journal article·2022-10-14

Direct H2S Decomposition by Plasmonic Photocatalysis: Efficient Remediation plus Sustainable Hydrogen Production

Minghe Lou, Junwei Lucas Bao, Linan Zhou, Gopal Narmada Naidu, Hossein Robatjazi, Aaron I. Bayles, Henry O. Everitt, Peter Nordlander, Emily A. Carter, Naomi J. Halas

ACS Energy Letters· Volume 7· Issue 10
Publisher page

Abstract

Plasmonic metal nanostructures have garnered rapidly increasing interest as heterogeneous photocatalysts, facilitating chemical bond activation and overcoming the high energy demands of conventional thermal catalysis. Here we report the highly efficient plasmonic photocatalysis of the direct decomposition of hydrogen sulfide into hydrogen and sulfur, an alternative to the industrial Claus process. Under visible light illumination and with no external heat source, up to a 20-fold reactivity enhancement compared to thermocatalysis can be observed. The substantially enhanced reactivity can be attributed to plasmon-mediated hot carriers (HCs) that modify the reaction energetics. With a shift in the rate-determining step of the reaction, a new reaction pathway is made possible with a lower apparent reaction barrier. Light-driven one-step decomposition of hydrogen sulfide represents an exciting opportunity for simultaneous high-efficiency hydrogen production and low-temperature sulfur recovery, important in many industrial processes.
Source: openalex_inverted_index · Quality: baseline

Research context

OpenAlex topics: Advanced Photocatalysis Techniques · Industrial Gas Emission Control · Gas Sensing Nanomaterials and Sensors

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

Affiliations

Department of Chemistry, Rice University, Houston, Texas 77005, United States

Laboratory of Nanophotonics, Rice University, Houston, Texas 77005, United States

Department of Mechanical and Aerospace Engineering and the Andlinger Center for Energy and the Environment, Princeton University, Princeton, New Jersey 08544, United States

Department of Chemistry, Boston College, Chestnut Hill, Massachusetts 02467, United States

Department of Electrical and Computer Engineering, Rice University, Houston, Texas 77005, United States

Syzygy Plasmonics Inc., Houston, Texas 77054, United States

U.S. Army DEVCOM Army Research Laboratory, Houston, Texas 77005, United States

Department of Physics and Astronomy, Rice University, Houston, Texas 77005, United States

Funding

Welch Foundation · Air Force Office of Scientific Research · Defense Threat Reduction Agency

References (60)

