Despite the important role of carboxymethyl cellulose (CMC) and styrene–butadiene rubber (SBR) binders in graphite electrodes for Li-ion batteries, the direct analysis of these binders remains challenging, particularly at very low concentrations as in practical graphite anodes. In this paper, we report the systematic investigation of the physiochemical behavior of the CMC and SBR binders and direct observations of their distributions in practical graphite electrodes. The key to this unprecedented capability is combining the advantages of several analytic techniques, including laser-ablation laser-induced break-down spectroscopy, time of flight secondary ion mass spectrometry, and a surface and interfacial cutting analysis system. By correlating the vertical distribution with the adsorption behaviors of the CMC, our study reveals that the CMC migration toward the surface during the drying process depends on the degree of cross-linked binder-graphite network generation, which is determined by the surface property of graphite and CMC materials. The suggested analytical techniques enable the independent tracing of CMC and SBR, disclosing the different vertical distribution of SBR from that of the CMC binder in our practical graphite anodes. This achievement provides additional opportunity to analyze the correlation between the binder distribution and mechanical properties of the electrodes.

Graphene has attracted great attention as an alternative to conventional metallic or transparent conducting electrodes. Despite its similarities with conventional electrodes, recent studies have shown that a single-atom layer of graphene possesses unique characteristics, such as a tunable work function and transparencies for electric potential, reactivity, and wetting. Nevertheless, a systematic analysis of graphene and semiconductor junction characteristics has not yet been carried out. Here, we report the photoresponse characteristics of graphene-on-GaN Schottky junction photodiodes (Gr-GaN SJPDs), showing a typical rectifying behavior and distinct photovoltaic and photoelectric responses. Following the initial abrupt response to UV illumination, the Gr-GaN SJPDs exhibited a distinct difference in photocarrier dynamics depending on the applied bias voltage, which is characterized by either a negative or positive change in photocurrent with time. We propose underlying mechanisms for the anomalous photocarrier dynamics based on the interplay between electrostatic molecular interactions over the one-atom-thick graphene and GaN junction and trapped photocarriers at the defect states in the GaN thin film.

The electrical double layer (EDL), consisting of two parallel layers of opposite charges, is foundational to many interfacial phenomena and unique in atomically thin materials. An important but unanswered question is how the "transparency" of atomically thin materials to their substrates influences the formation of the EDL. Here, we report that the EDL of graphene is directly affected by the surface energy of the underlying substrates. Cyclic voltammetry and electrochemical impedance spectroscopy measurements demonstrate that graphene on hydrophobic substrates exhibits an anomalously low EDL capacitance, much lower than what was previously measured for highly oriented pyrolytic graphite, suggesting disturbance of the EDL ("disordered EDL") formation due to the substrate-induced hydrophobicity to graphene. Similarly, electrostatic gating using EDL of graphene field-effect transistors shows much lower transconductance levels or even no gating for graphene on hydrophobic substrates, further supporting our hypothesis. Molecular dynamics simulations show that the EDL structure of graphene on a hydrophobic substrate is disordered, caused by the disruption of water dipole assemblies. Our study advances understanding of EDL in atomically thin limit.

With increasing demand for high-capacity and rapidly rechargeable anodes, problems associated with unstable evolution of a solid-electrolyte interphase on the active anode surface become more detrimental. Here, we report the near fatigue-free, ultrafast, and high-power operations of lithium-ion battery anodes employing silicide nanowires anchored selectively to the inner surface of graphene-based micro-tubular conducting electrodes. This design electrically shields the electrolyte inside the electrode from an external potential load, eliminating the driving force that generates the solid-electrolyte interphase on the nanowire surface. Owing to this electric control, a solid-electrolyte interphase develops firmly on the outer surface of the graphene, while solid-electrolyte interphase-free nanowires enable fast electronic and ionic transport, as well as strain relaxation over 2000 cycles, with 84% capacity retention even at ultrafast cycling (>20C). Moreover, these anodes exhibit unprecedentedly high rate capabilities with capacity retention higher than 88% at 80C (vs. the capacity at 1C).

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