Well-defined surface catalytic sites for solar CO 2 reduction: heterogenized molecular catalysts and single atom catalysts
Well-defined surface catalytic sites for solar CO 2 reduction: heterogenized molecular catalysts and single atom catalysts
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用于太阳能CO 2 还原的明确表面催化位点：多相分子催化剂和单原子催化剂
DOI：
10.1039/d3cc01821k
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发表时间：
2023
影响因子：
4.9
通讯作者：
Li, Gonghu
中科院分区：
文献类型：
--
作者：
Huang, Peipei;Shaaban, Ehab;Ahmad, Esraa;St. John, Allison;Jin, Tianqi;Li, Gonghu
在减少二氧化碳排放的太阳能燃料发电领域取得了令人振奋的进展。近年来，具有明确表面催化中心的新型光催化材料应运而生，包括多相分子催化剂和单原子催化剂。这篇专题文章总结了我们在这方面的最新研究，并简要讨论了相关文献。为了获得多相分子催化剂，我们将二亚胺-三羰基稀土(I)配合物和四氮杂大环钴(III)化合物共价连接到不同的表面，考察了配体的衍生化和表面性质对其结构和光催化活性的影响。单原子催化剂结合了均相催化和多相催化的优点。以石墨化碳氮化物为载体制备了单位钴催化剂，在可见光照射下表现出了良好的二氧化碳选择性还原活性。氮化碳和碳的掺杂对单位钴催化剂的结构和活性有深远的影响。我们的研究成果是为了强调如何将红外、紫外-可见、电子顺磁共振和X射线吸收光谱等光谱技术与催化剂的合成和计算模型相结合，在分子水平上了解明确定义的表面催化中心的结构和性质。这篇文章还强调了在太阳能二氧化碳减排的广泛背景下的挑战和机遇。
Exciting progress has been made in the area of solar fuel generation by CO2 reduction. New photocatalytic materials containing well-defined surface catalytic sites have emerged in recent years, including heterogenized molecular catalysts and single atom catalysts. This Feature Article summarizes our recent research in this area, together with brief discussions of relevant literature. In our effort to obtain heterogenized molecular catalysts, a diimine-tricarbonyl Re(I) complex and a tetraaza macrocyclic Co(III) compound were covalently attached to different surfaces, and the effects of ligand derivatization and surface characteristics on their structures and photocatalytic activities were investigated. Single atom catalysts combine the advantages of homogeneous and heterogeneous catalysis. A single-site cobalt catalyst was prepared on graphitic carbon nitride, which demonstrated excellent activity in selective CO2 reduction under visible-light irradiation. Doping carbon nitride with carbon was found to have profound effects on the structure and activity of the single-site cobalt catalyst. Our research achievements are presented to emphasize how spectroscopic techniques, including infrared, UV-visible, electron paramagnetic resonance, and X-ray absorption spectroscopies, could be combined with catalyst synthesis and computation modeling to understand the structures and properties of well-defined surface catalytic sites at the molecular level. This article also highlights challenges and opportunities in the broad context of solar CO2 reduction.