Antimony sulfide (Sb2S3) is a promising, environmentally friendly semiconductor for novel photodetectors in view of its superior optoelectronic properties. In particular, Sb2S3 has a quasi-one-dimensional (Q1D) crystallographic structure, which enables efficient charge-carrier transport for photodetectors if the film orientation can be well-controlled. In this work, high-performance Sb2S3 photodetectors are developed through crystallographic orientation engineering. Hydrothermal deposition processed [hk0]-oriented Sb2S3 films and close-spaced sublimation processed [hk1]-oriented Sb2S3 films were successfully designed to construct photoconductive and photovoltaic Sb2S3 devices, respectively. The careful studies reveal the correlation between the film orientation and device performance. The photoconductive detectors based on [hk0]-oriented films achieve enhanced responsivity of 2.032 A W-1 and detectivity of 2.24 × 1013 Jones in view of favorable horizontal charge-carrier transport. The photovoltaic detectors based on [hk1]-oriented films deliver improved responsivity of 8.35 × 10-2 A W-1 and detectivity of 4.15 × 1012 Jones through efficient vertical charge-carrier transport. This work provides more insights into the dependence of the optoelectronic properties of Sb2S3 devices on the crystal orientation, proving that tailoring preferential crystal orientations through deposition strategies is an effective approach to achieving high-performance photodetectors.
Solution-processed copper indium sulfide (CuInS2) is an attractive absorber for thin-film photovoltaics due to its non-toxicity and favorable optoelectronic properties. However, low-temperature processed planar heterojunction (PHJ) devices based on CuInS2 nanoparticles have long been constrained to power conversion efficiencies (η) below 5-6%, primarily due to poor crystallinity and high trap density in CuInS2. Here, we introduce an Ag+-mediated crystallization (AMC) strategy that dramatically enhances CuInS2 film quality. The incorporation of Ag+ cations into the precursor promotes the chalcopyrite phase formation, effectively passivates copper and sulfur vacancy defects, and downshifts the valence band of the resulting CuInS2 film. This synergistic suppression of deep-level defects, combined with valence band engineering, modulates the valence band offset at the CuInS2/CuSCN interface in all-inorganic PHJ devices, yielding an optimized band alignment. Consequently, the Ag+-mediated CuInS2 solar cell achieves a notable efficiency of η = 7.31% with a high open-circuit voltage (Voc) of 0.75 V, due to a significantly suppressed non-radiative recombination and a greatly enhanced charge collection efficiency. The Voc represents the highest value among the low-temperature processed all-inorganic CuInS2-based PHJ solar cells, while the efficiency approaches the current record for such devices. Our work establishes a powerful and versatile strategy for defect control and interfacial band engineering in solution-processed chalcogenide photovoltaics.
The molten salt assisted nitridation process was used in this research to produce Si3N4 composite ceramics from kerf loss silicon waste powder. Na3AlF6 molten salt was introduced into the system and the effects of Si-salt ratio, nitridation temperature on the nitriding product were investigated. These results indicated that Na3AlF6 salt promotes the conversion of waste silicon to Si2N2O, alpha-Si3N4 and beta-Si3N4, and 98.3 % conversion rate of waste silicon was obtained at 1350 degrees C when the silicon-salt ratio was 1:0.75. 90.7 % of Si2N2O phase and 2 %alpha-Si3N4 and 1 %(3-Si3N4 were obtained with the Si-salt ratio of 1:1.5 at 1350 degrees C. The main phase of the product changes from Si2N2O to (3-Si3N4 with the temperature increasing. The content of (3-Si3N4 phase reached 72.9 % with the Si-salt ratio of 1:0.75 at 1450 degrees C. The formation and transformation mechanisms were analyzed combined with the in-situ nitriding process. This work provides a feasible method to recycle the waste silicon powder.
