电化学（中英文） ›› 2022, Vol. 28 ›› Issue (2): 2108501. doi: 10.13208/j.electrochem.210850
所属专题： “电催化和燃料电池”专题文章
王雪1,2, 张丽1, 刘长鹏1,2, 葛君杰1,2, 祝建兵1,2,*(
), 邢巍1,2,*()
收稿日期:2021-11-01
修回日期:2021-12-02
出版日期:2022-02-28
发布日期:2021-12-18
Xue Wang1,2, Li Zhang1, Chang-Peng Liu1,2, Jun-Jie Ge1,2, Jian-Bing Zhu1,2,*(), Wei Xing1,2,*()
Received:2021-11-01
Revised:2021-12-02
Published:2022-02-28
Online:2021-12-18
Contact:
*Tel: (86-431)85262147, E-mail:
摘要：
碱性介质中的氧还原反应是金属-空气电池和阴离子交换膜燃料电池的重要电化学过程。但是,其动力学缓慢,因而引起了对高效电催化剂的广泛研究。其中,非贵金属催化剂可有效地规避铂基催化剂成本和储量的问题,而备受关注。但其挑战在于将性能提高到可与Pt基催化材料媲美。鉴于非贵金属催化剂的组成和结构对催化性能有着至关重要的影响,精准地调控催化剂的结构有望消除非贵金属催化剂和商业铂基催化剂的活性差距。在该评述中,我们致力于总结通过结构调控来提升性能的研究进展。我们首先介绍了四种极具代表性的非贵金属催化剂,包括非金属碳基材料、金属化合物、石墨化碳层包覆金属颗粒、原子分散的金属-氮-碳材料,突出了催化活性位点和催化机理。随后,针对于这些催化剂,我们归纳了从微纳尺度到原子层面的结构调控策略,如分级多孔结构的设计、界面工程、缺陷工程以及原子对活性位点的构建。我们着重讨论了结构和性能之间的依赖关系。从加速传质、增加可及的活性位点数量、可调控的电子状态和多组分之间的协同效应,讨论了这些结构变化引起的活性改进的起源。最后,我们对该领域存在的挑战以及未来的前景进行了展望。
王雪, 张丽, 刘长鹏, 葛君杰, 祝建兵, 邢巍. 碱性介质中非贵金属氧还原催化剂的结构调控进展[J]. 电化学（中英文）, 2022, 28(2): 2108501.
Xue Wang, Li Zhang, Chang-Peng Liu, Jun-Jie Ge, Jian-Bing Zhu, Wei Xing. Recent Advances in Structural Regulation on Non-Precious Metal Catalysts for Oxygen Reduction Reaction in Alkaline Electrolytes[J]. Journal of Electrochemistry, 2022, 28(2): 2108501.
Table 1
Reaction equations of ORR in alkaline conditions.
| Mechanism | Overall reaction | ||
|---|---|---|---|
| Four-electron process | Dissociation pathway | O2 + 2* → 2O* 2O* + 2e- + 2H2O → 2OH* + 2OH- 2OH* + 2e- → 2OH- + 2* | O2 + 2H2O + 4e- → 4OH- |
| Associative pathway | O2 + * → O2* O2* + H2O + e- → OOH* + OH- OOH* + e- → O* + OH- O* + H2O + e- → OH* + OH- OH* + e- → OH- + * | ||
| Two-electron process | O2 + * → O2* O2* + H2O + e- → OOH* + OH- OOH* + e- → HO2- +* | O2 + H2O + 2e- → HO2- + OH- | |
Figure 1
(A) Illustration of the edge defect reconstruction; (B) The HAADF-STEM image of N-G. The nitrogen atoms are marked with the red circles; (C) Expanded image of the dotted box in (B) (‘5’ indicates the pentagons). Reproduced with permission of Ref. 24, copyright 2019 Springer Nature. (color on line)
Figure 2
(A) Schematic illustration showing the synthesis of N, S co-doped carbon catalysts; (B, C) Free-energy diagrams of the ORR mechanism at different electrode potentials (U) on (B) N doped carbon and (C) N, S co-doped carbon. The * denotes the free C site on doped carbon structure. Insets: the optimized structure of N doped and N, S co-doped carbon structure. The gray, blue and yellow balls denote C, N and S, respectively. Reproduced with permission of Ref. 34, copyright 2016 Royal Society of Chemistry. (color on line)
Figure 3
(A) Flow diagram for the synthesis processes of 3D N-GQDs/NiCo2S4/CC composite; (B) Durability testing curves in 0.1 mol·L-1 KOH; (C) Relative Gibbs free energy diagram of NiCo2S4 for the ORR at different potentials. Reproduced with permission of Ref. 54, copyright 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim. (color on line)
Figure 4
(A, B) Transmission electron microscopic images of Fe3C encapsulated in N-doped carbon nanotubes/carbon black composite; (C) Results of the DFT calculations. PDOS of the p orbitals of C atoms bonded to Fe in Fe3C@SWNT compared with that in pure SWNT; (D) ORR polarization plots after 20000 cycles in O2-saturated 0.1 mol·L-1 KOH. Reproduced with permission of Ref. 63, copyright 2015 Royal Society of Chemistry. (color on line)
Figure 5
(A) Schematic illustration for the formation of Fe-N-C catalysts using ZIF-8 as an active site host; (B) Aberration-corrected HAADF-STEM image of the isolated Fe atoms involved Fe/N-G-SAC catalyst; (C) Fourier transforms of k3-weighted Fe K-edge EXAFS data. Reproduced with permission of Ref. 81, copyright 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim. (color on line)
Figure 6
(A) Graphical illustration for the synthesis process of Fe/N-CNRs; (B) N2 adsorption-desorption results and (C) Pore diameter distribution results for Fe/N-CNRs, N-CNRs, and Fe/N-CNRs-NW; (D) E1/2 and kinetic current density (Jk)@0.85V results of these catalysts. Reproduced with permission of Ref. 79, copyright 2021 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim. (color on line）
