用于氧还原电催化的Fe-M-N-C基双原子催化剂的研究进展

doi:10.1016/S1872-2067(23)64538-3

催化学报 ›› 2023, Vol. 54: 56-87.DOI: 10.1016/S1872-2067(23)64538-3

用于氧还原电催化的Fe-M-N-C基双原子催化剂的研究进展

樊哲琛^a, 万浩^a, 余浩^a, 葛君杰^a^,^b^,^*()

^a中国科学技术大学化学与材料科学学院应用化学系, 安徽合肥230026
^b中国科学院洁净能源创新研究院, 辽宁大连116023

收稿日期:2023-06-28 接受日期:2023-10-08 出版日期:2023-11-18 发布日期:2023-11-15
通讯作者: *电子信箱: gejunjie@ustc.edu.cn (葛君杰).
基金资助:
国家重点研发计划(2022YFB4004100);国家自然科学基金(U22A20396);安徽省自然科学基金(2208085UD04);中国科学院低碳转化科学与工程重点实验室开放课题资助项目(KLLCCSE-202202);中国科学院洁净能源创新研究院合作基金(DNL202010)

Rational design of Fe-M-N-C based dual-atom catalysts for oxygen reduction electrocatalysis

Zhechen Fan^a, Hao Wan^a, Hao Yu^a, Junjie Ge^a^,^b^,^*()

^aSchool of Chemistry and Materials Science, University of Science and Technology of China, Hefei 230026, Anhui, China
^bDalian National Laboratory for Clean Energy, Dalian 116023, Liaoning, China

Received:2023-06-28 Accepted:2023-10-08 Online:2023-11-18 Published:2023-11-15
Contact: *E-mail: gejunjie@ustc.edu.cn (J. Ge).
About author:Junjie Ge received her Ph.D. in physical chemistry from Chinese Academy of Sciences in 2010. She worked at University of South Carolina and University of Hawaii as a postdoc fellow for almost 5 years. She joined Changchun Institute of Applied Chemistry in 2015 as a professor and then joined University of Science and Technology of China in 2022 as a professor. Her research interests comprehend fuel cells, nanoscience, catalysis, and electrochemistry. She has published 100+ peer-reviewed papers on the highly reputable international journals including Nat. Sci. Rev., Joule, Chem, PNAS, J. Am. Chem. Soc., Nat. Commun., Angew. Chem. Int. Ed., Sci. Bull., Energy Environ. Sci., with several of them are ranked as highly cited papers. She serves actively as a referee for journals in ACS, Wiley, RSC, Science Direct, and several Chinese journals.
Supported by:
National Key R&D Program of China(2022YFB4004100);National Natural Science Foundation of China(U22A20396);Natural Science Foundation of Anhui Province(2208085UD04);Key Laboratory of Low-Carbon Conversion Science & Engineering, Shanghai Advanced Research Institute, Chinese Academy of Sciences(KLLCCSE-202202);Dalian National Laboratory for Clean Energy(DNL)CAS, the Research Innovation Fund(DNL202010)

摘要/Abstract

摘要：

实现质子交换膜燃料电池(PEMFC)的商业化应用亟需开发出低成本的高效氧还原(ORR)电催化剂以替代昂贵的Pt基材料. 过去十余年, 研究人员对由M-N_x活性位点和富缺陷碳质基底组成的热解M-N-C基单原子催化剂进行了深入的研究, 以期进一步提高催化剂的性能并降低成本. 其中, Fe-N-C基单原子催化剂表现出了较好的催化性能和巨大的应用潜力. 近年来人们发现, 在单原子催化剂中引入另一种金属原子组成的双原子催化剂具有特殊的几何构型和电子结构, 有利于反应过程中原子间相互作用, 使催化性能进一步提高. 其中, 在Fe-N-C基催化剂中引入另一种金属原子组成的Fe-M-N-C双原子催化剂(M代表金属)可以进一步激发Fe-N-C催化剂的本征活性, 相关研究也吸引了越来越多的关注.

本文综述了Fe-M-N-C基双原子催化剂催化ORR过程的研究进展. 首先, 讨论了双原子催化剂催化ORR的机制, 其中引入的第二种金属原子通过协同和/或调制效应发挥作用. 其后, 系统总结了Fe-M-N-C的合成方法、表征技术和计算方法, 以进一步推动双原子催化剂的研究. 再后, 根据金属原子之间的相互作用, 将双原子催化剂分为Marriage型和Conjunct型. 最后, 结合双原子位点的原子构型详细讨论了不同双原子催化剂的作用机制: 包括提供额外催化位点、改变吸附构型、调节电子结构等.

