Abstract
The gas-phase reactions of [IrC4H2]+ with methane and water have been explored by using mass spectrometry combined with quantum chemical calculations. Interestingly, under the employed conditions, two isomers of [IrC4H2]+ co-exist with different reactivity. One of them only activates methane while the other is solely reactive with water to produce CO. Apparently, upon varying the coordination patterns, the Ir center gains rather distinct capabilities of mediating the bond breaking and making processes. The reactivity toward methane mainly depends on the orbital orientation, while the π-aromaticity of the reaction complex matters for the conversion of water. The experimental and theoretical findings in this work do not only imply the promising role the Ir atom can play in the bulk-system methane conversion, but may also be instructive on how to construct a high-performance center for steam reforming of methane.
References
Wilhelm DJ, Simbeck DR, Karp AD, Dickenson RL. Fuel Processing Tech, 2001, 71: 139–148
Chen Y, Mu X, Luo X, Shi K, Yang G, Wu T. Energy Technol, 2020, 8: 1900750
Koumi Ngoh S, Njomo D. Renew Sustain Energy Rev, 2012, 16: 6782–6792
Barelli L, Bidini G, Gallorini F, Servili S. Energy, 2008, 33: 554–570
Sehested J. Catal Today, 2006, 111: 103–110
Ruifeng G, Zongqiang M. J Rare Earths, 2007, 25: 364–367
Wu H, La Parola V, Pantaleo G, Puleo F, Venezia A, Liotta L. Catalysts, 2013, 3: 563–583
Zhang H, Sun Z, Hu YH. Renew Sustain Energy Rev, 2021, 149: 111330
Morales-Cano F, Lundegaard LF, Tiruvalam RR, Falsig H, Skjøth-Rasmussen MS. Appl Catal A-Gen, 2015, 498: 117–125
Cheah SK, Massin L, Aouine M, Steil MC, Fouletier J, Gélin P. Appl Catal B-Environ, 2018, 234: 279–289
Mei D, Glezakou VA, Lebarbier V, Kovarik L, Wan H, Albrecht KO, Gerber M, Rousseau R, Dagle RA. J Catal, 2014, 316: 11–23
Zhang J, Li X, Chen H, Qi M, Zhang G, Hu H, Ma X. Int J Hydrogen Energy, 2017, 42: 19755–19775
Lu B, Inoue M, Abe T. Sustain Energy Fuels, 2018, 2: 795–802
Wu H, Wu XN, Jin X, Zhou Y, Li W, Ji C, Zhou M. JACS Au, 2021, 1: 1631–1638
Li HF, Zhao YX, Yuan Z, Liu QY, Li ZY, Li XN, Ning CG, He SG. J Phys Chem Lett, 2017, 8: 605–610
Liu Z, Wu H, Li W, Wu X. Molecules, 2021, 26: 6028
Li W, Wu H, Ding X, Wu X. Chin Chem Lett, 2022, doi:https://doi.org/10.1016/j.cclet.2022.02.002
León I, Ruipérez F, Ugalde JM, Wang LS. J Chem Phys, 2018, 149: 144307
Liu X, Li G, Liu Z, Zou J, Yang D, Du S, Yang W, Jiang L, Xie H. J Chem Phys, 2022, 156: 164302
Romanescu C, Galeev TR, Li WL, Boldyrev AI, Wang LS. Acc Chem Res, 2013, 46: 350–358
Geng C, Li J, Weiske T, Schwarz H. Chem Eur J, 2019, 25: 12940–12945
Yang L, Wang XY, Tang XY, Wang MY, Ni CY, Yu H, Song YL, Abrahams BF, Lang JP. Sci China Chem, 2022, 65: 1094–1099
Liu Z, Qin Z, Cui C, Luo Z, Yang B, Jiang Y, Lai C, Wang Z, Wang X, Fang X, Li G, Wang F, Xiao C, Yang X. Sci China Chem, 2022, 65: 1196–1203
Su P, Jiang Z, Chen Z, Wu W. J Phys Chem A, 2014, 118: 2531–2542
Mitoraj MP, Michalak A, Ziegler T. J Chem Theor Comput, 2009, 5: 962–975
Giambiagi M, de Giambiagi MS, Mundim KC. Struct Chem, 1990, 1: 423–427
Schleyer PR, Maerker C, Dransfeld A, Jiao H, van Eikema Hommes NJR. J Am Chem Soc, 1996, 118: 6317–6318
Chen Z, Wannere CS, Corminboeuf C, Puchta R, Schleyer PR. Chem Rev, 2005, 105: 3842–3888
Fallah-Bagher-Shaidaei H, Wannere CS, Corminboeuf C, Puchta R, Schleyer PR. Org Lett, 2006, 8: 863–866
Matito E. Phys Chem Chem Phys, 2016, 18: 11839–11846
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This work was supported by the National Natural Science Foundation of China (21878265, 21603037, 21973016).
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Yuan, B., Liu, Z., Wu, XN. et al. On the distinct reactivity of two isomers of [IrC4H2]+ toward methane and water. Sci. China Chem. 65, 1720–1724 (2022). https://doi.org/10.1007/s11426-022-1342-4
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DOI: https://doi.org/10.1007/s11426-022-1342-4