Issue

Vol. 16 (2024)

Recent Advances in Mechanistic Understanding of Metal-Free Carbon Thermocatalysis and Electrocatalysis with Model Molecules

https://doi.org/10.1007/s40820-023-01262-8
Wei Guo
CAS Key Laboratory of Design and Assembly of Functional Nanostructures, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002, People’s Republic of China
Linhui Yu
Institute of Urban Environment, Chinese Academy of Sciences, Xiamen 361021, People’s Republic of China
Ling Tang
CAS Key Laboratory of Design and Assembly of Functional Nanostructures, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002, People’s Republic of China
Yan Wan
CAS Key Laboratory of Design and Assembly of Functional Nanostructures, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002, People’s Republic of China
Yangming Lin
CAS Key Laboratory of Design and Assembly of Functional Nanostructures, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002, People’s Republic of China

Corresponding Author: Yangming Lin

xmlinyangming@fjirsm.ac.cn

Nano-Micro Letters, Vol. 16 (2024), Article Number: 125

Abstract

Metal-free carbon, as the most representative heterogeneous metal-free catalysts, have received considerable interests in electro- and thermo-catalytic reactions due to their impressive performance and sustainability. Over the past decade, well-designed carbon catalysts with tunable structures and heteroatom groups coupled with various characterization techniques have proposed numerous reaction mechanisms. However, active sites, key intermediate species, precise structure–activity relationships and dynamic evolution processes of carbon catalysts are still rife with controversies due to the monotony and limitation of used experimental methods. In this Review, we summarize the extensive efforts on model catalysts since the 2000s, particularly in the past decade, to overcome the influences of material and structure limitations in metal-free carbon catalysis. Using both nanomolecule model and bulk model, the real contribution of each alien species, defect and edge configuration to a series of fundamentally important reactions, such as thermocatalytic reactions, electrocatalytic reactions, were systematically studied. Combined with in situ techniques, isotope labeling and size control, the detailed reaction mechanisms, the precise 2D structure–activity relationships and the rate-determining steps were revealed at a molecular level. Furthermore, the outlook of model carbon catalysis has also been proposed in this work.


Highlights:
1 Mechanistic understandings of metal-free carbon thermocatalysis and electrocatalysis from the viewpoint of model method are summarized.
2 Active sites and reaction mechanisms are discussed with a focus on in-situ techniques and 2D structure–activity relationships.
3 The real contribution of each alien species, defect and edge configuration to catalytic reactions are systematically highlighted at a molecular level.

Keywords

Metal-free carbon catalysts Model catalyst Electrocatalysis Active site Reaction mechanisms
Guo, Wei, Linhui Yu, Ling Tang, Yan Wan, and Yangming Lin. 2024. “Recent Advances in Mechanistic Understanding of Metal-Free Carbon Thermocatalysis and Electrocatalysis With Model Molecules”. Nano-Micro Letters 16 (February):125. https://doi.org/10.1007/s40820-023-01262-8.
