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Over the past decades, the design of active catalysts has been the subject of intense research efforts. However, there has been significantly less deliberate emphasis on rationally designing a catalyst system with a prolonged stability. A major obstacle comes from the ambiguity behind how catalyst degrades. Several degradation mechanisms are proposed in literature,   but with a lack of systematic studies, the causal relations between degradation and those proposed mechanisms remain ambiguous. Here, a systematic study of a catalyst system comprising of small particles and single atoms of Pt sandwiched between graphene layers, GR/Pt/GR, is studied to  unravel the degradation mechanism of the studied electrocatalyst for oxygen reduction reaction(ORR). Catalyst suffers from atomic dissolution under ORR harsh acidic and oxidizing operation voltages. Single atoms trapped in point defects within the top graphene layer on their way hopping through toward the surface of GR/Pt/GR architecture. Trapping mechanism renders individual Pt atoms as single atom catalyst sites catalyzing ORR for thousands of cycles before washed away in the electrolyte. The GR/Pt/GR catalysts also compare favorably to state‐of‐the‐art commercial Pt/C catalysts and demonstrates a rational design of a hybrid nanoarchitecture with a prolonged stability for thousands of operation cycles.

Smart materials are versatile material systems which exhibit a measurable response to external stimuli. Recently, smart material systems have been developed which incorporate graphene in order to share on its various advantageous properties, such as mechanical strength, electrical conductivity, and thermal conductivity as well as to achieve unique stimuli‐dependent responses. Here, a graphene fiber‐based smart material that exhibits reversible electrical conductivity switching at a relatively low temperature (60 °C), is reported. Using molecular dynamics (MD) simulation and density functional theory‐based non‐equilibrium Green's function (DFT‐NEGF) approach, it is revealed that this thermo‐response behavior is due to the change in configuration of amphiphilic triblock dispersant molecules occurring in the graphene fiber during heating or cooling. These conformational changes alter the total number of graphene‐graphene contacts within the composite material system, and thus the electrical conductivity as well. Additionally, this graphene fiber fabrication approach uses a scalable, facile, water‐based method, that makes it easy to modify material composition ratios. In all, this work represents an important step forward to enable complete functional tuning of graphene‐based smart materials at the nanoscale while increasing commercialization viability.

The nature of the atomic configuration and the bonding within epitaxial Pt‐graphene films is investigated. Graphene‐templated monolayer/few‐multilayers of Pt, synthesized as contiguous 2D films by room temperature electrochemical methods, is shown to exhibit a stable {100} structure in the 1–2 layer range. The fundamental question being investigated is whether surface Pt atoms rendered in these 2D architectures are as stable as those of their bulk Pt counterparts. Unsurprisingly, a single layer Pt on the graphene (Pt_1ML/GR) shows much larger Pt dissociation energy (−7.51 eV) than does an isolated Pt atom on graphene. However, the dissociation energy from Pt_1ML/GR is similar to that of bulk Pt(100), −7.77 eV, while in bi‐layer Pt on the graphene (Pt_2ML/GR), this energy changes to −8.63 eV, surpassing its bulk counterpart. At Pt_2ML/GR, the dissociation energy also slightly surpasses that of bulk Pt(111). Bulk‐like stability of atomically thin Pt–graphene results from a combination of interplanar PtC covalent bonding and inter/intraplanar metallic bonding. This unprecedented stability is also accompanied by a metal‐like presence of electronic states at the Fermi level. Such atomically thin metal‐graphene architectures can be a new stable platform for synthesizing 2D metallic films with various applications in catalysis, sensing, and electronics.