Exploring the Tunability of Trimetallic MOF Nodes for Partial Oxidation of Methane to Methanol
Source abstract
Abstract
Density functional theory is used to study the tunability of trigonal prismatic SBUs found in metal–organic frameworks (MOFs) such as MIL-100, MIL-101, and PCN-250/MIL-127 of chemical composition M3+2M2+(μ3-O)(RCOO)6 for the partial oxidation of methane to methanol. We performed a combinatorial screening by varying the composition of the trimetallic node (M13+)2(M22+) (where M1 and M2 = V, Cr, Mn, Fe, Co, and Ni) and calculated the reaction pathway on both M1 and M2 sites. The systematic replacement of metals in the trimetallic cluster allowed us to study the influence of spectator atoms on the catalytic activity of a specific metal site in the cluster toward the N2O activation and C–H bond activation steps of the reaction. In the screening, we identified the top-performing node compositions with predicted barriers lower than those already reported for experimentally tested MOFs with trigonal prismatic SBUs. This work demonstrates the opportunity to tune the catalytic activity of MOFs for redox reactions by changing their metal node composition.
Source: openalex_inverted_index · Quality: baseline
Research context
OpenAlex topics: Metal-Organic Frameworks: Synthesis and Applications · Catalytic Processes in Materials Science · Gas Sensing Nanomaterials and Sensors
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
Affiliations
Department of Chemical and Biological Engineering, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States
Funding
Office of Science · National Science Foundation
References (73)
Show source-provided references
1. 10.1021/cr00036a00510.1021/cr00036a005 ↗
2. 10.1038/nchem.195610.1038/nchem.1956 ↗
3. 10.1021/jacs.9b0868610.1021/jacs.9b08686 ↗
4. 10.1038/nature0165010.1038/nature01650 ↗
5. 10.1021/ar000034b10.1021/ar000034b ↗
6. 10.1021/acscatal.9b0393210.1021/acscatal.9b03932 ↗
7. 10.1021/acscatal.8b0517810.1021/acscatal.8b05178 ↗
8. 10.1021/jacs.9b0400610.1021/jacs.9b04006 ↗
9. 10.1021/acscatal.8b0001210.1021/acscatal.8b00012 ↗
10. 10.1021/acscatal.8b0481310.1021/acscatal.8b04813 ↗
11. 10.1021/acsami.7b0219510.1021/acsami.7b02195 ↗
12. 10.1021/acs.inorgchem.7b0214310.1021/acs.inorgchem.7b02143 ↗
13. 10.1039/b817735j10.1039/b817735j ↗
14. 10.1021/ic050064g10.1021/ic050064g ↗
15. 10.1038/3501008810.1038/35010088 ↗
16. 10.1039/B202749F10.1039/B202749F ↗
17. 10.1002/anie.20045425010.1002/anie.200454250 ↗
18. 10.1039/B512169H10.1039/B512169H ↗
19. 10.1002/anie.20046059210.1002/anie.200460592 ↗
20. 10.1126/science.111627510.1126/science.1116275 ↗
21. 10.1039/b600709k10.1039/b600709k ↗
22. 10.1016/j.micromeso.2012.02.02710.1016/j.micromeso.2012.02.027 ↗
23. 10.1016/j.micromeso.2011.12.00110.1016/j.micromeso.2011.12.001 ↗
24. 10.1016/j.micromeso.2010.12.01610.1016/j.micromeso.2010.12.016 ↗
25. 10.1002/cplu.20160045610.1002/cplu.201600456 ↗
26. 10.1039/B704325B10.1039/B704325B ↗
27. 10.1021/ja906198y10.1021/ja906198y ↗
28. 10.1016/j.ijhydene.2010.12.04310.1016/j.ijhydene.2010.12.043 ↗
29. 10.1002/ejic.20120010610.1002/ejic.201200106 ↗
