journal article·2025-06-24

Feature-Extended Descriptor Construction for Prediction of Consecutive Elementary Reaction Energies in Methane Oxidation

Wangqiang Lin, Fangting Liu, Zhilong Song, Yehui Zhang, Qionghua Zhou, Chongyi Ling, Qiang Li, Jinlan Wang

Chemistry of Materials· Volume 37· Issue 12
Publisher page

Abstract

Conventional descriptor construction approaches are fundamentally limited by their narrow focus on predicting adsorption energies for structurally similar intermediates, failing to address the complexity of real catalytic systems involving multiple active sites and elementary reactions. To overcome these limitations, we develop a general feature extension approach that systematically expands descriptor functionality through two key innovations: structure extension for diverse active sites and reaction extension for consecutive elementary reactions, enabled by comparative analysis of active site characteristics. Applying this approach to methane oxidation to methanol with three consecutive elementary reactions and six possible active sites (totaling 1,026 metal-exchanged zeolite catalysts), we successfully mapped the complete reaction pathways, identified optimal bimetallic catalysts (including experimentally verified Ag and Cu bimetallic active sites), and extracted fundamental structure–activity relationships. Proof-of-concept verification supports the generalizability of the feature extension approach, establishing a paradigm shift in descriptor discovery that transcends traditional single-site/single-step limitations and offering a powerful framework for complex catalytic pathway analysis and rational catalyst design.
Source: openalex_inverted_index · Quality: baseline

Research context

OpenAlex topics: Catalysis and Oxidation Reactions · Catalytic Processes in Materials Science · CO2 Reduction Techniques and Catalysts

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Key Laboratory of Quantum Materials and Devices of Ministry of Education, School of Physics

Southeast University

Funding

National Key Research and Development Program of China · Basic Research Program of Jiangsu Province · Fundamental Research Funds for the Central Universities · National Natural Science Foundation of China

References (86)