Two-dimensional (2D) materials, all-inorganic perovskites, and their hybrid systems have attracted considerable interest for high-performance optoelectronics. Nevertheless, the controlled assembly of heterostructures and the precise management of perovskite film quality within such architectures continue to pose significant challenges and critical for further advancement. Herein, a seed-substrate dual assistance (SSDA) strategy-combining perovskite seeds and a nanostructured WS2 template-has been designed to fabricate a highly oriented, largegrained CsPbBr3 film and construct a novel FTO/WS2/CsPbBr3/Au heterojunction photodetector (PD). This synergistic regulation markedly enhances crystallinity and preferred orientation of CsPbBr3 films, effectively suppressing grain-boundary scattering and interfacial non-radiative recombination, thereby facilitating efficient and directional charge transport/separation. Benefiting from these structural and material optimizations, the asfabricated device exhibits distinct photoresponse across the UV-to-visible region (310-532 nm), particularly achieving a responsivity (R) of 0.503 A W-1 at 365 nm, a specific detectivity (D*) exceeding 8.87 & times; 1012 Jones at 365 nm, and an ultrafast response speed with rise and fall times of 4.71 and 55.9 mu s, respectively, under 532 nm illumination. This work not only offers a viable route for optimizing perovskite film quality in hybriddimensional systems, but also provides new mechanistic insights into the design of high-performance optoelectronic devices, advancing the practical deployment of 2D/perovskite hybrid platforms.
Antimony sulfide (Sb2S3) is a promising light-absorbing material for inorganic thin film solar cells. In this paper, for the first time, a tiny CH3NH3PbI3 (MAPbI3) seed-crystal passivation (TMSP) strategy has been developed to modify Sb2S3 grain boundaries (GBs), which suppresses carrier recombination and promotes efficient charge separation/transport of photogenerated carriers. The optical and electrical properties are investigated by the scanning electron microscopy (SEM), ultraviolet-visible spectroscopy (Uv-vis), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS). Furthermore, the energy band deflection induced by tiny MAPbI3 seed crystals is evaluated and revealed. The TMSP strategy can reduce interface electron recombination and increase electron lifetime of photogenerated carriers. Finally, the champion Sb2S3 solar cells with a Sb2S3 film thickness of ca.100 nm exhibits a power conversion efficiency (eta) of 5.95% with an encouraging open circuit voltage (Voc) of 0.73 V. This TMSP strategy, employing bidirectional interfacial passivation through chemical bonding, is applicable for defect passivation in other inorganic semiconductor films.
Antimony selenosulfide (Sb2(S,Se)3) has emerged as a promising light-harvester for thin-film photovoltaics, offering an eco-friendly and earth-abundant alternative with exceptional structural stability and tunable optoelectronic characteristics. However, solution-processed Sb2(S,Se)3 films encounter critical challenges, particularly non-equilibrium anion gradient distribution and pervasive vacancy/antisite defects, which fundamentally compromise carrier dynamics and ultimately limit photovoltaic performance. To address these dual challenges, we have developed an innovative sequential sulfur-selenium ion gradient engineering (SIGE) strategy. This approach involves preferential sulfur incorporation followed by controlled selenium infusion, enabling targeted defect passivation and optimal anion distribution. The SIGE strategy achieves transformative advancements through three synergistic mechanisms: (1) precise band alignment enabled by chalcogen composition regulation; (2) suppression of detrimental deep-level defects via targeted selenium-ion occupancy control; (3) enhanced carrier transport dynamics through a marked reduction in non-radiative recombination. Consequently, the resulting TS-Sb2(S,Se)3 device yields a power conversion efficiency of 10.84% and an open-circuit voltage of 0.584 V, achieving an efficiency enhancement of 25.75% compared to the original Sb2(S,Se)3 device. This innovative chalcogen gradient engineering approach establishes a universal framework for atomic-scale composition control, point defect passivation, and interface optimization in multinary semiconductors. The research findings also provide crucial insights for advancing high-performance metal chalcogenide photovoltaic technologies. (c) 2026 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights are reserved, including those for text and data mining, AI training, and similar technologies.
Inspired by biological materials, aperiodicity and disorder significantly expand the design freedom of mechanical structures and prove effective in optimizing linear elastic and elastoplastic properties. However, customizing the nonlinear force deflection responses of disordered metamaterials under dynamic impact remains challenging due to the vast design space, irregular structural forms, and complex structure-property relationships. In this work, a novel framework for the design of disordered metamaterials is proposed, consisting of a forward prediction network and an inverse design network, to enable programmable stress-strain behaviors. The disordered metamaterials are generated through a virtual growth program, which assembles predefined building blocks in a stochastic yet controllable manner. Unlike conventional methods, the proposed framework enables diverse equivalent stress-strain responses solely by altering the spatial distribution of building blocks, without changing the generation frequency. In addition, four distinct types of representative structures are identified through investigation of the energy absorption performance of disordered metamaterials. Structural chamber graphs and nodes with different coordination numbers are introduced to elucidate the mechanism by which the spatial distribution of building blocks affects macroscopic mechanical behavior. Furthermore, the inverse design framework generates an energy-absorbing structure that outperforms the maximum-SEAv sample in the dataset by 8.41%. Finally, dynamic experiments are conducted to validate the effectiveness of the proposed method. This framework provides a new pathway for realizing complex, predefined nonlinear force deflection responses and advances the data-driven design of disordered metamaterials.