Download Citation
Endnote/Zotero/Mendeley (RIS)
BibTeX
References
  1. D.S. Su, G. Wen, S. Wu, F. Peng, R. Schlögl, Carbocatalysis in liquid-phase reactions. Angew. Chem. Int. Ed. 56(4), 936–964 (2017). https://doi.org/10.1002/anie.201600906
  2. D. Yu, E. Nagelli, F. Du, L. Dai, Metal-free carbon nanomaterials become more active than metal catalysts and last longer. J. Phys. Chem. Lett. 1(14), 2165–2173 (2010). https://doi.org/10.1021/jz100533t
  3. X. Liu, L. Dai, Carbon-based metal-free catalysts. Nat. Rev. Mater. 1, 16064 (2016). https://doi.org/10.1038/natrevmats.2016.64
  4. H. Piao, G. Choi, X. Jin, S.-J. Hwang, Y.J. Song et al., Monolayer graphitic carbon nitride as metal-free catalyst with enhanced performance in photo- and electro-catalysis. Nano-Micro Lett. 14(1), 55 (2022). https://doi.org/10.1007/s40820-022-00794-9
  5. J. Zhang, J. Zhang, F. He, Y. Chen, J. Zhu et al., Defect and doping co-engineered non-metal nanocarbon ORR electrocatalyst. Nano-Micro Lett. 13(1), 65 (2021). https://doi.org/10.1007/s40820-020-00579-y
  6. Y. Wu, P. Xiong, J. Wu, Z. Huang, J. Sun et al., Band engineering and morphology control of oxygen-incorporated graphitic carbon nitride porous nanosheets for highly efficient photocatalytic hydrogen evolution. Nano-Micro Lett. 13(1), 48 (2021). https://doi.org/10.1007/s40820-020-00571-6
  7. M. Yamamoto, S. Goto, R. Tang, K. Yamazaki, Three-dimensionally ordered nanoporous graphene materials: template synthesis, structure, and applications. ChemRxiv (2023). https://doi.org/10.26434/chemrxiv-2023-1mgs8
  8. K. Srinivas, D. Liu, F. Ma, A. Chen, Z. Zhang et al., Defect-engineered mesoporous undoped carbon nanoribbons for benchmark oxygen reduction reaction. Small 19(34), e2301589 (2023). https://doi.org/10.1002/smll.202301589
  9. Y. Mou, X. Wu, C. Qin, J. Chen, Y. Zhao et al., Linkage microenvironment of azoles-related covalent organic frameworks precisely regulates photocatalytic generation of hydrogen peroxide. Angew. Chem. Int. Ed. 62(36), e202309480 (2023). https://doi.org/10.1002/anie.202309480
  10. H. Wang, Y. Wu, M. Feng, W. Tu, T. Xiao et al., Visible-light-driven removal of tetracycline antibiotics and reclamation of hydrogen energy from natural water matrices and wastewater by polymeric carbon nitride foam. Water Res. 144, 215–225 (2018). https://doi.org/10.1016/j.watres.2018.07.025
  11. X. Yan, B. Wang, J. Ren, X. Long, D. Yang, An unsaturated bond strategy to regulate active centers of metal-free covalent organic frameworks for efficient oxygen reduction. Angew. Chem. Int. Ed. 61(46), e202209583 (2022). https://doi.org/10.1002/anie.202209583
  12. X. Long, D. Li, B. Wang, Z. Jiang, W. Xu et al., Heterocyclization strategy for construction of linear conjugated polymers: efficient metal-free electrocatalysts for oxygen reduction. Angew. Chem. Int. Ed. 58(33), 11369–11373 (2019). https://doi.org/10.1002/anie.201905468
  13. Z. Zhao, B. Wang, Z. You, Q. Zhang, W. Song et al., Heterocyclic modulated electronic states of alkynyl-containing conjugated microporous polymers for efficient oxygen reduction. Small 19(17), e2207298 (2023). https://doi.org/10.1002/smll.202207298
  14. Z. You, B. Wang, Z. Zhao, Q. Zhang, W. Song et al., Metal-free carbon-based covalent organic frameworks with heteroatom-free units boost efficient oxygen reduction. Adv. Mater. 35(7), e2209129 (2023). https://doi.org/10.1002/adma.202209129
