Boosting Osmotic Energy Harvesting from Organic Solutions by Ultrathin Covalent Organic Framework Membranes.

Extracting osmotic energy from waste organic solutions via reverse electrodialysis represents a promising approach to reuse such industrial wastes and helps to mitigate the ever-growing energy needs. Herein, a molecularly thin membrane of covalent organic frameworks is engineered via interfacial polymerization to investigate its ion transport behavior in organic solutions. Interestingly, a significant deviation from linearity between ion conductance and reciprocal viscosity is observed, attributed to the nanoscale confinement effect on intermolecular interactions. This finding suggests a potential strategy to modulate the influence of apprarent viscosity on transmembrane transport. The osmotic energy harvesting of the ultrathin membrane in organic systems was studied, achieving an unprecedented output power density of over 84.5 W m-2 at a 1000-fold salinity gradient with a benign conversion efficiency and excellent stability. These findings provide a meaningful stepping stone for future studies seeking to fully leverage the potentials of organic systems in energy harvesting applications.

Induced Huge Optical Activity in Nanoplatelet Superlattice.

Chiral superstructures with unique chiroptical properties that are not inherent in the individual units are essential in applications such as 3D displays, spintronic devices, biomedical sensors, and beyond. Generally, chiral superstructures are obtained by tedious procedures exploring various physical and chemical forces to break spatial symmetry during the self-assembly of discrete nanoparticles. In contrast, we herein present a simple and efficient approach to chiral superstructures by intercalating small chiral molecules into preformed achiral superstructures. As a model system, the chiral CdSe nanoplatelet (NPL) superlattice exhibits a giant and tunable optical activity with the highest g-factor reaching 3.09 × 10-2 to the excitonic transition of the NPL superlattice, nearly 2 orders of magnitude higher than that of the corresponding separated chiral NPLs. The theoretical analysis reveals that the chiral deformation in the NPL superlattice induced by the chiral perturbation of the small chiral molecules is critical to the observed huge optical activity. We anticipate that this research lays a foundation for understanding and applying chiral inorganic nanosystems.

Oxygen Radical Coupling on Short-Range Ordered Ru Atom Arrays Enables Exceptional Activity and Stability for Acidic Water Oxidation.

The discovery of efficient and stable electrocatalysts for oxygen evolution reaction (OER) in acid is vital for the commercialization of the proton-exchange membrane water electrolyzer. In this work, we demonstrate that short-range Ru atom arrays with near-ideal Ru-Ru interatomic distances and a unique Ru-O hybridization state can trigger direct O*-O* radical coupling to form an intermediate O*-O*-Ru configuration during acidic OER without generating OOH* species. Further, the Ru atom arrays suppress the participation of lattice oxygen in the OER and the dissolution of active Ru. Benefiting from these advantages, the as-designed Ru array-Co3O4 electrocatalyst breaks the activity/stability trade-off that plagues RuO2-based electrocatalysts, delivering an excellent OER overpotential of only 160 mV at 10 mA cm-2 in 0.5 M H2SO4 and outstanding durability during 1500 h operation, representing one of the best acid-stable OER electrocatalysts reported to date. 18O-labeled operando spectroscopic measurements together with theoretical investigations revealed that the short-range Ru atom arrays switched on an oxide path mechanism (OPM) during the OER. Our work not only guides the design of improved acidic OER catalysts but also encourages the pursuit of short-range metal atom array-based electrocatalysts for other electrocatalytic reactions.

Steering Photooxidation of Methane to Formic Acid over A Priori Screened Supported Catalysts.

Efficient methane photooxidation to formic acid (HCOOH) has emerged as a sustainable approach to simultaneously generate value-added chemicals and harness renewable energy. However, the persistent challenge lies in achieving a high yield and selectivity for HCOOH formation, primarily due to the complexities associated with modulating intermediate conversion and desorption after methane activation. In this study, we employ first-principles calculations as a comprehensive guiding tool and discover that by precisely controlling the O2 activation process on noble metal cocatalysts and the adsorption strength of carbon-containing intermediates on metal oxide supports, one can finely tune the selectivity of methane photooxidation products. Specifically, a bifunctional catalyst comprising Pd nanoparticles and monoclinic WO3 (Pd/WO3) would possess optimal O2 activation kinetics and an intermediate oxidation/desorption barrier, thereby promoting HCOOH formation. As evidenced by experiments, the Pd/WO3 catalyst achieves an exceptional HCOOH yield of 4.67 mmol gcat-1 h-1 with a high selectivity of 62% under full-spectrum light irradiation at room temperature using molecular O2. Notably, these results significantly outperform the state-of-the-art photocatalytic systems operated under identical condition.

