School of Chemistry & Chemical Engineering, Anhui University of Technology, Ma'anshan, Anhui, 243002, P. R. China.
Hefei National Research Center for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.
Angew Chem Int Ed Engl. 2023 Apr 3;62(15):e202216837. doi: 10.1002/anie.202216837. Epub 2023 Jan 18.
Developing efficient and stable transition metal oxides catalysts for energy conversion processes such as oxygen evolution reaction and oxygen reduction reaction is one of the key measures to solve the problem of energy shortage. The spin state of transition metal oxides is strongly correlated with their catalytic activities. In an octahedral structure of transition metal oxides, the spin state of active centers could be regulated by adjusting the splitting energy and the electron pairing energy. Regulating spin state of active centers could directly modulate the d orbitals occupancy, which influence the strength of metal-ligand bonds and the adsorption behavior of the intermediates. In this review, we clarified the significance of regulating spin state of the active centers. Subsequently, we discussed several characterization technologies for spin state and some recent strategies to regulate the spin state of the active centers. Finally, we put forward some views on the future research direction of this vital field.
开发高效稳定的过渡金属氧化物催化剂对于解决能源短缺问题的能源转化过程，如析氧反应和氧还原反应，是关键措施之一。过渡金属氧化物的自旋态与其催化活性密切相关。在过渡金属氧化物的八面体结构中，通过调节分裂能和电子配对能可以调节活性中心的自旋态。调节活性中心的自旋态可以直接调制 d 轨道占据，从而影响金属-配体键的强度和中间物的吸附行为。在这篇综述中，我们阐明了调节活性中心自旋态的重要意义。随后，我们讨论了几种用于自旋态的表征技术和一些调节活性中心自旋态的最新策略。最后，我们对这一重要领域的未来研究方向提出了一些看法。