  15. E. Troschke, M. Oschatz, I.K. Ilic, Schiff-bases for sustainable battery and supercapacitor electrodes. Exploration 1(3), 20210128 (2021). https://doi.org/10.1002/EXP.20210128
  16. F. He, Y. Wang, J. Liu, X. Yao, One-dimensional carbon based nanoreactor fabrication by electrospinning for sustainable catalysis. Exploration 3, 20220164 (2023). https://doi.org/10.1002/EXP.20220164
  17. S. Zhao, X. Lu, L. Wang, J. Gale, R. Amal, Carbon-based metal-free catalysts for electrocatalytic reduction of nitrogen for synthesis of ammonia at ambient conditions. Adv. Mater. 31(13), e1805367 (2019). https://doi.org/10.1002/adma.201805367
  18. L. Liotta, Catalytic oxidation of volatile organic compounds on supported noble metals. Appl. Catal. B 100(3–4), 403–412 (2010). https://doi.org/10.1016/j.apcatb.2010.08.023
  19. E.W. McFarland, H. Metiu, Catalysis by doped oxides. Chem. Rev. 113(6), 4391–4427 (2013). https://doi.org/10.1021/cr300418s
  20. J.J. Sattler, J. Ruiz-Martinez, E. Santillan-Jimenez, B.M. Weckhuysen, Catalytic dehydrogenation of light alkanes on metals and metal oxides. Chem. Rev. 114(20), 10613–10653 (2014). https://doi.org/10.1021/cr5002436
  21. S. Navalon, A. Dhakshinamoorthy, M. Alvaro, H. Garcia, Carbocatalysis by graphene-based materials. Chem. Rev. 114(12), 6179–6212 (2014). https://doi.org/10.1021/cr4007347
  22. R. Paul, F. Du, L. Dai, Y. Ding, Z.L. Wang et al., 3d heteroatom-doped carbon nanomaterials as multifunctional metal-free catalysts for integrated energy devices. Adv. Mater. 31(13), e1805598 (2019). https://doi.org/10.1002/adma.201805598
  23. Z. Komeily-Nia, L.-T. Qu, J.-L. Li, Progress in the understanding and applications of the intrinsic reactivity of graphene-based materials. Small Sci. 1(2), 2000026 (2020). https://doi.org/10.1002/smsc.202000026
  24. F. Zoller, S. Haringer, D. Bohm, J. Luxa, Z. Sofer et al., Carbonaceous oxygen evolution reaction catalysts: From defect and doping-induced activity over hybrid compounds to ordered framework structures. Small 17(48), e2007484 (2021). https://doi.org/10.1002/smll.202007484
  25. K. Choi, S. Kim, Theoretical study of oxygen reduction reaction mechanism in metal-free carbon materials: defects, structural flexibility, and chemical reaction. ACS Nano 16(10), 16394–16401 (2022). https://doi.org/10.1021/acsnano.2c05607
  26. A.N. Eledath, A. Edathiparambil Poulose, A. Muthukrishnan, O-functionalization of n-doped reduced graphene oxide for topological defect-driven oxygen reduction. ACS Appl. Nano Mater. 5(8), 10528–10536 (2022). https://doi.org/10.1021/acsanm.2c01852
  27. R. Rabeya, S. Mahalingam, A. Manap, M. Satgunam, M. Akhtaruzzaman et al., Structural defects in graphene quantum dots: a review. Int. J. Quantum Chem. 122(12), e26900 (2022). https://doi.org/10.1002/qua.26900
  28. Z.H. Sun, X. Zhang, X.D. Yang, W.N. Shi, Y.Q. Huang et al., Identification of a pyrone-type species as the active site for the oxygen reduction reaction. Chem. Commun. 58(64), 8998–9001 (2022). https://doi.org/10.1039/d2cc03093d
  29. Y. Li, Y. Tong, F. Peng, Metal-free carbocatalysis for electrochemical oxygen reduction reaction: activity origin and mechanism. J. Energy Chem. 48, 308–321 (2020). https://doi.org/10.1016/j.jechem.2020.02.027
  30. S. Liu, Y. Zhang, B. Ge, F. Zheng, N. Zhang et al., Constructing graphitic-nitrogen-bonded pentagons in interlayer-expanded graphene matrix toward carbon-based electrocatalysts for acidic oxygen reduction reaction. Adv. Mater. 33(42), e2103133 (2021). https://doi.org/10.1002/adma.202103133
