In Situ Measurement of Strain Evolution in the Graphene Electrode during Electrochemical Lithiation and Delithiation

The strain/stress of the electrode materials induced in the electrochemical process is the key factor for lithium-ion batteries. However, in situ experimental techniques to quantitatively measure the strain/stress response of electrode materials at different length and time scales are still lacking. In this paper, in situ measurement of strain evolution in the graphene electrode during lithiation/delithiation was performed by micro-Raman spectroscopy. The Raman G and 2D peaks of the graphene electrode were obtained using a modified coin cell with an optical window. The stages of the Li-graphite intercalation compounds were characterized by the G peak, while the in-plane strain of the graphene electrode microstructure was characterized by the 2D peak. Evolution of the biaxial strain during the electrochemical cycles was obtained based on determination of the relationship between the Raman shift and the in-plane strain of the graphene electrode. The experimental results show that the biaxial tensile strain of the graphene electrode almost linearly increases during lithiation. The maximum biaxial tensile strain induced by lithiation is about 0.4%, corresponding to the Li-graphite intercalation compound at stage 3. This study provides an experimental basis for understanding the deformation mechanism of the graphene electrode and developing high-performance graphene-based batteries

Selectivity Control for Electrochemical CO₂ Reduction by Charge Redistribution on the Surface of Copper Alloys

Copper is a significant platform for CO2 electroreduction catalysts because it is the only known metal to produce multi-carbon products but suffers from poor selectivity. In the early stages of the reaction pathway, a selectivity-determining step dictates if the pathway leads to formate (a dead-end) or to CO (and on to multi-carbon products). Therefore, controlling the adsorption of key intermediates, in order to steer the reaction pathway as desired, is critical for selective CO2 electroreduction. Alloying copper is a strategy in which the composition and electronic properties of the alloy surface can be finely tuned to alter the reaction intermediate adsorption behavior. Herein, through in situ Raman spectroscopy and density functional theory (DFT) calculations, we investigate a composition-dependent selectivity toward CO and formate during CO2 electroreduction on a range of Cu–Sn alloy catalysts. We find that the selectivity shifts from CO to formate generation as the Sn content in the alloy catalyst increases because of a shift in adsorption preference from the C-bound *COOH intermediate to the O-bound *OCHO intermediate. Theoretical DFT calculation results indicate that this selectivity shift is due to a gradual weakening of *COOH adsorption and strengthening of *OCHO that occurs with increasing Sn content. A combination of theoretical Bader charge analysis and experimental X-ray photoelectron spectroscopy revealed the origin of such transformation: upon alloying, charge is redistributed from Sn to Cu, which creates regions of localized positive charge on the Sn sites. Therefore, with increasing tin content, these localized positive sites hinder the nucleophilic attack of the CO2 carbon, making *COOH adsorption (and the CO pathway) less favorable

Revisiting Frictional Characteristics of Graphene: Effect of In-Plane Straining

Supreme mechanical performance and tribological properties render graphene a promising candidate as a surface friction modifier. Recently, it has been demonstrated that applying in-plane strain can effectively tune friction of suspended graphene in a reversible manner. However, since graphene is deposited on solid surfaces in most tribological applications, whether such operation will result in a similar modulation effect becomes a critical question to be answered. Herein, by depositing graphene onto a stretchable substrate, the frictional characteristics of supported graphene under a wide range of strain are examined with an in situ tensile loading platform. The experimental results show that friction of supported graphene decreases with increasing graphene strain, similar to the suspended system. However, depending on the adherence state of the graphene/substrate interface, the system exhibits two distinct friction regimes with significantly different strain dependences. Assisted by detailed atomic force microscopy imaging, we attribute the unique behavior to the transition between two friction modulation modes, i.e., contact-quality-dominated friction and puckering-dominated friction. This work provides a more comprehensive view of the influence of strain on surface friction of graphene, which is beneficial for active modulation of graphene friction through strain engineering

Water-Processable Self-Doped Hole-Injection Layer for Large-Area, Air-Processed, Slot-Die-Coated Flexible Organic Light-Emitting Diodes