本文还对Fe-M-N-C基双原子催化剂面临的主要挑战和发展机遇进行了总结, 并对未来的研究方向进行了展望. 一些关键的发展方向应该得到充分的关注和发展, 包括Fe基双原子位点的精准合成、双原子位点的可靠识别、对催化机理的深入认识、Fe基催化剂在酸性环境中的稳定性以及具有最佳活性的双原子位点构型. 综上, 本文对Fe-M-N-C基双原子催化剂研究现状进行了系统的总结, 希望为未来理性设计催化剂提供一定的参考.

关键词: 氧还原反应, 铁基催化剂, 双原子催化剂, 催化活性, 原子构型

Abstract:

Fe-N-C based single-atom catalysts (SACs) with isolated Fe atoms dispersed on nitrogen-doped carbon matrix have achieved sustained attention for oxygen reduction reaction due to their great potential in replacing the Pt based noble catalysts in terms of catalytic activity. To further trigger the intrinsic activity of Fe-N-C, Fe based dual-atom catalysts (DACs, i.e., Fe-M-N-C) have been intensively studied, which confer the catalysts with readily tunable geometric configurations, electronic structures, thereby tailored catalytic properties. In this review, current progress on the rational design of Fe-M-N-C based DACs for enhanced oxygen reduction catalysis is summarized. Firstly, the ORR mechanisms on DACs are discussed where the second metal atoms can function through synergistic effect and/or modulation effect to promote the intrinsic catalytic activity. Moreover, the currently available synthetic approaches, characterization techniques and computational methods are systematically reviewed to aid the investigation of DACs. Then, DACs are classified into marriage-type and conjunct-type based on the interaction between metal atoms, whose properties are discussed at length with the atomic configuration. At last, the main challenges of Fe-M-N-C based DACs are summarized and some appealing directions towards highly efficient and stable energy applications are provided for their further enhancement.

Key words: Oxygen reduction reaction, Fe based catalyst, Dual-atom catalyst, Catalytic activity, Atomic configuration

樊哲琛, 万浩, 余浩, 葛君杰. 用于氧还原电催化的Fe-M-N-C基双原子催化剂的研究进展[J]. 催化学报, 2023, 54: 56-87.

Zhechen Fan, Hao Wan, Hao Yu, Junjie Ge. Rational design of Fe-M-N-C based dual-atom catalysts for oxygen reduction electrocatalysis[J]. Chinese Journal of Catalysis, 2023, 54: 56-87.

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图/表 27

Fig. 1. A timeline of development of Fe-M-N-C based DACs for ORR. (a) Reprinted with permission from Ref. [61]. Copyright 2011, American Chemical Society. (b) Reprinted with permission from Ref. [62]. Copyright 2007, American Association for the Advancement of Science. (c) Reprinted with permission from Ref. [64]. Copyright 2014, American Chemical Society. (d) Reprinted with permission from Ref. [65]. Copyright 2017, American Chemical Society. (e) Reprinted with permission from Ref. [67]. Copyright 2019, American Chemical Society. (f) Reprinted with permission from Ref. [70]. Copyright 2023, American Chemical Society.

Fig. 2. Overview of topics about Fe-M-N-C based DACs for ORR.

Fig. 3. Schematic depiction of possible ORR mechanisms.

Fig. 4. Schematic diagram of possible adsorption configurations of O2 at single-atom site and dual-atom site. Blue and purple represent Fe and M metal atoms, and red represents the adsorbed O2.

Fig. 5. (a) The two-step synthesis process of Fe2-N-C. Reprinted with permission from Ref. [66]. Copyright 2019, Elsevier. (b) The synthesis process of DACs via a macrocyclic precursor-mediated encapsulation-pyrolysis method. Reprinted with permission from Ref. [70]. Copyright 2023, American Chemical Society.

Fig. 6. (a) The fabrication process of the planar-like Fe2N6 structure supported on carbon support. Reprinted with permission from Ref. [68]. Copyright 2019, American Chemical Society. (b) Fe10 cluster with atomically dispersed Rh atom, and the formation of Rh-Fe paired atoms. Reprinted with permission from Ref. [115]. Copyright 2020, John Wiley and Son.

