ACS Catalysis
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2024
·
IF 11.3
Xue Yang,Lu Sun,Xingyu Liu,Zekai Yang,Han Sun,Weiwei Liu,Haijun Chen
The vacancy-engineering strategy has been successfully employed for electrochemical conversion by modulating the electronic structure and reaction kinetics of metal oxide-based electrode materials. The electrolysis of ammonia into hydrogen and nitrogen under mild conditions would be beneficial for utilizing ammonia as a zero-carbon fuel for mobile applications, such as cars and ships. Although platinum has been studied as the most effective state-of-the-art electrocatalyst for ammonia electrolysis, its high cost and rapid deactivation due to nitride poisoning make it difficult to be used commercially. Herein, we report that nanosized cerium oxides (CeOx) demonstrate highly efficient activity and enhanced stability for ammonia electrolysis in a nonaqueous electrolyte system. The Faradaic efficiency of N2 is approximately double that of a commercial Pt/C electrode, while its onset potential is lower than that of the latter. Cerium oxide with vacancy sites was found to be more favorable for NH3 adsorption and exhibits a significantly lower energy barrier for the initial step of NH3 dissociation compared to CeO2. Consequently, this contributes to the heightened activity of ammonia electrolysis on the electrode of cerium oxide following the G–M mechanism.
研究领域:
材料科学
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电化学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
Matter
·
2024
·
IF 17.3
Pei Li,Shuo Yang,Jiaxiong Zhu,Shengnan Wang,Yue Hou,Huilin Cui,Ze Chen,Rong Zhang,Zhuoxi Wu,Yiqiao Wang,Zhiquan Wei,Xinghui Liu,Shaoce Zhang,Xinliang Li,Chunyi Zhi
Chlorine-based electrochemical energy storage is a promising candidate for sustainable battery technology. The anionic redox reaction of Cl 0/−1 is of interest due to its superior redox potential (1.36 V vs . standard hydrogen electrode [SHE]), capacity (756 mAh g −1 ), high power, and low cost. Although Cl chemistry has been used in aqueous batteries for a long time, its deployment in organic lithium batteries has been significantly impeded due to the insolubility of Cl − ions (<0.1 M). Scarce oxidizable Cl − blocks redox reactions and the inevitable lithium chloride (LiCl) film passivates electrodes on discharge. We report a eutectic effect to improve the Cl − solubility in organic electrolytes (2 M or higher) by mixing a series of N-/P-centered chloride salts with lithium bis(trifluoromethanesulfonyl)imide at specific ratios. Based on an optimized Cl − concentration, a Li-Cl 2 cell using I as a chemical fixation can achieve a three-electron transfer with a specific capacity of 702 mAh g −1 and an energy density of 1,116 Wh kg −1 .
研究领域:
电化学
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能源材料科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Yihan Zhen,Cuijuan Zhang,Yongdan Li
Nonaqueous redox flow batteries (NARFBs) have promise for large-scale energy storage with high energy density. Developing advanced active materials is of paramount importance to achieve high stability and energy density. Herein, we adopt the molecular engineering strategy by coupling tetraalkylammonium and an ethylene glycol ether side chain to design anthraquinone-based ionic active species. By adjusting the length of the ethylene glycol ether chain, an ionic active species 2-((9,10-dioxo-9,10-dihydroanthracen-1-yl)amino)-N-(2-(2-methoxyethoxy)ethyl)-(N,N-dimethylethan-1-aminium)-bis(trifluoromethylsulfonyl)imide (AQEG2TFSI) with high solubility and stability is obtained. Paired with a FcNTFSI cathode, the full battery provides an impressive cycling performance with discharge capacity retentions of 99.96% and 99.74% per cycle over 100 cycles with 0.1 and 0.4 M AQEG2TFSI, respectively.
研究领域:
材料科学
·
能源存储技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yihan Zhen,Cuijuan Zhang,Yongdan Li
The non-aqueous redox flow battery (NARFB) is a very promising technology for the grid-scale energy storage; however, its wide application is seriously limited by the cycling stability. Here, we designed a ferrocene derivative by imidazole-functionalization and grafting an oligoether chain, 1-ferrocenylmethyl-3-(2-(2-(2-methoxyethoxy)ethoxy)ethyl) imidazolium-bis(trifluoromethylsulfonyl)imide (FcMITEGTFSI). The imidazolium cationic group induces a positive shift in the redox potential of the ferrocene core whilst ensuring the stability of the active species; the flexible oligoether side chain renders the molecule a liquid at room temperature (25 °C) and miscible with acetonitrile solvent. The flow battery shows robust cycling stability, with an overall discharge capacity retention of ≈95.5% after 200 cycles, corresponding to a capacity retention of ≈99.98% per cycle at 25 mA cm −2 with 0.1 M electrolyte.
