E fficient and cost-effective electrocatalysts play critical roles in energy conversion and storage [1][2][3] . Homogeneous and heterogeneous catalysts represent two parallel frontiers of electrocatalysts, each with their own merits and drawbacks 4,5 . Homogeneous catalysts are attractive for their highly uniform active sites, tunable coordination environment and maximized atom utilization efficiency, but are limited by their relatively poor stability and recyclability. Heterogeneous catalysts are appealing for their high durability, excellent recyclability, and easy immobilization and integration with electrodes, but usually have rather low atom utilization efficiency due to the limited surface sites accessible to reactants. To this end, considerable efforts have been devoted to developing nanoscale heterogeneous catalysts that can increase the exposed surface atoms 3 . However, the inhomogeneity in the distribution of particle sizes and facets poses a serious challenge for controlling active sites and fundamental mechanistic studies 6,7 . In contrast, homogeneous catalysts typically exhibit the well-defined atomic structure with tunable coordination environment that is essential for deciphering the catalytic reaction pathway and rational design of targeted catalysts with tailored catalytic properties 8 . Single-atom catalysts (SACs) with monodispersed single atoms supported on solid substrates are recently emerging as an exciting class of catalysts that combine the merits of both homogeneous and heterogeneous catalysts [9][10][11][12][13][14] . However, most SACs studied to date employ metal oxides (for example, TiO 2 , CeO 2 and FeO x ) as supporting substrates to prevent atom aggregation [15][16][17][18] , which cannot be readily applied in electrocatalytic applications due to their low electrical conductivity and/or poor stability in harsh liquid-phase electrolytes (for example, strong acid or base). Atomic transitionmetal-nitrogen moieties supported in carbon (M-N-Cs) represent a unique class of SACs with high electrical conductivity and superior (electro)chemical stability for electrocatalytic applications 19 . In particular, Fe-based M-N-Cs have been extensively studied as electrocatalysts towards the oxygen reduction reaction (ORR) with demonstrated activity and stability approaching those of commercial Pt/C catalysts 20,21 . In addition, as suggested by numerous theoretical studies, M-N-Cs are promising candidates for catalysing a wide range of electrochemical processes, such as hydrogen reduction/oxidation 22 , CO 2 /CO reduction 23 and N 2 reduction 24 . A significant advantage of SACs is that the well-defined single atomic site could allow precise understanding of the catalytic reaction pathway, and rational design of targeted catalysts with tailored activity (in a manner similar to homogeneous catalyst design). However, this perceived advantage has been investigated theoretically
Graphene-supported single atomic metals (G-SAMs) have recently attracted considerable research interest for their intriguing catalytic, electronic, and magnetic properties. The development of effective synthetic methodologies toward G-SAMs with monodispersed metal atoms is vital for exploring their fundamental properties and potential applications. A convenient, rapid, and general strategy to synthesize a series of monodispersed atomic transition metals (for example, Co, Ni, Cu) embedded in nitrogen-doped graphene by two-second microwave (MW) heating the mixture of amine-functionalized graphene oxide and metal salts is reported here. The MW heating is able to simultaneously induce the reduction of graphene oxide, the doping of nitrogen, and the incorporation of metal atoms into the graphene lattices in one simple step. The rapid MW process minimizes metal diffusion and aggregation to ensure exclusive single metal atom dispersion in graphene lattices. Electrochemical studies demonstrate that graphene-supported Co atoms can function as highly active electrocatalysts toward the hydrogen evolution reaction. This MW-assisted method provides a rapid and efficient avenue to supported metal atoms for wide ranges of applications.
Transformation of unipolar n-type semiconductor behavior to ambipolar and finally to unipolar p-type behavior in CH NH PbI microplate field-effect transistors by thermal annealing is reported. The photoluminescence spectra essentially maintain the same features before and after the thermal annealing process, demonstrating that the charge transport measurement provides a sensitive way to probe low-concentration defects in perovskite materials.
A solid-state thermoelectric device is attractive for diverse technological areas such as cooling, power generation and waste heat recovery with unique advantages of quiet operation, zero hazardous emissions, and long lifetime. With the rapid growth of flexible electronics and miniature sensors, the low-cost flexible thermoelectric energy harvester is highly desired as a potential power supply. Herein, a flexible thermoelectric copper selenide (Cu Se) thin film, consisting of earth-abundant elements, is reported. The thin film is fabricated by a low-cost and scalable spin coating process using ink solution with a truly soluble precursor. The Cu Se thin film exhibits a power factor of 0.62 mW/(m K ) at 684 K on rigid Al O substrate and 0.46 mW/(m K ) at 664 K on flexible polyimide substrate, which is much higher than the values obtained from other solution processed Cu Se thin films (<0.1 mW/(m K )) and among the highest values reported in all flexible thermoelectric films to date (≈0.5 mW/(m K )). Additionally, the fabricated thin film shows great promise to be integrated with the flexible electronic devices, with negligible performance change after 1000 bending cycles. Together, the study demonstrates a low-cost and scalable pathway to high-performance flexible thin film thermoelectric devices from relatively earth-abundant elements.
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