Advances in spin regulation of M-N-C single-atom catalysts and their applications in electrocatalysis

doi:10.1016/S1872-2067(24)60204-4

Chinese Journal of Catalysis ›› 2025, Vol. 69: 17-34.DOI: 10.1016/S1872-2067(24)60204-4

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Advances in spin regulation of M-N-C single-atom catalysts and their applications in electrocatalysis

Jiayi Cui^a^,^b, Xintao Yu^a^,^b, Xueyao Li^a^,^b, Jianmin Yu^a^,^b, Lishan Peng^a^,^b^,^*(), Zidong Wei^c^,^*()

^aKey Laboratory of Rare Earths, Ganjiang Innovation Academy, Chinese Academy of Sciences, Ganzhou 341119, Jiangxi, China
^bSchool of Rare Earths, University of Science and Technology of China, Hefei 230026, Anhui, China
^cNational Key Laboratory of Special Chemical Power Sources, National-Municipal Joint Engineering Laboratory for Chemical Process Intensification and Reaction, School of Chemistry and Chemical Engineering, Chongqing University, Chongqing 400044, China

Received:2024-11-10 Accepted:2024-11-14 Online:2025-02-18 Published:2025-02-10
Contact: *E-mail: lspeng@gia.cas.cn (L. Peng), zdwei@cqu.edu.cn (Z. Wei).
About author:Lishan Peng (Ganjiang Innovation Academy, Chinese Academy of Sciences) obtained his B.S. and Ph.D. degrees in 2014 and 2019, respectively, at Chongqing University. Subsequently, he worked as a postdoctoral researcher at Westlake University, the University of Auckland (New Zealand) and the Technical Institute of Physics and Chemistry, Chinese Academy of Sciences. His research interests include the design and theoretical study of advanced electrocatalysts for energy storage and conversion. He has coauthored more than 80 peer-reviewed papers with citation over 5000 times.
Zidong Wei (School of Chemistry and Chemical Engineering, Chongqing University) received Bachelor degree from Shaanxi University of Science and Technology (1984), and Ph.D. degree from Tianjin University (1994). He has been in the field of electrochemical catalysis for more than 30 years and has published more than 300 papers with citation over 22000 times. He has been the Chief Scientist of the National Key Research and Development Program and the Chief Scientist of the National Natural Science Foundation. He edited or participated in the compilation of “Electrochemical Catalysis”, “Chemical Process Intensification”, “Electrocatalysis”, “Electrocatalytic Oxygen Reduction Reaction” and other books. He won the first, second and third prizes of provincial and ministerial level natural sciences and technological progress once each. He is a council member in the Chemical Industry and Engineering Society of China, and Chinese Chemical Society.
Supported by:
National Natural Science Foundation of China(22209186);National Natural Science Foundation of China(22479149);Self-deployed Projects of Ganjiang Innovation Academy, CAS(E355F006);Natural Science Foundation of Jiangxi Province(20242BAB23016);"Double Thousand Plan" of Jiangxi Province(jxsq2023101056);Key Research and Development Program of Jiangxi Province(20223BBG74004);Key Research and Development Program of Jiangxi Province(20232BBG70003);Youth Innovation Promotion Association, Chinese Academy of Sciences(2023343)

Abstract

Abstract:

To enhance the efficiency of green energy harvesting and pollutant degradation, significant efforts are focused on identifying highly effective catalysts. Metal-nitrogen-carbon single-atom catalysts (M-N-C SACs) have emerged as pivotal in catalysis due to their unique geometric structures, electronic states, and catalytic capabilities. Notably, the incorporation of magnetic elements at the active centers of these single-atom catalysts has garnered attention for their role in efficient electrochemical conversions. The orientation of spin states critically influences the adsorption and formation of reactants and intermediates, making the precise control of spin alignment and magnetic moments essential for reducing energy barriers and overcoming spin-related limitations, thereby enhancing catalytic activity. Thus, understanding the catalytic role of spin and modulating spin density at M-N-C single-atom centers holds profound fundamental and technological significance. In this review, we elucidate the fundamental mechanisms governing spin states and its influence in electrocatalysis. We then discuss various strategies for adjusting the spin states of active centers in the M-N-C SACs and the associated characterization techniques. Finally, we outline challenges and future perspectives of spin regulation for high-performance catalysts. This review provides deep insights into the micro-mechanisms of catalytic phenomena and offers a roadmap for designing spin-regulated catalysts for advanced energy applications.