研究领域:
能源存储技术
·
电化学材料
✓ 已验证
产品关联
DOI
高影响因子
Nature Nanotechnology
·
2025
·
IF 34.9
Wang Hansen,Yan Xiaolin,Zhang Rupeng,Sun Juanjuan,Feng Fuxiang,Li Haoran,Liang Jinding,Wang Yuchun,Ye Guangzhou,Luo Xiaonan,Huang Shengyuan,Wan Pan,Hung Samantha T.,Ye Fangjun,Chen Fangyun,Wu Erxiao,Zhou Jinfei,Ulissi Ulderico,Ge Xiaoming,Liu Chengyong,Xu Bo,Liu Na,Ouyang Chuying
Unwanted side reactions occurring at electrode|electrolyte interfaces significantly impact the cycling life of lithium metal batteries. However, a comprehensive view that rationalizes these interfacial reactions and assesses them both qualitatively and quantitatively is not yet established. Here, by combining multiple analytical techniques, we systematically investigate the interfacial reactions in lithium metal batteries containing ether-based non-aqueous electrolyte solutions. We quantitatively monitor various nanoscale-driven processes such as the reduction and oxidation pathways of lithium salt and organic solvents, the formation of various solid-electrolyte interphase species, the gas generation within the cell and the cross-talk processes between the electrodes. We demonstrate that the consumption of lithium ions owing to the continuous decomposition of the lithium bis(fluorosulfonyl)imide salt, which dominates the interfacial reactions, results in ion depletion during the cell discharge and battery failure. On the basis of these findings, we propose an electrolyte formulation in which lithium bis(fluorosulfonyl)imide content is maximized without compromising dynamic viscosity and bulk ionic conductivity, aiming for long-cycling battery performance. Following this strategy, we assemble and test Li (20 μm thickness)||LiNi 0.8 Mn 0.1 Co 0. 1 O 2 (17.1 mg cm − 2 of active material) single-layer stack pouch cells in lean electrolyte conditions (that is, 2.1 g Ah −1 ), which can effectively sustain 483 charge (0.2 C or 28 mA)/discharge (1 C or 140 mA) cycles at 25 °C demonstrating a discharge capacity retention of about 77%.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Joule
·
2024
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IF 38.6
Dongyang Shen,Xinhua Zheng,Ruihao Luo,Taoli Jiang,Mingming Wang,Mingying Zhang,Qia Peng,Li Song,Shiming Zhou,Zhiguo Hou,Yitai Qian,Wei Chen
Owing to their high volumetric capacity, reasonably low redox potential, and budget friendliness, manganese metal batteries (MnMBs) are excellent candidates for batteries with a high energy-to-price ratio. However, since there is no suitable electrolyte ensuring reversible Mn plating/stripping due to the low redox potential of the Mn 2+ /Mn redox couple and the strong interaction between charge-dense Mn 2+ ions and solvents, the development of MnMBs has been largely constrained. Herein, a halogen-mediated non-aqueous electrolyte (HM-NAE) is developed to enable highly reversible Mn plating/stripping. Benefiting from this halogen-mediated mechanism, the asymmetric Mn cell can cycle stably more than 1,000 h with a Coulombic efficiency close to 100%. Moreover, a Mn|HM-NAE|Mo 6 S 8 full cell with high electrochemical performances is constructed and fully understood. This work offers a new avenue to the development of rechargeable, non-aqueous MnMB through electrolyte engineering, which can also shed light on other multivalent metal batteries and electroplating industry.
