Fe and Mo Dual-Site Single-Atom Catalysts for High-Efficiency Wide-pH Hydrogen Evolution and Alkaline Overall Water Splitting

The aqueous zinc-ion battery (AZIB) is a promising option for grid-scale energy storage, but it faces challenges from parasitic water-related reactions and limited operational temperature range. Replacing H2O molecules in...

Weakly solvating aqueous-based electrolyte facilitated by a soft co-solvent for extreme temperature operations of zinc-ion batteries

Understanding the self-stacking interactions in precursors can facilitate the preparation of high-performance carbon materials and promote the commercial application of zinc ion hybrid capacitors (ZIHCs). Here, a π-conjugated molecule mediated pyrolysis strategy is presented to prepare carbon materials. Taking intermolecular force simulation (reduced density gradient plots) as a guide, the relationship between the self-stacking interactions in π-conjugated molecules and the structural parameters of carbon materials can be extrapolated. The resultant self-doped hierarchical porous carbons (NHPCs) derived from 1, 8, 4, 5-naphthalenetetracarboxdiimide with suitable self-stacking interactions empower the highest specific surface areas (2038 m2/g) and surface opening macropores. The NHPCs-based ZIHCs deliver a high capacity of 220 mAh/g, a high energy density of 149.5 Wh kg−1 and a super-stable cycle lifespan with 93.2 % capacity retention after 200, 000 cycles. The excellent electrochemical performance roots in the superior hierarchical porous structure with surface opening macropores, which guarantees the structural stability of carbon cathodes upon repeated rounds. Meanwhile, the heteroatom doping further relieves the kinetics concern of Zn2+ uptake/removal to enhance O-Zn-N binding particularly at high discharge currents. Besides, the proton-assisted Zn2+ dual-ion storage mechanism plays an essential role in the energy storage process. This work demonstrates a facile synthesis method and advances the fundamental understanding of its dual-ion storage mechanism. 

π-Conjugated molecule mediated self-doped hierarchical porous carbons via self-stacking interaction for high-energy and ultra-stable zinc-ion hybrid capacitors.

Rapid fabrication of FexNi2-xP4O12 and graphene hybrids as electrocatalyst for highly efficient oxygen evolution reaction

Active and stable oxygen evolution electrocatalysts are essential in increasing the efficiency of the water electrolyzers. The Ni2P/Fe(O)OH heterostructure nanoparticles are prepared via solvothermal phosphidization of Ni metal-organic frameworks (MOF) followed by immersing in Fe3+ aqueous solution. Characterizations reveal that the Ni2P/Fe(O)OH heterostructure nanoparticles are 12.83 nm in size averagely, and the heterointerface induces electron interactions between the Ni2P and Fe(O)OH phases. When used to catalyze OER in alkaline solutions, the Ni2P/Fe(O)OH-40/nickel foam (NF) is the most active and exhibits 240 mV overpotential to reach 10 mA cm-2 oxygen evolution (OER) current densities, which is significantly better than the Ni2P/NF. Lower apparent activation energy, charge transfer resistance, and Tafel slope, along with higher electron rate constant are observed at Ni2P/Fe(O)OH-40/NF, which suggests that the OER kinetics is more facile at the heterostructure surface. Both Ni2P/Fe(O)OH-40/NF and Ni2P/NF involve decoupled electron and proton transfer process, and higher degree of lattice oxygen oxidation mechanism (LOM) participation is observed at Ni2P/Fe(O)OH-40/NF, which results from the increased acidity of the Ni3+ sites. Density functional theory calculations prove that the formation of heterostructure with Fe(O)OH alters the band structure and the OER intermediate adsorption energies, that lead to lower energy barrier in the rate-determining step. The Ni2P/Fe(O)OH-40/NF is also stable towards OER in alkaline solutions. 

Construction of nickel phosphide/iron oxyhydroxide heterostructure nanoparticles for oxygen evolution

Aqueous zinc-ion batteries (AZIBs) are emerging as one of the most reliable energy storage technologies for scale-up application, but still suffer from the instability of Zn anode, which is mainly caused by the undesirable dendrite growth and side reactions. To tackle these issues, we formulate a new aqueous electrolyte with weak solvation effect by introducing low-dielectric-constant acetone to achieve H2O-poor solvation structure of Zn2+. Experimental and theoretical calculation studies concurrently reveal that such solvation structure can: i) relieve the solvated H2O related side reactions, ii) suppress the dendrite growth by boosting the desolvation kinetics of Zn2+ and iii) in-situ form solid electrolyte interface (SEI) to synergistically inhibit the side reaction and dendrite growth. The synergy of these three factors prolongs the cycling life of Cu/Zn asymmetric cell from 30 h to more than 800 h at 1 mA cm-2/1 mAh cm-2, and can work at more harsh condition of 5 mA cm-2/5 mAh cm-2. More encouragingly, Zn/V2O5·nH2O full cell also shows enhanced cycling stability of 95.9% capacity retention after 1000 cycles, much better than that with baseline electrolyte (failing at ~700th cycle).

Weak Solvation Effect Induced Optimal Interfacial Chemistry Enables Highly Durable Zn Anodes for Aqueous Zn-Ion Batteries.

Iron-induced electron modulation of nickel hydroxide/carbon nanotubes composite to effectively boost the oxygen evolution activity

Investigating dendrite-free stripping/plating anodes is highly significant for advancing the practical application of aqueous alkaline batteries. Sn has been identified as a promising candidate for anode material, but its deposition/dissolution efficiency is hindered by the strong electrostatic repulsion between Sn(OH)3 - and the substrate. Herein, this work constructs a nondense copper layer which serves as stannophile and hydrogen evolution inhibitor to adjust the tendency of competing reactions on Sn foil surface, thus achieving a highly reversible Sn anode. The interactions between the deposited Sn and the substrates are also strengthened to prevent shedding. Notably, the ratio of Sn redox reaction is significantly boosted from ≈20% to ≈100%, which results in outstanding cycling stability over 560 h at 10 mA cm-2 . A Sn//Ni(OH)2 battery device is also demonstrated with capacities from 0.94 to 22.4 mA h cm-2 and maximum stability of 1800 cycles.

Tendency Regulation of Competing Reactions Toward Highly Reversible Tin Anode for Aqueous Alkaline Batteries.

Sulfur doped NiCo2O4 nanosheets as advanced cathode for flexible alkaline Zn batteries

NiCo2O4 for alkaline Zn-based batteries (AZBs) suffers from low capacity and an unsatisfactory cycling life. Meanwhile, the widespread application of NiCo2O4 is seriously limited by costly and tedious synthetic procedures. In this work, a facile and economically efficient surface corrosion strategy is demonstrated to fabricate a high-performance Mn-doped NiCo2O4 (SMNC) nanosheet cathode for AZBs. Compares to the undoped NiCo2O4 (SNC), the SMNC shows enhanced mass transfer ability and increased active sites. Consequently, the Zn/SMNC cell reaches a big areal capacity of 0.58 mA h cm–2 at 2 mA cm–2 as well as an ultralong cycle life with 95% capacity retention over 6000 cycles. This work provides an effective, low-cost, and method to prepare advanced cathode materials for AZBs. 

Surface Corrosion Engineering Endows Mn-Doped NiCo2O4 Nanosheets with High Capacity and Long Life for Alkaline Zn-Based Batteries

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