Highly efficient counter electrodes (CEs) for dye-sensitized solar cells (DSSCs) were developed using thin films of scalable and high-quality, nitrogen-doped graphene nanoplatelets (NGnP), which was synthesized by a simple two-step reaction sequence. The resultant NGnP was deposited on fluorine-doped SnO2 (FTO)/glass substrates by using electrospray (e-spray) coating, and their electrocatalytic activities were systematically evaluated for Co(bpy)3(3+/2+) redox couple in DSSCs with an organic sensitizer. The e-sprayed NGnP thin films exhibited outstanding performances as CEs for DSSCs. The optimized NGnP electrode showed better electrochemical stability under prolonged cycling potential, and its Rct at the interface of the CE/electrolyte decreased down to 1.73 Ω cm(2), a value much lower than that of the Pt electrode (3.15 Ω cm(2)). The DSSC with the optimized NGnP-CE had a higher fill factor (FF, 74.2%) and a cell efficiency (9.05%), whereas those of the DSSC using Pt-CE were only 70.6% and 8.43%, respectively. To the best of our knowledge, the extraordinarily better current-voltage characteristics of the DSSC-NGnP outperforming the DSSC-Pt for the Co(bpy)3(3+/2+) redox couple (in paticular, FF and short circuit current, Jsc) is highlighted for the first time.

Edge‐selectively fluorinated graphene nanoplatelets (FGnPs) are prepared by mechanochemically driven reaction between fluorine gas (20 vol% in argon) and activated carbon species from graphitic C–C bonds unzipped by high‐speed stainless steel balls with a high kinetic energy. The fluorination at edges of the unzipped graphene nanoplatelets (GnPs) is confirmed by various analytical techniques while the content of fluorine in FGnPs is determined to be 3.0 and 3.4 at% by X‐ray photoelectron spectroscopy and energy‐dispersive X‐ray spectroscopy, respectively. Because of the large difference in electronegativity between carbon (χ = 2.55) and fluorine (χ = 3.98) and the strong C–F bond, the edge‐fluorination of GnPs can provide the maximized charge polarization with an enhanced chemical stability. Thus, electrodes based on the resultant FGnPs demonstrate superb electrochemical performance with excellent stability/cycle life in dye‐sensitized solar cells (FF: 71.5%; Jsc: 14.44 mA cm−2; Voc: 970 mV; PCE: 10.01%) and lithium ion batteries (650.3 mA h g−1 at 0.5 C, charge retention of 76.6% after 500 cycles).

Nitrogen fixation is essential for the synthesis of many important chemicals (e.g., fertilizers, explosives) and basic building blocks for all forms of life (e.g., nucleotides for DNA and RNA, amino acids for proteins). However, direct nitrogen fixation is challenging as nitrogen (N2) does not easily react with other chemicals. By dry ball-milling graphite with N2, we have discovered a simple, but versatile, scalable and eco-friendly, approach to direct fixation of N2 at the edges of graphene nanoplatelets (GnPs). The mechanochemical cracking of graphitic C−C bonds generated active carbon species that react directly with N2 to form five- and six-membered aromatic rings at the broken edges, leading to solution-processable edge-nitrogenated graphene nanoplatelets (NGnPs) with superb catalytic performance in both dye-sensitized solar cells and fuel cells to replace conventional Pt-based catalysts for energy conversion.

Three new thieno[3,2‐b][1]benzothiophene (TBT)‐based donor–π–acceptor (D–π–A) sensitizers, coded as SGT‐121, SGT‐129, and SGT‐130, have been designed and synthesized for dye‐sensitized solar cells (DSSCs), for the first time. The TBT, prepared by fusing thiophene unit with the phenyl unit of triphenylamine donor, is utilized as the π‐bridge for all sensitizers with good planarity. They have been molecularly engineered to regulate the highest occupied molecular orbital (HOMO)‐lowest unoccupied molecular orbital (LUMO) energy levels and extend absorption range as well as to control the electron‐transfer process that can ensure efficient dye regeneration and prevent undesired electron recombination. The photovoltaic performance of SGT‐sensitizer‐based DSSCs employing Co(bpy)32+/3+ (bpy = 2,2′‐bipyridine) redox couple is systematically evaluated in a thorough comparison with Y123 as a reference sensitizer. Among them, SGT‐130 with benzothiadiazole‐phenyl (BTD‐P) unit as an auxiliary acceptor exhibits the highest power‐conversion efficiency (PCE) of 10.47% with Jsc = 16.77 mA cm−2, Voc = 851 mV, and FF = 73.34%, whose PCE is much higher than that of Y123 (9.5%). It is demonstrated that the molecular combination of each fragment in D–π–A organic sensitizers can be a pivotal factor for achieving the higher PCEs and an innovative strategy for strengthening the drawbacks of the π‐bridge.

Challenging precious Pt-based electrocatalysts for dye-sensitized solar cells (DSSCs), graphene nanoplatelets that are N-doped at the edges (NGnPs) are prepared via simply ball-milling graphite in the presence of nitrogen gas. DSSCs based on specific nanoplatelets designated "NGnP5" display superior photovoltaic performance (power conversion efficiency, 10.27%) compared to that of conventional Pt-based devices (9.96%). More importantly, the NGnP counter electrode exhibits outstanding electrochemical stability and electrocatalytic activity with a cobalt-complex redox couple.