ABSTRACT The pursuit of multifunctional photodetectors (PDs) that combine broadband responsivity, high specific detectivity under low‐light conditions, and robust operation across extreme temperatures is a cornerstone for advancing next‐generation optical communication and imaging systems. Herein, we report a self‐powered PD FTO/CdS/Sb2(S,Se)3/Au via a low‐cost solution‐processed method. At zero bias, the Sb2(S,Se)3‐based PD exhibits a responsivity of 0.6 A/W, a specific detectivity of 7.68 × 1012 Jones, ultrafast response/recovery times of 1.13/1.90 µs, and a 3 dB bandwidth of 175 kHz under 785 nm illumination (4.09 µW/cm2). Most strikingly, the unencapsulated device exhibits excellent stability from 10 to 575 K, which is rarely reported for Sb2(S,Se)3‐based PDs. The practical multifunctional applicability of this single PD is further validated by its successful integration as a high‐speed receiver in a visible light communication system and a sensing pixel for high‐resolution imaging. Compared with the reference Sb2(S,Se)3 sample, the performance enhancement of the Sb2(S,Se)3/CdS heterojunction PD arises from the built‐in electric field (Ebi) that enables the effective carrier separation/extraction, and the heterojunction structure that reduces the interface/bulk trap densities of the Sb2(S,Se)3 film. This work opens a promising avenue in near‐infrared imaging, light communication and extreme‐environment sensing.
As an emerging photovoltaic material, antimony selenosulfide (Sb2(S,Se)3) has attracted considerable attention and research enthusiasm. However, the current solution-processed Sb2(S,Se)3 layers suffer from severe unfavorable energy band structure problems attributed to the vertical gradient-variable Se/S atomic ratio, making it a challenging and prospective subject. Herein, a novel and convenient alkali metal Cs+-induced Se/S atomic ratio variation strategy has been developed for the first time to regulate Sb2(S,Se)3 energy band structure through hydrothermal-processed CdS nanorod-arrays (NAs)/Sb2(S,Se)3 bulk heterojunction (BHJ) films. The Cs+-induced regulation strategy narrows Se-elemental concentration gradient distribution adjusting effectively Se/S atomic ratio in longitudinal CdS-NAs/Sb2(S,Se)3 BHJ films. This generates a favorable energy band structure, contributing to rapid charge separation and extraction of photogenerated carriers of CdS-NAs/Sb2(S,Se)3 BHJ. Meanwhile, the Cs+-induced Se/S ratio variation not only passivates the defect-state concentration and enhances crystal size of CdS-NAs/Sb2(S,Se)3 film, bust also extend the carrier lifetime for Sb2(S,Se)3 BHJ photovoltaic devices. The resulting Cs-Sb2(S,Se)3 BHJ photovoltaic devices exhibit an impressing power conversion efficiency (η) of 8.23%, the highest one currently available for Sb2(S,Se)3 BHJ solar cells. This study will undoubtedly facilitate the development of efficient Sb2(S,Se)3 BHJ devices, and other similar inorganic semiconductor photovoltaic devices.
Sb-2(S,Se)(3) has garnered significant interest as a light-harvesting material owing to its exceptional photovoltaic properties. However, conventional hydrothermal synthesis yields Sb-2(S,Se)(3) films exhibiting detrimental energy-level inversion and high defect density (e.g., S vacancy/antisite defects) and severely limiting device performance. To address these limitations, we developed an Cs+ ion-modulated hydrothermal growth (IHG) strategy that eliminates programmed-temperature ramping, enabling direct construction of high-quality Sb-2(S,Se)(3) bulk heterojunctions (BHJs). This approach simultaneously enlarges grain dimensions and crystal size (0.40 mu m -> 0.75 mu m), and enhances out-of-plane charge transport along the [hkl, l not equal 0] orientation, effectively suppressing reversed unfavorable Se-gradients distribution while passivating deep-level defects of Sb-2(S,Se)(3) films. Ultimately, Sb-2(S,Se)(3) solar cells incorporating IHG-engineered BHJs demonstrate significantly reduced carrier recombination and extended carrier lifetimes (enhancing similar to 150.5 %), yielding a champion power conversion efficiency of 8.66 % - representing the state-of-the-art for BHJ Sb-2(S,Se)(3) photovoltaics. This IHG paradigm establishes a transformative pathway for fabricating high-performance Sb-2(S,Se)(3) BHJ films and next-generation photovoltaics, redefining quality standards beyond conventional synthesis limitations.