Large-Area Conductive MOF Ultrathin Film Controllably Integrating Dinuclear-Metal Sites and Photosensitizers to Boost Photocatalytic CO2 Reduction with H2O as an Electron Donor.

Owing to the electrical conductivity and periodic porosity, conductive metal-organic framework (cMOF) ultrathin films open new perspectives to photocatalysis. The space-selective assembly of catalytic sites and photosensitizers in/on cMOF is favorable for promoting the separation of photogenerated carriers and mass transfer. However, the controllable integration of functional units into the cMOF film is rarely reported. Herein, via the synergistic effect of steric hindrance and an electrostatic-driven strategy, the dinuclear-metal molecular catalysts (DMC) and perovskite (PVK) quantum dot photosensitizers were immobilized into channels and onto the surface of cMOF ultrathin films, respectively, affording [DMC@cMOF]-PVK film photocatalysts. In this unique heterostructure, cMOF not only facilitated the charge transfer from PVK to DMC but also guaranteed mass transfer. Using H2O as an electron donor, [DMC@cMOF]-PVK realized a 133.36 µmol·g-1·h-1 CO yield in photocatalytic CO2 reduction, much higher than PVK and DMC-PVK. Owing to the excellent light transmission of films, multilayers of [DMC@cMOF]-PVK were integrated to increase the CO yield per unit area, and the 10-layer device realized a 1115.92 µmol·m-2 CO yield in 4 h, which was 8-fold higher than that of powder counterpart. This work not only lightens the development of cMOF-based composite films but also paves a novel avenue for an ultrathin film photocatalyst.

Steering the Reconstruction of Oxide-Derived Cu by Secondary Metal for Electrosynthesis of n-Propanol from CO.

As fuel and an important chemical feedstock, n-propanol is highly desired in electrochemical CO2/CO reduction on Cu catalysts. However, the precise regulation of the Cu localized structure is still challenging and poorly understood, thus hindering the selective n-propanol electrosynthesis. Herein, by decorating Au nanoparticles (NPs) on CuO nanosheets (NSs), we present a counterintuitive transformation of CuO into undercoordinated Cu sites locally around Au NPs during CO reduction. In situ spectroscopic techniques reveal the Au-steered formation of abundant undercoordinated Cu sites during the removal of oxygen on CuO. First-principles accuracy molecular dynamic simulation demonstrates that the localized Cu atoms around Au tend to rearrange into disordered layer rather than a Cu (111) close-packed plane observed on bare CuO NSs. These Au-steered undercoordinated Cu sites facilitate CO binding, enabling selective electroreduction of CO into n-propanol with a high Faradaic efficiency of 48% in a flow cell. This work provides new insight into the regulation of the oxide-derived catalysts reconstruction with a secondary metal component.

Continuous Flow System for Highly Efficient and Durable Photocatalytic Oxidative Coupling of Methane.

Photocatalytic oxidative coupling of methane (OCM) into value-added industrial chemicals offers an appealing green technique for achieving sustainable development, whereas it encounters double bottlenecks in relatively low methane conversion rate and severe overoxidation. Herein, we engineer a continuous gas flow system to achieve efficient photocatalytic OCM while suppressing overoxidation by synergizing the moderate active oxygen species, surface plasmon-mediated polarization, and multipoint gas intake flow reactor. Particularly, a remarkable CH4 conversion rate of 218.2 µmol h-1 with an excellent selectivity of ∼90% toward C2+ hydrocarbons and a remarkable stability over 240 h is achieved over a designed Au/TiO2 photocatalyst in our continuous gas flow system with a homemade three-dimensional (3D) printed flow reactor. This work provides an informative concept to engineer a high-performance flow system for photocatalytic OCM by synergizing the design of the reactor and photocatalyst to synchronously regulate the mass transfer, activation of reactants, and inhibition of overoxidation.

Effect of Facet on Local Electron Density of Oxygen Vacancy in Catalysts for Nitrogen Electro-Reduction.

