Journal of Energy Chemistry
·
2025
·
IF 14.9
Botao Zhang,Yongxin Huang,Shengyu Gao,Ning Zhang,Yang Mei,Yanting Huang,Taifeng Ding,Xin Hu,Li Li,Feng Wu,Renjie Chen
Aqueous zinc-ion batteries (AZIBs) are pivotal for achieving net-zero goals, yet their commercialization is impeded by zinc dendrites, parasitic reactions, and interfacial instability. Current debates persist on the interplay between zincophilic-hydrophilic and zincophobic-hydrophobic interactions at the anode-electrolyte interface. Herein, a conceptual framework that decouples these competing effects was proposed, enabling the rational design of a dual-layer architecture with an inner zincophilic layer for Zn 2+ flux homogenization and an outer hydrophobic layer for water shielding. Through in situ and ex situ analyses, the synergistic mechanism was elucidated. During the cycling process, the zincophilic interface guides uniform Zn deposition, while the hydrophobic coating suppresses H 2 O-induced side reactions. This dual modification achieves a Zn||Cu cell with an unprecedented 99.89% Coulombic efficiency and 975-cycle stability. This work resolves the long-standing controversy over interfacial affinity design, offering a scalable and industrially viable strategy to enhance AZIBs’ durability without sacrificing energy density.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
iScience
·
2021
·
IF 5.458
Xiyang Cai,Cehuang Fu,Haldrian Iriawan,Fan Yang,Aiming Wu,Liuxuan Luo,Shuiyun Shen,Guanghua Wei,Yang Shao-Horn,Junliang Zhang
Summary Green synthesis of ammonia by electrochemical nitrogen reduction reaction (NRR) shows great potential as an alternative to the Haber-Bosch process but is hampered by sluggish production rate and low Faradaic efficiency. Recently, lithium-mediated electrochemical NRR has received renewed attention due to its reproducibility. However, further improvement of the system is restricted by limited recognition of its mechanism. Herein, we demonstrate that lithium-mediated NRR began with electrochemical deposition of lithium, followed by two chemical processes of dinitrogen splitting and protonation to ammonia. Furthermore, we quantified the extent to which the freshly deposited active lithium lost its activity toward NRR due to a parasitic reaction between lithium and electrolyte. A high ammonia yield of 0.410 ± 0.038 μg s −1 cm −2 geo and Faradaic efficiency of 39.5 ± 1.7% were achieved at 20 mA cm −2 geo and 10 mA cm −2 geo, respectively, which can be attributed to fresher lithium obtained at high current density.
研究领域:
化学
·
材料科学
·
环境科学
✓ 已验证
DOI
高影响因子
Journal of Energy Storage
·
2025
·
IF 9.8
Jiaqi Leng,Xiaofang Wang,Dan Li,Ruru Shi,Xingyun Zhu,Longsheng Cao,Qingda An
Aqueous zinc ion batteries (AZIBs) show promise for future energy storage due to affordability and safety. However, industrial application is hindered by parasitic reactions and zinc dendrites. We address this by adding 1-ethyl-3-methylimidazolium dicyandiamide ([Emim][DCA], or ED) to the electrolyte, suppressing water reduction and Zn dendrite growth. The strong coordination between zinc and nitrogen-containing ligands leads to DCA − anion adsorption on the zinc anode, forming a dense Zn(DCA) 2 layer. This layer aids zinc ion desolvation and isolates water molecules, enabling water-free deposition and facilitating reversible plating/stripping. Additionally, in the water-poor double electric layer, zinc cations introduce triflate anions to the zinc electrode surface, forming an in-situ fluorine-based SEI layer. This layer separates zinc electrodes from water, inhibiting corrosion, and hydrogen evolution. With ED additives, Zn||Zn symmetric cells maintain a cycle life of over 2500 h at 0.5 mA cm −2 and 0.5 mAh cm −2 . Zn||Ti asymmetric cells achieve 99.4 % Coulombic efficiency. The Zn||PANI full cell lasts for 1000 cycles at 4 A g −1 without a significant decrease in specific capacity.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Hanning Zhang,Tao Shui,Nosipho Moloto,An Li,Ruogu Zhang,Jiacheng Liu,Song-Zhu Kure-Chu,Takehiko Hihara,Wei Zhang,ZhengMing Sun