Hole-injection layers (HILs) play a pivotal role in organic light-emitting diodes (OLEDs) by enabling the efficient injection of positive charge carriers (holes) into the active layer, thus facilitating light emission. This research paper focuses on enhancing the processability and performance of solution-processed HILs in OLEDs by utilizing a water-processable self-doped polymer, P2. The P2 film, deposited via slot-die coating, exhibits exceptional uniformity, high transmittance (85%) across the visible spectrum, and a smooth surface (with a root-mean-square roughness of 1.4 nm) comparable to state-of-the-art poly­(3,4-ethylenedioxythiophene):poly­(styrenesulfonate) (PEDOT:PSS) films. The P2 HIL in a four-layer OLED structure, consisting of a PET/ITO/HIL/hole transport layer (HTL)/emissive layer (EML)/electron transport layer (ETL)/Ag, with poly­(9-vinylcarbazole) (PVK) as the HTL, Super Yellow (SY) as the EML, and poly­((9,9-bis­(3′-(N,N-dimethylamino)­propyl)-2,7-fluorene)-alt-2,7-(9,9-dioctylfluorene)) (PFN) as the ETL, demonstrates enhanced hole injection and transport properties. Flexible OLEDs incorporating P2 HILs, fabricated and tested under ambient conditions on a large-area (4 × 40 mm) indium–tin oxide (ITO)-coated polyethylene terephthalate (PET) substrate, demonstrate a maximum current efficiency of 1.24 cd/A, surpassing devices with PEDOT:PSS HILs by 82%. Moreover, a significant 50% reduction in turn-on voltage is observed compared with analogous devices using a PEDOT:PSS layer. This work contributes to the advancement of the OLED technology for various commercial optoelectronic applications

Water-Processable Self-Doped Hole-Injection Layer for Large-Area, Air-Processed, Slot-Die-Coated Flexible Organic Light-Emitting Diodes

Hole-injection layers (HILs) play a pivotal role in organic light-emitting diodes (OLEDs) by enabling the efficient injection of positive charge carriers (holes) into the active layer, thus facilitating light emission. This research paper focuses on enhancing the processability and performance of solution-processed HILs in OLEDs by utilizing a water-processable self-doped polymer, P2. The P2 film, deposited via slot-die coating, exhibits exceptional uniformity, high transmittance (85%) across the visible spectrum, and a smooth surface (with a root-mean-square roughness of 1.4 nm) comparable to state-of-the-art poly­(3,4-ethylenedioxythiophene):poly­(styrenesulfonate) (PEDOT:PSS) films. The P2 HIL in a four-layer OLED structure, consisting of a PET/ITO/HIL/hole transport layer (HTL)/emissive layer (EML)/electron transport layer (ETL)/Ag, with poly­(9-vinylcarbazole) (PVK) as the HTL, Super Yellow (SY) as the EML, and poly­((9,9-bis­(3′-(N,N-dimethylamino)­propyl)-2,7-fluorene)-alt-2,7-(9,9-dioctylfluorene)) (PFN) as the ETL, demonstrates enhanced hole injection and transport properties. Flexible OLEDs incorporating P2 HILs, fabricated and tested under ambient conditions on a large-area (4 × 40 mm) indium–tin oxide (ITO)-coated polyethylene terephthalate (PET) substrate, demonstrate a maximum current efficiency of 1.24 cd/A, surpassing devices with PEDOT:PSS HILs by 82%. Moreover, a significant 50% reduction in turn-on voltage is observed compared with analogous devices using a PEDOT:PSS layer. This work contributes to the advancement of the OLED technology for various commercial optoelectronic applications

Water-Processable Self-Doped Hole-Injection Layer for Large-Area, Air-Processed, Slot-Die-Coated Flexible Organic Light-Emitting Diodes