Oxygen-vacancy (Ov) engineering is an effective strategy to manipulate the electronic configuration of catalysts for electrochemical nitrogen reduction reaction (eNRR). The influence of the stable facet on the electronic configuration of Ov is widely studied, however, the effect of the reactive facet on the local electron density of Ov is unveiled. In this work, an eNRR electrode R(111)-TiO2/HGO is provided with a high proportion exposed reactive facet (111) of rutile-TiO2 (denoted as R(111)-TiO2) nanocrystals with Ov anchored in hierarchically porous graphite oxide (HGO) nanofilms. The R(111)-TiO2/HGO exhibits excellent eNRR performance with an NH3 yield rate of 20.68 µg h-1 cm-2, which is ≈20 times the control electrode with the most stable facet (110) exposed (R(110)-TiO2/HGO). The experimental data and theoretical simulations reveal that the crystal facet (111) has a positive effect on regulating the local electron density around the oxygen vacancy and the two adjacent Ti-sites, promoting the π-back-donation, minimizing the eNRR barrier, and transforming the rate determination step to *NNH→*NNHH. This work illuminates the effect of crystal facet on the performance of eNRR, and offers a novel strategy to design efficient eNRR catalysts.

Flexible Full-Inorganic Ultrathin Films with Stable Circularly Polarized Luminescence Covering the Visible to Near-Infrared Region.

Circularly polarized luminescence (CPL) materials hold significant value in various fields, including information storage, secure communication, three-dimensional displays, biological detection, and optoelectronic devices. Using the Langmuir-Schaeffer (LS) assembly technique, we successfully construct a series of large-area flexible optical ultrathin films. Impressively, the inorganic assembled ultrathin films exhibit excellent CPL optical activity covering the visible to near-infrared (NIR) region, with the luminescence asymmetry factor glum ranging from 0.59 to 0.72. Moreover, such ultrathin films also display outstanding mechanical flexibility, the optical activity of which even after 240 bending cycles shows almost no difference compared to the unbent samples. Owing to the ultra-broadband optical activity and ultra-stable optical activity of such full-inorganic assembled materials on flexible substrates, coupled with their excellent processability and outstanding mechanical flexibility, we anticipate they will find use in many fields such as communication technology and flexible optoelectronics.

Ultrastrong Graphene Sheets Assembled with Nanoconfined Water.

Highly ordered assembly of two-dimensional (2D) nanoplatelets plays a key role in enhancing the mechanical properties of layered nanocomposites. Layer-by-layer (LbL) assembly, vacuum-assisted filtration, and blade coating have been used to fabricate layered nanocomposites. However, the intrinsic wrinkles of 2D nanoplatelets and defects derived from assembling approaches make it difficult to align 2D nanoplatelets. Recently, the team of Prof. Qunfeng Cheng at Beihang University and their collaborator, Prof. Ray H. Baughman at the University of Texas at Dallas developed a novel approach for aligning graphene and Ti3C2Tx MXene nanoplatelets by nanoconfined assembly through continuous vacuum-assisted filtration. The resultant MXene-bridged sheet has ultrastrong mechanical properties and low porosity, providing a new concept for assembling 2D nanoplatelets into aligned and compact high-performance layered nanocomposites.

Best Practices for Experiments and Reports in Photocatalytic Methane Conversion.

Efficiently converting methane into valuable chemicals via photocatalysis under mild condition represents a sustainable route to energy storage and value-added manufacture. Despite continued interest in this area, the achievements have been overshadowed by the absence of standardized protocols for conducting photocatalytic methane oxidation experiments as well as evaluating the corresponding performance. In this review, we present a structured solution aimed at addressing these challenges. Firstly, we introduce the norms underlying reactor design and outline various configurations in the gas-solid and gas-solid-liquid reaction systems. This discussion helps choosing the suitable reactors for methane conversion experiments. Subsequently, we offer a comprehensive step-by-step protocol applicable to diverse methane-conversion reactions. Emphasizing meticulous verification and accurate quantification of the products, this protocol highlights the significance of mitigating contamination sources and selecting appropriate detection methods. Lastly, we propose the standardized performance metrics crucial for evaluating photocatalytic methane conversion. By defining these metrics, the community could obtain the consensus of assessing the performance across different studies. Moving forward, the future of photocatalytic methane conversion necessitates further refinement of stringent experimental standards and evaluation criteria. Moreover, development of scalable reactor is essential to facilitate the transition from laboratory proof-of-concept to potentially industrial production.

