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Single‐atom catalysts (SACs) supported on inorganic materials have attracted much attention in numerous research fields for their high catalytic performance. However, such SACs have been limited by the low metal loading, especially on different types of inorganic supports. Herein, a general approach is presented for preparing SACs on metallic, metal oxide, and perovskite nanosheet (NS) supports to reach a high metal loading of up to 3.94 wt%, by utilizing N‐doped graphene as a sacrificial template that spatially confines the single atoms (SAs). Specifically, the target support material precursors are adsorbed onto the SAs‐stabilized sacrificial template, followed by subsequent heat treatment to transfer the SAs to the support material and to remove the graphene layer. Pt SAs on oxide support exhibits little to no aggregation throughout >10 000 min of annealing at 275 °C, demonstrating high thermal stability, as also supported by ex situ post‐anneal electron microscopy and X‐ray absorption fine structure studies. As a proof‐of‐concept, Pt SACs on SnO2 NSs exhibit high catalytic activity toward chemiresistive sensing of acetone gas (response = 95.4 at 10 ppm, 7.6‐fold enhancement compared with pristine SnO2 NSs) and unprecedented stability under highly humid conditions (27.4% response deterioration at 95% relative humidity). [ABSTRACT FROM AUTHOR]

Single-crystal nanocrystals of catalytic metals and oxides are essential for understanding chemical interactions on well-defined catalyst surfaces. However, a comprehensive understanding of the crystallographic origins for such enhancement has been lacking. This work provides formal evidence of the structure–property relationship through a model study on single-crystal TiO 2. Our approach involves transient pulse heating to manipulate porosity and phase in epitaxially-grown TiO 2 nanosheets along the (0 0 1) plane. Furthermore, we could introduce high-entropy alloy nanoparticles into the system, which exhibited excellent catalytic activity toward CO oxidation, achieving T 90 at 143 °C. This improved performance is attributed to the interplay between the catalytic nanoparticles and the multiphase support, facilitating CO and O 2 adsorption. Our study contributes to a fundamental understanding of structure–property relationships in heterogeneous catalyst systems. Overall, our thermal shock synthesis approach shows much promise for developing single crystal-based advanced nanocatalysts with broad practical implications. [ABSTRACT FROM AUTHOR]

The lack of bifunctional features of perovskite oxide toward the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) significantly limits its use as a cathode catalyst for rechargeable Zn–air batteries (ZABs). Thus far, numerous techniques to disperse additional catalysts on a perovskite host have been suggested to overcome this problem; however, cost-effectiveness and catalyst lifespan remain unsatisfactory. Herein, we present cobalt-based-nanoparticle-decorated Sr 0.95 Nb 0.1 Co 0.7 Fe 0.2 O 3–δ (S0.95NCF) by a simple ex-solution method and use it as a novel air-electrode catalyst. We successfully implemented the socketed nanoparticles with various compositions at different reduction temperatures, achieving notably enhanced activity towards OER and ORR. More importantly, the newly designed catalyst exhibits record-high charge/discharge durability over 500 h (or 1500 consequent cycles) when used as the ZABs cathode. Our findings provide essential guidelines for designing heterostructured electrocatalysts for future energy devices, in which multifunctionality is desirable. [Display omitted] • Ex-solution is applied to Sr 0.95 Nb 0.1 Co 0.7 Fe 0.2 O 3 –δ at various reduction temperatures. • The exsolved metals are elaborately explored depending on ex-solution conditions. • CoFe-nanoalloy ex-solution enhances electrochemical performances for OER and ORR. • The designed catalyst exhibits record-high durability for the Zinc-air batteries. [ABSTRACT FROM AUTHOR]