Indigo, an organic carbonyl material, is a promising candidate for next-generation green energy storage systems. However, its practical application is hindered by sluggish reaction kinetics, poor electronic conductivity, and the detrimental shuttle effect caused by the dissolution of organic intermediates during charge–discharge cycling. To address these challenges, this paper proposes a dual “physical confinement and chemisorption” synergistic strategy. Low-cost biomass guar gum was used as a precursor to fabricate a nitrogen-doped porous carbon skeleton embedded with FeCo nanoalloys (N-MPC@FeCo) via a facile ball-milling and in situ pyrolysis process, serving as a robust host for indigo. Experimental and theoretical investigations reveal that the pore network physically confines indigo molecules and significantly shortens charge-transfer pathways. The dispersed FeCo nanoalloys and N-dopant sites serve as efficient electrocatalytic centers, accelerating redox kinetics and suppressing intermediate shuttling via strong chemisorption. This structural and chemical synergy enables the N-MPC@FeCo/Indigo composite cathode to deliver an initial specific capacity of 170.6mAh g−1 at 0.5C, with high capacity retention over 170 cycles and exceptional high-rate reversibility. Further incorporation of multiwalled carbon nanotubes (CNTs) as a supplementary conductive network yields an optimized N-MPC@FeCo/CNT/Indigo cathode that achieves an initial specific capacity of 202.3mAh g−1 at 0.2C—approaching the theoretical maximum of 204.58mAh g−1—while retaining a specific capacity of 173mAh g−1 after 400 cycles. This work enhances the electrochemical performance of lithium–indigo batteries and presents a versatile design paradigm for low-cost, high-performance biomass-derived organic energy storage systems.
Effective molecular engineering strategies are crucial for developing photosensitizers. In this study, we designed three triazatruxene (TAT)-based donor-π-bridge-acceptor (D-π-A) photosensitizers, denoted JM202, JM203, and JM204. JM203 and JM204, which have fluorine atoms at different positions, were assembled into single-dye-adsorbed and cosensitized dye-sensitized solar cells with JM202. Then, the effect of fluorine substitution on the photophysical properties and cosensitization was investigated. When the fluorine atom was near the electron acceptor (JM204), the molar extinction coefficient of the dye was enhanced, and charge transport was improved. JM204 also facilitated the adsorption of JM202, leading to higher dye loading and significantly enhanced short-circuit photocurrent density. Furthermore, the co-adsorption of JM202 reduced electronic recombination, resulting in a higher open-circuit voltage. Consequently, the JM202-JM204 cosensitized device achieved an optimal photoelectric conversion efficiency of 11.7%. The results of this study offer a new perspective for developing cosensitized dye-sensitized solar cells.
Photocatalytic plastic degradation is significant for achieving sustainable waste conversion and reducing environmental burden. Single component photocatalysts face challenges such as narrow absorption range and low charge separation efficiency, making efficient photocatalytic degradation plastics and hydrogen production a challenging task. Constructing Z-scheme heterojunctions a promising approach to effectively broaden the range of photo-response and improve the separation and transfer rate of photo-generated charge carriers. Herein, ZnO/ ZnSe Z-scheme heterojunction photocatalyst was in situ synthesized via simple anion exchange. The ZnO/ZnSe-2 heterojunction exhibits excellent photocatalytic plastic degradation performance, with an organic production reaching as high as 52.8 mu mol, which is 6.1 times and 2.9 times higher than pure ZnO and ZnSe, respectively. In addition, the photocatalytic hydrogen production rate of ZnO/ZnSe-2 heterojunction is optimized to be 123.2 mu mol h-1, which is 5.4 times and 2.8 times compared to pure ZnO and ZnSe, respectively. Time of flight (TOF) testing results indicate that the mobility of ZnO/ZnSe heterojunction is 15.74 times that of ZnSe, indicating that the significant improvement in plastic degradation performance can be attributed to the close contact interface between ZnO and ZnSe, which facilitates the migration of charge carriers. In addition, the Z-scheme heterojunction maintains stronger oxidation and reduction potentials.
