An official website of the United States government
Abstract Ion‐insertion capacitors show promise to bridge the gap between supercapacitors of high power densities and batteries of high energy densities. While research efforts have primarily focused on Li+‐based capacitors (LICs), Na+‐based capacitors (SICs) are theoretically cheaper and more sustainable. Owing to the larger size of Na+compared to Li+, finding high‐rate anode materials for SICs has been challenging. Herein, an SIC anode architecture is reported consisting of TiO2nanoparticles anchored on a sheared‐carbon nanotubes backbone (TiO2/SCNT). The SCNT architecture provides advantages over other carbon architectures commonly used, such as reduced graphene oxide and CNT. In a half‐cell, the TiO2/SCNT electrode shows a capacity of 267 mAh g−1at a 1 C charge/discharge rate and a capacity of 136 mAh g−1at 10 C while maintaining 87% of initial capacity over 1000 cycles. When combined with activated carbon (AC) in a full cell, an energy density and power density of 54.9 Wh kg−1and 1410 W kg−1, respectively, are achieved while retaining a 90% capacity retention over 5000 cycles. The favorable rate capability, energy and power density, and durability of the electrode is attributed to the enhanced electronic and Na+conductivity of the TiO2/SCNT architecture.
more »
« less
This content will become publicly available on February 16, 2026
Stable Cycling of Sodium All‐Solid‐State Batteries with High‐Capacity Cathode Presodiation
Abstract Sodium all‐solid‐state batteries (NaSSBs) with an alloy‐type anode (e.g., Sn and Sb) offer superior capacity and energy density compared to hard carbon anode. However, the irreversible loss of Na+at the alloy anode during the initial cycle results in diminished capacity and stability, impairing full‐cell performance. This study presents an easy‐to‐implement cathode presodiation strategy by employing a Na‐rich material to address these challenges. Leveraging the high theoretical capacity and suitable voltage window, Na2S is chosen as the Na donor, which is activated by creating a mixed electron‐ion conducting network, delivering a high capacity of 511.7 mAh g−1. By adding a small amount (i.e., 3 wt.%) of Na2S to the cathode composite, a NaCrO2|| Sn full cell demonstrated capacity improvement from 90.8 to 118.2 mAh g−1(based on cathode mass). The capacity‐balanced full cell can thus cycle to more than 300 times with >90% capacity retention. This work provides a practical solution to enhance the full‐cell performance and advance the transformation from half‐cell to full‐cell applications of NaSSBs.
more »
« less
- Award ID(s):
- 2134764
- PAR ID:
- 10572137
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Energy Materials
- Volume:
- 15
- Issue:
- 23
- ISSN:
- 1614-6832
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
Abstract A full cell chemistry of aqueous dual‐ion battery (DIB) was reported, comprising the graphite cathode and 3,4,9,10‐perylenetetracarboxylic diimide (PTCDI) as the anode. This DIB employed a mixture aqueous electrolyte: 5 mtributylmethylammonium (TBMA) chloride plus 5 mMgCl2, where [MgCl3]−and TBMA+serve as the charge carriers for cathode and anode of the DIB, respectively. This novel full cell exhibited a specific capacity of around 41 mAh g−1based on the total active mass of both electrodes with an average operation voltage of 1.45 V and stable cycling for 400 cycles.more » « less
-
Abstract This is the first report of molybdenum carbide‐based electrocatalyst for sulfur‐based sodium‐metal batteries. MoC/Mo2C is in situ grown on nitrogen‐doped carbon nanotubes in parallel with formation of extensive nanoporosity. Sulfur impregnation (50 wt% S) results in unique triphasic architecture termed molybdenum carbide–porous carbon nanotubes host (MoC/Mo2C@PCNT–S). Quasi‐solid‐state phase transformation to Na2S is promoted in carbonate electrolyte, with in situ time‐resolved Raman, X‐ray photoelectron spectroscopy, and optical analyses demonstrating minimal soluble polysulfides. MoC/Mo2C@PCNT–S cathodes deliver among the most promising rate performance characteristics in the literature, achieving 987 mAh g−1at 1 A g−1, 818 mAh g−1at 3 A g−1, and 621 mAh g−1at 5 A g−1. The cells deliver superior cycling stability, retaining 650 mAh g−1after 1000 cycles at 1.5 A g−1, corresponding to 0.028% capacity decay per cycle. High mass loading cathodes (64 wt% S, 12.7 mg cm−2) also show cycling stability. Density functional theory demonstrates that formation energy of Na2Sx(1 ≤x ≤ 4) on surface of MoC/Mo2C is significantly lowered compared to analogous redox in liquid. Strong binding of Na2Sx(1 ≤x ≤ 4) on MoC/Mo2C surfaces results from charge transfer between the sulfur and Mo sites on carbides’ surface.more » « less
-
Abstract Developing low‐voltage carboxylate anode materials is critical for achieving low‐cost, high‐performance, and sustainable Na‐ion batteries (NIBs). However, the structure design rationale and structure‐performance correlation for organic carboxylates in NIBs remains elusive. Herein, the spatial effect on the performance of carboxylate anode materials is studied by introducing heteroatoms in the conjugation structure and manipulating the positions of carboxylate groups in the aromatic rings. Planar and twisted organic carboxylates are designed and synthesized to gain insight into the impact of geometric structures to the electrochemical performance of carboxylate anodes in NIBs. Among the carboxylates, disodium 2,2’‐bipyridine‐5,5’‐dicarboxylate (2255‐Na) with a planar structure outperforms the others in terms of highest specific capacity (210 mAh g−1), longest cycle life (2000 cycles), and best rate capability (up to 5 A g−1). The cyclic stability and redox mechanism of 2255‐Na in NIBs are exploited by various characterization techniques. Moreover, high‐temperature (up to 100 °C) and all‐organic batteries based on a 2255‐Na anode, a polyaniline (PANI) cathode, and an ether‐based electrolyte are achieved and exhibited exceptional electrochemical performance. Therefore, this work demonstrates that designing organic carboxylates with extended planar conjugation structures is an effective strategy to achieve high‐performance and sustainable NIBs.more » « less
-
Abstract A dual‐layer interphase that consists of an in‐situ‐formed lithium carboxylate organic layer and a thin BF3‐doped monolayer Ti3C2MXene on Li metal is reported. The honeycomb‐structured organic layer increases the wetting of electrolyte, leading to a thin solid electrolyte interface (SEI). While the BF3‐doped monolayer MXene provides abundant active sites for lithium homogeneous nucleation and growth, resulting in about 50% reduced thickness of inorganic‐rich components among the SEI layer. A low overpotential of less than 30 mV over 1000 h cycling in symmetric cells is received. The functional BF3 groups, along with the excellent electronic conductivity and smooth surface of the MXene, greatly reduce the lithium plating/stripping energy barrier, enabling a dendrite‐free lithium‐metal anode. The battery with this dual‐layer coated lithium metal as the anode displays greatly improved electrochemical performance. A high capacity‐retention of 175.4 mAh g−1at 1.0 C is achieved after 350 cycles. In a pouch cell with a capacity of 475 mAh, the battery still exhibits a high discharge capacity of 165.6 mAh g−1with a capacity retention of 90.2% after 200 cycles. In contrast to the fast capacity decay of pure Li metal, the battery using NCA as the cathode also displays excellent capacity retention in both coin and pouch cells. The dual‐layer modified surface provides an effective approach in stabilizing the Li‐metal anode.more » « less