  31. G. Gan, S. Fan, X. Li, J. Wang, C. Bai et al., Nature of intrinsic defects in carbon materials for electrochemical dechlorination of 1,2-dichloroethane to ethylene. ACS Catal. 11(22), 14284–14292 (2021). https://doi.org/10.1021/acscatal.1c03701
  32. A. Biswas, S. Kapse, R. Thapa, R.S. Dey, Oxygen functionalization-induced charging effect on boron active sites for high-yield electrocatalytic NH3 production. Nano-Micro Lett. 14(1), 214 (2022). https://doi.org/10.1007/s40820-022-00966-7
  33. J. Quílez-Bermejo, E. Morallón, D. Cazorla-Amorós, Metal-free heteroatom-doped carbon-based catalysts for ORR: a critical assessment about the role of heteroatoms. Carbon 165, 434–454 (2020). https://doi.org/10.1016/j.carbon.2020.04.068
  34. X.-K. Kong, C.-L. Chen, Q.-W. Chen, Doped graphene for metal-free catalysis. Chem. Soc. Rev. 43(8), 2841–2857 (2014). https://doi.org/10.1039/C3CS60401B
  35. T. Koretsune, S. Saito, Electronic structure of boron-doped carbon nanotubes. Phys. Rev. B 77(16), 165417 (2008). https://doi.org/10.1103/PhysRevB.77.165417
  36. V. Likodimos, S. Glenis, C. Lin, Electronic properties of boron-doped multiwall carbon nanotubes studied by Esr and static magnetization. Phys. Rev. B 72(4), 045436 (2005). https://doi.org/10.1103/PhysRevB.72.045436
  37. J. Zhang, X. Liu, R. Blume, A. Zhang, R. Schlögl et al., Surface-modified carbon nanotubes catalyze oxidative dehydrogenation of n-butane. Science 322(5898), 73–77 (2008). https://doi.org/10.1126/science.1161916
  38. W. Xia, C. Jin, S. Kundu, M. Muhler, A highly efficient gas-phase route for the oxygen functionalization of carbon nanotubes based on nitric acid vapor. Carbon 47(3), 919–922 (2009). https://doi.org/10.1016/j.carbon.2008.12.026
  39. S. Wu, L. Yu, G. Wen, Z. Xie, Y. Lin, Recent progress of carbon-based metal-free materials in thermal-driven catalysis. J. Energy Chem. 58, 318–335 (2021). https://doi.org/10.1016/j.jechem.2020.10.011
  40. K. Gong, F. Du, Z. Xia, M. Durstock, L. Dai, Nitrogen-doped carbon nanotube arrays with high electrocatalytic activity for oxygen reduction. Science 323, 760–764 (2009). https://doi.org/10.1126/science.1168049
  41. W. Wei, H. Liang, K. Parvez, X. Zhuang, X. Feng et al., Nitrogen-doped carbon nanosheets with size-defined mesopores as highly efficient metal-free catalyst for the oxygen reduction reaction. Angew. Chem. Int. Ed. 53, 1570–1574 (2014). https://doi.org/10.1002/anie.201307319
  42. H. Jiang, J. Gu, X. Zheng, M. Liu, X. Qiu et al., Defect-rich and ultrathin n doped carbon nanosheets as advanced trifunctional metal-free electrocatalysts for the Orr, OER and HER. Energy Environ. Sci. 12, 322–333 (2019). https://doi.org/10.1039/C8EE03276A
  43. Q. Lv, W. Si, J. He, L. Sun, C. Zhang et al., Selectively nitrogen-doped carbon materials as superior metal-free catalysts for oxygen reduction. Nat. Commun. 9, 3376 (2018). https://doi.org/10.1038/s41467-018-05878-y
  44. H. Xu, J. Yang, R. Ge, J. Zhang, Y. Li et al., Carbon-based bifunctional electrocatalysts for oxygen reduction and oxygen evolution reactions: optimization strategies and mechanistic analysis. J. Energy Chem. 71, 234–265 (2022). https://doi.org/10.1016/j.jechem.2022.03.022
  45. J. Quílez-Bermejo, E. Morallón, D. Cazorla-Amorós, On the deactivation of n-doped carbon materials active sites during oxygen reduction reaction. Carbon 189, 548–560 (2022). https://doi.org/10.1016/j.carbon.2021.12.086
