Aqueous zinc-ion batteries (AZIBs) are one of the promising energy storage systems, which consist of electrode materials, electrolyte, and separator. The first two have been significantly received ample development, while the prominent role of the separators in manipulating the stability of the electrode has not attracted sufficient attention. In this work, a separator (UiO-66-GF) modified by Zr-based metal organic framework for robust AZIBs is proposed. UiO-66-GF effectively enhances the transport ability of charge carriers and demonstrates preferential orientation of (002) crystal plane, which is favorable for corrosion resistance and dendrite-free zinc deposition. Consequently, Zn|UiO-66-GF-2.2|Zn cells exhibit highly reversible plating/stripping behavior with long cycle life over 1650 h at 2.0 mA cm-2, and Zn|UiO-66-GF-2.2|MnO2 cells show excellent long-term stability with capacity retention of 85% after 1000 cycles. The reasonable design and application of multifunctional metal organic frameworks modified separators provide useful guidance for constructing durable AZIBs. 

/pdf/metal-organic-frameworks-functionalized-separators-for-2nfyl7ug.pdf

Metal–Organic Frameworks Functionalized Separators for Robust Aqueous Zinc-Ion Batteries

Electrocatalytic oxygen reduction reaction (ORR), oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) have attracted widespread attention because of their important role in the application of various energy storage and conversion devices, such as fuel cells, metal-air batteries and water splitting devices. However, the sluggish kinetics of the HER/OER/ORR and their dependency on expensive noble metal catalysts (e.g., Pt) obstruct their large-scale application. Hence, the development of efficient and robust bifunctional or trifunctional electrocatalysts in nanodimension for both oxygen reduction/evolution and hydrogen evolution reactions is highly desired and challenging for their commercialization in renewable energy technologies. This review describes some recent developments in the discovery of bifunctional or trifunctional nanostructured catalysts with improved performances for application in rechargeable metal-air batteries and fuel cells. The role of the electronic structure and surface redox chemistry of nanocatalysts in the improvement of their performance for the ORR/OER/HER under an alkaline medium is highlighted and the associated reaction mechanisms developed in the recent literature are also summarized.

Multifunctional nanostructured electrocatalysts for energy conversion and storage: current status and perspectives.

Multifunctional interfacial engineering on the Zn anode to conquer dendrite growth, hydrogen evolution, and the sluggish kinetics associated with Zn deposition is highly desirable for boosting the commercialization of aqueous zinc‐ion batteries. Herein, a spontaneous construction of carbonyl‐containing layer on a Zn anode (Zn@ZCO) is rationally designed as an ion redistributor and functional protective interphase. It has strong zincphilicity and dendrite suppression ability due to the significant interaction of the highly electronegative and highly nucleophilic carbonyl oxygen, favoring ion transport and homogenizing Zn deposition effectively. On the other side, the hydrogen bond formed by the proton acceptor of oxygen atom in ZCO regulates the Zn‐ion desolvation process at the interfaces, thus bounding water activity and then mitigating water‐induced parasitic reactions. Consequently, the Zn@ZCO anode exhibits an extended cycling lifespan of 5000 h (>208 days) with a dendrite‐free surface and negligible by‐products. More encouragingly, the effectiveness is also convincing in NH4V4O10‐based full‐cells with excellent rate performance and cyclic stability. The stabilized Zn anode enabled by the strategy of spontaneous construction of functional solid electrolyte interphase brings forward a facile and instructive approach toward high‐performance zinc‐storage systems.

Spontaneous Construction of Nucleophilic Carbonyl‐Containing Interphase toward Ultrastable Zinc‐Metal Anodes

Achieving long-term stable zinc anodes at high currents/capacities remains a great challenge for practical rechargeable zinc-ion batteries. Herein, we report an imprinted gradient zinc electrode that integrates gradient conductivity and hydrophilicity for long-term dendrite-free zinc-ion batteries. The gradient design not only effectively prohibits side reactions between the electrolyte and the zinc anode, but also synergistically optimizes electric field distribution, zinc ion flux and local current density, which induces preferentially deposited zinc in the bottom of the microchannels and suppresses dendrite growth even under high current densities/capacities. As a result, the imprinted gradient zinc anode can be stably cycled for 200 h at a high current density/capacity of 10 mA cm-2/10 mAh cm-2, with a high cumulative capacity of 1000 mAh cm-2, which outperforms the none-gradient counterparts and bare zinc. The imprinted gradient design can be easily scaled up, and a high-performance large-area pouch cell (4*5 cm2) is also demonstrated. 

