journal article·2023-02-10

Single Atoms in Photocatalysis: Low Loading Is Good Enough!

Shanshan Qin, Johannes Will, Hyesung Kim, Nikita Denisov, Simon Carl, Erdmann Spiecker, Patrik Schmuki

ACS Energy Letters· Volume 8· Issue 2
Publisher page

Abstract

We disperse Pt single atoms (SAs) with different loading densities on anatase TiO 2 thin films and evaluate the photocatalytic H 2 generation as a function of the incident light intensity. We show that under common illumination intensities (such as terrestrial solar illumination), a minuscule Pt SA loading of ∼10 5 atoms μm –2 (surface Pt content ∼0.1 at.%) is sufficient to achieve a maximized H 2 production rate. This results in a maximum turnover frequency at a single Pt atom site of ∼300 H 2 molecules s –1 . For a vast majority of illumination conditions and a suitable surface configuration, it is not the density of co-catalytic sites that is rate-determining (a high loading is not needed!), but the charge carrier generation (and flux of photoelectrons to the co-catalytic centers) determines the overall reaction rate. This is in stark contrast to SA catalysis of classic chemical reactions where generally a maximum loading of reactive SA delivers a maximum activity.
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Research context

OpenAlex topics: Advanced Photocatalysis Techniques · Electrocatalysts for Energy Conversion · TiO2 Photocatalysis and Solar Cells

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

Affiliations

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

Institute of Micro- and Nanostructure Research & Center for Nanoanalysis and Electron Microscopy (CENEM), University of Erlangen-Nuremberg, IZNF, Cauerstraße 3, 91058 Erlangen, Germany

Regional Centre of Advanced Technologies and Materials, Czech Advanced Technology and Research Institute, Palacky University, Olomouc, 779 00, Czech Republic

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

Funding

European Regional Development Fund · Ministerstvo ?kolstv?, Ml?de?e a Telov?chovy · Deutsche Forschungsgemeinschaft

References (50)

Show source-provided references
1. 10.1016/j.joule.2021.12.01110.1016/j.joule.2021.12.011 ↗
2. 10.1021/acs.chemrev.9b0084010.1021/acs.chemrev.9b00840 ↗
3. 10.1021/ar300361m10.1021/ar300361m ↗
4. 10.1021/acscatal.8b0188610.1021/acscatal.8b01886 ↗
5. 10.1002/chem.20130336610.1002/chem.201303366 ↗
6. 10.1002/adma.20180488310.1002/adma.201804883 ↗
7. 10.1002/chem.20140298910.1002/chem.201402989 ↗
8. 10.1039/C7TA01914A10.1039/C7TA01914A ↗
9. 10.1002/adma.20190340410.1002/adma.201903404 ↗
10. 10.1021/acsenergylett.2c0012210.1021/acsenergylett.2c00122 ↗
11. 10.1021/ar00143a00110.1021/ar00143a001 ↗
12. 10.1002/adma.20200330010.1002/adma.202003300 ↗
13. 10.1038/s41929-021-00650-w10.1038/s41929-021-00650-w ↗
14. 10.1016/0047-2670(79)80037-410.1016/0047-2670(79)80037-4 ↗
15. 10.1002/admi.20220080810.1002/admi.202200808 ↗
16. 10.1002/anie.20191243910.1002/anie.201912439 ↗
17. 10.1002/smll.20210489210.1002/smll.202104892 ↗
18. 10.1021/cr100164510.1021/cr1001645 ↗
19. 10.1021/jp406523w10.1021/jp406523w ↗
20. 10.1039/C7TA04410K10.1039/C7TA04410K ↗
21. 10.1016/j.apcatb.2006.05.00710.1016/j.apcatb.2006.05.007 ↗
22. 10.1016/j.jcat.2009.11.00610.1016/j.jcat.2009.11.006 ↗
23. 10.1002/cctc.20200028110.1002/cctc.202000281 ↗
24. 10.1021/acs.chemrev.0c0057610.1021/acs.chemrev.0c00576 ↗
25. 10.1038/s41565-018-0197-910.1038/s41565-018-0197-9 ↗
26. 10.1126/sciadv.abb982310.1126/sciadv.abb9823 ↗
27. 10.1002/adfm.20210284310.1002/adfm.202102843 ↗
28. 10.1002/solr.20210102610.1002/solr.202101026 ↗
29. 10.1016/j.electacta.2022.14012910.1016/j.electacta.2022.140129 ↗
30. 10.1007/s10853-022-07420-410.1007/s10853-022-07420-4 ↗
31. 10.1002/adma.20190850510.1002/adma.201908505 ↗
32. 10.1021/acsomega.0c0574910.1021/acsomega.0c05749 ↗
33. 10.1021/acscatal.7b0084510.1021/acscatal.7b00845 ↗
34. 10.1016/j.apcata.2020.11770310.1016/j.apcata.2020.117703 ↗
35. 10.1021/jp972002k10.1021/jp972002k ↗
36. 10.1021/acscatal.9b0421410.1021/acscatal.9b04214 ↗
37. 10.1016/j.jcat.2019.05.03310.1016/j.jcat.2019.05.033 ↗
38. 10.1002/adma.20220656910.1002/adma.202206569 ↗
39. 10.1021/acsenergylett.1c0024610.1021/acsenergylett.1c00246 ↗
40. 10.1016/j.isci.2021.10293810.1016/j.isci.2021.102938 ↗
41. 10.1039/c3ta13167j10.1039/c3ta13167j ↗
42. 10.3390/app1014469910.3390/app10144699 ↗
43. 10.1021/jp034773w10.1021/jp034773w ↗
44. 10.1103/PhysRevB.73.04532610.1103/PhysRevB.73.045326 ↗
45. 10.1038/srep0135210.1038/srep01352 ↗
46. 10.1016/j.nanoso.2017.03.00610.1016/j.nanoso.2017.03.006 ↗
47. 10.1002/aenm.20180098110.1002/aenm.201800981 ↗
48. 10.1002/anie.20190405810.1002/anie.201904058 ↗
49. 10.1002/cctc.20210191610.1002/cctc.202101916 ↗
50. 10.1002/adma.20180164910.1002/adma.201801649 ↗