  46. S. Park, J. Kim, K. Kwon, A review on biomass-derived n-doped carbons as electrocatalysts in electrochemical energy applications. Chem. Eng. J. 446, 137116 (2022). https://doi.org/10.1016/j.cej.2022.137116
  47. Y. Shen, Y. Li, G. Yang, Q. Zhang, H. Liang et al., Lignin derived multi-doped (N, S, Cl) carbon materials as excellent electrocatalyst for oxygen reduction reaction in proton exchange membrane fuel cells. J. Energy Chem. 44, 106–114 (2020). https://doi.org/10.1016/j.jechem.2019.09.019
  48. H.B. Yang, J. Miao, S.-F. Hung, J. Chen, H.B. Tao et al., Identification of catalytic sites for oxygen reduction and oxygen evolution in n-doped graphene materials: development of highly efficient metal-free bifunctional electrocatalyst. Sci. Adv. 2(4), e1501122 (2016). https://doi.org/10.1126/sciadv.1501122
  49. L. Chen, Y. Hernandez, X. Feng, K. Müllen, From nanographene and graphene nanoribbons to graphene sheets: chemical synthesis. Angew. Chem. Int. Ed. 5(31), 7640–7654 (2012). https://doi.org/10.1002/anie.201201084
  50. L. Xue, Y. Li, X. Liu, Q. Liu, J. Shang et al., Zigzag carbon as efficient and stable oxygen reduction electrocatalyst for proton exchange membrane fuel cells. Nat. Commun. 9, 3819 (2018). https://doi.org/10.1038/s41467-018-06279-x
  51. R. Panico, W. Powell, J.-C. Richer, A Guide to IUPAC Nomenclature of Organic Compounds: Recommendations 1993 (Blackwell Scientific Publications, Oxford, 1993)
  52. E.M. Adkins, J.H. Miller, Towards a taxonomy of topology for polynuclear aromatic hydrocarbons: linking electronic and molecular structure. Phys. Chem. Chem. Phys. 19(41), 28458–28469 (2017). https://doi.org/10.1039/c7cp06048c
  53. L. Zhi, K. Müllen, A bottom-up approach from molecular nanographenes to unconventional carbon materials. J. Mater. Chem. 18, 1472–1484 (2008). https://doi.org/10.1039/B717585J
  54. P. Puschnig, D. Lüftner, Simulation of angle-resolved photoemission spectra by approximating the final state by a plane wave: from graphene to polycyclic aromatic hydrocarbon molecules. J. Electron Spectros. Relat. Phenom. 200, 193–208 (2015). https://doi.org/10.1016/j.elspec.2015.06.003
  55. C. Hu, L. Dai, Doping of carbon materials for metal-free electrocatalysis. Adv. Mater. 31(7), 1804672 (2019). https://doi.org/10.1002/adma.201804672
  56. M. Pykal, P. Jurečka, F. Karlický, M. Otyepka, Modelling of graphene functionalization. Phys. Chem. Chem. Phys. 18(9), 6351–6372 (2016). https://doi.org/10.1039/C5CP03599F
  57. Y. Jia, L. Zhang, L. Zhuang, H. Liu, X. Yan et al., Identification of active sites for acidic oxygen reduction on carbon catalysts with and without nitrogen doping. Nat. Catal. 2(8), 688–695 (2019). https://doi.org/10.1038/s41929-019-0297-4
  58. H. Wu, C. Su, R. Tandiana, C. Liu, C. Qiu et al., Graphene-oxide-catalyzed direct CH−CH-type cross-coupling: the intrinsic catalytic activities of zigzag edges. Angew. Chem. Int. Ed. 57, 10848 (2018). https://doi.org/10.1002/anie.201802548
  59. S. Fujii, T. Enoki, Nanographene and graphene edges: electronic structure and nanofabrication. Acc. Chem. Res. 46(10), 2202–2210 (2013). https://doi.org/10.1021/ar300120y
  60. M. Li, B. Yin, C. Gao, J. Guo, C. Zhao et al., Graphene: preparation, tailoring, and modification. Exploration 3, 20210233 (2023). https://doi.org/10.1002/EXP.20210233
  61. Y. Jiao, Y. Zheng, M. Jaroniec, S.Z. Qiao, Origin of the electrocatalytic oxygen reduction activity of graphene-based catalysts: a roadmap to achieve the best performance. J. Am. Chem. Soc. 136(11), 4394–4403 (2014). https://doi.org/10.1021/ja500432h