/pdf/gradient-design-of-imprinted-anode-for-stable-zn-ion-3s8j5yyb.pdf

Gradient design of imprinted anode for stable Zn-ion batteries

Ultrathin separators are indispensable to high‐energy‐density zinc‐ion batteries (ZIBs), but their easy failure caused by zinc dendrites poses a great challenge. Herein, 23 µm‐thick functional ultrathin separators (FUSs), realizing superb electrochemical stability of zinc anodes and outstanding long‐term durability of ultrathin separators, are reported. In the FUSs, an ultrathin but mechanically strong nanoporous membrane substrate benefits fast and flux‐homogenized Zn2+ transport, while a metal–organic framework (MOF)‐derived C/Cu nanocomposite decoration layer provides rich low‐barrier zinc nucleation sites, thereby synergistically stabilizing zinc anodes to inhibit zinc dendrites and dendrite‐caused separator failure. Investigation of the zinc affinity of the MOF‐derived C/Cu nanocomposites unravels the high zincophilicity of heteroatom‐containing C/Cu interfaces. Zinc anodes coupled with the FUSs present superior electrochemical stability, whose operation lifetime exceeds 2000 h at 1 mA cm−2 and 600 h at 10 mA cm−2, 40–50 times longer than that of the zinc anodes using glass‐fiber separators. The reliability of the FUSs in ZIBs and zinc‐ion hybrid supercapacitors is also validated. This work proposes a new strategy to stabilize zinc anodes and provides theoretical guidance in developing ultrathin separators for high‐energy‐density zinc‐based energy storage.

Functional Ultrathin Separators Proactively Stabilizing Zinc Anodes for Zinc‐Based Energy Storage

The practical application of Zn‐metal anodes (ZMAs) is mainly impeded by the limited lifespan and low Coulombic efficiency (CE) resulting from the Zn dendrite growth and side reactions. Herein, a 3D multifunctional host consisting of N‐doped carbon fibers embedded with Cu nanoboxes (denoted as Cu NBs@NCFs) is rationally designed and developed for stable ZMAs. The 3D macroporous configuration and hollow structure can lower the local current density and alleviate the large volume change during the repeated cycling processes. Furthermore, zincophilic Cu and in‐situ‐formed Cu–Zn alloy can act as homogeneous nucleation sites to minimize the Zn nucleation overpotential, further guiding uniform and dense Zn deposition. As a result, this Cu NBs@NCFs host exhibits high CE of Zn plating/stripping for 1000 cycles. The Cu NBs@NCFs–Zn electrode shows low voltage hysteresis and prolonged cycling life (450 h) with dendrite‐free behaviors. As a proof‐of‐concept demonstration, a Zn‐ion full cell is fabricated based on this Cu NBs@NCFs–Zn anode, which demonstrates decent rate capability and improved cycling performance.

Nitrogen‐Doped Carbon Fibers Embedded with Zincophilic Cu Nanoboxes for Stable Zn‐Metal Anodes

Single-atom catalysts (SACs) are being pursued as economical electrocatalysts. However, their low active-site loading, poor interactions, and unclear catalytic mechanism call for significant advances. Herein, atomically dispersed Ni/Co dual sites anchored on nitrogen-doped carbon (a-NiCo/NC) hollow prisms are rationally designed and synthesized. Benefiting from the atomically dispersed dual-metal sites and their synergistic interactions, the obtained a-NiCo/NC sample exhibits superior electrocatalytic activity and kinetics towards the oxygen evolution reaction. Moreover, density functional theory calculations indicate that the strong synergistic interactions from heteronuclear paired Ni/Co dual sites lead to the optimization of the electronic structure and the reduced reaction energy barrier. This work provides a promising strategy for the synthesis of high-efficiency atomically dispersed dual-site SACs in the field of electrochemical energy storage and conversion.

Highly Efficient Electrocatalytic Oxygen Evolution Over Atomically Dispersed Synergistic  Ni/Co Dual Sites.

