| 碳基无金属电催化剂的本征缺陷研究进展 |
| Recent Advances in Intrinsic Defects of Carbon-Based Metal-Free Electrocatalysts |
| 作者 | 单位 | E-mail | | 周子为 | 吉林大学化学学院, 无机合成与制备化学国家重点实验室, 长春 130012 | | | 何志敏 | 华中科技大学材料科学与工程学院, 材料成形与模具技术国家重点实验室, 武汉 430074 | | | 郭昆 | 华中科技大学材料科学与工程学院, 材料成形与模具技术国家重点实验室, 武汉 430074 | guok@hust.edu.cn | | 黄科科 | 吉林大学化学学院, 无机合成与制备化学国家重点实验室, 长春 130012 | kkhuang@jlu.edu.cn | | 卢兴 | 华中科技大学材料科学与工程学院, 材料成形与模具技术国家重点实验室, 武汉 430074 | lux@hust.edu.cn |
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| 摘要: 自首次报道氮掺杂碳纳米管具有优良的氧还原催化性能以来，碳基无金属材料作为贵金属基电催化剂的潜在替代品而被寄予厚望。碳骨架中普遍存在的本征缺陷位点是影响碳材料物理化学性质的重要因素。特定碳缺陷的引入可以打破原本完整的sp2碳骨架而形成局部畸变，改变邻近碳原子的电荷或自旋密度分布，进而优化催化过程反应物和中间产物的吸附/脱附，提升活性位点的催化活性。因此，在碳基材料中设计创造特定的缺陷结构成为了制备高活性电催化剂的重要研究方向。本文对近年来碳基无金属电催化剂中本征缺陷的研究进展进行了综述，归纳了碳材料中常见的3类本征缺陷（边界、空位或孔洞、拓扑畸变）的制备策略和表征手段，并深入讨论了不同类型碳缺陷的构型和电子结构与其电催化活性的内在关系。最后，我们对目前本征碳缺陷在电催化领域的研究挑战和未来前景进行了总结和展望。 |
| 关键词: 碳基无金属材料 边界 空位 孔洞 拓扑畸变 电子结构 电催化反应 |
| 基金项目: 国家自然科学基金（No.21925104）和湖北省自然科学基金（No.2021CFA020）资助 |
| Abstract: Since the first discovery of nitrogen-doped carbon nanotubes with outstanding catalytic performance toward the oxygen reduction reaction, carbon-based metal-free materials hold great potential as promising alternatives to noble metal-based electrocatalysts prevailingly used in common energy technologies. In addition to the positive role of dopants, the ubiquitous intrinsic defects in the carbon skeleton are also important factors that affect the physical and chemical properties of carbon materials. Specifically, the carbon defects can induce localized charge and/or spin density redistribution and optimize the adsorption and/or desorption behaviors of key species, thereby improving the catalytic activity of adjoining carbon atoms. Rational design and creation of well-defined defects in carbon skeleton have recently become a crucial research frontier of carbon-based metal-free electrocatalysts. In this paper, we present an overview of recent advances in the intrinsic defects of carbon materials for electrocatalytic applications. Special focus is placed on three types of intrinsic defects, including edges, vacancies/holes, and topological defects. The fundamental features of these defects are first discussed, followed by summarizing the preparation and characterization methodology of such defects. According to both experimental and theoretical studies, the underlying correlations between the electronic structure and the electrocatalytic performance of these differentlyconfigured carbon defects are systematically elaborated. Finally, facing challenges and future perspectives on the intrinsic carbon defects for electrocatalysis are also provided. |
| Keywords: carbon-based metal-free materials edge vacancy hole topological defect electronic structure electrocatalytic reaction |
| 投稿时间：2022-03-25 修订日期：2022-08-05 |
| 摘要点击次数: 4692 |
| 全文下载次数: 489 |
| 周子为,何志敏,郭昆,黄科科,卢兴.碳基无金属电催化剂的本征缺陷研究进展[J].无机化学学报,2022,38(11):2113-2126. |
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