Highly active single-layer 2H-MoS2 for CO2 hydrogenation to methanol
Few-layer MoS2 were recently discovered as promising catalyst for CO2 hydrogenation to methanol, despite extreme conditions proposed for its synthesis. Herein, we developed an exceptionally facile, safe, and scalable strategy to prepare single-layer MoS2 (s-MoS2) at ambient pressure using instantane...
| Main Authors: | , , , , , |
|---|---|
| Other Authors: | |
| Format: | Journal Article |
| Language: | English |
| Published: |
2024
|
| Subjects: | |
| Online Access: | https://hdl.handle.net/10356/180134 |
| _version_ | 1811684578626109440 |
|---|---|
| author | Zhou, Shenghui Ma, Wenrui Kosari, Mohammadreza Lim, Alvin M.H. Kozlov, Sergey M. Zeng, Hua Chun |
| author2 | School of Chemistry, Chemical Engineering and Biotechnology |
| author_facet | School of Chemistry, Chemical Engineering and Biotechnology Zhou, Shenghui Ma, Wenrui Kosari, Mohammadreza Lim, Alvin M.H. Kozlov, Sergey M. Zeng, Hua Chun |
| author_sort | Zhou, Shenghui |
| collection | NTU |
| description | Few-layer MoS2 were recently discovered as promising catalyst for CO2 hydrogenation to methanol, despite extreme conditions proposed for its synthesis. Herein, we developed an exceptionally facile, safe, and scalable strategy to prepare single-layer MoS2 (s-MoS2) at ambient pressure using instantaneous self-assembled micelles of didodecyldimethylammonium (DA)−MoS4 complexes as precursor. During the pyrolysis, the presence and subsequent decomposition of coordinated DA inhibited the growth and sheet-stacking of MoS2 in c-direction, resulting in discrete s-MoS2 molecular sheets which maximize the exposure of in-plane S vacancies (Sv). Remarkably, s-MoS2 displayed 77% methanol selectivity and methanol space time yield of 1.54 g·gMoS2–1·h–1, representing the top levels among reported MoS2 catalysts under similar conditions. Density functional theory (DFT) simulations attribute high activity of s-MoS2 to its ability to stabilize in-plane low-coordinated Mo atoms in the vicinity of Sv on both sides of monolayer. The superior performance of s-MoS2 creates new prospects for technological applications beyond CO2 hydrogenation. |
| first_indexed | 2024-10-01T04:30:52Z |
| format | Journal Article |
| id | ntu-10356/180134 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T04:30:52Z |
| publishDate | 2024 |
| record_format | dspace |
| spelling | ntu-10356/1801342024-09-18T05:58:18Z Highly active single-layer 2H-MoS2 for CO2 hydrogenation to methanol Zhou, Shenghui Ma, Wenrui Kosari, Mohammadreza Lim, Alvin M.H. Kozlov, Sergey M. Zeng, Hua Chun School of Chemistry, Chemical Engineering and Biotechnology Department of Chemical and Biomolecular Engineering, NUS The Cambridge Centre for Advanced Research and Education, Singapore Engineering Density functional theory Facile and scalable fabrication Few-layer MoS2 were recently discovered as promising catalyst for CO2 hydrogenation to methanol, despite extreme conditions proposed for its synthesis. Herein, we developed an exceptionally facile, safe, and scalable strategy to prepare single-layer MoS2 (s-MoS2) at ambient pressure using instantaneous self-assembled micelles of didodecyldimethylammonium (DA)−MoS4 complexes as precursor. During the pyrolysis, the presence and subsequent decomposition of coordinated DA inhibited the growth and sheet-stacking of MoS2 in c-direction, resulting in discrete s-MoS2 molecular sheets which maximize the exposure of in-plane S vacancies (Sv). Remarkably, s-MoS2 displayed 77% methanol selectivity and methanol space time yield of 1.54 g·gMoS2–1·h–1, representing the top levels among reported MoS2 catalysts under similar conditions. Density functional theory (DFT) simulations attribute high activity of s-MoS2 to its ability to stabilize in-plane low-coordinated Mo atoms in the vicinity of Sv on both sides of monolayer. The superior performance of s-MoS2 creates new prospects for technological applications beyond CO2 hydrogenation. Agency for Science, Technology and Research (A*STAR) National Research Foundation (NRF) The authors gratefully acknowledge the financial supports provided by the National University of Singapore and by the National Research Foundation (NRF), Prime Minister’s Office, Singapore, under its Campus for Research Excellence and Technological Enterprise (CREATE C4T Programme). This work is also supported by the National University of Singapore (A-0009169–00–00) and Agency for Science, Technology and Research (A*STAR) through Low Carbon Energy Research Finding Initiative (LCERFI01–0033 | U2102d2006). 2024-09-18T05:58:18Z 2024-09-18T05:58:18Z 2024 Journal Article Zhou, S., Ma, W., Kosari, M., Lim, A. M., Kozlov, S. M. & Zeng, H. C. (2024). Highly active single-layer 2H-MoS2 for CO2 hydrogenation to methanol. Applied Catalysis B: Environment and Energy, 349, 123870-. https://dx.doi.org/10.1016/j.apcatb.2024.123870 0926-3373 https://hdl.handle.net/10356/180134 10.1016/j.apcatb.2024.123870 2-s2.0-85186521829 349 123870 en LCERFI01–0033 U2102d2006 CREATE C4T A-0009169–00–00 Applied Catalysis B: Environment and Energy © 2024 Elsevier B.V. All rights reserved. |
| spellingShingle | Engineering Density functional theory Facile and scalable fabrication Zhou, Shenghui Ma, Wenrui Kosari, Mohammadreza Lim, Alvin M.H. Kozlov, Sergey M. Zeng, Hua Chun Highly active single-layer 2H-MoS2 for CO2 hydrogenation to methanol |
| title | Highly active single-layer 2H-MoS2 for CO2 hydrogenation to methanol |
| title_full | Highly active single-layer 2H-MoS2 for CO2 hydrogenation to methanol |
| title_fullStr | Highly active single-layer 2H-MoS2 for CO2 hydrogenation to methanol |
| title_full_unstemmed | Highly active single-layer 2H-MoS2 for CO2 hydrogenation to methanol |
| title_short | Highly active single-layer 2H-MoS2 for CO2 hydrogenation to methanol |
| title_sort | highly active single layer 2h mos2 for co2 hydrogenation to methanol |
| topic | Engineering Density functional theory Facile and scalable fabrication |
| url | https://hdl.handle.net/10356/180134 |
| work_keys_str_mv | AT zhoushenghui highlyactivesinglelayer2hmos2forco2hydrogenationtomethanol AT mawenrui highlyactivesinglelayer2hmos2forco2hydrogenationtomethanol AT kosarimohammadreza highlyactivesinglelayer2hmos2forco2hydrogenationtomethanol AT limalvinmh highlyactivesinglelayer2hmos2forco2hydrogenationtomethanol AT kozlovsergeym highlyactivesinglelayer2hmos2forco2hydrogenationtomethanol AT zenghuachun highlyactivesinglelayer2hmos2forco2hydrogenationtomethanol |