Vacancy engineering of two-dimensional W 2 N 3 nanosheets for efficient CO 2 hydrogenation
Source abstract
Abstract
Peaking carbon emissions and achieving carbon neutrality have become the consensus goal of the international community to solve the environmental problems threatening mankind caused by accumulative greenhouse gases like CO2. Herein we proposed vacancy engineering of two-dimensional (2D) topological W2N3 for efficient CO2 hydrogenation into high value-added chemicals and fuels. Spherical aberration corrected scanning transmission electron microscopy (Cs-corrected STEM) confirmed a large amount of N vacancies on the catalyst surface, which significantly reduced the energy barrier for the formation of the essential intermediates of *CO and *CHO as revealed by density functional theory (DFT) calculations. Consequently, the highly stable catalyst exhibited efficient CO2 hydrogenation superior to many previous reports with a maximum CO2 conversion rate of 24% and a high selectivity of 23% for C2+ hydrocarbons. This work provided not only insight into the vacancy-controlled CO2 hydrogenation mechanism, but also fresh ammunition to bring the remaining potential of 2D topological transition metal nitrides in the field of catalysis.
Source: europepmc · Quality: candidate unverified · Source record ↗
Research context
OpenAlex topics: Advanced Photocatalysis Techniques · MXene and MAX Phase Materials · Electronic and Structural Properties of Oxides
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
Affiliations
State Key Laboratory of Applied Organic Chemistry (SKLAOC), Key Laboratory of Advanced Catalysis of Gansu Province, College of Chemistry and Chemical Engineering, Key Laboratory of Special Function Materials and Structure Design, Ministry of Education, Lanzhou University, Lanzhou, 730000, China
Electron Microscopy Centre of Lanzhou University and Key Laboratory for Magnetism and Magnetic Materials of Ministry of Education, Lanzhou University, Lanzhou 730000, China
Funding
National Natural Science Foundation of China
References (51)
Show source-provided references
1. Markewitz · Energy Environ. Sci. · 2012 · 5 · 728110.1039/c2ee03403d ↗
2. Aitbekova · Angew. Chem., Int. Ed. · 2019 · 58 · 1745110.1002/anie.201910579 ↗
3. Wang · ACS Catal. · 2020 · 10 · 638910.1021/acscatal.0c00810 ↗
4. Ramirez · ACS Catal. · 2018 · 8 · 917410.1021/acscatal.8b02892 ↗
5. Hwang · ACS Catal. · 2021 · 11 · 226710.1021/acscatal.0c04358 ↗
6. Zhao · Angew. Chem., Int. Ed. · 2021 · 60 · 449610.1002/anie.202015017 ↗
7. Das · Chem. Soc. Rev. · 2020 · 49 · 293710.1039/C9CS00713J ↗
8. Skupinska · Chem. Rev. · 1991 · 91 · 61310.1021/cr00004a007 ↗
9. Shen · ACS Catal. · 2020 · 10 · 1458110.1021/acscatal.0c03471 ↗
10. Tan · Chem. Rev. · 2017 · 117 · 622510.1021/acs.chemrev.6b00558 ↗
11. Deng · Nat. Nanotechnol. · 2016 · 11 · 21810.1038/nnano.2015.340 ↗
