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Oxidation self-charging batteries have emerged with the demand for powering electronic devices around the clock. The low efficiency of self-charging has been the key challenge at present. Here, a more efficient autoxidation self-charging mechanism is realized by introducing hemoglobin (Hb) as a positive electrode additive in the polyaniline (PANI)-zinc battery system. The heme acts as a catalyst that reduces the energy barrier of the autoxidation reaction by regulating the charge and spin state of O2. To realize self-charging, the adsorbed O2 molecules capture electrons of the reduced (discharged state) PANI, leading to the desorption of zinc ions and the oxidation of PANI to complete self-charging. The battery can discharge for 12 min (0.5 C) after 50 self-charging/discharge cycles, while there is nearly no discharge capacity in the absence of Hb. This biology-inspired electronic regulation strategy may inspire new ideas to boost the performance of self-charging batteries.
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Theoretically, tandem quantum-dot light-emitting diodes (QLEDs) hold great promise for achieving both high efficiency and high stability in display applications. However, in practice, their operational stability remains considerably inferior to that of state-of-the-art devices. In this study, we developed a new tandem structure with optimal electrical and optical performance to simultaneously improve the efficiency and stability of tandem QLEDs. Electrically, upon development of a barrier-free interconnecting layer enabled by an indium-zinc oxide bridging layer and a conductive ZnMgO layer, the driving voltage of the tandem QLEDs is remarkably reduced. Optically, upon development of a top-emitting structure and optimization of the cavity length guided by a theoretical simulation, a maximum light extraction efficiency is achieved. As a result, the red tandem QLEDs exhibit a maximum external quantum efficiency of 49.01% and a T95 lifetime at 1000 cd/m2 of >50â¯000 h, making them one of the most efficient and stable QLEDs ever reported.
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Graphene has tremendous potential in future electronics due to its superior force, electrical, and thermal properties. However, the development of graphene devices is limited by its complex, high-cost, and low-efficiency preparation process. This study proposes a novel laser bidirectional graphene printing (LBGP) process for the large-scale preparation of patterned graphene films. In LBGP, a sandwich sample composed of a thermoplastic elastomer (TPE) substrate, carbon precursor powder, and a glass cover is irradiated by a nanosecond pulsed laser. The laser photothermal effect converts the carbon precursor into graphene, with partial graphene sheets deposited directly on the TPE substrate and the remaining transferred to the glass cover via a laser-induced plasma plume. This method simultaneously prepares two face-to-face graphene films in a single laser irradiation, integrating synthesis, transfer, and patterning. The resulting graphene patterns demonstrate good performance in flexible pressure sensing and Joule heating, showcasing high sensitivity (7.7 kPa-1), fast response (37 ms), and good cycling stability (2000 cycles) for sensors, and high heating rate (1 °C s-1) and long-term stability (3000 s) for heaters. It is believed that the simple, low-cost, and efficient LBGP process can promote the development of graphene electronics and laser manufacturing processes.
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Inverted perovskite solar cells (PSCs) are considered as the most promising avenue for the commercialization of PSCs due to their potential inherent stability. However, suboptimal interface contacts between electron transport layer (ETL) (such as C60) and the perovskite absorbing layer within inverted PSCs always result in reduced efficiency and poor stability. Herein, a surface state manipulation strategy has been developed by employing a highly electronegative 4-fluorophenethylamine hydrochloride (p-F-PEACl) to effectively address the issue of poor interface contacts in the inverted PSCs. The p-F-PEACl demonstrates a robust interaction with perovskite film through bonding of amino group and Cl- with I- and Pb2+ ions in the perovskite, respectively. As such, the surface defects of perovskite film can be significantly reduced, leading to suppressed non-radiative recombination. Moreover, p-F-PEACl also plays a dual role in enhancing the surface potential and improving energy-level alignment at the interfaces between the perovskite and C60 carrier transport layer, which directly contributes to efficient charge extraction. Finally, the open-circuit voltage (Voc) of devices increases from 1.104 V to 1.157 V, leading to an overall efficiency improvement from 22.34% to 24.78%. Furthermore, the p-F-PEACl-treated PSCs also display excellent stability.
