First-Principles Theory for the H + CH 4 → H 2 + CH 3 Reaction
10.1126/science.1104085
Crossref journal-article
American Association for the Advancement of Science (AAAS)
Science (221)
Abstract

A full-dimensional quantum dynamics simulation of a hydrogen atom reacting with methane on an accurate ab initio potential energy surface is reported. Based on first-principles theory, thermal rate constants are predicted with an accuracy comparable to (or even exceeding) experimental precision. The theoretical prediction is within the range of the significantly varied experimental rate constants reported by different groups. This level of accuracy has previously been achieved only for smaller, three-or four-atom reactive systems. Comparison with classical transition state theory confirms the importance of quantum mechanical tunneling for the rate constant below 400 kelvin.

Bibliography

Wu, T., Werner, H.-J., & Manthe, U. (2004). First-Principles Theory for the H + CH 4 → H 2 + CH 3 Reaction. Science, 306(5705), 2227–2229.

Authors 3
  1. Tao Wu (first)
  2. Hans-Joachim Werner (additional)
  3. Uwe Manthe (additional)
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Dates
Type When
Created 20 years, 8 months ago (Dec. 26, 2004, 11:34 p.m.)
Deposited 1 year, 7 months ago (Jan. 9, 2024, 10:57 p.m.)
Indexed 4 weeks, 1 day ago (Aug. 6, 2025, 9:51 a.m.)
Issued 20 years, 8 months ago (Dec. 24, 2004)
Published 20 years, 8 months ago (Dec. 24, 2004)
Published Print 20 years, 8 months ago (Dec. 24, 2004)
Funders 0

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@article{Wu_2004, title={First-Principles Theory for the H + CH 4 → H 2 + CH 3 Reaction}, volume={306}, ISSN={1095-9203}, url={http://dx.doi.org/10.1126/science.1104085}, DOI={10.1126/science.1104085}, number={5705}, journal={Science}, publisher={American Association for the Advancement of Science (AAAS)}, author={Wu, Tao and Werner, Hans-Joachim and Manthe, Uwe}, year={2004}, month=dec, pages={2227–2229} }