Metal-Organic Framework-Based Hetero-Phase Nanostructure Photocatalysts with Molecular-Scale Tunable Energy Levels.

As an effective method to modulate the physicochemical properties of materials, crystal phase engineering, especially hetero-phase, plays an important role in developing high-performance photocatalysts. However, it is still a huge challenge but significant to construct porous hetero-phase nanostructures with adjustable band structures. As a kind of unique porous crystalline materials, metal-organic frameworks (MOFs) might be the appropriate candidate, but the MOF-based hetero-phase is rarely reported. Herein, we developed a secondary building unit (SBU) regulating strategy to prepare two crystal phases of Ti-MOFs constructed by titanium and 1,4-dicarboxybenzene, i.e., COK and MIL-125. Besides, COK/MIL-125 hetero-phase was further constructed. In the photocatalytic hydrogen evolution reaction, COK/MIL-125 possessed the highest H2 yield compared to COK and MIL-125, ascribing to the Z-Scheme homojunction at hetero-phase interface. Furthermore, by decorating with amino groups (i.e., NH2-COK/NH2-MIL-125), the light absorbing capacity was broadened to visible-light region, and the visible-light-driven H2 yield was greatly improved. Briefly, the MOF-based hetero-phase possesses periodic channel structures and molecularly adjustable band structures, which is scarce in traditional organic or inorganic materials. As a proof of concept, our work not only highlights the development of MOF-based hetero-phase nanostructures, but also paves a novel avenue for designing high-performance photocatalysts.

Regulating the Layered Stacking of a Covalent Triazine Framework Membrane for Aromatic/Aliphatic Separation.

Membrane separation of aromatics and aliphatics is a crucial requirement in chemical and petroleum industries. However, this task presents a significant challenge due to the lack of membrane materials that can endure harsh solvents, exhibit molecular specificity, and facilitate easy processing. Herein, we present a novel approach to fabricate a covalent triazine framework (CTF) membrane by employing a mix-monomer strategy. By incorporating a spatial monomer alongside a planar monomer, we were able to subtly modulate both the pore aperture and membrane affinity, enabling preferential permeation of aromatics over aliphatics with molecular weight below 200 Dalton (Da). Consequently, we achieved successful all-liquid phase separation of aromatic/aliphatic mixtures. Our investigation revealed that the synergistic effects of size sieving and the affinity between the permeating molecules and the membrane played a pivotal role in separating these closely resembling species. Furthermore, the membrane exhibited remarkable robustness under practical operating conditions, including prolonged operation time, various feed compositions, different applied pressure, and multiple feed components. This versatile strategy offers a feasible approach to fabricate membranes with molecule selectivity toward aromatic/aliphatic mixtures, taking a significant step forward in addressing the grand challenge of separating small organic molecules through membrane technology.

Anomalous Mechanical and Electrical Interplay in a Covalent Organic Framework Monolayer Membrane.

Ion transport through nanoconfinement, driven by both electrical and mechanical forces, has drawn ever-increasing attention, due to its high similarity to stress-sensitive ion channels in biological systems. Previous studies have reported only pressure-induced enhancement in ion conductance in low-permeable systems such as nanotubes, nanoslits, or single nanopores. This enhancement is generally explained by the ion accumulation caused by the capacitive effect in low-permeable systems. Here, we fabricate a highly permeable COF monolayer membrane to investigate ion transport behavior driven by both electrical and mechanical forces. Our results show an anomalous conductance reduction activated by external mechanical force, which is contrary to the capacitive effect-dominated conductance enhancement observed in low-permeable nanopores or channels. Through simulations, we uncovered a distinct electrical-mechanical interplay mechanism that depends on the relative rate between the ion diffusion from the boundary layer to the membrane surface and the ion transport through the membrane. The high pore density of the COF monolayer membrane reduces the charge accumulation caused by the capacitive effect, resulting in fewer accumulated ions near the membrane surface. Additionally, the high membrane permeability greatly accelerates the dissipation of the accumulated ions under mechanical pressure, weakening the effect of the capacitive layer on the streaming current. As a result, the ions accumulated on the electrodes, rather than in the capacitive layer, dominating the streaming current and giving rise to a distinct electrical-mechanical interplay mechanism compared to that in low-permeable nanopores or channels. Our study provides new insights into the interplay between electrical and mechanical forces in ultra-permeable systems.