Key words: Electrocatalysis, M-N-C materials, Single-atom catalyst, Electron spin effect, Spin regulation

Jiayi Cui, Xintao Yu, Xueyao Li, Jianmin Yu, Lishan Peng, Zidong Wei. Advances in spin regulation of M-N-C single-atom catalysts and their applications in electrocatalysis[J]. Chinese Journal of Catalysis, 2025, 69: 17-34.

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Figures/Tables 10

Fig. 1. Regulation strategies and characterization methods for spin state of SACs.

Fig. 2. (a) Molecular orbital diagram of triplet and singlet oxygen. (b) Distinctive reshaping of the wavefunction for the 3Σg? (left) states and 1Δg (right). Because of the Fermi hole that mitigates electronic repulsions; unpaired electrons do not share the center of the 3Σg? O2 molecule. Therefore, triplet oxygen (yellow shading, left) is much more stable than singlet oxygen (blue shading, right). Reprinted with permission from Ref. [36]. Copyright 2021, The Authors. (c) Calculated PDOS diagrams for Co(OH)2, Co3(SOH)x, and Co3S4 and the corresponding magnetic moments of O2 excited via the magnetization effect of the catalysts. Reprinted with permission from Ref. [45]. Copyright 2017, American Chemical Society.

Fig. 3. (a) Crystal field splitting of d orbitals in an octahedral structure. Red and blue spheres represent O and 3d metal atoms, respectively. Electron configurations of Co3+ in different orbitals under low-spin (b), intermediate-spin (c) and high-spin (d) states. Reprinted with permission from Ref. [52]. Copyright 2023, Wiley-VCH GmbH. (e) The relationship of the ORR overpotential versus ?G*OOH for all the carbon active sites with joint participation of the charge, spin and ligand effects. The distribution of ?G*OOH for all the carbon active sites with separate participation of the spin density effect (f). Reprinted with permission from Ref. [54]. Copyright 2021, The Authors.

Fig. 4. (a) The proposed ORR mechanism for the Fe1-N4SC. (b) Content of different Fe moieties of the three catalysts. (c) LSV curves for the catalysts acquired in O2-saturated 0.1 mol L?1 KOH solution on a rotating ring disc electrode (RRDE) at a rotation speed of 1600 r min?1 and a scan rate of 5 mV s?1. Reprinted with permission from Ref. [65]. Copyright 2021, Wiley-VCH GmbH. (d) FT-EXAFS fitting results of FeSA-NSC-900. (e) Molecular orbital diagram of N2 and possible Fe spin configurations in FeN4 and FeN3S1. (f) NH3 yields of FeSA-NSC-800, FeSA-NSC-900, FeSA-NSC-1000, FeSA-NSC-1100, and FeSA-N4C. Reprinted with permission from Ref. [67]. Copyright 2022, Wiley-VCH GmbH.

Fig. 5. (a) Schematic illustration of the preparation of SA Fe-N-C. (b) EPR spectra of Fe-N-C. (c) LSV curves at a rotation rate of 900?r min-1 of Fe-N-C in 0.1 mol L?1 HClO4. Reprinted with permission from Ref. [76]. Copyright 2022, Elsevier. (d) Schematic illustration for preparation of Ru1/NC-T catalysts. (e) Reusability tests at different conversion levels. Reprinted with permission from Ref. [78]. Copyright 2021, The Authors. (f) Configurations of Fe anchored N2O2-C, N2C2-C and C2O2-C. Dark golden rod sphere: iron; brown sphere: carbon; blue sphere: nitrogen; and red sphere: oxygen. (g) Free energy diagram for the NRR at U = 0 V on Fe-N2C2-C with distal and alternative reaction pathways. Reprinted with permission from Ref. [80]. Copyright 2022, Royal Society of Chemistry.