Show source-provided references
1. 10.1002/anie.20210300710.1002/anie.202103007 ↗
2. 10.1021/jacs.3c0426010.1021/jacs.3c04260 ↗
3. Luo Y.-R. · 200710.1201/9781420007282 ↗
4. Haynes W. M. · 201410.1201/b17118 ↗
5. 10.1039/C4EE00604F10.1039/C4EE00604F ↗
6. 10.1126/science.aam903510.1126/science.aam9035 ↗
7. 10.1016/j.chempr.2019.05.00810.1016/j.chempr.2019.05.008 ↗
8. 10.1002/aenm.20200215410.1002/aenm.202002154 ↗
9. 10.1021/ja047158u10.1021/ja047158u ↗
10. 10.1038/ncomms854610.1038/ncomms8546 ↗
11. 10.1021/jacs.7b0647210.1021/jacs.7b06472 ↗
12. 10.1039/C8CY02414F10.1039/C8CY02414F ↗
13. 10.1039/D1CS00783A10.1039/D1CS00783A ↗
14. 10.1021/jacs.4c0064610.1021/jacs.4c00646 ↗
15. 10.1021/acs.chemrev.2c0031510.1021/acs.chemrev.2c00315 ↗
16. 10.1002/cctc.20170076810.1002/cctc.201700768 ↗
17. 10.1002/anie.20151106510.1002/anie.201511065 ↗
18. 10.1039/C7CC00467B10.1039/C7CC00467B ↗
19. 10.1021/acs.chemrev.2c0043910.1021/acs.chemrev.2c00439 ↗
20. 10.1021/acs.chemrev.6b0062410.1021/acs.chemrev.6b00624 ↗
21. 10.1002/anie.20100642410.1002/anie.201006424 ↗
22. 10.1021/acscatal.6b0300510.1021/acscatal.6b03005 ↗
23. 10.1002/anie.20240317910.1002/anie.202403179 ↗
24. 10.1021/acs.chemmater.9b0422310.1021/acs.chemmater.9b04223 ↗
25. 10.1021/acscatal.9b0153410.1021/acscatal.9b01534 ↗
26. 10.1021/acs.chemrev.7b0034410.1021/acs.chemrev.7b00344 ↗
27. 10.1073/pnas.091046110610.1073/pnas.0910461106 ↗
28. 10.1038/s41578-019-0152-x10.1038/s41578-019-0152-x ↗
29. 10.1103/PhysRevLett.99.01610510.1103/PhysRevLett.99.016105 ↗
30. 10.1103/PhysRevB.89.11511410.1103/PhysRevB.89.115114 ↗
31. 10.1039/D3MH00157A10.1039/D3MH00157A ↗
32. 10.1039/D2MH01197B10.1039/D2MH01197B ↗
33. 10.1021/jacs.3c1197210.1021/jacs.3c11972 ↗
34. 10.1021/jacs.2c0454010.1021/jacs.2c04540 ↗
35. 10.1021/acscatal.2c0325010.1021/acscatal.2c03250 ↗
36. 10.1021/jacsau.3c0055810.1021/jacsau.3c00558 ↗
37. 10.1103/PhysRevB.54.1116910.1103/PhysRevB.54.11169 ↗
38. 10.1103/PhysRevB.50.1795310.1103/PhysRevB.50.17953 ↗
39. 10.1103/PhysRevLett.77.386510.1103/PhysRevLett.77.3865 ↗
40. 10.1063/1.47293310.1063/1.472933 ↗
41. 10.1002/jcc.2049510.1002/jcc.20495 ↗
42. 10.1063/1.338234410.1063/1.3382344 ↗
43. 10.1016/j.jcat.2016.03.01410.1016/j.jcat.2016.03.014 ↗
44. 10.1002/smtd.20180026610.1002/smtd.201800266 ↗
45. 10.1016/j.cpc.2021.10803310.1016/j.cpc.2021.108033 ↗
46. International Zeolite Association. IZA Structure database; https://www.iza-structure.org/databases/ (accessed 18 April 2024).
47. 10.1063/1.132967210.1063/1.1329672 ↗
48. Abu-Mostaf Y. S. · 2012
49. Pedregosa F. · J. Mach. Learn. Res. · 2011 · 12 · 2825
50. 10.1038/npjcompumats.2016.2810.1038/npjcompumats.2016.28 ↗
51. Mentel, L. M. mendeleev - A Python resource for properties of chemical elements, ions and isotopes. 2014. https://github.com/lmmentel/mendeleev (accessed 18 April 2024).
52. 10.1021/acscatal.6b0172110.1021/acscatal.6b01721 ↗
53. 10.1038/s41467-018-03235-710.1038/s41467-018-03235-7 ↗
54. 10.1002/anie.20160470810.1002/anie.201604708 ↗
55. 10.1002/advs.20230214310.1002/advs.202302143 ↗
56. 10.1126/science.aaw110810.1126/science.aaw1108 ↗
57. 10.1016/j.apcatb.2021.12012410.1016/j.apcatb.2021.120124 ↗
58. 10.1002/cctc.20180180910.1002/cctc.201801809 ↗
59. 10.1039/D0CP01257B10.1039/D0CP01257B ↗
60. 10.1016/j.ces.2022.11781810.1016/j.ces.2022.117818 ↗
61. 10.1016/j.ccr.2023.21543810.1016/j.ccr.2023.215438 ↗
62. 10.1021/acscatal.6b0189510.1021/acscatal.6b01895 ↗
63. 10.1021/la501184b10.1021/la501184b ↗
64. 10.1039/D0CP06696F10.1039/D0CP06696F ↗
65. 10.1021/acs.jctc.6b0016810.1021/acs.jctc.6b00168 ↗
66. 10.1016/j.jcat.2019.08.00210.1016/j.jcat.2019.08.002 ↗
67. 10.1021/jp711191j10.1021/jp711191j ↗
68. 10.1002/anie.20090280010.1002/anie.200902800 ↗
69. 10.1038/nmat476010.1038/nmat4760 ↗
70. 10.1021/acs.iecr.0c0545710.1021/acs.iecr.0c05457 ↗
71. 10.1021/acs.jpcc.0c0443210.1021/acs.jpcc.0c04432 ↗
72. 10.1039/D0TA04615A10.1039/D0TA04615A ↗
73. 10.1039/C9TA13404B10.1039/C9TA13404B ↗
74. 10.1002/aenm.20190394910.1002/aenm.201903949 ↗
75. 10.1039/D0TA06583H10.1039/D0TA06583H ↗
76. 10.1039/C9TA12608B10.1039/C9TA12608B ↗
77. 10.1021/acs.jpcc.0c0226510.1021/acs.jpcc.0c02265 ↗
78. 10.1021/acs.jpclett.0c0383910.1021/acs.jpclett.0c03839 ↗
79. 10.1016/j.cattod.2011.04.00110.1016/j.cattod.2011.04.001 ↗
80. 10.1039/D1CY00687H10.1039/D1CY00687H ↗
81. 10.1039/D0CP01284J10.1039/D0CP01284J ↗
82. 10.1016/j.cattod.2005.09.02810.1016/j.cattod.2005.09.028 ↗
83. 10.1039/C4CC09645B10.1039/C4CC09645B ↗
84. 10.1021/acscatal.6b0237210.1021/acscatal.6b02372 ↗
85. 10.1039/C9CY00013E10.1039/C9CY00013E ↗
86. 10.1038/s41467-024-46924-210.1038/s41467-024-46924-2 ↗