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Small · 2024 · IF 13

Harmonizing Wide Voltage Window and High Energy Density toward Asymmetric All-Solid-State Supercapacitor

Gang Zhao,Huanchi Chen,Bingzhe Jia,Shanshan Bai,Xinrui Qiang,Xinming Wu

All-solid-state supercapacitors are known for their safety, stability, and excellent cycling performance. However, their limited voltage window results in lower energy density, restricting their widespread application in practical scenarios. Therefore, in this work, CC/MoO 3 @Ti 3 C 2 T x negative electrode and Mo 1 Al 1 -MnO 2 /CC positive electrode materials are synthesized and prepared by electrochemical deposition co-coating and one-step hydrothermal methods, respectively, and assembled into an asymmetric supercapacitor (ASC) device based on the two electrode materials. The study reveals that the surface capacitances of the positive and negative electrodes are 1685.5 mF cm −2 and 1134.98 mF cm −2 correspondingly, with potential windows of both as high as 1.1 V. Surprisingly, the potential window of the all-solid-state supercapacitor assembled based on the two electrodes reaches 2.2 V, and the energy density reaches 0.44 m W h cm −2 , which is much higher than the performance indicators based on similar electrodes. The resulting excellent performance parameters are mainly attributed to the efficient synergy between the pseudo-capacitance effect of the MoO 3 film and the high electrical conductivity of the Ti 3 C 2 T x sheets, as well as the great improvement of the intrinsic electron mobility and ion diffusion channel stability of MnO 2 by Mo and Al bimetallic doping.

研究领域: 材料科学 · 能源存储
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JOURNAL OF POWER SOURCES · 2022 · IF 9.794

3D hierarchical porous carbon from fulvic acid biomass for high energy density supercapacitor with high withstanding voltage

Panpan Chang,Jie Zheng,Yongbing Cen,Fan Yang,Xuguang Li,Qingruo Xie,Jinshi Dong

Biomass-derived porous carbons (BD-PC) have evoked wide attention in the field of supercapacitors . However, the oxygen-containing groups (OFGs) in BD-PC bring a great threat to the structural stability of porous carbons in organic electrolyte at the voltage window higher than 2.7 V. Therefore, it is a worthwhile challenge to construct BD-PC with very-low content of OFGs which can operate stably at the ultrahigh voltage window. Herein, the green and renewable fulvic acid biomass is used as carbon precursor to construct 3D hierarchical porous carbon (HPC) with high yield of 13.3% by KOH activation and annealing method. This HPC presents continuous carbon network with ultrathin nanosheets of 50 nm. It has high specific surface area of 3028 m 2  g −1 , good e -conductivity of 43 S m −1 , ultrahigh C/O ratio of 27.4 and high sp 2 carbon content of 90%. Thus, the voltage window upper limits can be raised up to 3 V in TEABF 4 /PC and 3.5 V in EMIMBF 4 electrolytes. In TEABF 4 /PC electrolyte, this HPC displays high C g of 124 F g −1 at 0.05 A g −1 with C 10/0.05 as high as 70.8% and ultralong lifespan of 94% after 20,000 cycles. In EMIMBF 4 electrolyte, the energy density can reach up to 56.6 Wh kg −1 .

研究领域: 材料科学 · 能源存储
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Self-supported VO(PO3)2 electrode for 2.8 V symmetric aqueous supercapacitors

Yujing Liu,Qi Liu,Xin Zhou,Xiaohui Liu,Mingyue Li,Zhongqiu Liu,Anguo Ying

Improving the voltage window of aqueous supercapacitors beyond 2.5 V without diminishing their capacitance performance is a big challenge to achieve excellent energy density because of the undesirable water decomposition. Herein, this study developed a novel vanadium phosphate (VPO) of the VO(PO 3 ) 2 aerogel as the electrode to enlarge the device voltage, which could effectively raise HER/OER overpotentials and thus achieving a stable wide electrochemical window of −1 ∼ 1 V (vs. SCE) with remarkably improved capacitance. The VPO microstructure is organized by nanowire-stacked lamellar bricks via engineering a controllable phase-transformation using the V-P-citric acid-aerogel as the precursor. Examined as the supercapacitor electrode, in-situ X-ray powder diffraction analysis uncovers that the VO(PO 3 ) 2 undergoes a reversible phase-transformation reaction associated with Na + intercalation/de-intercalation in Na 2 SO 4 and a typical redox pseudocapacitance process in KOH. For the first time, a 2.8 V symmetric aqueous supercapacitor was further assembled with an energy density of 123.1 Wh kg −1 at the power density of 580 W kg −1 , which is much superior to those of all reported V-base supercapacitors. The underlying mechanisms of the VO(PO 3 ) 2 on ultrahigh voltage window and charge storage are further elucidated, which provide the fundamental guidance for structuring VPO-based electrodes used for commercial energy storage devices.

