State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, P. R. China.
Department of Medical Technology, Suzhou Chien-shiung Institute of Technology, Taicang 215411, P. R. China.
Nanoscale Horiz. 2022 Oct 24;7(11):1340-1387. doi: 10.1039/d2nh00362g.
Due to the elusive structure-function relationship, traditional nanocatalysts always yield limited catalytic activity and selectivity, making them practically difficult to replace natural enzymes in wide industrial and biomedical applications. Accordingly, single-atom catalysts (SACs), defined as catalysts containing atomically dispersed active sites on a support material, strikingly show the highest atomic utilization and drastically boosted catalytic performances to functionally mimic or even outperform natural enzymes. The molecular characteristics of SACs (, unique metal-support interactions and precisely located metal sites), especially single-atom iron catalysts (Fe-SACs) that have a similar catalytic structure to the catalytically active center of metalloprotease, enable the accurate identification of active centers in catalytic reactions, which afford ample opportunity for unraveling the structure-function relationship of Fe-SACs. In this review, we present an overview of the recent advances of support materials for anchoring an atomic dispersion of Fe. Subsequently, we highlight the structural designability of support materials as two sides of the same coin. Moreover, the applications described herein illustrate the utility of Fe-SACs in a broad scope of industrially and biologically important reactions. Finally, we present an outlook of the major challenges and opportunities remaining for the successful combination of single Fe atoms and catalysts.
由于结构-功能关系难以捉摸，传统的纳米催化剂通常表现出有限的催化活性和选择性，使得它们在广泛的工业和生物医学应用中实际上难以替代天然酶。因此，单原子催化剂（SACs）被定义为在载体材料上含有原子分散的活性位点的催化剂，它们显著地表现出最高的原子利用率，并极大地提高了催化性能，以功能模拟甚至超过天然酶。SACs 的分子特征（独特的金属-载体相互作用和精确定位的金属位点），特别是具有类似于金属蛋白酶催化活性中心的催化结构的单原子铁催化剂（Fe-SACs），使人们能够在催化反应中准确识别活性中心，从而为揭示 Fe-SACs 的结构-功能关系提供了充分的机会。在这篇综述中，我们介绍了用于锚定原子分散铁的载体材料的最新进展。随后，我们强调了载体材料的结构设计性是同一枚硬币的两面。此外，本文所述的应用说明了 Fe-SACs 在广泛的工业和生物重要反应中的实用性。最后，我们提出了在成功结合单个铁原子和催化剂方面仍然存在的主要挑战和机遇。