Enabling Specific Photocatalytic Methane Oxidation by Controlling Free Radical Type.

Selective CH4 oxidation to CH3OH or HCHO with O2 in H2O under mild conditions provides a desired sustainable pathway for synthesis of commodity chemicals. However, manipulating reaction selectivity while maintaining high productivity remains a huge challenge due to the difficulty in the kinetic control of the formation of a desired oxygenate against its overoxidation. Here, we propose a highly efficient strategy, based on the precise control of the type of as-formed radicals by rational design on photocatalysts, to achieve both high selectivity and high productivity of CH3OH and HCHO in CH4 photooxidation for the first time. Through tuning the band structure and the size of active sites (i.e., single atoms or nanoparticles) in our Au/In2O3 catalyst, we show alternative formation of two important radicals, •OOH and •OH, which leads to distinctly different reaction paths to the formation of CH3OH and HCHO, respectively. This approach gives rise to a remarkable HCHO selectivity and yield of 97.62% and 6.09 mmol g-1 on In2O3-supported Au single atoms (Au1/In2O3) and an exceptional CH3OH selectivity and yield of 89.42% and 5.95 mmol g-1 on In2O3-supported Au nanoparticles (AuNPs/In2O3), respectively, upon photocatalytic CH4 oxidation for 3 h at room temperature. This work opens a new avenue toward efficient and selective CH4 oxidation by delicate design of composite photocatalysts.

Modulating Charges of Dual Sites in Multivariate Metal-Organic Frameworks for Boosting Selective Aerobic Epoxidation of Alkenes.

Selective aerobic epoxidation of alkenes without any additives is of great industrial importance but still challenging because the competitive side reactions including C═C bond cleavage and isomerization are difficult to avoid. Here, we show fabricating Cu(I) single sites in pristine multivariate metal-organic frameworks (known as CuCo-MOF-74) via partial reduction of Cu(II) to Cu(I) ions during solvothermal reaction. Impressively, CuCo-MOF-74 is characteristic with single Cu(I), Cu(II), and Co(II) sites, and they exhibit the substantially enhanced selectivity of styrene oxide up to 87.6% using air as an oxidant at almost complete conversion of styrene, ∼25.8% selectivity increased over Co-MOF-74, as well as good catalytic stability. Contrast experiments and theoretical calculation indicate that Cu(I) sites contribute to the substantially enhanced selectivity of epoxides catalyzed by Co(II) sites. The adsorption of two O2 molecules on dual Co(II) and Cu(I) sites is favorable, and the projected density of state of the Co-3d orbital is closer to the Fermi level by modulating with Cu(I) sites for promoting the activation of O2 compared with dual-site Cu(II) and Co(II) and Co(II) and Co(II), thus contributing to the epoxidation of the C═C bond. When other kinds of alkenes are used as substrates, the excellent selectivity of various epoxides is also achieved over CuCo-MOF-74. We also prove the universality of fabricating Cu(I) sites in other MOF-74 with various divalent metal nodes.

Intrinsic Strain-Mediated Ultrathin Ceria Nanoantioxidant.

Metal oxide nanozymes have emerged as the most efficient and promising candidates to mimic antioxidant enzymes for treatment of oxidative stress-mediated pathophysiological disorders, but the current effectiveness is unsatisfactory due to insufficient catalytic performance. Here, we report for the first time an intrinsic strain-mediated ultrathin ceria nanoantioxidant. Surface strain in ceria with variable thicknesses and coordinatively unsaturated Ce sites was investigated by theoretical calculation analysis and then was validated by preparing ∼1.2 nm ultrathin nanoplates with ∼3.0% tensile strain in plane/∼10.0% tensile strain out of plane. Compared with nanocubes, surface strain in ultrathin nanoplates could enhance the covalency of the Ce-O bond, leading to increasing superoxide dismutase (SOD)-mimetic activity by ∼2.6-fold (1533 U/mg, in close proximity to that of natural SOD) and total antioxidant activity by ∼2.5-fold. As a proof of concept, intrinsic strain-mediated ultrathin ceria nanoplates could boost antioxidation for improved ischemic stroke treatment in vivo, significantly better than edaravone, a commonly used clinical drug.

Single Site Coordination Enabled Construction of Metal-Diketimine-Linked Covalent Organic Frameworks for Boosted Electrooxidation of Biomass Derivative.

