DataVXACS Applied Materials & InterfacesPaper
journal article·2023-07-05

Activation of Osmium by the Surface Effects of Hydrogenated TiO2 Nanotube Arrays for Enhanced Hydrogen Evolution Reaction Performance

Mila N. Krstajić Pajić, Ana S. Dobrota, Anca Mazare, Slađana Đurđić, Imgon Hwang, Natalia V. Skorodumova, Dragan Manojlović, Rastko Vasilić, Igor A. Pašti, Patrik Schmuki, Uroš Lačnjevac

ACS Applied Materials & Interfaces· Volume 15· Issue 26
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Source abstract

Abstract

Efficient cathodes for the hydrogen evolution reaction (HER) in acidic water electrolysis rely on the use of expensive platinum group metals (PGMs). However, to achieve economically viable operation, both the content of PGMs must be reduced and their intrinsically strong H adsorption mitigated. Herein, we show that the surface effects of hydrogenated TiO 2 nanotube (TNT) arrays can make osmium, a so far less-explored PGM, a highly active HER electrocatalyst. These defect-rich TiO 2 nanostructures provide an interactive scaffold for the galvanic deposition of Os particles with modulated adsorption properties. Through systematic investigations, we identify the synthesis conditions (OsCl 3 concentration/temperature/reaction time) that yield a progressive improvement in Os deposition rate and mass loading, thereby decreasing the HER overpotential. At the same time, the Os particles deposited by this procedure remain mainly sub-nanometric and entirely cover the inner tube walls. An optimally balanced Os@TNT composite prepared at 3 mM/55 °C/30 min exhibits a record low overpotential (η) of 61 mV at a current density of 100 mA cm –2, a high mass activity of 20.8 A mg Os –1 at 80 mV, and a stable performance in an acidic medium. Density functional theory calculations indicate the existence of strong interactions between the hydrogenated TiO 2 surface and small Os clusters, which may weaken the Os–H* binding strength and thus boost the intrinsic HER activity of Os centers. The results presented in this study offer new directions for the fabrication of cost-effective PGM-based catalysts and a better understanding of the synergistic electronic interactions at the PGM|TiO 2 interface.
Source: openalex_inverted_index · Quality: baseline

Research context

Energy storageNanomaterialsCompositesCatalysis & surfacesMaterials processing

OpenAlex topics: Electrocatalysts for Energy Conversion · Advanced battery technologies research · Fuel Cells and Related Materials

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

Affiliations

University of Belgrade – Faculty of Technology and Metallurgy, Karnegijeva 4, 11000 Belgrade, Serbia

University of Belgrade – Faculty of Physical Chemistry, Studentski trg 12-16, 11000 Belgrade , Serbia

Department of Materials Science, WW4-LKO, Friedrich-Alexander-University of Erlangen-Nuremberg, Martensstraße 7, 91058 Erlangen, Germany

Advanced Institute for Materials Research (AIMR), National University Corporation Tohoku University (TU), Sendai 980-8577, Japan

University of Belgrade – Faculty of Chemistry, Studentski trg 12-16, 11000 Belgrade, Serbia

Department of Materials Science and Engineering, School of Industrial Engineering and Management, KTH−Royal Institute of Technology, Brinellvägen 23, SE-100 44 Stockholm, Sweden

University of Belgrade – Faculty of Physics, Studentski trg 12-16, 11000 Belgrade, Serbia

Regional Centre of Advanced Technologies and Materials, Šlechtitelů 27, 78371 Olomouc, Czech Republic

Department of Chemistry, Faculty of Science, King Abdulaziz University, P.O. Box 80203, 21569 Jeddah, Saudi Arabia

University of Belgrade – Institute for Multidisciplinary Research, Kneza Višeslava 1, 11030 Belgrade, Serbia

Funding

Vetenskapsr?det · Ministerstvo ?kolstv?, Ml?de?e a Telov?chovy · Deutsche Forschungsgemeinschaft · Science Fund of the Republic of Serbia · Ministarstvo Prosvete, Nauke i Tehnolo?kog Razvoja · Schw?bisch Gm?nd · Bilateral cooperation program between the Republic of Serbia and the Federal Republic of Germany

References (70)