研究领域:
材料科学
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电化学
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能源存储
✓ 已验证
DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
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2018
·Vol. 165
·期 5
·A757
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IF 3.662
Shijia Mu,Ding Zhu,Wei Liu,Shengrong Cai,Kaifang Zhang,Yungui Chen
Due to the sluggish oxygen reduction reaction (ORR) process of an O2 cathode, the power delivery of aprotic Li-O2 batteries (A-LOBs) is widely considered to be very poor. However, this work demonstrates the transient high-power output of A-LOBs based on the capacitive feature of the O2 cathode, including the intrinsic capacitance of cathode material and the ORR pseudocapacitance of the absorbed O2 on the cathode surface, by using graphene with high specific surface area. The O2 cathode delivers a high specific power of 12 026 W kggraphene−1 while also providing a large specific energy of 1216 Wh kggraphene−1. Pulse-discharge tests show that A-LOBs can achieve the transient high power output at high current via the "capacitor-type", while maintaining the high energy output at low current due to the "battery-type" (ORR). This work indicates that A-LOBs can deliver both high energy density and high transient power, which may be an appeal for the next-generation electric vehicles.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2022
·Vol. 13
·期 1
·1-13
·
IF 17.694
Zhang Ziheng,Avdeev Maxim,Chen Huaican,Yin Wen,Kan Wang Hay,He Guang
Prussian blue analogues (PBAs) are appealing active materials for post-lithium electrochemical energy storage. However, PBAs are not generally suitable for non-aqueous Li-ion storage due to their instability upon prolonged cycling. Herein, we assess the feasibility of PBAs with various lithium content for non-aqueous Li-ion storage. We determine the crystal structure of the lithiated PBAs via neutron powder diffraction measurements and investigate the influence of water on structural stability and Li-ion migration through operando X-ray diffraction measurements and bond valence simulations. Furthermore, we demonstrate that a positive electrode containing Li 2-x FeFe(CN) 6 ⋅ nH 2 O (0 ≤ x ≤ 2) active material coupled with a Li metal electrode and a LiPF 6 -containing organic-based electrolyte in coin cell configuration delivers an initial discharge capacity of 142 mAh g −1 at 19 mA g −1 and a discharge capacity retention of 80.7% after 1000 cycles at 1.9 A g −1 . By replacing the lithium metal with a graphite-based negative electrode, we also report a coin cell capable of cycling for more than 370 cycles at 190 mA g −1 with a stable discharge capacity of about 105 mAh g −1 and a discharge capacity retention of 98% at 25 °C.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2018
·
IF 5.116
Q. Xu,L.Y. Qin,Y.N. Ji,P.K. Leung,H.N. Su,F. Qiao,W.W. Yang,A.A. Shah,H.M. Li
Compared with conventional aqueous electrolyte , due to unique merits of deep eutectic solvents including a wide electrochemical window, ease in preparation, low vapor pressure and low cost, they have been used as electrolyte in the non-aqueous flow battery . This work reports a reline deep eutectic solvent, which is prepared as the anolyte and catholyte of a vanadium-iron redox flow battery . Since the solubility of the vanadium and iron species in deep eutectic solvent has been improved, an increased specific capacity can be obtained, up to 54.6% compared with the aqueous electrolyte one. However, the viscosity of this electrolyte is much larger than that of aqueous electrolyte, which causes more pumping losses. With the increase of operating temperature, the viscosity experiences a huge drop. The open-circuit voltage of such an non-aqueous system begins near 0.9 V with a decrease rate of 0.005 V h −1 , suggesting a better capacity retention ability than does the aqueous flow battery. The cycling performance of this redox flow battery is evaluated at a current density of 2.0 mA cm −2 under the temperature of 30 °C. The coulombic efficiency is up to 94.8%, while voltage efficiency and energy efficiency are just 68.3% and 64.7%, respectively. The low voltage efficiency stems from the sluggish redox kinetics of the vanadium ions , and large internal ohmic resistance. With an improved thermal stability, this vanadium-iron redox flow battery is preferred to be operated at elevated temperature, which helps to greatly reduce the ohmic loss and pumping loss, such that to increase the system energy efficiency.
