精准调控自旋态：可持续催化领域的创新理念

引用本文: 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 shu

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

精准调控自旋态：可持续催化领域的创新理念

任伟 ^1, ,
李金河 ^1, ,
朱成章 ^{2,
,} ,
王伟康 ^1, ,
刘芹芹 ^{1,
,}

1.
江苏大学材料科学与工程学院, 江苏镇江 212013
2.
南京工业大学环境科学与工程学院, 江苏南京 210009

通讯作者: Email: zhucz@njtech.edu.cn (朱成章); qqliu@ujs.edu.cn (刘芹芹)

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:

English

Tailored spin states: a transformative paradigm for sustainable catalysis

Wei Ren ^1, ,
Jinhe Li ^1, ,
Chengzhang Zhu ^{2,
,} ,
Weikang Wang ^1, ,
Qinqin Liu ^{1,
,}

1.
School of Materials Science and Engineering, Jiangsu University, Zhenjiang 212013, Jiangsu Provicne, China
2.
School of Environmental Science and Engineering, Nanjing Tech University, Nanjing 210009, Jiangsu Provicne, China

Corresponding author: Email: zhucz@njtech.edu.cn (Chengzhang Zhu); qqliu@ujs.edu.cn (Qinqin Liu)

Received Date: 18 July 2025
Accepted Date: 01 September 2025
Revised Date: 29 August 2025
Available Online: 15 April 2026

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.

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精准调控自旋态：可持续催化领域的创新理念

通讯作者: Email: zhucz@njtech.edu.cn (朱成章); qqliu@ujs.edu.cn (刘芹芹)

English

Tailored spin states: a transformative paradigm for sustainable catalysis

Corresponding author: Email: zhucz@njtech.edu.cn (Chengzhang Zhu); qqliu@ujs.edu.cn (Qinqin Liu)

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

精准调控自旋态：可持续催化领域的创新理念

通讯作者: Email: zhucz@njtech.edu.cn (朱成章); qqliu@ujs.edu.cn (刘芹芹)

English

Tailored spin states: a transformative paradigm for sustainable catalysis

Corresponding author: Email: zhucz@njtech.edu.cn (Chengzhang Zhu); qqliu@ujs.edu.cn (Qinqin Liu)

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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