Lithium-sulfur batteries (LSBs) hold promise for high-energy storage; however, lithium polysulfide (LiPSs) shuttling, chaotic migration, and slow redox kinetics persist. A new strategy based on a MoS2/CoP2 interlayer is proposed to tune the D-band center and interfacial charge rearrangements through electrical coupling between the heterostructural components and built-in electric field (BIEF). Experimental and theoretical calculations demonstrate that this heterostructural design optimizes the D-band center of the Mo sites in MoS2, thus enhancing the adsorption and catalytic ability of LiPSs. The different work functions of MoS2 and CoP2 enable the spontaneous formation of BIEF at the MoS2/CoP2 interface to promote the directional migration for LiPSs from the highly adsorbed MoS2 to the strongly catalytic CoP2 via a "trapping-directional migration-catalytic" mechanism that results in high-efficiency catalytic conversion. The synergistic effect lowers the reaction barrier for the LiPSs redox reaction and enhances the bidirectional catalytic conversion of LiPSs. The initial specific capacity of the resulting LSBs is ultra-high (1320.7 mAh g- 1 at 0.2 C), with performance sustained at 2 C for 700 cycles, and areal capacity of 6.31 mAh cm- 2 at a high sulfur loading (7.06 mg cm- 2). Rational design of the D-band center and BIEF to control the polysulfide behavior advances LSBs towards commercialization.
Nickel oxide (NiOx) is extensively utilized as a hole transport material in inverted perovskite solar cells (p-i-n PSCs) due to its exceptional chemical stability and high transmittance. However, the energy level mismatch and numerous interfacial defects between NiOx and perovskite impede enhancements in device efficiency and stability. In this study, we introduce an organic small molecule, ZL003, derived from triazatruxene (TAT), as an interfacial modification material aimed at optimizing the buried interface of NiOx-based inverted PSCs. ZL003 features a donor-it-bridge-acceptor (D-it-A) molecular structure, which facilitates the extraction and transport of interfacial charges, thereby minimizing carrier recombination losses. Additionally, the hydrophobic characteristics of ZL003 contribute to improved crystal quality in perovskite films and a reduction in defect density. Consequently, the p-i-n PSCs utilizing ZL003-modified NiOx achieve a peak power conversion efficiency (PCE) of 23.66 %, significantly surpassing that of the control device. Furthermore, the unencapsulated NiOx + ZL003based PSCs demonstrate enhanced device stability, maintaining 90 % of their initial efficiency after over 1000 h of exposure to air with a relative humidity (RH) of 50-60 %.
A compact electron donor-acceptor dyad, NI-ICz, with 6,12-diphenyl-indolo[3,2-b]carbazole (ICz) as the electron donor and naphthalimide (NI) as the acceptor, was prepared to study its electron transfer (ET) and thermally activated delayed fluorescence (TADF) properties. The rigid and bulky electron donor reduced the reorganization energy (lambda = 0.96 eV) for ET, which facilitated the formation of a long-lived charge separated (CS) state in NI-ICz by exploiting the Marcus inverted region effect on charge recombination (CR). Transient absorption (TA) spectroscopy revealed the formation of CS triplet (3CS) states (tau = 8.6 mu s in n-hexane, 1.4 mu s in toluene, and 0.13 mu s in acetonitrile). TADF of this dyad was observed in n-hexane but was absent in polar solvents, indicating that 3CS -> 1CS reversed ISC (RISC) was inefficient, which is solid experimental evidence for the spin-vibronic coupling mechanism of TADF. The small zero-field splitting (ZFS) parameter (|D| = 900 MHz) for the triplet state of NI-ICz confirmed the formation of the 3CS state. These results demonstrate the feasibility of achieving a long-lived CS state in compact electron donor-acceptor dyads. The findings also highlight the crucial role of the closely lying 3LE, 1CS and 3CS states in enabling TADF, where the 3LE state serves as an essential intermediate state to facilitate RISC in TADF systems.
Colloidal quantum dot-based photodetectors (PDs) have been undergoing a blooming boost for their prominent photoelectric performance and convenient solution processability. However, the widely used hole transport layer (HTL) 1,2-ethanedithiol (EDT) retains several drawbacks such as a mismatched energy level, existing defects, need for oxidation, and multilayer fabrication. Organic p-type materials, which possess commendable characteristics and synthetic adaptability, have emerged as promising alternatives for the traditional EDT HTL. Herein, we proposed an indeno[1,2-b]carbazole-based organic HTL, named MeOP-DSF. Owing to the optimized band alignment and enhanced interfacial charge dynamics, the carrier generation and collection process are effectively enhanced. The MeOP-DSF-based PDs demonstrate a photoresponsivity of 0.44 A/W, a noise current of 1.1 x 10(-9) A Hz(-0.5), a specific detectivity of 6.9 x 10(8) Jones, and a broad linear dynamic range of 104 dB, outperforming the performance of EDT-based devices on all fronts. This work demonstrates the outstanding potential of organic p-type materials and may provide a universal approach for high-performance PDs.