研究领域:
电化学
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材料科学
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能源存储
✓ 已验证
DOI
高影响因子
Processes
·
2022
·Vol. 10
·期 4
·649
·
IF 3.352
Ping Lu,Peizhuo Sun,Qiang Ma,Huaneng Su,Puiki Leung,Weiwei Yang,Qian Xu
Redox flow batteries hold promise as large-scale energy storage systems for off-grid electrification. The electrolyte is one of the key components of redox batteries. Inspired by the mechanism involved in solvents for extraction, a ternary deep eutectic solvent (DES) is demonstrated, in which glycerol is introduced into the original binary ethaline DES. Redox pairs (active substance) dissolved in the solvent have low charge transfer resistance. The results show that the viscosity of the solvent with the ratio of choline chloride to ethylene glycol to glycerol of 1:2:0.5 decreases from 51.2 mPa·s to 40.3 mPa·s after adding the redox pair, implying that the mass transfer resistance of redox pairs in this solvent is reduced. Subsequent cyclic voltammetry and impedance tests show that the electrochemical performance with the ternary DES as the electrolyte in redox flow batteries is improved. When the ratio of 1:2:0.5 ternary DES is used as the electrolyte, the power density of the battery (9.01 mW·cm−2) is 38.2% higher than that of the binary one (6.52 mW·cm−2). Fourier transform infrared spectroscopy further indicates that the introduction of glycerol breaks the hydrogen bond network of the solvent environment where the redox pair is located, unraveling the hydrogen bond supramolecular complex. Rational solvent design is an effective strategy to enhance the electrochemical performance of redox batteries.
研究领域:
能源材料科学
·
电化学
✓ 已验证
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2020
·Vol. 30
·期 40
·2004247
·
IF 16.836
Maoxin Chen,Lei Wang,Xinghao Sheng,Tao Wang,Jian Zhou,Shengyang Li,Xiaohua Shen,Meng Zhang,Qiusheng Zhang,Xinzhi Yu,Jian Zhu,Bingan Lu
Potassium-ion hybrid capacitors (PIHCs) show great potential in large-scale energy storage due to the advantages of electrochemical capacitors and potassium-ion batteries. However, their development remains at the preliminary stage and is mainly limited by the kinetic imbalance between the two electrodes. Herein, an architecture of NbSe 2 nanosheets embedded in N, Se co-doped carbon nanofibers (NbSe 2 /NSeCNFs) as flexible, free-standing, and binder-free anodes for PIHCs is reported. The NbSe 2 /NSeCNFs with hierarchically porous structure and N, Se co-doping afford highly efficient channels for fast transportation of potassium ions and electrons during repeated cycling process. Furthermore, excellent electrochemical reversibility of the NbSe 2 /NSeCNFs electrode is demonstrated through in situ XRD, in situ Raman, ex situ transmission electron microscopy and element mapping. Thus, PIHCs with the NbSe 2 /NSeCNFs anode and active carbon cathode achieve a high energy of 145 W h kg −1 at a current density of 50 mA g −1 , as well as an ultra-long cycle life of over 10 000 cycles at a high current density of 2 A g −1 . These results indicate that the assembled PIHCs display great potential for applications in the field of ultra-long cycling energy storage devices.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Nanoscale Advances
·
2022
·Vol. 5
·期 2
·435-442
·
IF 5.598
Mao Chen,Hongning Chen
Nonaqueous redox flow batteries (NRFBs) have been regarded as promising large-scale electrochemical energy storage technology due to the wider solvent stable potential windows and greater selection of materials. However, the application of NRFBs is greatly limited considering the low capacity and high cost of active materials. In this work, we design and demonstrate a high-capacity polysulfide (PS)–polyiodide (PI) NRFB in Li-ion based 1,3-dioxolane (DOL) and 1,2-dimethoxyethane (DME) (v/v ∼ 1 : 1) organic electrolyte. The high solubility and low cost of PS (5 M) and PI (4 M) can achieve the high capacity and high applicability of NRFBs, which is attractive for realizing large-scale stationary energy storage. The highest volumetric capacity of 28 Ah L−1 based on a full cell is achieved with 1.5 M PS-4 M PI. The high coulombic efficiency (∼100%) and capacity retention (>99%) for 100 cycles in the PS–PI system is demonstrated by using a Li-ion conducting ceramic membrane. Voltage control is applied for both PS and PI to avoid the formation of irreversible solid Li2S and I2, which ensures the high stability of battery reaction. In situ UV-vis spectroscopy reveals the high reversibility of PS and PI in DOL/DME. A continuous flow mode test of the PS–PI system is also demonstrated to realize >300 hours stable cycling performance which implies good applicability for a long-term process. The successful demonstration of this high-capacity PS–PI nonaqueous system provides a new direction to promote the application of NRFBs in more fields.
研究领域:
能源存储技术
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）