Hybrid materials, integrating the merits of individual components, are ideal structures for efficient oxygen evolution reaction (OER). However, the rational construction of hybrid structures with decent physical/electrochemical properties is yet challenging. Herein, a promising OER electrocatalyst composed of trimetallic metal‐organic frameworks supported over S/N‐doped carbon macroporous fibers (S/N‐CMF@FexCoyNi1‐x‐y‐MOF) via a cation‐exchange strategy is delicately fabricated. Benefiting from the trimetallic composition with improved intrinsic activity, hollow S/N‐CMF matrix facilitating exposure of active sites, as well as their robust integration, the resultant S/N‐CMF@FexCoyNi1‐x‐y‐MOF electrocatalyst delivers outstanding activity and stability for alkaline OER. Specifically, it needs an overpotential of 296 mV to reach the benchmark current density of 10 mA cm−2 with a small Tafel slope of 53.5 mV dec−1. In combination with X‐ray absorption fine structure spectroscopy and density functional theory calculations, the post‐formed Fe/Co‐doped γ‐NiOOH during the OER operation is revealed to account for the high OER performance of S/N‐CMF@FexCoyNi1‐x‐y‐MOF.

Supporting Trimetallic Metal‐Organic Frameworks on S/N‐Doped Carbon Macroporous Fibers for Highly Efficient Electrocatalytic Oxygen Evolution

Zn dendrite growth and undesired parasitic reactions severely restrict the practical use of deep-cycling Zn metal anodes (ZMAs). Herein, we demonstrate an elaborate design of atomically dispersed Cu and Zn sites anchored on N,P-codoped carbon macroporous fibers (denoted as Cu/Zn-N/P-CMFs) as a three-dimensional (3D) versatile host for efficient ZMAs in mildly acidic electrolyte. The 3D macroporous frameworks can alleviate the structural stress and suppress Zn dendrite growth by spatially homogenizing Zn2+ flux. Moreover, the well-dispersed Cu and Zn atoms anchored by N and P atoms maximize the utilization as abundant active nucleation sites for Zn plating. As expected, the Cu/Zn-N/P-CMFs host presents a low Zn nucleation overpotential, high reversibility, and dendrite-free Zn deposition. The Cu/Zn-N/P-CMFs-Zn electrode exhibits stable Zn plating/stripping with low polarization for 630 h at 2 mA cm-2 and 2 mAh cm-2. When coupled with a MnO2 cathode, the fabricated full cell also shows impressive cycling performance even when tested under harsh conditions.

Atomically Dispersed Zincophilic Sites in N,P-Codoped Carbon Macroporous Fibers Enable Efficient Zn Metal Anodes.

Manipulating the intrinsic activity of heterogeneous catalysts at the atomic level is an effective strategy to improve the electrocatalytic performances but remains challenging. Here, atomically dispersed Ni anchored on CeO2 particles entrenched on peanut-shaped hollow nitrogen-doped carbon structures (a-Ni/CeO2@NC) is rationally designed and synthesized. The as-prepared a-Ni/CeO2@NC catalyst exhibits substantially boosted intrinsic activity and greatly reduced overpotential for the electrocatalytic oxygen evolution reaction. Experimental and theoretical results demonstrate that the decoration of isolated Ni species over the CeO2 induces electronic coupling and redistribution, thus resulting in the activation of the adjacent Ce sites around Ni atoms and greatly accelerated oxygen evolution kinetics. This work provides a promising strategy to explore the electronic regulation and intrinsic activity improvement at the atomic level, thereby improving the electrocatalytic activity.

https://www.science.org/doi/pdf/10.1126/sciadv.adh1320?download=true

Atomically dispersed Ni activates adjacent Ce sites for enhanced electrocatalytic oxygen evolution activity

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Nitrogen‐Doped Carbon Fibers Embedded with Zincophilic Cu Nanoboxes for Stable Zn‐Metal Anodes

Highly Efficient Electrocatalytic Oxygen Evolution Over Atomically Dispersed Synergistic Ni/Co Dual Sites.

Supporting Trimetallic Metal‐Organic Frameworks on S/N‐Doped Carbon Macroporous Fibers for Highly Efficient Electrocatalytic Oxygen Evolution

Atomically Dispersed Zincophilic Sites in N,P-Codoped Carbon Macroporous Fibers Enable Efficient Zn Metal Anodes.

Atomically dispersed Ni activates adjacent Ce sites for enhanced electrocatalytic oxygen evolution activity