The efficiency and stability of lithium-sulfur (Li-S) batteries are mainly limited by slow reaction kinetics and lithium dendrite growth. To deal with these issues, in this study, Co(bpy)3(PF6)2 was employed as a dual-functional additive to improve the performance of Li-S batteries. In the case of sulfur cathodes, as evidenced by electrochemical measurements and density functional theory calculations, Co(bpy)3(PF6)2 exhibits a strong affinity toward lithium polysulfides (LiPSs), accelerating the LiPS conversion process. Conversely, in the case of Li anodes, due to LiF-rich solid electrolyte interphases formed by PF6 - anions, Co(bpy)3(PF6)2 can react with the Li metal anode to reduce Li dendrite growth. Batteries incorporating Co(bpy)3(PF6)2 were prepared and subjected to charging and discharging cycles. These batteries achieved a first-cycle discharge capacity of 1228 mAh g-1 at 0.2 C and a capacity of 914.4 mAh g-1 at 2 C. They retained 99.7% of their initial capacity when returning to 0.2 C. Co(bpy)3(PF6)2 was commonly used in dye-sensitized solar cell electrolytes and responsible for charge transport. This study demonstrates that Co(bpy)3(PF6)2 can be used as a dual-functional additive, and it offers avenues for advancing practical Li-S batteries and fresh perspectives for integrated optical energy storage devices.
Colloidal quantum dots (CQDs) have garnered considerable attention for photodetectors (PDs), attributable to exceptional photoelectric properties and ease solution-based processing. However, the prevalent use of 1,2-ethanedithiol (EDT) as a hole transport layer (HTL) has limitations, such as energy level discrepancies, requisite oxidation, and intricate multilayer assembly. Organic p-type materials, lauded for their superior attributes and synthetic versatility, are now stepping forward as viable substitutes for conventional EDT HTLs. In this work, we introduced an organic HTL derived from indolo[3,2-b]carbazole, named ZL004, leading to a marked improvement in carrier generation and collection, facilitated by the optimized band alignment and enhanced interfacial charge dynamics. The ZL004-based PDs exhibit a photoresponsivity of 0.45 A/W, a noise current of 1.8 x 10(-11) A Hz(-0.5), a specific detectivity of 4.6 x 10(9) Jones, and an expansive linear dynamic range of 107 dB & horbar;surpassing EDT-based devices across the board, demonstrating the extraordinary property of organic p-type materials for CQD-based PDs.
A triazatruxene-based HTM, 3Ka-DBT-3Ka, enhances band alignment and augments charge generation and collection in devices. The PbS CQD solar cells employing 3Ka-DBT-3Ka as the HTM achieve a peak power conversion efficiency (PCE) of 11.4%.
Ammonium salts are essential low-dimensional perovskite materials and are synthesized by a protonation reaction, giving the amino group a positive charge.
Colloidal quantum dots (CQDs) are promising optoelectronic materials for solution-processed thin film optoelectronic devices. However, the large surface area with abundant surface defects of CQDs and trap-assisted non-radiative recombination losses at the interface between CQDs and charge-transport layer limit their optoelectronic performance. To address this issue, an interface heterojunction strategy is proposed to protect the CQDs interface by incorporating a thin layer of polyethyleneimine (PEIE) to suppress trap-assisted non-radiative recombination losses. This thin layer not only acts as a protective barrier but also modulates carrier recombination and extraction dynamics by forming heterojunctions at the buried interface between CQDs and charge-transport layer, thereby enhancing the interface charge extraction efficiency. This enhancement is demonstrated by the shortened lifetime of carrier extraction from 0.72 to 0.46 ps. As a result, the resultant PbS CQD solar cells achieve a power-conversion-efficiency (PCE) of 13.4% compared to 12.2% without the heterojunction.
