TY - JOUR
T1 - Discovery of New Synthetic Routes of Amino Acids in Prebiotic Chemistry
AU - Li, Xiao Tian
AU - Mi, Sixuan
AU - Xu, Yuzhi
AU - Li, Bo Wen
AU - Zhu, Tong
AU - Zhang, John Z.H.
N1 - Publisher Copyright:
© 2024 The Authors. Published by American Chemical Society.
PY - 2024/12/23
Y1 - 2024/12/23
N2 - The origin of life on Earth remains one of the most perplexing challenges in biochemistry. While numerous bottom-up experiments under prebiotic conditions have provided valuable insights into the spontaneous chemical genesis of life, there remains a significant gap in the theoretical understanding of the complex reaction processes involved. In this study, we propose a novel approach using a roto-translationally invariant potential (RTIP) formulated with pristine Cartesian coordinates to facilitate the simulation of chemical reactions. By employing RTIP pathway sampling to explore the reactivity of primitive molecules, we identified several low-energy reaction mechanisms, such as two-hydrogen-transfer hydrogenation and HCOOH-catalyzed hydration and amination. This led to the construction of a comprehensive reaction network, illustrating the synthesis pathways for glycine, serine, and alanine. Further thermodynamic analysis highlights the pivotal role of formaldimine as a key precursor in amino acid synthesis, owing to its more favorable reactivity in coupling reactions compared to the traditionally recognized hydrogen cyanide. Our study demonstrates that the RTIP methodology, coupled with a divide-and-conquer strategy, provides new insights into the simulation of complex reaction processes, offering promising applications for advancing organic design and synthesis.
AB - The origin of life on Earth remains one of the most perplexing challenges in biochemistry. While numerous bottom-up experiments under prebiotic conditions have provided valuable insights into the spontaneous chemical genesis of life, there remains a significant gap in the theoretical understanding of the complex reaction processes involved. In this study, we propose a novel approach using a roto-translationally invariant potential (RTIP) formulated with pristine Cartesian coordinates to facilitate the simulation of chemical reactions. By employing RTIP pathway sampling to explore the reactivity of primitive molecules, we identified several low-energy reaction mechanisms, such as two-hydrogen-transfer hydrogenation and HCOOH-catalyzed hydration and amination. This led to the construction of a comprehensive reaction network, illustrating the synthesis pathways for glycine, serine, and alanine. Further thermodynamic analysis highlights the pivotal role of formaldimine as a key precursor in amino acid synthesis, owing to its more favorable reactivity in coupling reactions compared to the traditionally recognized hydrogen cyanide. Our study demonstrates that the RTIP methodology, coupled with a divide-and-conquer strategy, provides new insights into the simulation of complex reaction processes, offering promising applications for advancing organic design and synthesis.
KW - RTIP
KW - chemical space exploration
KW - origin of life
KW - prebiotic synthesis of amino acid
KW - reaction pathway sampling
UR - https://www.scopus.com/pages/publications/85209717271
U2 - 10.1021/jacsau.4c00685
DO - 10.1021/jacsau.4c00685
M3 - 文章
AN - SCOPUS:85209717271
SN - 2691-3704
VL - 4
SP - 4757
EP - 4768
JO - JACS Au
JF - JACS Au
IS - 12
ER -