Figure 7
(A) Synthetic scheme for the preparation of SA-Fe-Nx-MPCS catalyst; (B) Schematic illustration of the air electrodes and their SEM images; (C) COMSOL multiphysics modeling of O2 diffusion into the air electrode; (D) Polarization and power density curves of flow batteries with the prepared catalysts and Pt/C. Reproduced with permission of Ref. 80, copyright 2021 Elsevier. (color on line)
Figure 8
(A) Schematic illustration revealing the synthetic strategy of the TMs@NCx composite; (B) ORR polarization curves for TMs@NCx samples in O2-saturated 0.1 mol·L-1 KOH at scan rate of 5 mV·s-1 and rotation speed of 1600 r·min-1; (C) Jk of ORR at different potentials on different catalysts. Reproduced with permission of Ref. 70, copyright 2016 American Chemical Society. (color on line)
Figure 9
(A) Schematic illustration for the Ni doping strategy to regulate the interface structure of the as-derived catalysts; (B) RTEM image, and (C, D) FFT patterns derived from the regions of the areas 1 and 2 in (B). Reproduced with permission of Ref. 97, copyright 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim. (color on line)
Figure 10
(A-D) Various Fe cluster/Fe-N4 site configurations and the corresponding formation energy (Ef); (E) ORR Gibbs free energy diagrams on the edge and in-plane sites; (F) ORR polarization curves of the Fe/N-G-SAC, other Fe-based counterparts and the commercial Pt/C. Reproduced with permission of Ref. 81, copyright 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim. (color on line)
Figure 11
(A) Schematic illustration for the synthetic procedure of diatomic IrCo-N-C catalyst; (B, C) Partial density of states for Co-3d orbitals in (B) CoN4, (C) IrCoN5; (D) Fourier transformed extended X-ray adsorption fine structure (FT-EXAFS) spectra at Co K-edge; (E) The ORR polarization curves of IrCo-N-C, single-atom Co-N-C and Ir-N-C, and commercial Pt/C in 0.1 mol·L-1 KOH solution. Reproduced with permission of Ref. 103, copyright 2021 American Chemical Society. (color on line)
Table 2
The ORR performance and synthesis method of the representative NPMCs reported in literature.
| Sample | E1/2 (V vs. RHE) | Synthesis method |
|---|---|---|
| N-doping carbon[ | 0.853 | Template method |
| N, S co-doping carbon[ | 0.83 | Hummers’ method |
| N, S, O tri-doped carbon nanosheet[ | 0.86 | Template method |
| VACNTs-MnO2[ | / | Nebulized ethanol assisted infiltration and pyrolysis method |
| Mn@LaCoO3[ | 0.72 | Polyol-assisted solvothermal method |
| FeNiCo-P[ | 0.84 | Pyrolysis method |
| Co2P -Co, N, and P multi-doped carbon material[ | 0.843 | Phosphidation |
| C@CoCx[ | 0.8 | Solid-solid separation method |
| Fe3C@rGO[ | 0.8 | Pyrolysis method |
| FexN@N-doped carbon[ | 0.84 | NH3- histidine assisted method |
| NiCo-P[ | 0.82 | Electrospinning route |
| NiCo2S4@g-C3N4-CNT[ | 0.76 | Two-step hydrothermal |
| N-GQDs@NiCo2S4[ | 0.86 | Hydrothermal, sulfuration and electrophoretic deposition |
| Fe3C/N-doped carbon[ | 0.86 | Pyrolysis method |
| CoFe/N, P co-doped carbon nanovesicles[ | 086 | Impregnation and pyrolysis method |
| Co/N, S co-doped carbon[ | 0.85 | Two-step calcination methods |
| Pt1/FeOx[ | / | Pyrolysis method |
| Fe/N-CNRs[ | 0.9 | Pyrolysis method |
| SA-Fe-Nx-MPCS[ | 0.88 | Template method |
| Fe/N-G-SAC[ | 0.89 | Template method |
| Co-Nx-C[ | / | Template method |
| CoO@Mn3O4[ | / | Adsorption and reduction method |
| carbon-CoP[ | 0.81 | Phosphorization method |
| FexN[ | 0.89 | Pyrolysis method |
| CoO/CoxP[ | 0.86 | Phosphorization method |
| FexN@N-doped GO[ | / | Pyrolysis method |
| TiCoNx-rGO[ | 0.902 | Pyrolysis method |
| Co2N5[ | 0.79 | Pyrolysis method |
| FeCoN5[ | 0.86 | Pyrolysis method |
| IrCoN5[ | 0.911 | ZIFs-assisted host-guest method |
| FeNi-SAs@NC[ | 0.907 | Pyrolysis method |
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