Single dyes typically exhibit limited light absorption in dye-sensitized solar cells (DSSCs). Thus, cosensitization using two or more dyes to enhance light-harvesting efficiency has been explored; however, the aggregation of dyes can adversely affect electron injection capabilities. This study focused on the design and synthesis of three dyes with a common carbazole donor for DSSCs: DZ102, TZ101, and JM102. JM102 broadens the absorption spectrum by replacing the benzoic acid electron acceptor of TZ101 with acetylenic benzoic acid. A cosensitized DSSC device based on CO-1 [DZ102:TZ101 = 1:1 (50 μM:50 μM)] achieved a short-circuit current density of 19.4 mA/cm2 and a power conversion efficiency of 10.9%. For the first time, the molecular interactions between the dyes in the photoanode were demonstrated using cyclic voltammetry, which revealed the presence of intermolecular forces. Adsorption kinetics further indicated that these forces promoted the self-assembly of dyes during adsorption, which resulted in a cosensitization adsorption amount greater than the sum of the individual dye adsorptions. This study provides novel insights into the selection of cosensitizing dyes for DSSCs.
有一个词,叫病耻感,指的是患者因自己所患疾病而产生的负面情绪,因病而羞、因病而耻、因病而卑是病耻感的典型特征. 最初,病耻感多用于精神疾病.后来,随着社会越来越关注心理健康,发现很多患者其实也有类似的感受.皮肤科当然也不例外,如狐臭、脚气、私处毛囊炎等疾病,往往给患者带来巨大的心理压力.
Two-dimensional Ruddlesden-Popper perovskites (2D-RPPs) have emerged as promising candidates for efficient solar cells. However, compositional complexity and their multiphase nature make them particularly susceptible to strain, which can have detrimental effects on their device performance and stability. Here, we focus on cyclohexane methylamine (CMA)-based 2D-RPPs and modulate the strain by substituting iodide with bromide. These mixed-halide 2D-RPPs show excellent optical properties, with mixability and tunable band gap. As the substitution ratio increases, the 2D-RPP framework undergoes a sudden rearrangement in crystal lattice, effectively releasing the strain in lattices. Benefiting from the strain relaxation, the 2D-RPPs exhibit evident improvement in crystallinity, which significantly suppresses recombination in the device and enhances carrier transport across it. Consequently, we achieve an increase of 1.15% in efficiency with the strain-released devices containing (CMA)2MA8Pb9I26.4Br1.6. This device shows significantly improved stability, retaining 93% of the initial efficiency after exposure to 55%-85% relative humidity (RH) for 120 days.
Rigid and coplanar molecular structures are important for photosensitizers, but their packing status on the surface of nanocrystalline mesoporous titanium dioxide (TiO2) films requires more attention. Here, we designed three indolo[3,2-b]carbazole-based organic dyes ZL002, ZL004, and ZL006 with a coplanar structure by introducing flexible Z-type double and triple bonds having a smaller stereo-effect, and a rigid backbone from a benzene ring connected by a single bone. We studied the properties of photoelectricity, electron injection, and charge transport based on the ZL dyes adsorbed on the surface of TiO2, and their dye-sensitized solar cell performance. We found that rigid single bonds and triple bonds widen absorption and preserve the vertical coplanar status of the dyes on TiO2. The coplanar and rigid dye ZL004 densely packed on the surface of TiO2 gives smaller relaxation loss, higher electron-injection efficiency, and longer charge-recombination lifetime. As a result, the best efficiency of 11.6% based on dye ZL004 is achieved from their densely packed structure on the surface of TiO2.
日本有一部电影《裂口女》,女主的嘴角裂开了长长的一道口子,看着不仅吓人,而且感觉很痛. 日常生活中,大部分的人都经历过烂嘴角,虽然不像裂口女那样夸张,但是嘴角裂开,吃不下饭,说不好话,甚至都笑不出来.就怕一动就牵扯到嘴角的伤口.
A chlorophyll derivative, sodium copper chlorophyllin (NaCu-Chl), is utilized to passivate the defects at the perovskite film surface via a solution post-treatment method. It is found that NaCu-Chl not only suppresses the defect-induced nonradiative recombination but also improves the film morphology. Moreover, NaCu-Chl treatment also facilitates efficient hole extraction from perovskite to Spiro-OMeTAD. As a result, NaCu-Chl-treated MAPbI(3) PSCs produce an optimal power conversion efficiency (PCE) of 20.27% with better ambient and thermal stability. This work offers an insight into the application of natural products and derivatives for fabrication of PSCs.