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With the rapid advancement of electronic technology, traditional textiles are challenged to keep up with the demands of wearable electronics. It is anticipated that multifunctional textile-based electronics incorporating energy storage, electromagnetic interference (EMI) shielding, and photothermal conversion are expected to alleviate this problem. Herein, a multifunctional cotton fabric with hierarchical array structure (PPy/NiCoAl-LDH/Cotton) is fabricated by the introduction of NiCoAl-layered double hydroxide (NiCoAl-LDH) nanosheet arrays on cotton fibers, followed by polymerization and growth of continuous dense polypyrrole (PPy) conductive layers. The multifunctional cotton fabric shows a high specific areal capacitance of 754.72 mF cm-2 at 5 mA cm-2 and maintains a long cycling life (80.95% retention after 1000 cycles). The symmetrical supercapacitor assembled with this fabric achieves an energy density of 20.83 µWh cm-2 and a power density of 0.23 mWcm-2. Moreover, the excellent electromagnetic interference shielding (38.83 dB), photothermal conversion (70.2 °C at 1000 mW cm-2), flexibility and durability are also possess by the multifunctional cotton fabric. Such a multifunctional cotton fabric has great potential for using in new energy, smart electronics, and thermal management applications.
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Two types of functional surfaces with the same roughness but completely different surface topographies are prepared, namely positively skewed surfaces filled with micropillar arrays (Sa ≈4.4 µm, Ssk >0) and negatively skewed surfaces filled with microcavity arrays (Sa ≈4.4 µm, Ssk <0), demonstrating promoting droplet splashing. Remarkably, the critical Weber number for generating satellite droplets on the negatively skewed surfaces is significantly lower than that on the positively skewed surfaces, indicating that the negatively skewed surface with microcavity arrays is more likely to promote droplet splashing. It is mainly attributed to the fact that air on the negatively skewed surface can make the liquid film take on a Cassie-Baxter state on the surface so that the stabilizing capillary force of the liquid film exceeds the destabilizing stress of the air film. Moreover, the surface topography promoting droplet spreading and the mechanical properties of three-phase moving contact lines are analyzed from the perspective of microscopic interface mechanics. Finally, it is demonstrated the designed positively skewed surfaces can be employed for large-area heat dissipation by means of high-efficiency evaporation.
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Piezo-catalysis emerges as an efficient, safe, and affordable strategy for removing hazardous substances from aquatic environments. Here, the BiFeO3@In2Se3 heterojunction demonstrates remarkable prowess as a piezo-catalyst, enabling the high-efficiency removal of uranium (U) from U(VI)-containing water. A total U(VI) removal efficiency of 94.6% can be achieved under ultrasonic vibration without any sacrificial agents. During the entire catalytic process, piezo-induced electrons, hydroxyl radicals, and superoxide radicals play important roles in U(VI) removal, while the generated H2O2 is responsive to the transformation of soluble U(VI) into insoluble (UO2)O2â¢2H2O and UO3. Furthermore, auxiliary illumination can accelerate the increase of free charges, enabling the piezo-catalyst to retain more charges. This leads to an improved U(VI) removal efficiency of 98.8% and a significantly increased reaction rate constant. This study offers a comprehensive analysis of the fabrication of high-efficiency piezo-catalysts in the removal or extraction of U(VI) from U(VI)-containing water.
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Mesocrystals (MCs) with high-index facets may have superior catalytic properties to those with low-index facets and their nanocrystal counterparts. However, synthesizing such mesocrystal materials is still very challenging because of the metastability of MCs and energetic high-index crystal facets. This work reports a successful solvothermal method followed by calcination for synthesizing copper oxide-based MCs possessing a core-shell structure (denoted as Cu2 O@CuO HIMCs). Furthermore, these MCs are predominantly bounded by the high-index facets such as {311} or {312} with a high-density of stepped atoms. When used as catalysts in Si hydrochlorination to produce trichlorosilane (TCS, the primary feedstock of high-purity crystalline Si), Cu2 O@CuO HIMCs exhibit significantly enhanced Si conversion and TCS selectivity compared to those with flat surfaces and their nanostructured counterparts. Theoretical calculations reveal that both the core-shell structure and the high-index surface contribute to the increased electron density of Cu sites in Cu2 O@CuO HIMCs, promoting the adsorption and dissociation of HCl and stabilizing the dissociated Cl* intermediate. This work provides a simple method for synthesizing high-index faceted MCs and offers a feasible strategy to enhance the catalytic performance of MCs.
