through three steps: 1) at the catalyst surface, the reactants diffuse toward the active sites; 2) the reactants are adsorbed at the active sites and transformed into products via consecutive elementary reaction steps; 3) the products diffuse from the surface via chemical desorption. [4][5][6] To facilitate this transformational process, the catalytically active surface should contain many highly catalytically active sites. [7][8][9][10] However, in conventional bulk catalysts, typically, only a few surface atoms provide catalytic activity, and most of the subsurface atoms cannot directly participate in the reactions, thus resulting in atomic waste. [11][12][13][14][15] Recently, more efficient catalysts have been prepared by changing the active sites from those of a bulk catalyst to isolated atoms; these systems are known as single-atom catalysts (SACs). Thus, the term SAC is given to materials whose catalytically active sites are single atoms. The first discussion of SACs can be traced back to 2011, Zhang et al. reported Pt atoms anchored on FeO x (Pt 1 /FeO x ) for CO oxidation. [16] Crucially, when the size of catalysts reaches the atomic scale, distinctive properties that affect their chemical activities, conversion efficiencies, and stabilities emerge. In particular, unlike bulk catalysts, SACs maximize the use of the catalytically active metal atoms (nearly 100% atom efficiency). [17][18][19][20] Further, compared with bulk catalysts, SACs have unique advantages: 1) an unsaturated coordination environment that affects the affinity of the catalyst for intermediate species; 2) distinctive quantum size effects that yield discrete energy levels and frontier molecular orbital (FMO) occupancies; 3) strong atom support interactions that facilitate surface charge redistribution; 4) appropriate polarity to restrain shuttle effects during catalytic processes; 5) breaking of the energy scaling relationship based on the Sabatier principle for enhanced catalytic activity; and 6) site-to-site interactions between single atoms that enhance the catalytic kinetics. [21][22][23][24][25][26][27][28] In recent years, the use of transition-metal-based SACs [29][30][31] and precious-metal-based SACs [32][33][34] has developed rapidly, especially in the field of energy catalysis. In particular, research has focused on Fe, [35][36][37] Co, [38,39] Ni, [40,41] Mn, [42] Pt, [43,44] Ir, [45][46][47] Pd. [48,49] Owing to the strong atom-support interactions, the coupling of the metal and ligand orbitals in the support can result in changes in the d-band center (ε d ) of the metal atoms, [50,51] and this spin-orbit coupling, which results in a range of electronic states, is key to the success of heterogeneous Single-atom catalysts (SACs) provide well-defined active sites with 100% atom utilization, and can be prepared using a wide range of support materials. Therefore, they are attracting global attention, especially in the fields of energy conversion and storage. To date, research has focused on transitionmetal and precious-metal-bas...