20–40 μm size) as the starting material mixed with Mg (OH)2 as a source of H2O for the hydrous experiments. The experiments revealed that the diamond-to-graphite transformation at P = 1GPa and T = 1300 °C was triggered by the presence of H2O and was accomplished through a three-stage process. Stage 1: diamond reacts with a supercritical H2O producing an intermediate 200–500 nm size “globular carbon” phase. This phase is a linear carbon chain; i.e. a polyyne or carbyne. Stage 2: the linear carbon chains are unstable and highly reactive, and they decompose by zigzagging and cross-linking to form sp2-bonded structures. Stage 3: normal, disordered, and onion-like graphite is produced by the decomposition of the sp-hybridized carbon chains which are re-organized into sp2 bonds. Our experiments show that there is no direct transformation from sp3 C-bonds into sp2 C-bonds. Our hydrous high-pressure and high-temperature experiments show that the diamond-to-graphite transformation requires an intermediate metastable phase of a linear hydrocarbon. This process provides a simple mechanism for the substitution of other elements into the graphite structure (e.g. H, S, O).