研究领域: 材料科学 · 电化学 · 能源存储
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ChemElectroChem · 2020 ·Vol. 7 ·期 4 ·928-936 · IF 4.154

Maximized Energy Density of RuO2//RuO2 Supercapacitors through Potential Dependence of Specific Capacitance

Yilun Wang,Dawei Gu,Jiaren Guo,Mingyang Xu,Hongshun Sun,Jishu Li,Lei Wang,Linjiang Shen

Graphical One step at a time : A stepwise cyclic voltammetry approach is proposed to construct the potential dependence of specific capacitance. The working voltage window and energy density of RuO 2 //RuO 2 supercapacitors (SCs) are maximized by modulating the mass ratio based on the relationship between specific capacitance and potential. The voltage window and energy density of RuO 2 //RuO 2 with m + /m − =3.03 reach 0.750 V and 4.81 Wh/kg, respectively. These values are 188 % and 304 % higher than those of RuO 2 //RuO 2 with a mass ratio of 0.56. The source of wasted potential window on the electrodes in RuO 2 //RuO 2 is explained in an effort to design and produce better SCs. In this study, a stepwise cyclic voltammetry approach was proposed to clarify the potential dependence of specific capacitance for reduced graphene oxide and ruthenium oxide electrodes. Based on the relationship between specific capacitance and potential, the working voltage window and energy density of RuO 2 //RuO 2 supercapacitors (SCs) were maximized by modulating the mass ratio. The working voltage window of RuO 2 //RuO 2 with a mass ratio of 2.03 (close to optimum mass ratio ) was extended by about 188 % when compared to that calculated at a mass ratio of 0.56. The former was equivalent to a 304 % increase in energy density. In addition, the source of wasted potential window of electrodes on RuO 2 //RuO 2 was investigated in an effort to design and produce better SCs.

研究领域: 材料科学 · 电化学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2022 · IF 9.965

Design of Boron Carbonitrides-Polyaniline (BCN-PANI) assembled supercapacitor with high voltage window

Dong Shi,Mingzhi Yang,Baoguo Zhang,Haixiao Hu,Zizheng Ai,Yongliang Shao,Jianxing Shen,Yongzhong Wu,Xiaopeng Hao

Boron carbonitrides (BCN) have been widely concerned in the field of energy storage and conversion. However, the energy storage mechanism of electrical double-layer behavior and their stacked-layer structure severely limit the improvement of capacitance, thereby hindering their further development in energy storage. Therefore, an ultrasonic-ball milling method was first chosen to obtain BCN nanosheets, together with a feasible way of polyaniline (PANI) modification performed to boost the capacitive reaction of BCN nanosheets. For the first time, a BCN-PANI-based symmetric supercapacitor device can reach a high voltage window of 3.0 V when 1 M Et 4 N·BF 4 was chosen as the electrolyte. The working voltage of 3.0 V is three times that of a device with pure PANI with the ultrahigh energy density of 67.1 W h kg −1 , superior to most of the reported PANI-based devices. The eminent electrochemical performance provides a promising strategy to pave the way for configuring carbon-based multiple composite electrodes for other energy storage devices.

CAS / MDL: 62-53-3
研究领域: 材料科学 · 能源存储
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SYNTHETIC METALS · 2020 · IF 3.286

Enhanced electrochemical performance and high voltage window for supercapacitors based on fabric electrodes derived from tannin-Fe3+ complexes

Lei Hu,Limin Zang,Wusheng Zuo,Qifan Liu,Chao Yang,Chunliu Liang,Jianhui Qiu

The acquisition of high energy density for aqueous supercapacitors (SCs) is effective in extending the operating voltage and increasing the capacitance, which has drawn a great deal of attention in recent years. A scalable approach has been proposed by dip coating and carbonizing tannin-Fe 3+ (TA-Fe 3+ ) coordination compounds to prepare fabric electrodes, which can provide tannin carbon (TC) and Fe 3 O 4 for extended voltage windows and high specific capacitances, respectively. A fabric electrode with a chemically stable carbon core-shell structure was shown to improve its decomposition overpotential of water, which contributed to a wide operating voltage of 2.4 V for aqueous symmetric supercapacitors (SSCs). The assembled all solid-state SSCs achieved both an ultrahigh energy density of 51.26 μWh cm −2 , which was higher than most SSCs and even some asymmetric SCs, and the ability to connect them in series to function as practical energy storage devices. This work opens up the possibility for high operating voltage aqueous SCs and even more possibilities for SCs.