  62. S. Lu, Y. Shi, W. Zhou, Z. Zhang, F. Wu et al., Dissolution of the heteroatom dopants and formation of ortho-quinone moieties in the doped carbon materials during water electrooxidation. J. Am. Chem. Soc. 144(7), 3250–3258 (2022). https://doi.org/10.1021/jacs.1c13374
  63. S. Lu, C. Cheng, Y. Shi, Z. Zhang, B. Zhang, Unveiling structure transformation and activity origin of the heteroatom-doped carbons for hydrogen evolution. Proc. Natl. Acad. Sci. 120(20), e2300549120 (2023). https://doi.org/10.1073/pnas.2300549120
  64. H. Li, F. Pan, C. Qin, T. Wang, K.J. Chen, Porous organic polymers-based single-atom catalysts for sustainable energy-related electrocatalysis. Adv. Energy Mater. 13(28), 2301378 (2023). https://doi.org/10.1002/aenm.202301378
  65. Z. Wang, M. Cheng, Y. Liu, Z. Wu, H. Gu et al., Dual-atomic-site catalysts for molecular oxygen activation in heterogeneous thermo-/electro-catalysis. Angew. Chem. Int. Ed. 62(22), e202301483 (2023). https://doi.org/10.1002/anie.202301483
  66. B.C. Smith, Fundamentals of Fourier Transform Infrared Spectroscopy, 2nd edn. (CRC Press, 2011). https://doi.org/10.1201/b10777
  67. E.K. Rideal, W.M. Wright, Clxxxiv—low temperature oxidation at charcoal surfaces. Part I. The behaviour of charcoal in the absence of promoters. J. Chem. Soc. Trans. 127, 1347 (1925). https://doi.org/10.1039/CT9252701347
  68. X. Guo, W. Qi, W. Liu, P. Yan, F. Li et al., Oxidative dehydrogenation on nanocarbon: revealing the catalytic mechanism using model catalysts. ACS Catal. 7(2), 1424–1427 (2017). https://doi.org/10.1021/acscatal.6b02936
  69. D.S. Su, S. Perathoner, G. Centi, Nanocarbons for the development of advanced catalysts. Chem. Rev. 113(8), 5782–5816 (2013). https://doi.org/10.1021/cr300367d
  70. Y. Lin, X. Sun, D.S. Su, G. Centi, S. Perathoner, Catalysis by hybrid sp2/sp3 nanodiamonds and their role in the design of advanced nanocarbon materials. Chem. Soc. Rev. 47, 8438–8473 (2018). https://doi.org/10.1039/C8CS00684A
  71. J.L. Figueiredo, M.F. Pereira, M.M. Freitas, J.J. Órfão, Characterization of active sites on carbon catalysts. Ind. Eng. Chem. Res. 46(12), 4110–4115 (2007). https://doi.org/10.1021/ie061071v
  72. J. Zhang, X. Wang, Q. Su, L. Zhi, A. Thomas et al., Metal-free phenanthrenequinone cyclotrimer as an effective heterogeneous catalyst. J. Am. Chem. Soc. 131(32), 11296–11297 (2009). https://doi.org/10.1021/ja9046735
  73. Y. Lin, Z. Liu, Y. Niu, B. Zhang, Q. Lu et al., Highly efficient metal-free nitrogen-doped nanocarbons with unexpected active sites for aerobic catalytic reactions. ACS Nano 13(12), 13995–14004 (2019). https://doi.org/10.1021/acsnano.9b05856
  74. A.D. Zdetsis, E.N. Economou, A pedestrian approach to the aromaticity of graphene and nanographene: Significance of huckel’s (4n+2)π electron rule. J. Phys. Chem. C 119(29), 16991–17003 (2015). https://doi.org/10.1021/acs.jpcc.5b04311
  75. J. Zhang, D. Su, A. Zhang, D. Wang, R. Schlögl et al., Nanocarbon as robust catalyst: mechanistic insight into carbon-mediated catalysis. Angew. Chem. Int. Ed. 46(38), 7319–7323 (2007). https://doi.org/10.1002/anie.200702466
  76. X. Guo, W. Qi, W. Liu, C. Liang, A. Zheng et al., Conjugated polymers with defined chemical structure as model carbon catalysts for nitro reduction. RSC Adv. 6(101), 99570–99576 (2016). https://doi.org/10.1039/C6RA18201A
  77. E. Louis, E. San-Fabián, G. Chiappe, J.A. Vergés, Electron enrichment of zigzag edges in armchair–oriented graphene nano–ribbons increases their stability and induces pinning of the fermi level. Carbon 154, 211–218 (2019). https://doi.org/10.1016/j.carbon.2019.07.102