Show source-provided references
1. 10.1126/science.aad499810.1126/science.aad4998 ↗
2. 10.1038/nature1147510.1038/nature11475 ↗
3. 10.1021/acs.chemrev.9b0024810.1021/acs.chemrev.9b00248 ↗
4. 10.1002/smll.20210455910.1002/smll.202104559 ↗
5. 10.1039/c4cs00448e10.1039/c4cs00448e ↗
6. 10.1002/smll.20190305710.1002/smll.201903057 ↗
7. 10.1038/s41467-021-24079-810.1038/s41467-021-24079-8 ↗
8. 10.1002/smll.20210482410.1002/smll.202104824 ↗
9. 10.1002/adfm.20210846410.1002/adfm.202108464 ↗
10. 10.1021/acsami.0c1047610.1021/acsami.0c10476 ↗
11. 10.1002/advs.20210034710.1002/advs.202100347 ↗
12. 10.1002/adfm.20200977010.1002/adfm.202009770 ↗
13. 10.1016/j.cej.2021.13130910.1016/j.cej.2021.131309 ↗
14. 10.1039/d0ta02681f10.1039/d0ta02681f ↗
15. 10.1002/anie.20200811710.1002/anie.202008117 ↗
16. 10.1039/c8ta12219a10.1039/c8ta12219a ↗
17. 10.1002/anie.20211416010.1002/anie.202114160 ↗
18. 10.1021/acscatal.2c0321410.1021/acscatal.2c03214 ↗
19. 10.1021/acsami.2c0950710.1021/acsami.2c09507 ↗
20. 10.1038/s41467-021-23306-610.1038/s41467-021-23306-6 ↗
21. 10.1016/j.nanoen.2019.05.03410.1016/j.nanoen.2019.05.034 ↗
22. 10.1002/anie.20210712310.1002/anie.202107123 ↗
23. 10.1002/adma.20190384110.1002/adma.201903841 ↗
24. 10.1016/j.mtener.2022.10104210.1016/j.mtener.2022.101042 ↗
25. 10.1016/j.jechem.2021.10.03110.1016/j.jechem.2021.10.031 ↗
26. 10.1002/cssc.20210155910.1002/cssc.202101559 ↗
27. 10.1039/d0nr01316a10.1039/d0nr01316a ↗
28. 10.1016/j.apsusc.2019.14467910.1016/j.apsusc.2019.144679 ↗
29. 10.1002/smll.20180213210.1002/smll.201802132 ↗
30. 10.1021/acs.jpcc.8b0167810.1021/acs.jpcc.8b01678 ↗
31. 10.1016/j.electacta.2015.04.01210.1016/j.electacta.2015.04.012 ↗
32. 10.1016/j.nanoen.2018.03.04010.1016/j.nanoen.2018.03.040 ↗
33. 10.1039/d0ta07492f10.1039/d0ta07492f ↗
34. 10.1002/adma.20060254910.1002/adma.200602549 ↗
35. 10.1021/ja710899q10.1021/ja710899q ↗
36. 10.1039/c6cp01799a10.1039/c6cp01799a ↗
37. 10.1016/j.electacta.2013.10.09210.1016/j.electacta.2013.10.092 ↗
38. 10.1002/adma.20190850510.1002/adma.201908505 ↗
39. 10.1002/adfm.20210284310.1002/adfm.202102843 ↗
40. 10.1016/j.isci.2021.10293810.1016/j.isci.2021.102938 ↗
41. 10.1002/adfm.20220784910.1002/adfm.202207849 ↗
42. 10.1002/adma.20220656910.1002/adma.202206569 ↗
43. 10.1016/j.electacta.2022.14012910.1016/j.electacta.2022.140129 ↗
44. 10.1002/smll.20210489210.1002/smll.202104892 ↗
45. 10.1039/d1ta04809k10.1039/d1ta04809k ↗
46. 10.1002/anie.20220864210.1002/anie.202208642 ↗
47. 10.1038/s41467-022-28805-810.1038/s41467-022-28805-8 ↗
48. 10.1002/aenm.20210023410.1002/aenm.202100234 ↗
49. 10.1016/j.jcis.2018.12.04110.1016/j.jcis.2018.12.041 ↗
50. 10.1016/j.jcat.2019.01.01010.1016/j.jcat.2019.01.010 ↗
51. 10.1016/j.nanoen.2017.07.00910.1016/j.nanoen.2017.07.009 ↗
52. 10.1002/cphc.20150017410.1002/cphc.201500174 ↗
53. 10.1002/celc.20220008110.1002/celc.202200081 ↗
54. 10.1016/j.electacta.2008.08.00410.1016/j.electacta.2008.08.004 ↗
55. Wanger C. D. · 1992
56. 10.1021/cr500061m10.1021/cr500061m ↗
57. 10.1016/j.apsusc.2022.15368110.1016/j.apsusc.2022.153681 ↗
58. 10.1016/j.actbio.2016.08.05010.1016/j.actbio.2016.08.050 ↗
59. 10.1016/s0022-0728(03)00256-010.1016/s0022-0728(03)00256-0 ↗
60. 10.1016/j.jpowsour.2012.03.06710.1016/j.jpowsour.2012.03.067 ↗
61. 10.1039/a907161j10.1039/a907161j ↗
62. 10.1016/s0013-4686(02)00329-810.1016/s0013-4686(02)00329-8 ↗
63. 10.1016/j.jcis.2005.03.03910.1016/j.jcis.2005.03.039 ↗
64. 10.1016/s0022-0728(96)04907-810.1016/s0022-0728(96)04907-8 ↗
65. 10.1021/acscatal.0c0178310.1021/acscatal.0c01783 ↗
66. Bao X. · 2022
67. 10.1016/j.cej.2020.12833310.1016/j.cej.2020.128333 ↗
68. Kittel C. · 2005
69. 10.1149/1.185698810.1149/1.1856988 ↗
70. 10.1016/j.susc.2011.12.01710.1016/j.susc.2011.12.017 ↗