Navigating the Chemical Space of HCN Polymerization and Hydrolysis: Guiding Graph Grammars by Mass Spectrometry Data

作者：Andersen Jakob L; Andersen Tommy; Flamm Christoph; Hanczyc Martin M; Merkle Daniel^*; Stadler Peter F

来源：Entropy, 2013, 15(10): 4066-4083.

DOI：10.3390/e15104066

• hydrogen cyanide
• graph grammars
• chemical space
• mass spectrometry
• chemical motif
• polymerization
• autocatalysis

Polymers of hydrogen cyanide and their hydrolysis products constitute a plausible, but still poorly understood proposal for early prebiotic chemistry on Earth. HCN polymers are generated by the interplay of more than a dozen distinctive reaction mechanisms and form a highly complex mixture. Here we use a computational model based on graph grammars as a means of exploring the chemical spaces of HCN polymerization and hydrolysis. A fundamental issue is to understand the combinatorial explosion inherent in large, complex chemical systems. We demonstrate that experimental data, here obtained by mass spectrometry, and computationally predicted free energies together can be used to guide the exploration of the chemical space and makes it feasible to investigate likely pathways and chemical motifs even in potentially open-ended chemical systems.

• 出版日期2013-10
• 单位上海生物信息技术研究中心