Fig. 8. (a) The synthesis process of Mn-Fe-N/S@mC catalysts based on the self-assembly of colloidal nanocrystals. Reprinted with permission from Ref. [117]. Copyright 2017, Elsevier. (b) The preparation of Fe-N-HCM and FeCo-N-HCN. Reprinted with permission from Ref. [118]. Copyright 2021, John Wiley and Son.

Fig. 9. (a) Aberration-corrected (AC)-HAADF-STEM image of Fe2-N6-C-o, and the corresponding yellow and red patterns represent the single and bimetallic Fe pairs, respectively. (b) Statistical study of the single and dual Fe sites and the Fe-Fe distance in Fig. (e). (c) HAADF-STEM image and elemental mappings of Fe2-N6-C-o. Reprinted with permission from Ref. [120]. Copyright 2022, American Chemical Society. (d) HAADF-STEM image of Fe-N4/Pt-N4@NC. (e) Magnified HAADF-STEM images of Fe-N4/Pt-N4@NC, and the corresponding dashed rectangles represents the atomically dispersed Fe atoms and Pt atoms. (f) The average intensity profiles of Fe/Pt atoms (indicated by dashed rectangles). Reprinted with permission from Ref. [84]. Copyright 2021, John Wiley and Son. (g) Magnified HAADF-STEM images of the (Fe,Co)/CNT, showing that Fe-Co dual sites are dominant in the (Fe,Co)/CNT. (h) The EEL spectrum recorded from the red rectangle in (g), indicating that Fe, Co is coordinated with N at the atomic scale. (i) Corresponding EELS mapping images of Co, Fe and N. Reprinted with permission from Ref. [71]. Copyright 2018, RSC Publishing.

Fig. 10. (a) Fe K-edge XANES spectra of the (Fe,Co)/CNT. (b) Fourier transformed (FT) k3-weighted χ(k)-function of the EXAFS spectra for the Fe K-edge of the (Fe,Co)/CNT. (c) The corresponding Fe K-edge EXAFS fitting curves of the (Fe,Co)/CNT. (d) Proposed architecture of Fe-Co dual sites. Reprinted with permission from Ref. [71]. Copyright 2018, RSC Publishing.

Fig. 11. (a) Experimental 57Fe M?ssbauer transmission spectra measured for (Fe,Co)/N-C, and corresponding fitting results. Reprinted with permission from Ref. [65]. Copyright 2021, American Chemical Society. 57Fe M?ssbauer spectra of (b) NCAG/Fe-Cu and (c) NCAG/Fe. Reprinted with permission from Ref. [105]. Copyright 2021, John Wiley and Son.

Fig. 12. Operando XANES spectra (a) and corresponding FTs (b) of Fe K-edge EXAFS oscillations of planar-like Fe2N6 structure at different applied potentials in 0.5 mol L-1 H2SO4. Reprinted with permission from Ref. [68]. Copyright 2020, Elsevier. Fe K-edge in situ XANES and the first-derivative of XANES spectra in the left figure for FeNx/C (c,e) and FeCoNX/C (d,f). Reprinted with permission from Ref. [67]. Copyright 2021, American Chemical Society.

Fig. 13. In-situ Raman spectra with applied potentials during the ORR process in (a) alkaline and (b) acidic solutions. Reprinted with permission from Ref. [92]. Copyright 2022, Elsevier. (c) In-situ Raman characterizations of Ni66Fe34-NC in O2-saturated 0.1 mol L-1 KOH. Reprinted with permission from Ref. [76]. Copyright 2021, Elsevier.

Fig. 14. Schematic of widely used computational methods for the rational design of DACs.

Fig. 15. (a) HAADF-STEM images and corresponding elemental mappings for FeCo2-NPC-900. (b) LSV curves FeCox-900 in O2-saturated 0.1 mol L-1 KOH solution. (c) LSV curves for FeCox-900 in O2-saturated 0.1 mol L-1 HClO4 solution. Reprinted with permission from Ref. [149]. Copyright 2017, John Wiley and Son. (d) HAADF-STEM image of Mn-Fe-N/S@mC. (e) Theoretical model of catalyst comprising Fe-N4 and Mn-N2S2 dual-metal sites. (f) The calculated free energy pathways of ORR on Mn-Fe-N/S@mC and Fe-N/S@mC. Reprinted with permission from Ref. [76]. Copyright 2020, Elsevier. (g) Reaction between ROS and ABTS (chemical probe); and photographs showing the color change of the solution after the Fenton reaction. (h) UV-vis absorption spectra of 0.1 mol L-1 HClO4 solutions including ABTS, H2O2 and/or catalysts. (i) The detected gas generation from H2O2 solution decomposition over Fe,Ce-N-C catalysts, or Fe-N-C catalyst. Inset presents the corresponding TOF values calculated with Fe,Ce-N-C, Fe-N-C, and Ce-N-C. Reprinted with permission from Ref. [151]. Copyright 2023, Elsevier.