12. Tang · Adv. Mater. · 2019 · 31 · 190199610.1002/adma.201901996 ↗
13. Anjum · Adv. Mater. · 2018 · 30 · 170710510.1002/adma.201707105 ↗
14. Ren · Adv. Energy Mater. · 2017 · 7 · 160165710.1002/aenm.201601657 ↗
15. Zhao · Nat. Energy · 2016 · 1 · 1618410.1038/nenergy.2016.184 ↗
16. Handoko · J. Mater. Chem. A · 2018 · 6 · 2188510.1039/C8TA06567E ↗
17. Johansson · Surf. Sci. Rep. · 1995 · 21 · 17910.1016/0167-5729(94)00005-0 ↗
18. Houston · Science · 1974 · 185 · 25810.1126/science.185.4147.258 ↗
19. Jin · Adv. Mater. · 2019 · 31 · 190270910.1002/adma.201902709 ↗
20. You · Phys. Rev. B · 2021 · 103 · 10450310.1103/PhysRevB.103.104503 ↗
21. Li · Appl. Phys. Lett. · 2020 · 116 · 07050110.1063/1.5143800 ↗
22. Kong · Nat. Chem. · 2011 · 3 · 84510.1038/nchem.1171 ↗
23. Wang · Phys. Rev. Lett. · 2012 · 108 · 09640410.1103/PhysRevLett.108.096404 ↗
24. Ma · ChemNanoMat · 2021 · 7 · 36810.1002/cnma.202100051 ↗
25. Zhai · Phys. Chem. Chem. Phys. · 2020 · 22 · 2214010.1039/D0CP02841J ↗
26. Li · Chem. Rec. · 2020 · 20 · 41310.1002/tcr.201900050 ↗
27. Jin · Adv. Mater. · 2019 · 31 · 190270910.1002/adma.201902709 ↗
28. Jin · Adv. Funct. Mater. · 2019 · 29 · 190064910.1002/adfm.201900649 ↗
29. Huang · Adv. Funct. Mater. · 2020 · 30 · 190848610.1002/adfm.201908486 ↗
30. Wang · Chem. Mater. · 2012 · 24 · 302310.1021/cm301516w ↗
31. Lin · Adv. Funct. Mater. · 2022 · 32 · 210881410.1002/adfm.202108814 ↗
32. Yu · Adv. Mater. · 2018 · 30 · 180565510.1002/adma.201805655 ↗
33. Tan · Nano Res. · 2020 · 13 · 143410.1007/s12274-020-2687-y ↗
34. Yu · Adv. Mater. · 2018 · 30 · 180565510.1002/adma.201805655 ↗
35. Dorner · Energy Environ. Sci. · 2010 · 3 · 88410.1039/c001514h ↗
36. Saeidi · Renewable Sustainable Energy Rev. · 2017 · 80 · 129210.1016/j.rser.2017.05.204 ↗
37. Feng · ACS Catal. · 2021 · 11 · 470410.1021/acscatal.0c05410 ↗
38. Vermaire · J. Catal. · 1989 · 116 · 30910.1016/0021-9517(89)90098-5 ↗
39. Wu · ChemCatChem · 2020 · 12 · 200410.1002/cctc.201902131 ↗
40. Chen · ACS Appl. Mater. Interfaces · 2019 · 11 · 3100910.1021/acsami.9b11285 ↗
41. Chen · J. Catal. · 2019 · 379 · 12110.1016/j.jcat.2019.09.022 ↗
42. Goud · ACS Catal. · 2020 · 10 · 1425810.1021/acscatal.0c03799 ↗
43. Liu · ACS Sustainable Chem. Eng. · 2018 · 6 · 1018210.1021/acssuschemeng.8b01491 ↗
44. Zhong · Chem. Soc. Rev. · 2020 · 49 · 138510.1039/C9CS00614A ↗
45. Roy · ACS Energy Lett. · 2018 · 3 · 193810.1021/acsenergylett.8b00740 ↗
46. Xu · Angew. Chem., Int. Ed. · 2020 · 59 · 2173610.1002/anie.202009620 ↗
47. Yao · Nat. Commun. · 2020 · 11 · 639510.1038/s41467-020-20214-z ↗
48. Zhang · Nat. Catal. · 2020 · 3 · 41110.1038/s41929-020-0440-2 ↗
49. Frei · J. Catal. · 2018 · 361 · 31310.1016/j.jcat.2018.03.014 ↗
50. Kattel · Angew. Chem., Int. Ed. · 2016 · 55 · 796810.1002/anie.201601661 ↗
51. Chen · Adv. Mater. · 2018 · 30 · 170466310.1002/adma.201704663 ↗