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Semiconducting materials show high potential for solar energy harvesting due to their suitable bandgaps, which allow the efficient utilization of light energy larger than their bandgaps. However, the photon energy smaller than their bandgap is almost unused, which significantly limits their efficient applications. Herein, plasmonic Pd/SnS2 microcubes with abundant Pd nanoparticles attached to the SnS2 nanosheets are fabricated by an in situ photoreduction method. The as-prepared Pd/SnS2 microcubes extend the light-harvesting ability of SnS2 beyond its cutoff wavelength, which is attributed to the localized surface plasmon resonance (LSPR) effect of the Pd nanoparticles and the 3D structure of the SnS2 microcubes. Pd nanoparticles can also enhance the light absorption of TiO2 nanoparticles and NiPS3 nanosheets beyond their cutoff wavelengths, revealing the universality for promoting absorption above the cutoff wavelength of the semiconductors. When the plasmonic Pd/SnS2 microcubes are integrated into a hydrophilic sponge acting as the solar evaporator, a solar-to-vapor efficiency of up to 89.2% can be achieved under one sun. The high solar-to-vapor conversion efficiency and the broad applicability of extending the light absorption far beyond the cutoff wavelength of the semiconductor comprise the potential of innovative plasmonic nanoparticle/semiconductor composites for solar desalination.
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Quasi-2D perovskites exhibit impressive optoelectronic properties and hold significant promise for future light-emitting devices. However, the efficiency of perovskite light-emitting diodes (PeLEDs) is seriously limited by defect-induced nonradiative recombination and imbalanced charge injection. Here, the defect states are passivated and charge injection balance is effectively improved by introducing the additive cyclohexanemethylammonium (CHMA) to bromide-based Dion-Jacobson (D-J) structure quasi-2D perovskite emission layer. CHMA participates in the crystallization of perovskite, leading to high quality film composed of compact and well-contacted grains with enhanced hole transportation and less defects. As a result, the corresponding PeLEDs exhibit stable pure blue emission at 466 nm with a maximum external quantum efficiency (EQE) of 9.22%. According to current knowledge, this represents the highest EQE reported for pure-blue PeLEDs based on quasi-2D bromide perovskite thin films. These findings underscore the potential of quasi-2D perovskites for advanced light-emitting devices and pave the way for further advancements in PeLEDs.
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Reducing the defect density of perovskite films during the crystallization process is critical in preparing high-performance perovskite solar cells (PSCs). Here, a multi-functional molecule, 3-phenyl-4-aminobutyric acid hydrochloride (APH), with three functional groups including a benzene ring, âNH3 + and âCOOH, is added into the perovskite precursor solution to improve perovskite crystallization and device performance. The benzene ring increases the hydrophobicity of perovskites, while âNH3 + and âCOOH passivate defects related to I- and Pb2+, respectively. Consequently, the power conversion efficiency (PCE) of the optimal device increased to 24.65%. Additionally, an effective area of 1 cm2 with a PCE of 22.45% is also prepared using APH as an additive. Furthermore, PSCs prepared with APH exhibit excellent stability by 87% initial PCE without encapsulation after exposure at room temperature under 25% humidity for 5000 h and retaining 70% of initial PCE after aging at 85 °C in an N2 environment for 864 h.
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The power conversion efficiency (PCE) of perovskite solar cells (PSCs) has exceeded those of conventional thin-film solar cell technologies, and the speed at which this increase has been achieved is unprecedented in the history of photovoltaics. Despite the significant progress achieved by PSCs at the laboratory level, their commercial prospects still face two significant challenges: scaling up in size and ensuring long-term stability. Small-area devices (~1 cm2) are typically fabricated using spin-coating. However, this approach may not be suitable for preparing the large-area (>100 cm2) substrates required for commercialization. Thus, new materials and methods must be developed to facilitate the coating of large-area PSCs. This review will discuss the development of scaling up organic-inorganic hybrid PSCs and the challenges of increasing the device area. Furthermore, it will provide an overview of the methodologies for achieving high-efficiency perovskite solar modules.