Table 1 Summery of active sites and function of reported marriage-type DACs.

Catalyst	Active site	Function of another atom	Ref.
FeCo₂-NPC-900	FeN_x+CoN_x	synergistically catalyzing ORR	[149]
Fe,Mn-N/C	FeN₄+MnN₄	synergistically catalyzing ORR	[150]
Mn-Fe-N/S@mC	FeN₄+MnN₂S₂	synergistically catalyzing ORR	[76]
Fe/Ni(1:3)-NG	FeN₄+NiN₄	catalyzing OER	[101]
Ni-N₄/GHSs/Fe-N₄	FeN₄+NiN₄	catalyzing OER	[102]
Fe,Ce-N-C	FeN₄+CeN₄	catalyzing radical scavenging reaction	[151]

Fig. 16. (a-c) The k3-weighted Fourier-transform experimental Fe K-edge EXAFS spectrum (black line) and the fitting curve (red line) of Fe2-N-C (a), Fe1-N-C (b), and Fe3-N-C (c). The insets of show the optimized structural model. (d) LT-FTIR spectra after O2 adsorption on Fe1-N-C, Fe2-N-C, and Fe3-N-C. The optimized adsorption configurations, adsorption energies (EO2) and O-O bond lengths (LO-O) for O2 molecules on Fe1-N-C (e), Fe2-N-C (f), and Fe3-N-C (g). (h) ORR polarization curves in O2-saturated 0.5 mol L-1 H2SO4 solution. (i) ORR durability tests of Fe2-N-C after 5000, 10000, and 20000 cycles at an accelerated sweep rate of 50 mV s-1 at 0.6-1.0 V. Reprinted with permission from Ref. [66]. Copyright 2019, Elsevier. (j) Fe-Fe shell length calculated from operando EXAFS spectra. Inset: deductive oxygenated intermediates adsorption state on the planar-like Fe2N6 structure. (k) Proposed ORR reaction pathways on the planar-like Fe2N6 structure. (l) ORR polarization curves of isolated FeN4, planar-like Fe2N6 structure and Fe-N nanoparticle catalysts in O2-saturated 0.5 mol L-1 H2SO4 solution. Reprinted with permission from Ref. [68]. Copyright 2020, Elsevier.

Fig. 17. (a) Illustration of proposed various structures. (b) Proposed ORR mechanism on 2L-Up sites. (c) Gibbs free energy diagrams at 1.23 V. (d) Calculated charge density differences for 2L-Up and FeN4. The charge accumulation and depletion are colored in cyan and yellow. (e) LSV curves of Fe(Zn)-N-C and reference samples measured with RRDE obtained in O2 saturated 0.1 mol L-1 HClO4. (f) The durability tests of Fe(Zn)-N-C. Reprinted with permission from Ref. [154]. Copyright 2020, John Wiley and Son.

Table 2 Summery of active sites, activity and durability of reported homonuclear DACs.

Catalyst	Active site	Performance		Durability test ∆E_1/2 (cycle number)	Ref.
Catalyst	Active site	E_1/2 (V)	Electrolyte	Durability test ∆E_1/2 (cycle number)	Ref.
Fe₂-N-C	Fe₂N₆	0.78	0.5 mol L^-1 H₂SO₄	20 mV (20k)	[66]
Fe₂N₆	Fe₂N₆	0.84	0.5 mol L^-1 H₂SO₄	24 mV (10k)	[68]
Fe(Zn)-N-C	HO-FeN₄-O-FeN₄-OH	0.83	0.1 mol L^-1 HClO₄	14 mV (10k)	[154]
Fe2@PDA-ZIF-900	Fe₂N₆	0.816	0.5 mol L^-1 H₂SO₄	—	[155]

Fig. 18. (a) Counter plot of ηORR versus the Fe-M distance and d electrons of M. (b) The structure of FeMN6-DAC and FeMN8-DAC. (c) The spatial spin density of FeNiN6-DAC. (d) Side view of charge transfer within the system of FeNiN6-DAC. Reprinted with permission from Ref. [94]. Copyright 2023, Elsevier. (e) Linear correlation between the magnetic moment on Fe and the ORR activity of the eight configurations with two metal atoms. The atomic structures of each configuration are shown with their respective Fe-Cu interatomic distance. Reprinted with permission from Ref. [120]. Copyright 2021, American Chemical Society. The free energy diagrams of ORR and OER on mode 1 (f), model 2 (g), model 3 (h) of FeCoN6 and Fe-N-C (Co-N-C) (i) at 0 V. Reprinted with permission from Ref. [160]. Copyright 2020, Elsevier.