Aromatic aldehydes are widely used for the construction of covalent organic frameworks (COFs). However, due to the high flexibility, high steric hindrance, and low reactivity, it remains challenging to synthesize COFs using ketones as building units, especially the highly flexible aliphatic ones. Here, the single nickel site coordination strategy is reported to lock the configurations of the highly flexible diketimine to transform discrete oligomers or amorphous polymers into highly crystalline nickel-diketimine-linked COFs (named as Ni-DKI-COFs). The strategy has been successfully extended to the synthesis of a series of Ni-DKI-COFs by the condensation of three flexible diketones with two tridentate amines. Thanks to the ABC stacking model with high amount and easily accessible single nickel (II) sites on their 1D channels, Ni-DKI-COFs are exploited as well-defined electrocatalyst platforms for efficiently electro-upgrading biomass-derived 5-Hydroxymethylfurfural (HMF) into value-added 2,5-furandicarboxylic acid (FDCA) with a 99.9% yield and a 99.5% faradaic efficiency as well as a high turnover frequency of 0.31 s-1 .

Modulation of Nano-superstructures and Their Optical Properties.

Self-assembly, which enables spontaneous arrangement of objects, is of particular importance for nanomaterials in both fundamental and applied research fields. Multiple types of nanoparticle superstructures have been successfully built in highly controllable and efficient manners through balancing the nanoscale interactions. Uniform and proper arrangement of nanoparticles inside the assembled superstructures is essential to exhibit their constant, reliable, and homogeneous functionalities. To be specific, the long-range ordered superlattices not only succeed with their building blocks' intrinsic property, but also, more importantly, can display collective properties that are absent both in individual nanoparticles and in their bulk states. One of the most attractive aspects of nanomaterials is their exceptional optical properties that have tremendous application potential in multidisciplinary fields. In this regard, constructing the superstructures from optical nano units like noble metal nanostructures, semiconductor nanoparticles, or hybrid nanomaterials is critical for attaining the unique optical properties and exploring their practical applications in multiple fields including photonics, optoelectronics, optical sensing, photocatalysis, etc. In this Account, we provide guidelines for self-assembly strategies to fabricate the superstructures and discuss the optical properties that the superstructures display. In the first part, we categorize and discuss the key factors that strongly affect the self-assembly process and determine the configurational and integral quality of the superstructures. On one hand, the diversity and designability of nanoparticles offer the intrinsic complexity of the building blocks, including geometry, size, composition, and surface ligand, which efficiently tailors the assembly process and superstructure configuration. On the other hand, multiple factors originating from the introduction of extrinsic features are recognized to facilitate the metastable or dynamic self-assembly process. Such extrinsic features include both matter like DNA origami, peptides, small molecules, etc. and nonmatter involved with electric fields, magnetic fields, light, temperature, etc. In the second part, we introduce the state-of the art progress on the collective optical performances of the assembled superstructures, including (1) chiral optics, such as circular dichroism and circularly polarized luminescence, (2) plasmonic properties and related applications, and (3) luminescence related optics and their applications. Finally, we summarize the existing problems and main challenges briefly, and some future directions of this field are proposed. We envision that, with deep understanding of the assembly mechanism and development of the synthetic and surface chemistry, rational modulation of nanoassemblies will be the trend of this field, which is beneficial to achieve the emerging collective performances and create new generation devices with advanced functions.

Copper Activation Enabling Reversible Aqueous Cu-ZnS Battery Chemistry.

The aqueous metal-sulfide batteries (AMSBs) have attracted research interest due to their high capacity, environmentally friendly qualities, and the accessibility of raw materials. However, the design strategies for metal-sulfide cathode have rarely been reported. Here, the copper-activated sphalerite in which Zn2+ is substituted by Cu2+ through ion exchange has been introduced for the first time as cathode for aqueous Cu/ZnS batteries. After sphalerite transformed to CuS, a two-step conversion of CuS→Cu7 S4 →Cu2 S storage mechanism has been proposed. At 0.7 A g-1 current density, the capacity can reach 532.4 mAh g-1 after 100 cycles. When cycled once at a current density of 35 mA g-1 , the initial reversible capacity can reach 461 mAh g-1 under 1 A g-1 . Furthermore, the assembled Zn//ZnS hybrid ion cell delivers an energy of up to 460 Wh kg-1 , which is better than for many AMSBs.