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Large amounts of wastewater containing low-concentration (<10 ppm) rare-earth ions (REIs) are discharged annually in China's rare-earth mining and processing industry, resulting in severe environmental pollution and economic losses. Hence, achieving efficient selective recovery of low-concentration REIs from REIs-containing wastewater is essential for environmental protection and resource recovery. In this study, a pseudocapacitance system was designed for highly efficient capacitive selective recovery of REIs from wastewater using the titanium dioxide/P/C (TiO2/P/C) composite electrode, which exhibited over 99% recovery efficiency for REIs, such as Eu3+, Dy3+, Tb3+, and Lu3+ in mixed solution. This system maintained high efficiency and more than 90 times the enrichment concentration of REIs even after 100 cycles. Ti4+ of TiO2 was reduced to Ti3+ of Ti3O5 under forward voltage in the system, which trapped the electrons of phosphorus site and caused it to be oxidized to phosphate with a strong affinity for REIs, thus improving the selectivity of REIs. Under reverse voltage, Ti3O5 was oxidized to TiO2, which transferred electrons to phosphate and transformed to the phosphorus site, resulting in the desorption and enrichment of REIs and the regeneration of the electrode. This study provides a promising method for the efficient recovery of REIs from wastewater.
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Eletrodos , Metais Terras Raras , Fósforo , Titânio , Águas Residuárias , Águas Residuárias/química , Metais Terras Raras/química , Fósforo/química , Adsorção , Titânio/química , Poluentes Químicos da Água/química , ÍonsRESUMO
Organic contaminants are ubiquitous in the environment, with mounting evidence unequivocally connecting them to aquatic toxicity, illness, and increased mortality, underscoring their substantial impacts on ecological security and environmental health. The intricate composition of sample mixtures and uncertain physicochemical features of potential toxic substances pose challenges to identify key toxicants in environmental samples. Effect-directed analysis (EDA), establishing a connection between key toxicants found in environmental samples and associated hazards, enables the identification of toxicants that can streamline research efforts and inform management action. Nevertheless, the advancement of EDA is constrained by the following factors: inadequate extraction and fractionation of environmental samples, limited bioassay endpoints and unknown linkage to higher order impacts, limited coverage of chemical analysis (i.e., high-resolution mass spectrometry, HRMS), and lacking effective linkage between bioassays and chemical analysis. This review proposes five key advancements to enhance the efficiency of EDA in addressing these challenges: (1) multiple adsorbents for comprehensive coverage of chemical extraction, (2) high-resolution microfractionation and multidimensional fractionation for refined fractionation, (3) robust in vivo/vitro bioassays and omics, (4) high-performance configurations for HRMS analysis, and (5) chemical-, data-, and knowledge-driven approaches for streamlined toxicant identification and validation. We envision that future EDA will integrate big data and artificial intelligence based on the development of quantitative omics, cutting-edge multidimensional microfractionation, and ultraperformance MS to identify environmental hazard factors, serving for broader environmental governance.