Antimony selenosulfide (Sb₂(S,Se)₃) is a promising earth‐abundant photovoltaic material owing to its excellent optical and electrical properties. Currently, solution‐processed Sb₂(S,Se)₃ photovoltaics face a critical selenium paradox: uncontrolled gradient formation induces band misalignment while creating sulfur vacancies ( V S ) and antimony antisites (Sb S/Se ). Here, an ambient aqueous selenide ion treatment (ASIT) acting as atomic‐scale “ionic scalpel” is pioneered that surgically reconstructs selenium distribution. Through room‐temperature ionic diffusion, this liquid‐phase ion engineering achieves dual breakthroughs: 1) Gradient reversal via surface and bulk selenium enrichment flattening valence band offset from 0.12 to 0.03 eV and establishing ideal Type‐II band alignment, 2) Autogenous deep‐level defects healing via Se−V S /Sb S bond reconfiguration. Significantly, time‐resolved photoluminescence (TRPL) characterization unveils, for the first time, the ultrafast charge‐transfer dynamics at the heterointerface of CdS/Sb₂(S,Se)₃ films fabricated via the ASIT strategy. Ultimately, the resultant Sb₂(S,Se)₃ solar cell shatters performance ceiling with a 10.38% efficiency and record open‐circuit voltage of 0.694 V, showing 57% carrier lifetime enhancement. The water‐based process compatibility with roll‐to‐roll manufacturing positions ASIT as a game‐changer for scalable production of gradient‐engineered absorbers beyond antimony‐based systems.
Antimony trisulfide (Sb 2 S 3 ) is a promising low‐cost photovoltaic material, but practical Sb 2 S 3 solar cells suffer from multiple defects, anisotropic transport, and interfacial energy‐level mismatches, limiting power conversion efficiency ( η ) to 6%‐7%. Herein, a degradable full‐dimensional penetration passivation strategy using phenethylammonium iodide (PEAI) is proposed to synergistically address these issues. PEAI pretreatment of amorphous Sb 2 S 3 films enables [ hk 1]‐oriented crystallization, full‐dimensional defect passivation (bulk and interfaces), and dual‐interface energy‐level reconstruction via Cd‐I and Sb─I bonding. The PEAI reduces CdS surface energy and preferentially adsorbs on Sb 2 S 3 (211) planes, promoting [ hk 1] orientation and enhancing carrier transport. Moreover, the penetrated PEAI leads to a 3.7‐fold increase in carrier lifetime, verifying effective defect suppression. The resultant bulk heterojunction (BHJ) solar cells achieve a η of 8.21%, which is the highest efficiency of BHJ Sb 2 S 3 solar cells. This work establishes a quadruple‐integrated paradigm (defect passivation, orientation control, energy‐level optimization, and architecture design), providing a universal roadmap for high‐efficiency, sustainable photovoltaics.
Optoelectronic devices based on 2D materials/3D van der Waals heterostructures (vdWhs) have garnered considerable interest owing to their seamless integration and remarkable photodetection capabilities. However, the present device structure‐dependent photogenerated carrier transport and extraction still suffers from more serious challenges. Here, vertically oriented WS 2 nanosheet arrays are prepared controllably via magnetron sputtering technique on an n‐type silicon substrate, accompanied by a follow‐up transversely distributed 2D MXene layer, to construct a dual orthogonal‐stacked (DOS) heterostructure. This DOS strategy effectively utilizes the efficient charge transport channel properties inside a 2D‐material plane to fundamentally suppress carrier recombination and promote efficient carrier transport and extraction. The photodetectors (PDs) demonstrate excellent broadband photoresponsefrom ultraviolet to short‐wavelength infrared (254–1650 nm), achieving a photoresponsivity of 793 mA W −1 , a high light‐to‐dark current ratio of over 10 3 at 500 nW cm −2 , high response speeds (500 ns/31.1 µs) and a specific detectivity of 1.03 × 10 14 Jones at zero bias. Additionally, the PDs maintain good long‐term stability and repeatability under high pulsed light (500 kHz). This research provides a guidepost and theoretical support for the design of high‐performance 2D/3D heterojunction PDs and promotes the development and advancement of inorganic 2D‐based PDs.