Fig. 6. (a) Projected DOS diagrams of Fe-N-C and Fe-N-C/PdNC. (b) Spin density diagrams of Fe-N-C and Fe-N-C/PdNC (the isosurface is 0.1 a.u.). (c) Tafel plots (B) and the JK curves (C) of catalysts. Reprinted with permission from Ref. [87]. Copyright 2022, Elsevier. (d) Pyrolytic synthesis of FeNx/g-C3N4 catalysts. (e) Room-temperature 57Fe M?ssbauer spectra of I-FeNx/g-C3N4-5 catalyst: (a) fresh catalyst, (b) after the first cycle, and (c) after the second cycle. Reprinted with permission from Ref. [89]. Copyright 2018, American Chemical Society. (f) Schematic representation of N2 coordinated with three Fe(I)-ion homogeneous complexes in the side-on/end-on/end-on (μ3?η2:η1η1) configuration. (g) Schematic representation of N2 coordinated with heterogeneous Fe3/θ-Al2O3 (010) in the same configuration. (h) The major interactions and energy levels of the scalar relativistic Kohn-Sham β-spin MOs of isolated Fe3N2 with correlation to the orbitals from Fe3 and N2 fragments. (i) TOFs per site of ammonia synthesis over the three catalysts as a function of N2 partial pressure at 700?K and 100?bar. Reprinted with permission from Ref. [92]. Copyright 2018, The Authors.

Fig. 7. (a) Schematic illustration of synthesis procedure for Fe,Mn/N-C catalysts. (b) Magnetic susceptibility of Fe,Mn/N-C. (c) LSV curves of Fe,Mn/N-C, Fe/N-C, Mn/N-C, and Pt/C catalyst in O2-saturated 0.1 mol L?1 KOH solution. Reprinted with permission from Ref. [104]. Copyright 2021, The Authors. (d) ΔG1*H and (e) ΔG2*H for Fe/M-N-C (M = Mn, Fe, Co, Ni, Cu, and Zn) (f) Schematic illustration of the structure of the Fe/Zn-N-C DAC. (g) LSV curves of Fe/Zn-N-C, Fe-N-C, Zn-N-C and Pt/C for the ORR in O2-saturated 0.1 mol L?1 KOH solution. Reprinted with permission from Ref. [105]. Copyright 2022, Royal Society of Chemistry. (h) Room-temperature 57Fe M?ssbauer spectroscopy measurements of Fe1Se1-NC and (i) Fe1-NC (j) Content of different Fe moieties of the two catalysts (k) LSV curves for the catalysts acquired in O2-saturated 0.1 mol L?1 KOH solution on a rotating disc electrode (RDE) at 1600?r min?1 and a scanning rate of 5 mV s?1. Reprinted with permission from Ref. [106]. Copyright 2022, Elsevier.

Fig. 8. (a) Schematic for sensing the dipole-dipole interaction between a sensor atom (Fe) and a target atom. Electron spin resonance of individual Fe atoms on bilayer MgO/Ag(100) is driven by a radiofrequency electric field at the tunnelling junction due to VRF. The out-of-plane magnetic field Bz sets the resonance frequency. An in-plane magnetic field Bx mixes the spin states of Fe to increase the ESR signal. A spin-polarized (SP) STM tip measures the spin resonance signal via tunnelling magnetoresistance. The target atom creates a local magnetic field (dipolar field) that is detected by the sensor atom (Fe). (b) Constant-current STM image of four Fe atoms (～0.17 nm apparent height) on the surface. Imaging conditions are VDC = 0.1 V, I = 10 pA, Bz = 0.18 T, Bx = 5.7 T and T = 1.2 K. Reprinted with permission from Ref. [116]. Copyright 2017, Springer Nature.

Fig. 9. (a) A photograph of a homemade silicon nitride membrane with four electrical contacts. (b) A schematic showing the local Joule heating on a Pt/YIG FIB lamella for in-situ heating STEM-EELS experiments. Reprinted with permission from Ref. [128]. Copyright 2013, IEEE.

Fig. 10. (a) The synthesis process of o-MQFe. (b) 57Fe M?ssbauer spectroscopy. (c) 1/χm plots for PQD-Fe and o-MQFe-10:20:5. Reprinted with permission from Ref. [139]. Copyright 2022, Wiley-VCH GmbH.

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Advances in spin regulation of M-N-C single-atom catalysts and their applications in electrocatalysis

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