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Monitoramento Ambiental , Monitoramento Ambiental/métodos , Poluentes Ambientais , Fracionamento QuímicoRESUMO
Dye-sensitized solar cells, represent the alternate technology in solar research due to their cost effective, easy fabrication processes, higher efficiencies, and design flexibility. In this research, dual donor group modified zinc porphyrin dyes, have been synthesized for DSSCs. The complexes of zinc porphyrin functioned as acceptor or attaching groups within each mesophenyl ring and carboxylic acid. These complexes exhibited diverse alkyl substituents and sizable electron-donating substituents, contributing to their varied chemical structures and potential applications. The dual Donor-π bridge -Acceptor group sensitizers, Zn[5,15-diphenylcarbazole-10,20-(4-carboxyphenyl) Porphyrin] (KSR-1) and Zn [5,15-thiadiazole-10,20-(4-carboxyphenyl) Porphyrin] (KSR-2) have been synthesized and adopted for DSSCs implementation. The molar absorption coefficients (ε) of KSR-2 and KSR-1 Soret bands were 0.56 x 105 mol/L/cm and 0.47 x 105 mol/L/cm, respectively. The Q bands of the KSR-1 and KSR-2 dyes were 1.10 x 105 mol/L/cm and 1.0 x 105 mol/L/cm, respectively and the molar absorption coefficient of the KSR-1 dye was greater when compared to the KSR-2 dye. The molar absorption coefficient of 0.71 x 105 mol/L/cm was visible in the KSR -1 Q-band. DFT calculations and the electrochemical characteristics of the KSR-1 and KSR-2 dyes have been studied and discussed. The exploration involved in investigating the photophysical properties and photovoltaic performance which were affected by varying the length and number of the donor entities. The wall-plug efficiency of the KSR-1 based solar panel was Voc = 0.68 V, Jsc = 8.94 mA/m2, FF = 56 and Efficiency (µ) = 3.44%. The wall-plug efficiency of the KSR-2 based solar panel was Voc = 0.63 V, Jsc = 5.42 mA/m2, FF = 53 and Efficiency (µ) = 1.83%.
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Corantes , Metaloporfirinas , Energia Solar , Corantes/química , Metaloporfirinas/química , Fontes de Energia Elétrica , Zinco/químicaRESUMO
Photocatalytic degradation is an effective technology for degrading water pollution that plays a significant role in environmental remediation. Ternary 2D ternary V-VI-VIIA semiconductors are ideal candidates for photocatalytic degradation of pollutants due to effective light absorption and high charge carrier mobility. In this work, high-quality SbSeI crystals were prepared using the chemical vapor transport (CVT) method and their photocatalytic degradation performance for multiple pollutants was studied. SbSeI exhibits excellent photocatalytic performance in the degradation of potassium dichromate (Cr (VI)), rhodamine B (RhB), tetracycline hydrochloride (TC-HCl) and methyl orange (MO). More than 98% of Cr (VI) and RhB can be removed after irradiation with an Xe lamp for 10 min and 40 min, respectively. The capture experiments and electron spin resonance results indicated that ·O2- plays a major role in reducing Cr (VI), while h+ plays a primary role in the degradation of MO, RhB and TC-HCl. Interestingly, the degradation rate of Cr (VI) is 1.3 times higher than that of a single pollutant system, and the degradation rate of RhB is 1.6 times higher, due to the enhanced separation and utilization of holes and electrons. The results demonstrate that SbSeI is a potential photocatalytic degradation material.
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Benzovindiflupyr (BEN) has emerged as one of the fastest-growing SDHI fungicides in recent years, but it is considered "very highly toxic" to aquatic fish, invertebrates and crustaceans (EC50 or LC50, 0.0035-0.056â¯mg/L, acute toxicity). The comprehensive study on bioactivity, toxicity, and degradation behaviors of BEN at the enantiomeric level would facilitate the development of a high-efficiency and low-risk application method. The bioactivities of 1S, 4R-(-)-BEN against five target pathogens (Alternaria alternata, Phoma multirostrata, Selerotium rolfsii, Magnaporthe oryzae, and Rhizoctonia solani) (EC50, 0.00562-0.329â¯mg/L, high-efficiency) were 6.7-1029 times higher than 1R, 4S-(+)-BEN, demonstrating significant enantioselectivity. For Danio rerio, 1S, 4R-(-)-BEN (LC50, 0.0360â¯mg/L, "very highly toxic") exhibited higher toxicity than 1â¯R, 4S-(+)-BEN, but the toxic interaction was concentration addition (TUrac, 0.94), indicating an enhanced toxicity in the presence of 1R, 4S-(+)-BEN. Molecular docking was employed to offer insights at the molecular level and elucidate the factors influencing enantioselectivity. The stronger binding affinity of 1S, 4R-(-)-BEN with SDH was in line with the quantitative experimental findings. The degradation of two BEN enantiomers in four different fruits followed the first-order degradation kinetics equation, and displayed enantioselectivity. The preferential degradation of 1R, 4S-(+)-BEN was found in pears and grapes, while varying enantioselectivity was found at different stages in tomatoes and watermelons. The residual concentrations of BEN in grapes were higher than the EU's MRL, which in the other three fruits were below the MRLs during the sampling. In conclusion, 1S, 4R-(-)-BEN proved to be the more effective monomer. Utilizing the pure monomer could not only reduce the dosage of racemate by about 44-59â¯%, but also mitigate the risk of introducing inefficient monomer into the environment (especially for fish).
