A series of metal-free organic dyes bridged by anthracene-containing π-conjugations were designed and synthesized as new chromophores for the application of dye-sensitized solar cells (DSCs). Detailed investigations on the relationship between the dye structures, photophysical properties, electrochemical properties, and performances of DSCs are described. With the introduction of the anthracene moiety, together with a triple bond for the fine-tuning of molecular planar configurations and to broaden absorption spectra, the short-circuit photocurrent densities (J sc ) and open-circuit photovoltages (V oc ) of DSCs were improved to a large extent. The improvement of J sc is attributed to much broader absorption spectra of the dyes with the anthracene moiety. Electrochemical impedance spectroscopy (EIS) analysis reveals that the introduction of the anthracene moiety suppresses the charge recombination arising from electrons in TiO 2 films with I 3 ions in the electrolyte, thus improving V oc considerably. On the basis of optimized molecular structures and DSC test conditions, the dye TC501 shows a prominent solar energy conversion efficiency (η) up to 7.03% (J sc ) 12.96 mA • cm -2 , V OC ) 720 mV, ff ) 0.753) under simulated AM 1.5 irradiation (100 mW • cm -2 ).
Due to low density, extremely high electrical and thermal conductivities, graphene has great potential to construct lightweight thermal conductive paper for high-power electric devices. However, the remarkable properties of graphene are on a molecular level and difficult to achieve when processed into macroscopic paper. Here, an effective route to construct ultrahigh conductive graphene paper is developed. First, large-volume, high-concentration, planedefect-free, few-layer graphene dispersion is fast produced from graphite at high yield through ball milling. The exfoliated graphene dispersion is further processed into graphene paper through fast filtration, thermal treatment, and mechanical compression. The electrical and thermal conductivities of the resultant graphene paper are as high as 2231 S cm −1 and 1529 W m −1 K −1 , superior to previously reported graphene papers. Structural analyses confirm that the ultrahigh conductivities are attributed to high quality of graphene sheets, their compact ordered stacking, and large graphitic crystalline domain size, which improve electron and phonon transport within basal plane of graphene sheet and between graphene sheets.
Dye-sensitized solar cells (DSCs) based on two novel carbazole dyes (TC301 and TC306) and a Br(-)/Br(3)(-) redox mediator in dried CH(3)CN solutions as electrolytes yielded a V(oc) of 1.156 V and a eta value of 3.68% and a V(oc) of 0.939 V and a eta value of 5.22% under simulated AM 1.5, respectively. The dyes TC301 and TC306 have more positive HOMO levels (1.59 and 1.38 V vs NHE) than the redox potential of Br(-)/Br(3)(-)-based electrolytes, which have sufficient driving force to regenerate dyes. Under similar conditions with an I(-)/I(3)(-) instead of a Br(-)/Br(3)(-) redox mediator, DSCs sensitized by the dyes TC301 and TC306 produced a V(oc) of 0.696 V and a eta value of 2.36% and a V(oc) of 0.621 V and a eta value of 4.10%, respectively.
High-strength, flexible, and multifunctional characteristics are highly desirable for electromagnetic interference (EMI) shielding materials in the field of electric devices. In this work, inspired by natural nacre, we fabricated large-scale, layered MXene/amarid nanofiber (ANF) nanocomposite papers by blade-coating process plus sol–gel conversion step. The as-synthesized papers possess excellent mechanical performance, that is, exceptional tensile strength (198.80 ± 5.35 MPa), large strain (15.30 ± 1.01%), and good flexibility (folded into various models without fracture), which are ascribed to synergetic interactions of the interconnected three-dimensional network frame and hydrogen bonds between MXene and ANF. More importantly, the papers with extensive continuous conductive paths formed by MXene nanosheets present a high EMI shielding effectiveness of 13188.2 dB cm2 g–1 in the frequency range of 8.2–12.4 GHz. More interestingly, the papers show excellent Joule heating performance with a fast thermal response (<10 s) and a low driving voltage (≤4 V). As such, the large-scale MXene/ANF papers are considered as promising alternatives in a wide range of applications in electromagnetic shielding and thermal management.
