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

摘要/Abstract

摘要：

在全球可持续发展与能源环境危机日益加剧的背景下，催化剂的创新正面临关键转折点。电子自旋调控作为一种新兴理念，有望在量子层面重构反应路径，打破传统电子结构与几何构型的限制。本综述阐述了自旋活性中心如何通过调控轨道对称匹配、自旋极化电子转移和过渡态能垒来调节催化反应活性、选择性和效率。涵盖金属氧化物(如Co₃O₄、Y₂Ru₂O₇)、硫化物、合金及配位化合物(如MOF-Co/Cu/Ni)等多种催化材料，我们阐明了如何通过配位工程(掺杂/缺陷引入、配体调控)、价态调制、尺寸控制(量子限域)和外场刺激(磁耦合)等策略实现自旋态调控，实现动态调整d轨道占据数以优化中间体吸附，突破热力学的限制。特定的自旋构型能够加速电荷转移动力学，从而加快决速步的速率并提升整体催化性能。通过将先进的自旋表征与理论计算相结合，本综述总结了在反应中如何通过精准调控的高/低自旋态来实现性能提升，这些反应包括氧还原、二氧化碳(CO₂)还原、析氢、尿素合成及电池相关的反应；并提出了非平衡自旋调控与自旋相关催化将有望成为下一代可持续能源技术的先驱。

关键词: 自旋控制, 催化反应, 自旋调控方法, 表征技术

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

任伟, 李金河, 朱成章, 王伟康, 刘芹芹. 精准调控自旋态：可持续催化领域的创新理念[J]. 物理化学学报, 2026, 42(4), 100178. doi: 10.1016/j.actphy.2025.100178

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

链接本文: https://www.whxb.pku.edu.cn/CN/10.1016/j.actphy.2025.100178

https://www.whxb.pku.edu.cn/CN/Y2026/V42/I4/100178

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表1

表2

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]

表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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