  78. D. Guo, R. Shibuya, C. Akiba, S. Saji, T. Kondo et al., Active sites of nitrogen-doped carbon materials for oxygen reduction reaction clarified using model catalysts. Science 351(6271), 361–365 (2016). https://doi.org/10.1126/science.aad0832
  79. Y. Lin, Z. Liu, L. Yu, G.-R. Zhang, H. Tan et al., Overall oxygen electrocatalysis on nitrogen-modified carbon catalysts: Identification of active sites and in situ observation of reactive intermediates. Angew. Chem. Int. Ed. 60(6), 3299–3306 (2021). https://doi.org/10.1002/anie.202012615
  80. K. Takeyasu, M. Furukawa, Y. Shimoyama, S.K. Singh, J. Nakamura, Role of pyridinic nitrogen in the mechanism of the oxygen reduction reaction on carbon electrocatalysts. Angew. Chem. Int. Ed. 60(10), 5121–5124 (2021). https://doi.org/10.1002/anie.202014323
  81. R. Shibuya, T. Kondo, J. Nakamura, Bottom-up design of nitrogen-containing carbon catalysts for the oxygen reduction reaction. ChemCatChem 10(9), 2019–2023 (2018). https://doi.org/10.1002/cctc.201701928
  82. R.J. Kahan, W. Hirunpinyopas, J. Cid, M.J. Ingleson, R.A. Dryfe, Well-defined boron/nitrogen-doped polycyclic aromatic hydrocarbons are active electrocatalysts for the oxygen reduction reaction. Chem. Mater. 31(6), 1891–1898 (2019). https://doi.org/10.1002/cctc.201701928
  83. M. Wang, B. Wang, W. Song, X. Wang, X. Peng et al., Oxygen reduction activity of B←N-Containing organic molecule affected by asymmetric regulation. Small 18(3), 2105524 (2022). https://doi.org/10.1002/smll.202105524
  84. D. Li, B. Wang, X. Long, W. Xu, Y. Xia et al., Controlled asymmetric charge distribution of active centers in conjugated polymers for oxygen reduction. Angew. Chem. Int. Ed. 60(51), 26483–26488 (2021). https://doi.org/10.1002/anie.202109057
  85. H.W. Kim, M.B. Ross, N. Kornienko, L. Zhang, J. Guo et al., Efficient hydrogen peroxide generation using reduced graphene oxide-based oxygen reduction electrocatalysts. Nat. Catal. 1, 282–290 (2018). https://doi.org/10.1038/s41929-018-0044-2
  86. Z. Lu, G. Chen, S. Siahrostami, Z. Chen, K. Liu et al., High-efficiency oxygen reduction to hydrogen peroxide catalysed by oxidized carbon materials. Nat. Catal. 1(2), 156–162 (2018). https://doi.org/10.1038/s41929-017-0017-x
  87. G.-F. Han, F. Li, W. Zou, M. Karamad, J.-P. Jeon et al., Building and identifying highly active oxygenated groups in carbon materials for oxygen reduction to H2O2. Nat. Commun. 11(1), 2209 (2020). https://doi.org/10.1038/s41467-020-15782-z
  88. L. Yu, L. Tang, W. Guo, C. Li, D. Shin et al., Disclosing the natures of carbon edges with gradient nanocarbons for electrochemical hydrogen peroxide production. Matter 5(6), 1909–1923 (2022). https://doi.org/10.1016/j.matt.2022.04.010
  89. Y. Lin, K.-H. Wu, Q. Lu, Q. Gu, L. Zhang et al., Electrocatalytic water oxidation at quinone-on-carbon: a model system study. J. Am. Chem. Soc. 140(44), 14717–14724 (2018). https://doi.org/10.1021/jacs.8b07627
  90. Z. Gu, Y. Chen, Z. Wei, L. Qian, A.M. Al-Enizi et al., Precise tuning of heteroatom positions in polycyclic aromatic hydrocarbons for electrocatalytic nitrogen fixation. J. Colloid Interface Sci. 580, 623–629 (2020). https://doi.org/10.1016/j.jcis.2020.07.046
Read More
Author biographies are not available.
Download this PDF file
PDF
Statistic
Read Counter : 2203 Download : 1653

Most read articles by the same author(s)