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Fungicidas Industriais , Fungicidas Industriais/toxicidade , Fungicidas Industriais/química , Animais , Estereoisomerismo , Peixe-Zebra , Poluentes Químicos da Água/toxicidade , Poluentes Químicos da Água/química , Simulação de Acoplamento MolecularRESUMO
Low desulfurization efficiency impedes the wide application of dry desulfurization technology, which is a low-cost and simple process, and one significant solution is the development and manufacture of high-performance desulfurizers. In this study, firstly, a steam jet mill was used to digest quicklime; then, we utilized numerical simulation to study the flow field distribution and analyze the driving factors of quicklime digestion; and lastly, the desulfurization performance of the desulfurizer was evaluated under different relative humidities. The results show that the desulfurizer prepared via the steam jet mill had better apparent activity than traditional desulfurizers. Also, the entire jet flow field of the steam jet mill is in a supersonic and highly turbulent flow state, with high crushing intensity and good particle acceleration performance. Sufficient contact with the nascent surface maximizes the formation of slaked lime. The experiments demonstrated that the operating time with 100% desulfurization efficiency and the "break-through" time for the desulfurizer prepared via the steam jet mill is longer than that of traditional desulfurizers, and has significant advantages, especially at low flue gas relative humidity. Compared with traditional desulfurizers, the desulfurizer prepared via steam jet mill expands the range of acceptable flue gas temperature, and the failure temperature is 1.625 times that of traditional desulfurizers. This work breaks through the technical bottleneck of low dry desulfurization efficiency, which is an important step in pushing forward the application of dry desulfurization.
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Cálcio , Vapor , Umidade , ÓxidosRESUMO
Currently, purely organic compounds showing ambient phosphorescence with high efficiency (ΦP ) and ultra-long lifetime (τP ) are quite rare and often need to be achieved in hydrophilic poly(vinyl alcohol)-based hosts. This severely limits their applications. Here, we provide a solution to this issue by constructing an ortho-linked donor-acceptor (D-A) dyad whose D moiety has not only a long-lived T1 state to achieve a long τP , but also a Tn state that is close to the S1 state of the dyad to trigger effective spin-orbit charge transfer intersystem crossing (SOCT-ISC). The rationality of this strategy was validated by a new phosphor OF-BCz that is able to show a τP of 1.92â s and a ΦP of 30 % even in a less rigid matrix of poly(methyl methacrylate) (PMMA). Excitingly, OF-BCz exhibited its potential as both a photocuring initiator and an in situ quality indicator, allowing for the visual detection of defects in photolithographic patterning.
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Efficient exciton dissociation at low energy offsets is key to overcoming voltage losses in organic solar cells. In this work, we developed two dimeric acceptors, i-YT and o-YT, by precisely controlling the position of an asymmetric electron-donating linker. It induced the foldamer conformation of i-YT with a para linkage (relative to the dicyano groups), while retaining the unfold conformation for o-YT. This subtle structural modification influenced the molecular assembly properties, enabled near-zero energy offset exciton dissociation and power conversion efficiencies exceeding 18% for i-YT based organic solar cells. Detailed excitonic dynamics further revealed that the linker position critically influences three processes: the formation of delocalized singlet excited states, ultrafast charge transfer (~5 ps) in solid blends, and the suppression of exciton recombination. Additionally, devices based on i-YT demonstrated outstanding long-term stability, retaining over 85% of their initial efficiency after 1,400 hours of continuous illumination. These findings introduce a new class of dimeric acceptors that combine high efficiency with exceptional stability, offering a promising pathway toward low-energy-loss organic photovoltaics.