30. 10.1021/cm103644b10.1021/cm103644b ↗
31. 10.1021/cg401205810.1021/cg4012058 ↗
32. 10.1126/science.113797510.1126/science.1137975 ↗
33. 10.1002/cctc.20190105010.1002/cctc.201901050 ↗
34. 10.1021/acs.organomet.6b0083410.1021/acs.organomet.6b00834 ↗
35. 10.1021/acs.cgd.8b0135310.1021/acs.cgd.8b01353 ↗
36. 10.1039/b718371b10.1039/b718371b ↗
37. 10.1002/chem.20140437710.1002/chem.201404377 ↗
38. 10.1016/j.catcom.2015.10.00610.1016/j.catcom.2015.10.006 ↗
39. 10.1016/j.jcat.2012.11.02910.1016/j.jcat.2012.11.029 ↗
40. 10.1039/b902699a10.1039/b902699a ↗
41. 10.1039/c2cc31877f10.1039/c2cc31877f ↗
42. 10.1002/adsc.20100051610.1002/adsc.201000516 ↗
43. 10.1016/j.cattod.2014.01.01010.1016/j.cattod.2014.01.010 ↗
44. 10.1038/ncomms672310.1038/ncomms6723 ↗
45. 10.1021/acsami.7b0604110.1021/acsami.7b06041 ↗
46. 10.1039/C5CC02550H10.1039/C5CC02550H ↗
47. 10.1039/C4CS00002A10.1039/C4CS00002A ↗
48. 10.1039/c3ce42006j10.1039/c3ce42006j ↗
49. 10.1021/ja502328310.1021/ja5023283 ↗
50. 10.1002/anie.20180358710.1002/anie.201803587 ↗
51. 10.1021/jacs.6b0872410.1021/jacs.6b08724 ↗
52. 10.1039/C9TA01948K10.1039/C9TA01948K ↗
53. Frisch, M. J.; Trucks, G. W.; Schlegel, H. B.; Scuseria, G. E.; Robb, M. A.; Cheeseman, J. R.; Scalmani, G.; Barone, V.; Mennucci, B.; Petersson, G. A.; Nakatsuji, H.; Caricato, M.; Li, X.; Hratchian, H. P.; Izmaylov, A. F.; Bloino, G. Z.; Sonnenberg, J. L.; Hada, M.; Ehara, M.; Toyota, K.; Fukuda, R.; Hasegawa, J.; Ishida, M.; Nakajima, T.; Honda, Y.; Kitao, O.; Nakai, H.; Vreven, T. J. A.; Montgomery, J.; Peralta, J. E.; Ogliaro, F.; Bearpark, M.; Heyd, J. J.; Brothers, E.; Kudin, K. N.; Staroverov, V. N.; Kobayashi, R.; Normand, J.; Raghavachari, K.; Rendell, A.; Burant, J. C.; Iyengar, S. S.; Tomasi, J.; Cossi, M.; Rega, N.; Millam, J. M.; Klene, M.; Knox, J. E.; Cross, J. B.; Bakken, V.; Adamo, C.; Jaramillo, J.; Gomperts, R.; Stratmann, R. E.; Yazyev, O.; Austin, A. J.; Cammi, R.; Pomelli, C.; Ochterski, J. W.; Martin, R. L.; Morokuma, K.; Zakrzewski, V. G.; Vot, G. A.; Salvador, P.; Dannenberg, J. J.; Dapprich, S.; Daniels, A. D.; Farkas, Ö.; Foresman, J. B.; Ortiz, J. V.; Cioslowski, J.; Fox, D. J. Gaussian 16; rev. Gaussian, Inc.: Wallingford CT, 2016.
54. 10.1063/1.237099310.1063/1.2370993 ↗
55. 10.1021/jp402884h10.1021/jp402884h ↗
56. 10.1021/acs.jpcc.6b0736210.1021/acs.jpcc.6b07362 ↗
57. 10.1007/s00214005024410.1007/s002140050244 ↗
58. 10.1016/0009-2614(95)00621-A10.1016/0009-2614(95)00621-A ↗
59. Cramer C. J. · 2004
60. 10.1021/jp205508z10.1021/jp205508z ↗
61. 10.1039/c2sc01030e10.1039/c2sc01030e ↗
62. 10.1021/ct200866d10.1021/ct200866d ↗
63. 10.1039/C7CY01229B10.1039/C7CY01229B ↗
64. 10.1038/s41929-019-0273-z10.1038/s41929-019-0273-z ↗
65. 10.1021/acscatal.8b0022010.1021/acscatal.8b00220 ↗
66. 10.1006/jcat.2002.361510.1006/jcat.2002.3615 ↗
67. 10.1006/jcat.2000.308710.1006/jcat.2000.3087 ↗
68. 10.1007/BF0076411410.1007/BF00764114 ↗
69. 10.1021/acscatal.7b0359710.1021/acscatal.7b03597 ↗
70. 10.1038/nmat476010.1038/nmat4760 ↗
71. 10.1021/acs.jpcc.6b0460410.1021/acs.jpcc.6b04604 ↗
72. 10.1002/anie.20090536410.1002/anie.200905364 ↗
73. 10.1021/jp004613+10.1021/jp004613+ ↗