As a layered two-dimensional material, MoSe2 exhibits interlayer-tunable properties and exceptional theoretical capacities, making it a promising candidate for sodium/potassium ion storage systems. Nevertheless, its inadequate conductivity and irreversible reactions during charge and discharge seriously affect its electrochemical performance. Herein, a hierarchical interlayer-expanded MoSe2/C (IE-MoSe2/C) hybrid architecture with interlinked hollow nanospheres is engineered via a two-stage fabrication process combining hydrothermal self-assembly and controlled pyrolysis. The interlayer spacing increases to 1.02 nm, which accelerates the transport of sodium and potassium ions. Additionally, the strong interface between carbon and MoSe2 improves the conductivity, thereby enhancing the electrochemical kinetics of sodium-ion batteries (SIBs) and potassium-ion batteries (PIBs). On the other hand, the unique hierarchical IE-MoSe2/C structure with hollow nanospheres can effectively mitigate variations in volume during cycling. Thus, IE-MoSe2/C exhibits outstanding electrochemical characteristics as an anode material for SIBs and PIBs. Specifically, IE-MoSe2/C exhibits better rate capability (98 mAh g-1 at 20 A g-1 in SIBs) and cycling performance (269/174 mAh g-1 at 2.0/5.0 A g-1 over 1100 cycles in SIBs and 133/96 mAh g-1 at 1.0/2.0 A g-1 over 1000 cycles for PIBs). Additionally, at 0.5C, the full cell of IE-MoSe2/C||Na3V2(PO4)3 can display a consistent capacity of 93 mAh g-1, demonstrating the potential for future practical applications.
Antimony selenosulfide (Sb2(S,Se)3) has garnered considerable interest as a high-absorption photovoltaic material due to its exceptional light-harvesting properties. However, bulk heterojunction (BHJ) Sb2(S,Se)3 solar cells-though promising for efficient charge dissociation-still suffer from inefficient carrier extraction and high non-radiative losses, primarily caused by disordered crystallization and defective interfaces. Herein, we propose an interlayer-mediated oriented growth and defect passivation (IOD) strategy, utilizing a CdS seed layer (SL-CdS), to fabricate high-quality Sb2(S,Se)3 BHJ films with controlled morphology and optoelectronic properties. The SL-CdS interlayer guides the crystallization process, inducing preferential growth along the [h k l, l ≠ 0] crystallographic direction while suppressing [hk0]-oriented domains, thereby facilitating anisotropic charge transport along the c-axis and reducing carrier scattering. Moreover, this approach significantly reduces defect density by 47.37 % and diminishes non-radiative recombination by 74.64 %, while also enhancing charge carrier mobility and strengthening the built-in electric field. As a result, the champion BHJ Sb2(S,Se)3 solar cell achieves a remarkable power conversion efficiency (PCE) of 8.46 %-one of the highest reported for such BHJ architectures-representing a nearly threefold improvement over control device. Through multiscale characterization and detailed performance analysis, we conclusively correlate the enhanced photovoltaic performance with tailored grain orientation and size, effective interface passivation, and optimized carrier dynamics. This work provides a new materials design paradigm via interlayer engineering for high-performance and low-loss chalcogenide photovoltaics.
Developing hydrogen sensors with high performances is imperative for facilitating H2-related industries. Metal oxide semiconductor (MOS) based gas sensors are simple structures with low cost that are a promising approach for H2 detection. However, detection speed and selectivity of MOS-based sensors currently face great challenges. Herein, we design palladium single atoms (SAs) doped tin oxide (SnO2/Pdatom) for H2 detection. Actual sensing tests show an ultrafast response speed toward H2 (3s to 10 ppm H2), with detection limit of 50 ppb and superior selectivity. Using in-situ THz time-domain spectroscopy and density functional theory calculations, it proves that an extra energy band near Fermi level appeared in SnO2/Pdatom, and Pd SAs doped on SnO2 enhance signally concentration of free carrier in SnO2/Pdatom. Partial density of states reveals that coupling hybridization between Pd 4d orbital and O 2p orbital promotes electron injection from Pd 4d orbital into O π2p orbital, improving production of more O- ions on sensing surfaces. Consequentially, the sensing dynamics involving O- ions spillover at SnO2-Pdatom interface is discussed. Metal oxide semiconductor-based sensors are promising for hydrogen detection but their detection speed and selectivity are still limited. Here, a hydrogen sensor consisting of palladium single atom-doped tin oxide shows a response speed to hydrogen of 3 s and a detection limit of 50 parts per billion.