Show source-provided references
1. Apodaca L. E. · 2020 · 160
2. 2010 · 9 · 173
3. 2017 National Emissions Inventory Data. https://www.epa.gov/air-emissions-inventories/2017-national-emissions-inventory-nei-data (accessed 2022-02-14).
4. 10.1016/S0920-5861(03)00071-310.1016/S0920-5861(03)00071-3 ↗
5. 10.1021/acs.iecr.7b0466710.1021/acs.iecr.7b04667 ↗
6. 10.1016/j.ijhydene.2018.10.03510.1016/j.ijhydene.2018.10.035 ↗
7. 10.1080/17415993.2015.101053310.1080/17415993.2015.1010533 ↗
8. 10.1007/s11244-013-0061-y10.1007/s11244-013-0061-y ↗
9. 10.1016/j.cej.2016.11.05710.1016/j.cej.2016.11.057 ↗
10. 10.1016/j.ijhydene.2017.10.15610.1016/j.ijhydene.2017.10.156 ↗
11. 10.1039/C9EE03231B10.1039/C9EE03231B ↗
12. 10.1002/er.505010.1002/er.5050 ↗
13. 10.1016/j.apcatb.2016.02.06810.1016/j.apcatb.2016.02.068 ↗
14. 10.1039/c1gc15515f10.1039/c1gc15515f ↗
15. 10.1016/j.renene.2010.04.03710.1016/j.renene.2010.04.037 ↗
16. 10.1039/D0CC05894G10.1039/D0CC05894G ↗
17. 10.1021/acsomega.1c0729410.1021/acsomega.1c07294 ↗
18. 10.3390/molecules2713429610.3390/molecules27134296 ↗
19. 10.1016/j.jechem.2020.04.05110.1016/j.jechem.2020.04.051 ↗
20. 10.1016/j.cattod.2019.02.03210.1016/j.cattod.2019.02.032 ↗
21. 10.1039/D0CY01145B10.1039/D0CY01145B ↗
22. 10.1016/j.fuel.2020.11872910.1016/j.fuel.2020.118729 ↗
23. 10.1016/j.ijhydene.2018.04.21710.1016/j.ijhydene.2018.04.217 ↗
24. 10.1016/j.cattod.2018.11.00810.1016/j.cattod.2018.11.008 ↗
25. Robatjazi H. · 2021 · 36310.1021/bk-2021-1398.ch016 ↗
26. 10.1038/nnano.2014.31110.1038/nnano.2014.311 ↗
27. 10.1038/nmat345410.1038/nmat3454 ↗
28. 10.1038/ncomms1454210.1038/ncomms14542 ↗
29. 10.1073/pnas.160976911310.1073/pnas.1609769113 ↗
30. 10.1038/nmat428110.1038/nmat4281 ↗
31. 10.1021/acs.nanolett.7b0541010.1021/acs.nanolett.7b05410 ↗
32. 10.1038/s41467-017-00055-z10.1038/s41467-017-00055-z ↗
33. 10.1038/s41560-019-0517-910.1038/s41560-019-0517-9 ↗
34. 10.1016/j.apcatb.2017.02.08010.1016/j.apcatb.2017.02.080 ↗
35. 10.1038/s41929-020-0466-510.1038/s41929-020-0466-5 ↗
36. 10.1038/nchem.103210.1038/nchem.1032 ↗
37. 10.1021/acsenergylett.2c0014210.1021/acsenergylett.2c00142 ↗
38. 10.1021/ja060471710.1021/ja0604717 ↗
39. 10.1126/science.aat696710.1126/science.aat6967 ↗
40. Huber M. L. · 2011
41. 10.1021/nn401924n10.1021/nn401924n ↗
42. 10.1038/s41377-020-00345-010.1038/s41377-020-00345-0 ↗
43. 10.1039/c3cs60364d10.1039/c3cs60364d ↗
44. 10.1002/kin.2132510.1002/kin.21325 ↗
45. 10.1021/jp046475k10.1021/jp046475k ↗
46. 10.1016/j.susc.2005.03.02310.1016/j.susc.2005.03.023 ↗
47. 10.1016/j.apsusc.2014.04.19710.1016/j.apsusc.2014.04.197 ↗
48. 10.1016/0039-6028(94)90210-010.1016/0039-6028(94)90210-0 ↗
49. 10.1016/j.susc.2008.07.00110.1016/j.susc.2008.07.001 ↗
50. 10.1126/sciadv.aao471010.1126/sciadv.aao4710 ↗
51. 10.1146/annurev-physchem-061020-05350110.1146/annurev-physchem-061020-053501 ↗
52. 10.1021/jacs.9b0680410.1021/jacs.9b06804 ↗
53. 10.1016/S0920-5861(96)00208-810.1016/S0920-5861(96)00208-8 ↗
54. 10.1023/A:102018142305510.1023/A:1020181423055 ↗
55. 10.1016/j.cattod.2020.03.05210.1016/j.cattod.2020.03.052 ↗
56. 10.1002/adma.20210097210.1002/adma.202100972 ↗
57. 10.1021/acscatal.7b0317410.1021/acscatal.7b03174 ↗
58. 10.1021/nl502571b10.1021/nl502571b ↗
59. 10.1021/acsenergylett.0c0197810.1021/acsenergylett.0c01978 ↗
60. 10.1021/acsnano.8b0035210.1021/acsnano.8b00352 ↗