Hole-injection layers (HILs) play a pivotal role in organic light-emitting diodes (OLEDs) by enabling the efficient injection of positive charge carriers (holes) into the active layer, thus facilitating light emission. This research paper focuses on enhancing the processability and performance of solution-processed HILs in OLEDs by utilizing a water-processable self-doped polymer, P2. The P2 film, deposited via slot-die coating, exhibits exceptional uniformity, high transmittance (85%) across the visible spectrum, and a smooth surface (with a root-mean-square roughness of 1.4 nm) comparable to state-of-the-art poly­(3,4-ethylenedioxythiophene):poly­(styrenesulfonate) (PEDOT:PSS) films. The P2 HIL in a four-layer OLED structure, consisting of a PET/ITO/HIL/hole transport layer (HTL)/emissive layer (EML)/electron transport layer (ETL)/Ag, with poly­(9-vinylcarbazole) (PVK) as the HTL, Super Yellow (SY) as the EML, and poly­((9,9-bis­(3′-(N,N-dimethylamino)­propyl)-2,7-fluorene)-alt-2,7-(9,9-dioctylfluorene)) (PFN) as the ETL, demonstrates enhanced hole injection and transport properties. Flexible OLEDs incorporating P2 HILs, fabricated and tested under ambient conditions on a large-area (4 × 40 mm) indium–tin oxide (ITO)-coated polyethylene terephthalate (PET) substrate, demonstrate a maximum current efficiency of 1.24 cd/A, surpassing devices with PEDOT:PSS HILs by 82%. Moreover, a significant 50% reduction in turn-on voltage is observed compared with analogous devices using a PEDOT:PSS layer. This work contributes to the advancement of the OLED technology for various commercial optoelectronic applications

Water-Processable Self-Doped Hole-Injection Layer for Large-Area, Air-Processed, Slot-Die-Coated Flexible Organic Light-Emitting Diodes

Hole-injection layers (HILs) play a pivotal role in organic light-emitting diodes (OLEDs) by enabling the efficient injection of positive charge carriers (holes) into the active layer, thus facilitating light emission. This research paper focuses on enhancing the processability and performance of solution-processed HILs in OLEDs by utilizing a water-processable self-doped polymer, P2. The P2 film, deposited via slot-die coating, exhibits exceptional uniformity, high transmittance (85%) across the visible spectrum, and a smooth surface (with a root-mean-square roughness of 1.4 nm) comparable to state-of-the-art poly­(3,4-ethylenedioxythiophene):poly­(styrenesulfonate) (PEDOT:PSS) films. The P2 HIL in a four-layer OLED structure, consisting of a PET/ITO/HIL/hole transport layer (HTL)/emissive layer (EML)/electron transport layer (ETL)/Ag, with poly­(9-vinylcarbazole) (PVK) as the HTL, Super Yellow (SY) as the EML, and poly­((9,9-bis­(3′-(N,N-dimethylamino)­propyl)-2,7-fluorene)-alt-2,7-(9,9-dioctylfluorene)) (PFN) as the ETL, demonstrates enhanced hole injection and transport properties. Flexible OLEDs incorporating P2 HILs, fabricated and tested under ambient conditions on a large-area (4 × 40 mm) indium–tin oxide (ITO)-coated polyethylene terephthalate (PET) substrate, demonstrate a maximum current efficiency of 1.24 cd/A, surpassing devices with PEDOT:PSS HILs by 82%. Moreover, a significant 50% reduction in turn-on voltage is observed compared with analogous devices using a PEDOT:PSS layer. This work contributes to the advancement of the OLED technology for various commercial optoelectronic applications

Electrode Materials for Enhancing the Performance and Cycling Stability of Zinc Iodide Flow Batteries at High Current Densities

Aqueous redox flow battery systems that use a zinc negative electrode have a relatively high energy density. However, high current densities can lead to zinc dendrite growth and electrode polarization, which limit the battery’s high power density and cyclability. In this study, a perforated copper foil with a high electrical conductivity was used on the negative side, combined with an electrocatalyst on the positive electrode in a zinc iodide flow battery. A significant improvement in the energy efficiency (ca. 10% vs using graphite felt on both sides) and cycling stability at a high current density of 40 mA cm–2 was observed. A long cycling stability with a high areal capacity of 222 mA h cm–2 is obtained in this study, which is the highest reported areal capacity for zinc–iodide aqueous flow batteries operating at high current density, in comparison to previous studies. Additionally, the use of a perforated copper foil anode in combination with a novel flow mode was discovered to achieve consistent cycling at exceedingly high current densities of >100 mA cm–2. In situ and ex situ characterization techniques, including in situ atomic force microscopy coupled with in situ optical microscopy and X-ray diffraction, are applied to clarify the relationship between zinc deposition morphology on the perforated copper foil and battery performance in two different flow field conditions. With a portion of the flow going through the perforations, a significantly more uniform and compact zinc deposition was observed compared to the case where all of the flow passed over the surface of the electrode. Results from modeling and simulation support the conclusion that the flow of a fraction of electrolyte through the electrode enhances mass transport, enabling a more compact deposit