CAS / MDL: 7705-08-0 1401-55-4
研究领域: 材料科学 · 能源存储技术
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Energy & Environmental Science · 2023 ·Vol. 16 ·期 10 ·4679-4692 · IF 32.5

A wide temperature 10 V solid-state electrolyte with a critical current density of over 20 mA cm−2

Yiqi Wei,Zhenglong Li,Zichong Chen,Panyu Gao,Mingxi Gao,Chenhui Yan,Zhijun Wu,Qihang Ma,Yinzhu Jiang,Xuebin Yu,Xin Zhang,Yongfeng Liu,Yaxiong Yang,Mingxia Gao,Wenping Sun,Zhiguo Qu,Jian Chen,Hongge Pan

The use of solid-state electrolytes in all-solid-state batteries is a technology with prospects for increasing energy densities. However, poor oxidative stability and issues with dendrite growth significantly hamper their applicability. LiBH4 is considered as one of the most promising candidates due to the thermodynamic stability of Li. Herein, an in situ melting reaction is proposed to generate covalently bonded coordination on the particle surfaces of electrolytes to resolve these issues. This coordination thermodynamically shuts down the electronic exchanges during the anionic oxidation decomposition by covalently bonding the local high-concentration electrons on the anions, and it kinetically blocks electronic percolation on the particle surfaces of electrolytes; this phenomenon leads to an unprecedented voltage window (0–10 V) with a peak oxidation current that is 97.2 times lower and an electronic conductivity that is 3 orders of magnitude lower than that of the counterpart at 25 °C. The coordination can act as a binder to bond electrolyte particles, achieving a remarkable Young's modulus of 208.45 GPa; this modulus is twice as high as that of the counterpart. The remarkable mechanical property of the coordination is capable of adapting the sustained stress–strain release in Li plating and stripping. With these merits, the electrolyte displays a record-breaking critical current density of 21.65 mA cm−2 at 25 °C (twice the best-reported data in Li-ion solid-state electrolytes), cycling stabilities at 10.83 mA cm−2 for 6000 h and under 10 V for 1000 h, and an operational temperature window of −30 to 150 °C. The Li–LiCoO2 cells exhibit superior reversibility at high voltage. Our findings illuminate a clear direction for oxidative stability and dendrite suppression in solid-state electrolytes, making tremendous progress in high-voltage lithium batteries.

研究领域: 材料科学 · 电化学
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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

High-Voltage aqueous supercapacitors based on l-lysine pH Self-Buffering Coating-modified carbon cloth electrode

Ang Xu,Jie Gao,Huan Li,Xiyu Song,Bo Xu,Ying Liu,Yuanyuan Yu,Ping Wang,Qiang Wang,Man Zhou

Achieving a high working voltage window beyond the water electrolysis limit (1.23 V) is always a challenge for aqueous supercapacitors (SCs). Increasing the oxygen evolution reaction (OER) overpotential or hydrogen evolution reaction (HER) overpotential of the carbon-based electrode is an effective way to broaden the voltage window of SCs. In this work, we propose an efficient strategy of surface engineering to autonomously regulate the pH of the electrode/electrolyte interface microenvironment by using the amphoteric dissociation of amino acids, which suppress the OER and consequently broadens voltage window. L-Lysine was modified on the surface of carbon cloth to prepare the SC positive electrode. The voltage window of SCs based on L-Lysine modified electrode is enhanced from 1.2 V to 1.5 V and the energy density has increased by 59.42 % at 0.5 A g −1 . This is a promising strategy to design and engineer carbon-based aqueous SCs with a boosted energy density.

研究领域: 材料科学 · 电化学 · 能源存储
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Journal of Materials Chemistry A · 2024 ·Vol. 12 ·期 22 ·13106-13115 · IF 10.7

The role of Mn in widening the potential window of solid solution derived electrodes for aqueous supercapacitors

Ziying Shi,Enzuo Liu,Biao Chen,Junwei Sha,Lihua Qian,Zhijia Zhang,Xiaopeng Han,Wenbin Hu,Chunnian He,Naiqin Zhao,Jianli Kang

The interaction mechanism of the multi-element oxide electrodes remains a challenge, despite the fact that their synergy can not only improve the electronic structure, but also broaden the working potential window to some extent. Herein, the simple NiMn alloy system was taken up as a model to investigate the origin of the wide voltage window. Compared with conventional electrodes, this sandwich-type nanoporous-NiO(MnOx)@Ni electrode derived from a NiMn alloy could exhibit a wide working potential window of 1.5 V in aqueous electrolyte. The facilitated successive redox reactions between NiO and MnOx throughout the entire potential window strongly promote the capacitance extension without water decomposition, despite the fact that the cycling lifespan was limited by chemical dissolution of MnOx. The assembled quasi-solid-state supercapacitor can overcome the irreversible conversion and exhibit a remarkable lifespan of 5000 cycles at 10 A cm−3 (91% retention) and high energy density (37.67 mW h cm−3 at 0.2 A cm−3). This work provides new perceptions for the design of multi-element collaborative energy storage electrodes.