Fig. 19. (a) Proposed model of Fe-Co dual sites. (b) RDE polarization curves of Pt/C, Co SAs/N-C, Fe SAs/N-C, and (Fe,Co)/N-C in O2-saturated 0.1 mol L-1 HClO4. (c) DFT calculated energies of intermediates and transition states in mechanism of ORR at (Fe,Co)/N-C. Reprinted with permission from Ref. [65]. Copyright 2017, American Chemical Society. (d) Top and front views for the different adsorption models of OO* on the CuN4, CuCuN6, FeCuN6, FeN4, and FeFeN6. (e) The formation energy of OO* for five different models. (f) The Gibbs free energy diagram for ORR on different models at 0 V. Reprinted with permission from Ref. [78]. Copyright 2021, John Wiley and Son. (g) The cleavage of adsorbed OOH* on FeMnN6 site. The adsorbed OOH* in the “laying down” configuration, the transition state and the split OOH*. Reprinted with permission from Ref. [83]. Copyright 2022, John Wiley and Son.

Fig. 20. (a) The Fe K-edge EXAFS fitting curves and atomic configuration of Fe/Mn-N-C. ORR free energy diagrams for graphite, Fe-N-C, Mn-N-C, Fe/Mn-N-C (FeNx site), and Fe/Mn-N-C (MnNx site) at 0 V (b), 1.23 V (c). (d) Scheme of cascade mechanism on the FeNx site and MnNx site. Reprinted with permission from Ref. [163]. Copyright 2021, Elsevier. (e) The synthesis procedure and active sites of Fe-Zn@SNC. (f) Pathways and free energy diagrams of Fe-Zn@SNC with different Fe-Zn distances. (g) Overpotential of Fe-Zn@SNC models with different Fe-Zn distances. Barder charge of Fe-Zn@SNC models with Fe-Zn distances of 3.16 (h) and 2.46 ? (i). (j) Total charge transfer between O2* and Fe-Zn bridge site of three Fe-Zn@SNC models. (k) LSV curves in O2-saturated 0.5 mol L-1 H2SO4. (l) Stability of RDE polarization curves of Fe-Zn@SNC before and after 2000 potential cycles. Reprinted with permission from Ref. [80]. Copyright 2023, John Wiley and Son.

Fig. 21. (a) Calculating models of FeN4CuN4, FeN4FeN4, CuN4CuN4, FeN4 and CuN4. (b) ELF images of different models, blue represents the poor-electron region and red represents the rich-electron region. (c) O2 adsorption model and relative Ead. (d) PDOS images of Fe 3d in different models with the O 2p orbit. (e) Free energy diagram for the ORR with different models. (f) LSV curves for the ORR on different samples in O2-saturated 0.5 mol L-1 H2SO4 solution. Reprinted with permission from Ref. [164]. Copyright 2020, RSC Publishing. (g) O2 adsorption models of Fe-N4 and Fe-N4/Pt-N4. (h) Calculated projected density of states of Fe-N4/Pt-N4 after OOH* adsorption. (i) Calculated projected density of states of and Fe-N4/Pt-N4 after OH* adsorption. σ and π represent the bonding molecular orbitals between d orbital of Fe and p orbital of O. σ* and π* represent the antibonding molecular orbitals. Reprinted with permission from Ref. [75]. Copyright 2020, John Wiley and Son.