The low electronic conductivity and ion diffusion rate of lithium iron phosphate (LiFePO4) are the main factors limiting its further development as a positive electrode material for lithium-ion batteries. Element doping is an effective method to improve these limitations. In this study, the method of co-doping with cations and anions has been attempted to improve the electrochemical performance of lithium iron phosphate cathode materials. V-Cl co-doped LiFePO4/C samples were successfully prepared using the high temperature solid-phase method. The controlled particle size LiFe0.95V0.05PO0.95Cl0.05/C was characterized using XRD, XPS, SEM, and the band structure changes of the system were calculated using the first-principles calculations. The results show that V-Cl co-doped lithium iron phosphate materials could significantly enhance the electrochemical performance of lithium iron phosphate batteries, especially at 1C and 5C rates (1C = 170 mAh/g), where the capacities of the modified lithium iron phosphate battery electrodes could still maintain 89 % and 83 % after 1000 cycles. The synergistic effect of anions and cations in V-Cl co-doped system has been confirmed by the first-principles calculations, could effectively reduce the energy barrier for electronic band transitions and improve electronic conductivity.
Organic-inorganic hybrid perovskite films with excellent surface morphology and large grain sizes are crucial for achieving high-performance perovskite solar cells (PSCs). To reduce production costs and meet the growing demand for lightweight thin solar cells, developing ultra-thin absorber layers is an effective approach. However, defects and trap sites are inevitably formed on the surfaces of solution-processed perovskite films. Herein, we present an innovative method that directly incorporates graphite carbon nitride/carbon quantum dots (g-C3N4/ CQDs) into the perovskite precursor solution, using them as structural template to modulate film growth. The gC3N4/CQDs delay crystallization through the formation of a MA & sdot;g-C3N4/CQDs intermediate adduct, which reduces light absorption loss by increasing enlarge grain size and minimizing numerous pinhole defects in thin perovskite films. Additionally, the amide bond formed between g-C3N4 and CQDs can accelerate charge transport, as demonstrated by density functional theory calculation. As a result, the PSCs based on high-quality 360 nm MAPbI3:g-C3N4/CQDs films achieved a champion power conversion efficiency of 20.49 %. The devices retained more than 90 % of their initial efficiency for over 500 h in air without encapsulation. This work not only provides valuable insights into the role of 2D/0D carbon-based heterojunctions in PSCs, but also provides a straightforward technique for crystallization regulation to achieve efficient and stable PSCs.
Dendrite proliferation and parasitic side reaction seriously deteriorate the electrochemical reversibility of zinc metal anode (ZMAs), thus impeding the commercial application of rechargeable aqueous zinc-ion batteries. Herein, a novel strategy, which enables more stable interface chemistry of ZMAs, is proposed based on the construction of a dynamic electrostatic shielding layer. Specially, the trace amount of Al3+cations added into the ZnSO4 base-line electrolyte will preferentially adsorb onto the surface of Zn electrode and further establish a dynamic electrostatic shielding layer, which can effectively homogenize the Zn2+cations and electric field. Consequently, the Zn nucleation energy was reduced and the Zn2+deposition kinetic process was boosted. As a result, a long cycle life exceeding 3500 h was observed on the ZMA deployed in symmetric Zn||Zn cell (1 mA cm-2 and 0.5 mAh cm-2) with the ZnSO4/Al3+ hybrid electrolyte, along with an average Coulombic efficiency of 99.8 % in Zn||Cu cell (2 mA cm-2 and 1 mAh cm-2). Furthermore, the assembled full Zn||MnO2/CNT pouch cell with the ZnSO4/Al3+ hybrid electrolyte acquires a maximal specific capacity of 274.5 mAh g-1 and a high retention of 75 % after 2000 cycles. This work offers a novel pathway for stabilizing the interface chemistry of ZMAs, thus inhibiting Zn dendrite growth for enhanced electrochemical reversibility.