Abstract
Graphene nanoribbons with zigzag edges(ZGNRs) have attracted much attention for their spin-polarized edge states predicted more than 15 years ago. Since the ZGNRs are fabricated on metal substrates using molecular precursors, due to their strong coupling with metal substrates, experimental detection of the spin-polarized edge states is still difficult. Here, we design a partially hydrogenated graphene(PHGr), in which periodic hexagonal graphene nanoflakes(GNFs) with zigzag boundaries are embedded in a hydrogenated graphene layer. Using density functional theory(DFT) based first-principles calculations, we find that the hexagonal GNFs exhibit spin-polarized boundary states at their opposite zigzag boundaries, which is similar with the bow-tie-shaped GNFs and ZGNRs. DFT calculations demonstrate that the PHGr is a semiconductor with an antiferromagnetic ground state. Moreover, the antiferromagnetic boundary states and semiconducting properties keep unchanged when the size of GNF varies from 1.4 nm to 2.3 nm. The robustness of the spin-polarized boundary states enables this PHGr as a robust material for detecting spin-polarized boundary states coming from zigzag boundaries. In addition, we find that single Au atoms selectively adsorbed on boundaries catalyze H2 dissociation and therefore lower the barrier of graphene hydrogenation. Therefore, the PHGr can be used not only in carbon-based spintronic devices but also as a platform for single atom catalyst.
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References
Geim A. K., Novoselov K. S., Nat. Mater., 2007, 6(3), 183
Castro Neto A. H., Guinea F., Peres N. M. R., Novoselov K. S., Geim A. K., Rev. Mod. Phys., 2009, 81(1), 109
Avouris P., Nano Lett., 2010, 10(11), 4285
Tan Y., Xia X.-S., Liao X.-L., Li J.-B., Zhong H.-H., Liang S., Xiao S., Liu L.-H., Luo J.-H., He M.-D., Chen L.-Q., Carbon, 2020, 157, 724
Li Y. Y., Chen M. X., Weinert M., Li L., Nat. Commun., 2014, 5(1), 4311
Dutta S., Pati S. K., J. Mater. Chem., 2010, 20(38), 8207
Nakada K., Fujita M., Dresselhaus G., Dresselhaus M. S., Phys. Rev. B, 1996, 54(24), 17954
Magda G. Z., Jin X., Hagymási I., Vancsó P., Osváth Z., Nemes-Incze P., Hwang C., Biró L. P., Tapasztó L., Nature, 2014, 514(7524), 608
Fujita M., Wakabayashi K., Nakada K., Kusakabe K., J. Phys. Soc. JPN, 1996, 65(7), 1920
Son Y.-W., Cohen M. L., Louie S. G., Nature, 2006, 444(7117), 347
Wang W. L., Yazyev O. V., Meng S., Kaxiras E., Phys. Rev. Lett., 2009, 102(15), 157201
Yazyev O. V., Katsnelson M. I., Adv. Funct. Mater., 2012, 2, 71
Siemion F., Peter E. J., Sachsb H., Croat. Chem. Acta, 2005, 78, 195
Lieb E. H., Phys. Rev. Lett., 1989, 62(10), 1201
Dutta S., Pati S. K., J. Phys. Chem. B, 2008, 112(5), 1333
Ruffieux P., Wang S., Yang B., Sánchez-Sánchez C., Liu J., Dienel T., Talirz L., Shinde P., Pignedoli C. A., Passerone D., Dumslaff T., Feng X., Müllen K., Fasel R., Nature, 2016, 531(7595), 489
Shinde P. P., Liu J., Dienel T., Gröning O., Dumslaff T., Mühlinghaus M., Narita A., Müllen K., Pignedoli C. A., Fasel R., Ruffieux P., Passerone D., Carbon, 2021, 175, 50
Mishra S., Beyer D., Eimre K., Kezilebieke S., Berger R., Gröning O., Pignedoli C. A., Müllen K., Liljeroth P., Ruffieux P., Feng X., Fasel R., Nat. Nanotechnol., 2020, 15(1), 22
Li Y., Zhang W., Morgenstern M., Mazzarello R., Phys. Rev. Lett., 2013, 110(21), 216804
Chen H., Que Y., Tao L., Zhang Y.-Y., Lin X., Xiao W., Wang D., Du S., Pantelides S. T., Gao H.-J., Nano Res., 2018, 11(7), 3722
Li Y., Zhou Z., Cabrera C. R., Chen Z., Sci. Rep., 2013, 3, 2030
Chen H., Bao D.-L., Wang D., Que Y., Xiao W., Qian G., Guo H., Sun J., Zhang Y.-Y., Du S., Pantelides S. T., Gao H.-J., Adv. Mater., 2018, 30(32), 1801838
Blöchl P. E., Phys. Rev. B, 1994, 50(24), 17953
Kresse G., Joubert D., Phys. Rev. B, 1999, 59(3), 1758
Kresse G., Furthmüller J., Phys. Rev. B, 1996, 54(16), 11169
Kresse G., Furthmüller J., Comput. Mater. Sci., 1996, 6(1), 15
Monkhorst H. J., Pack J. D., Phys. Rev. B, 1976, 13(12), 5188
Henkelman G., Uberuaga B. P., Jónsson H., J. Chem. Phys., 2000, 113(22), 9901
Henkelman G., Jónsson H., J. Chem. Phys., 2000, 113(22), 9978
Lin X., Lu J. C., Shao Y., Zhang Y. Y., Wu X., Pan J. B., Gao L., Zhu S. Y., Qian K., Zhang Y. F., Bao D. L., Li L. F., Wang Y. Q., Liu Z. L., Sun J. T., Lei T., Liu C., Wang J. O., Ibrahim K., Leonard D. N., Zhou W., Guo H. M., Wang Y. L., Du S. X., Pantelides S. T., Gao H. J., Nat. Mater., 2017, 16(7), 717
Liu Z.-L., Lei B., Zhu Z.-L., Tao L., Qi J., Bao D.-L., Wu X., Huang L., Zhang Y.-Y., Lin X., Wang Y.-L., Du S., Pantelides S. T., Gao H.-J., Nano Lett., 2019, 19(8), 4897
Righi G., Magri R., Selloni A., J. Phys. Chem. C, 2019, 123(15), 9875
Miura Y., Kasai H., Diño W., Nakanishi H., Sugimoto T., J. Appl. Phys., 2003, 93(6), 3395
Acknowledgements
This work was supported by the National Natural Science Foundation of China (No.61888102), the National Key Research and Development Projects of China (Nos.2016YFA0202300, 2018YFA0305800), and the Strategic Priority Research Program of the Chinese Academy of Sciences, China(No.XDB30000000).
Computational resources were provided by the National Supercomputing Center in Tianjin, China.
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Song, Y., Tao, L., Zhang, Y. et al. A DFT Investigation on the Electronic Structures and Au Adatom Assisted Hydrogenation of Graphene Nanoflake Array. Chem. Res. Chin. Univ. 37, 1110–1115 (2021). https://doi.org/10.1007/s40242-021-1163-x
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DOI: https://doi.org/10.1007/s40242-021-1163-x