Fig. 22. (a) Illustration of atomic configurations of Fe-N4, Co2-N6, and Co2/Fe-N10. (b) The projected density of states (PDOS) of Fe-d orbitals in Fe-N4 and Co2/Fe-N10. (c) Free energy diagrams for Fe-N4 site in Co2/Fe-N1, Fe-N4, and Co2-N6 at 0 and 1.23 V. Reprinted with permission from Ref. [167]. Copyright 2021, John Wiley and Son. (d) Optimal configurations of single FeN4 sites in the basal plane (Fe1-1) (i) and at the nanopore (Fe1-2) (ii), and adjacent bimetal sites of Fe1/Fe1-1 (iii), Cu1/Fe1-1 (iv), Fe1/Fe1-2 (v) and Cu1/Fe1-2 (vi). (e) Magnetic moment and ΔGOH*, inset: their correlation for different models. (f) Free energy diagrams of the different models at their respective limiting potentials. (g) Fe 3d DOS of Fe1/Fe1-2 and Cu1/Fe1-2. (h) DOS of the Fe 3d orbitals in Cu1/Fe1-2. Reprinted with permission from Ref. [105]. Copyright 2022, John Wiley and Son.

Table 3 Summery of active sites, activity and durability of reported heteronuclear. DACs.

Catalyst	Active site	Interatomic distance (Å)	Performance		Durability test ∆E_1/2 (Cycle number)	Ref.
Catalyst	Active site	Interatomic distance (Å)	E_1/2 (V)	Electrolyte	Durability test ∆E_1/2 (Cycle number)	Ref.
FeNiN₈-DAC	FeN₄-NiN₄	7.68 *	0.84	0.5 mol L^-1 H₂SO₄	—	[94]
(Fe,Co)/N-C	FeCoN₆	2.50	0.863	0.1 mol L^-1 HClO₄	~0 mV (50k)	[75]
f-FeCoNC900	FeCoN₆	2.56	0.81	0.1 mol L^-1 HClO₄	—	[70]
Fe, Co SAs-PNCF	FeCoN₆	2.30	0.78	0.1 mol L^-1 HClO₄	~0 mV (5k)	[92]
Fe-Zn@SNC	FeZnN₅S	2.98	0.86	0.5 mol L^-1 H₂SO₄	25 mV (2k)	[80]
Fe/Ni-N_x/OC	FeN₄-NiN₄	—	0.84	0.1 mol L^-1 HClO₄	~0 mV (5k)	[75]
Co₂/Fe-N@CHC	FeN₄-Co₂N₆	2.41 (Co-Co)	0.812	0.1 mol L^-1 HClO₄	9 mV (5k)	[167]
Fe,Mn/N-C	FeMnN₆	2.5	0.804	0.1 mol L^-1 HClO₄	18 mV (8k)	[69]
FeCe-SAD/HPNC	FeN₄-CeN₆	3.77	0.81	0.1 mol L^-1 HClO₄	—	[168]
Fe/Zn-N-C	FeZnN₆	2.36	0.808	0.1 mol L^-1 HClO₄	28 mV (5k)	[171]
FeCoN₅P₁/C	FeCoN₅P	2.2	0.771	0.5 mol L^-1 H₂SO₄	—	[175]
FeCoN_x/C	FeCoN₅-OH	2.15	0.86	0.1 mol L^-1 HClO₄	13 mV (5k)	[67]

Fig. 23. (a) H2O2 reduction polarization curves for Fe DACs and reference samples. Gibbs free energy diagram of the Fenton-like (b) and hydrogen peroxide reduction reaction (HPRR) (c) processes. Reprinted with permission from Ref. [70]. Copyright 2023, American Chemical Society. Calculated free energies required for two-step protonation: ΔG1*H (d) and ΔG2*H (e) for Fe/M-N-C. (f) Protonation diagram of Fe/Zn-N-C. (g) Schematic illustration of the protonation process. Reprinted with permission from Ref. [171]. Copyright 2022, RSC publishing.

Fig. 24. (a) Geometric structure of M-N-C SACs. Reprinted with permission from Ref. [10]. Copyright 2021, John Wiley and Son. (b) Illustration of the FeCoN6 site with P doping in FeCo-NPC. (c) Free energy diagram for the OER and ORR processes of the FeCo-NPC, FeCo-NC, Fe-NPC and Co-NPC at 1.23 V. Reprinted with permission from Ref. [176]. Copyright 2023, Elsevier. (d) Schematic of FeCoN5-OH site. (e) Gibbs free energy diagrams at 1.23 V on CoN4, FeN4, and FeCoN5-OH sites. (f) Proposed ORR mechanism on the FeCoN5-OH site. Reprinted with permission from Ref. [67]. Copyright 2019, American Chemical Society.

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用于氧还原电催化的Fe-M-N-C基双原子催化剂的研究进展

Rational design of Fe-M-N-C based dual-atom catalysts for oxygen reduction electrocatalysis

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