CAS / MDL: 7783-20-2
研究领域: 材料科学 · 电化学
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CARBON · 2024 · IF 10.5

High-voltage aqueous supercapacitors enabled by polysiloxane passivation coating-modified carbon cloth electrode

Wenjun Meng,Huan Li,Zengyu Luo,Yifan Cui,Ang Xu,Chengjian Yao,Ping Wang,Qiang Wang,Man Zhou

The voltage window plays a crucial role in determining the energy density of supercapacitors. The limited energy density of carbon-based supercapacitors poses a significant challenge to their widespread adoption. Here, we propose a novel approach to modify carbon cloth by implementing a polysiloxane (PSiO) passivation coating. This forms an ion-conductive and electron-insulating thin film on the surface, effectively impeding electron conduction from electrode surface to electrode/electrolyte interface and suppressing electrolyte electrolysis. Consequently, an expanded voltage window is realized, thereby enhancing the energy density of aqueous carbon-based supercapacitors. The carbon cloth electrode modified with the PSiO passivation coating (CC-A-KH560) exhibits exceptional electrochemical performance, with a significantly increased 78.6 % widened applicable potential range compared to the activated carbon cloth electrode (CC-A). In a two-electrode configuration, the voltage window is broadened from 0.8 V for CC-A to 1.4 V for CC-A-KH560, and the energy density based on CC-A-KH560 is 8 times that based on CC-A. The good stability and durability are also obtained for the firm C–O–Si bonds during PSiO modification. More importantly, this design provides a generic solution of PSiO passivation coating-modified carbon electrode, applicable for diversified silicane couple agents, to realize a high-voltage energy storage performance for aqueous supercapacitors.

研究领域: 材料科学 · 电化学
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Energy & Environmental Materials · 2023 · IF 15

Strong Interaction Between Redox Mediators and Defect-Rich Carbons Enabling Simultaneously Boosted Voltage Windows and Capacitance for Aqueous Supercapacitors

Lu Guan,Yifan Zhu,Yi Wan,Mengdi Zhang,Qiang Li,Xiaoling Teng,Yunlong Zhang,Hao Yang,Yan Zhang,Han Hu,Mingbo Wu

Energy density, the Achilles' heel of aqueous supercapacitors, is simultaneously determined by the voltage window and specific capacitance of the carbon materials, but the strategy of synchronously boosting them has rarely been reported. Herein, we demonstrate that the rational utilization of the interaction between redox mediators (RMs) and carbon electrode materials, especially those with rich intrinsic defects, contributes to extended potential windows and more stored charges concurrently. Using 4-hydroxy-2,2,6,6-tetramethylpiperidinyloxyl (4OH-TEMPO) and intrinsic defect-rich carbons as the RMs and electrode materials, respectively, the potential window and capacitance are increased by 67% and sixfold in a neutral electrolyte. Moreover, this strategy could also be applied to alkaline and acid electrolytes. The first-principle calculation and experimental results demonstrate that the strong interaction between 4OH-TEMPO and defect-rich carbons plays a key role as preferential adsorbed RMs may largely prohibit the contact of free water molecules with the electrode materials to terminate the water splitting at elevated potentials. For the RMs offering weaker interaction with the electrode materials, the water splitting still proceeds with a thus sole increase of the stored charges. The results discovered in this work could provide an alternative solution to address the low energy density of aqueous supercapacitors.

CAS / MDL: 5144-89-8
研究领域: 材料科学 · 电化学
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Wide-voltage-window amphiphilic supramolecule excluded-volume electrolytes for ultra-durable full-cell aqueous potassium-Ion batteries

Jie Wei,Pengbo Zhang,Yuzhu Liu,Mengfei Zhu,Tengfei Dai,Zuoxiu Tie,Zhong Jin

Aqueous potassium-ion batteries (AKIBs) are promising candidates for large-scale energy storage. However, the performance of AKIBs is restricted the dissolution of electrode materials and the narrow voltage window of aqueous electrolytes. Herein, we report the amphiphilic supramolecule modified aqueous K-ion electrolytes with synergistic functions of excluded-volume effect and hydrogen bond networks, which greatly reduce the activity of water molecules, inhibit the dissolution of active materials, and expand the operation voltage window (>3.4 V). Moreover, the as-assembled full-cell AKIBs exhibit an open-circuit voltage of 2.0 V, good rate capability, wide operating temperature range (−20 to 90 °C), and ultralong cycling life (with a capacity retention of 97.8 % after 10,000 cycles at 10 C). The study makes it possible for aqueous electrolytes to possess wide voltage window and temperature endurance, greatly expanding the choices of practicable electrolyte and paving the way of high-voltage aqueous batteries towards sustainable, safety and low-cost energy storage.

研究领域: 材料科学 · 电化学 · 能源存储
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