精准调控自旋态：可持续催化领域的创新理念

doi:10.1016/j.actphy.2025.100178

Abstract

Abstract:

Amid escalating global sustainability pressures and energy-environmental crises, catalytic innovation has reached a pivotal inflection point. Electron spin manipulation emerges as a transformative paradigm, fundamentally rewiring reaction pathways at the quantum level, transcending classical electronic and geometric constraints. This review frames spin-engineered active centers as molecular spin switches, governing orbital symmetry matching, spin-polarized electron transfer, and transition-state energy landscapes. Covering diverse catalytic materials including metal oxides (e.g., Co₃O₄, Y₂Ru₂O₇), sulfides, alloys, and coordination compounds (e.g., MOF-Co/Cu/Ni), we elucidate how targeted spin-state modulation—achieved via coordination engineering (doping/defect introduction, ligand regulation), valence modulation, size control (quantum confinement), and external stimuli (magnetic coupling)—dynamically tailors d-orbital occupancy to optimize intermediate adsorption and overcome thermodynamic scaling limitations. Critically, these engineered spin configurations mediate accelerated charge-transfer kinetics, thereby expediting rate-determining steps and elevating overall catalytic performance. By integrating advanced spin-sensitive characterization with theoretical calculation, this review summarizes how precisely tailored high- and low-spin states yield unprecedented enhancements in key reactions such as oxygen reduction, CO₂ reduction, hydrogen evolution, urea synthesis, and battery-related reactions. The perspective advances an innovation framework where nonequilibrium spin control and spin-coherent catalysis will pioneer next-generation sustainable energy technologies.

Key words: Spin controlling, Catalytic reaction, Spin modulation method, Characterization technique

Wei Ren, Jinhe Li, Chengzhang Zhu, Weikang Wang, Qinqin Liu. Tailored spin states: a transformative paradigm for sustainable catalysis[J]. Acta Phys. -Chim. Sin. 2026, 42(4), 100178. doi: 10.1016/j.actphy.2025.100178

Figures/Tables 15

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Table 1

Table 2

Applications of spin state regulation in electrocatalysis."