A series of novel metal-free organic dyes TC301-TC310 with relatively high HOMO levels were synthesized and applied in dye-sensitized solar cells (DSCs) based on electrolytes that contain Br(-)/Br(3)(-) and I(-)/I(3)(-). The effects of additive Li(+) ions and the HOMO levels of the dyes have an important influence on properties of the dyes and performance of DSCs. The addition of Li(+) ions in electrolytes can broaden the absorption spectra of the dyes on TiO(2) films and shift both the LUMO levels of the dyes and the conduction band of TiO(2), thus leading to the increase of J(sc) and the decrease of V(oc). Upon using Br(-)/Br(3)(-) instead of I(-)/I(3)(-), a large increase of V(oc) is attributed to the enlarged energy difference between the redox potentials of electrolyte and the Fermi level of TiO(2), as well as the suppressed electron recombination. Incident photon to current efficiency (IPCE) action spectra, electrochemical impedance spectra, and nanosecond laser transient absorption reveal that both the electron collection yields and the dye regeneration yields (Φ(r)) depend on the potential difference (the driving forces) between the oxidized dyes and the Br(-)/Br(3)(-) redox couple. For the dyes for which the HOMO levels are more positive than the redox potential of Br(-)/Br(3)(-) sufficient driving forces lead to the longer effective electron-diffusion lengths and almost the same efficient dye regenerations, whereas for the dyes for which the HOMO levels are similar to the redox potential of Br(-)/Br(3)(-), insufficient driving forces lead to shorter effective electron-diffusion lengths and inefficient dye regenerations.
A highly flexible all-solid-state symmetric supercapacitor using an aramid nanofibers/PEDOT:PSS (ANFs/PEDOT:PSS) film exhibits excellent energy density and cycling stability.
Aluminum‐ion batteries (AIBs) are regarded as one of the most promising types of energy storage device in light of the safety, natural abundance, and electrochemical properties of aluminum. However, the rate capabilities of AIBs are limited owing to the sluggish kinetics of chloroaluminate anions. In this study, a covalent organic framework (COF) is adopted as the cathode material in AIBs. Theoretical and experimental results suggest that the COFs allow fast anion diffusion and intercalation without structure collapse, owing to the robust frameworks and the hierarchical pores with a large specific surface area of 1794 m2 g−1. The resultant AIB exhibits remarkable long‐term stability, with a reversible discharge capacity of 150 mAh g−1 after 13 000 cycles at 2 A g−1. It also shows an excellent rate capability of 113 mAh g−1 at 5 A g−1. This work fully demonstrates the potential of COFs in the storage of chloroaluminate anions and other large‐sized ions.
The electrochemical CO2 reduction reaction (CO2RR) to produce CO and H2 (syngas) is a promising method for clean energy, but challenges remain, such as controlling the CO/H2 ratios required for the syngas yield. Herein, hydrophobic exfoliated MoS2 (H‐E‐MoS2) nanosheets are fabricated from bulk MoS2 by a cost‐effective ball‐milling method, followed by decoration with fluorosilane (FAS). H‐E‐MoS2 is a cost‐effective electrocatalyst capable of directly reducing CO2 and H2O for tuneable syngas production with a wide range of CO/H2 ratios (from 1:2 to 4:1). In addition, H‐E‐MoS2 shows a high current density, 61 mA cm−2 at −1.1 V, and the highest CO FE of 81.2% at −0.9 V, which are higher than those of unmodified MoS2. According to density functional theory calculations, FAS decoration on the surface of MoS2 electrode can change the electronic properties of the edge Mo atom, which facilitates the rate‐limiting CO‐desorption step, thus promoting CO2RR. Moreover, the hydrophobic surface of H‐E‐MoS2 depressed the H2 evolution reaction and created abundant three‐phase contact points that provided sufficient CO2. The hydrophobization of the electrode may provide an effective strategy for easily tuning the CO/H2 ratio of syngas in a large range for the direct electroreduction CO2 to syngas with an optimized CO/H2 ratio.
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