Inﬂuence factor	Material design	Performance	Ref.
Defect engineering	MnO₂/V_O	NRR: MnO₂/V_O, 147.2 μg h⁻¹ mg_cat⁻¹; FE_NH3 = 11%.	[100]
Defect engineering	FePcTa-PPy/V_N	NRR: FePcTa-PPy/V_N, 31.47 μg h⁻¹ mg_cat⁻¹; FE_NH3 = 20.24%.	[101]
Defect engineering	Co₉S₈/Nb₂CT_x-P (V_S)	NRR: Co₉S₈/Nb₂CT_X-P (V_S), 62.62 μg h⁻¹ mg_cat⁻¹; FE_NH3 = 30.33%.	[102]
Dopant integration	F-doped LaCoO₃	OER/ORR: F doped LaCoO₃, overpotential of 390 mV at j = 10 mA cm⁻²; half-wave potential of 0.68 V.	[122]
Dopant integration	N-doped LaCoO₃	OER: N doped LaCoO₃, overpotential of 1.69 V at 50 mA cm⁻².	[123]
Dopant integration	Nd-doped CuCo₂S₄	OER: CuCo_1.75Nd_0.25S₄, overpotential of 320 mV at 500 mA cm⁻².	[124]
Dopant integration	Fe, Zn/N-C	Zn-air batteries: Fe, Zn/N-C, power densities of 211.7 mW cm⁻² (alkaline) and 95.0 mW cm⁻² (neutral).	[125]
Dopant integration	Mn-doped CoSe₂	HER: Mn doped CoSe₂, overpotential of 174 mV; Tafel slope of 36 mV dec⁻¹.	[126]
Dopant integration	Mg-doped Fe-N-C	OER: Mg doped Fe-N-C, overpotential of 224 mV at 10 mA cm⁻²; Tafel slope of 51.74 mV dec⁻¹.	[127]
Dopant integration	Cr-doped Mn@C	¹O₂: Cr doped Mn@C, 13.1 μmol L⁻¹ min⁻¹.	[128]
Dopant integration	Ni-doped Co₃O₄	Gram-negative ESBL-producing Escherichia coli: Ni doped Co₃O₄, 1 × 10⁶ CFU mL⁻¹ (5 min).	[129]
Dopant integration	Se-doped CuO	OH: Se doped CuO, 37.4 μmol L⁻¹ in 100 min.	[130]
Dopant integration	Mo-doped Co₄N	NRR: Mo doped Co₄N, 74.5 mg h⁻¹ cm⁻²; FE_NH3 = 93.4 %.	[131]
Valence modulation	ZnCo₂O₄	OER: ZnCo₂O₄, overpotential of 343 mV at 10 mA cm⁻².	[140]
Ligand regulation	MOF CoBDC-FcCA (CoBDC with FcCA-ligands)	OER: CoBDC-FcCA, overpotential of 280 mV at 10 mA cm⁻².	[150]
Ligand regulation	MOF Co-PMDA-2-mbIM (Co-PMDA with 2-mbIM-ligands)	Urea: Co-PMDA-2-mbIM, 14.47 mmol h⁻¹ g⁻¹; FE_urea = 48.97 %.	[151]
Ligand regulation	MOF Cu-BDC-X (Cu-BDC with F, 2F, H, OH, NH₂-ligands)	Urea: Cu-BDC-NH₂ and Cu-BDC-OH, first and second C-N coupling barriers of 0.75/0.81 and 0.72/0.62 eV.	[152]
Ligand regulation	MOF DD-Ni-NDA (DD-Ni with 2-NDA-ligands)	OER: DD-Ni-NDA, overpotential of 260 mV at 10 mA cm⁻².	[153]
Ligand regulation	FeN₂B₂ (FeN₄ with B-ligands)	NRR: FeN₂B₂, 115 μg h⁻¹ mg_cat⁻¹; FE_NH3 = 24.8 %.	[154]
Ligand regulation	F-Fe: TiO₂ (Fe: TiO₂ with F-ligands)	NRR: F-Fe: TiO₂, 27.86 μg h⁻¹ mg_cat⁻¹; FE_NH3 = 27.67 %.	[155]
Ligand regulation	Ti₄N₃X_X/FePc (FeN₄-X-Ti, X are O, Cl-ligands)	ORR: Ti₄N₃Cl_X/FePc, half-wave potential of +0.91 V, Tafel slope of 39.18 mV dec⁻¹.	[156]
Ligand regulation	Co-MOFs-X (Co-MOFs-X, X are OH, NH₂, SH-ligands)	ORR: Co-MOFs-OH, overpotential of 0.23 V.	[157]
Ligand regulation	Ni-N₄C (Ni-N₄C, N are pyridinic, pyrrolic-ligands)	CO₂RR (CO): Ni-Npyridinic-C, FE_CO ≈ 100 %.	[158]

Table 2

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Inﬂuence factor	Material design	Performance	Ref.
Size modulation	Ni-SA/CTF (Ni single atoms); Ni-AC/CTF (Ni clusters); NiO-NP/CTF (NiO nanoparticles)	2, 2′, 4, 4′-tetrahydrox-ybenzophenoe and RhB: Ni-AC/CTF, 624.4 μmol g⁻¹, 3.01 h⁻¹.	[94]
Defect engineering	ZnO/V_Zn	HER: ZnO/V_Zn, 5846.8 μmol g⁻¹ h⁻¹; ZnO, 103.7 μmol g⁻¹ h⁻¹.	[85]
Dopant integration	Al-doped ZnO	HER: Al/O-ZnO, 398 μmol g⁻¹ h⁻¹; ZnO, 100.1 μmol g⁻¹ h⁻¹.	[118]
Dopant integration	Mn-doped C₃N₄	BPA: Mn doped C₃N₄-Dark, 97.7 %; Mn doped C₃N₄-Light, 89.1 %.	[119]
Dopant integration	Mn-doped C₃N₄	HER: Mn doped C₃N₄, 13479.19 μmol g⁻¹ h⁻¹; C₃N₄, 418.61 μmol g⁻¹ h⁻¹.	[120]
Magnetic field regulation	Fe-BiVO₄-Magnetic (0-5000 Oe)	HER: 1Fe-BiVO₄-Magnetic, 118.54 μmol g⁻¹ h⁻¹; 1Fe-BiVO₄, 61.51 μmol g⁻¹ h⁻¹.	[161]
Magnetic field regulation	2D FeO/Cu₂O-Magnetic (1000 G)	CO₂RR (ethanol): 2D FeO/Cu₂O-Magnetic, 9.69 μmol g⁻¹ h⁻¹.	[162]

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