Considering the desired energy density, safety and cost-effectiveness, rechargeable zinc-ion batteries (ZIBs) are regarded as one of the most promising energy storage units in next-generation energy systems. Nonetheless, the service life of the current ZIBs is significantly limited by rampant dendrite growth and severe parasitic reactions occurring on the anode side. To overcome these issues caused by poor interfacial ionic conduction and water erosion, we have developed a facile strategy to fabricate a uniform zinc borate layer at the zinc anode/electrolyte interface (ZnBO). Such protective layer integrates superhydrophobic-zincopholic properties, which can effectively eliminate the direct contact of water molecules on the anode, and homogenize the interfacial ionic transfer, thereby enhancing the cyclic stability of the zinc plating/stripping. As a result, the as-prepared ZnBO-coated anode exhibits extended lifespan of 1200 h at 1 mA cm −2 and demonstrates remarkable durability of 570 h at 20 mA cm −2 in Zn||Zn symmetric cells. Additionally, when coupled to an NH 4 V 4 O 10 (NVO) cathode, it also delivers a superior cyclability (203.5 mAh/g after 2000 cycles at 5 A/g, 89.3 % capacity retention) in coin full cells and a feasible capacity of 2.5 mAh at 1 A/g after 200 cycles in pouch full cells. This work offers a unique perspective on integrating hydrophobicity and zincophilicity at the anode/electrolyte interface through an artificial layer, thereby enhancing the cycle lifespan of ZIBs.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Yu Bai,Haiping Zhou,Jia-Lin Yang,Qingqing Pan,Jiawei Wang,Yunpeng Wu,Xing-Long Wu
Aqueous zinc-ion batteries (AZIBs) have great potential for large-scale energy storage applications. However, the parasitic reactions, such as continuous hydrogen evolution reaction (HER), seriously hamper the reversibility and cycling stability of the zinc metal anode (ZMA), limiting its practical application. In this paper, a pre-growth interfacial layer strategy is adopted to grow the enol/ketone conversion interfacial layer on the surface of ZMA (denoted as Zn@AA). H + can be reversible “lock/unlock” during reversible enol/ketone conversion reaction. It not only broadens the capacity of AZIBs (Zn 2+ /H + co-insertion), but also inhibits the HER reaction (the amounts of H 2 evolution decreased obviously in both Zn@AA||Zn@AA and Zn@AA||VO 2 ·H 2 O@Ppy (Ppy denote as polypyrrole) cells by on-line differential electrochemical mass spectrometry analysis), thereby improving its stability performance. The cycle life of the assembled Zn@AA||Zn@AA cell exceeded 3200 h at 1 mA cm −2 and 1 mA h cm −2 . Furtherly, the Zn@AA||VO 2 ·H 2 O@Ppy full cell also exhibited excellent cycling stability and capacity retention. This work provides new ideas for modifying the ZMA interfacial layer to inhibit the HER, which guides the development of AZIBs.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Energy Storage Materials
·
2022
·
IF 20.831
Wenkang Wang,Cheng Yang,Xiaowei Chi,Jiahe Liu,Bo Wen,Yu Liu
Vanadium-based cathodes with high specific capacity have attracted wide attention in aqueous zinc ion batteries . The main barriers of the development of vanadium-based cathodes are vanadium dissolution, structure degradation, instability of cathode electrolyte interlayer (CEI) and parasitic reactions in aqueous electrolyte. In this work, for the first time, we propose a new type of ultralow-water-activity electrolyte that tackles all these problems. Our design is realized by the introduction of pioneering inert electrolyte filler (trimethyl phosphate). It is discovered that highly concentrated ZnCl 2 H 2 O clusters are surrounded by this electrolyte filler, reaching the lowest free solvation water composition (2.5%) reported so far. The ultralow water activity significantly inhibits parasitic reactions and vanadium dissolution, boosting the achievement of the highest columbic efficiency (99.98%). The biggest bottleneck of vanadium-based cathodes dissolution and water shuttle has been broken through by stable CEI. As a proof of concept , the V 6 O 13 cathode demonstrates exceptional stability of 99.43% capacity retention after 3 000 cycles at 1 A g −1 , and sets a new record for cycle life of 30 000 cycles (capacity retention of 90.34% at 10 A g −1 ) in zinc ion batteries , even reaching the level of supercapacitors (∼100 000 cycles).
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Chenbei Zhang,Xiaohu Qian,Dong Wang,Chengtao Chen,Yingdong Chen,Tao Chen,Jiajun Fu
The instability of zinc metal anode caused by zinc dendrite growth and severe parasitic reactions has significantly restricted the extensive application of rechargeable aqueous zinc-ion batteries (RAZBs). Herein, based on the strategy of dynamic hard domains, we develop an ion-conductive supramolecular elastomer consisting of Zn salts and the polyurethane-urea-polypropylene glycol polymer skeleton. This elastomer combines high mechanical strength, high ionic conductivity, decent hydrophobicity, and high adhesion to stabilize the electrode–electrolyte interface. In the elastomer system, this elastomer can dynamically adapt to the volume changes of Zn anodes during repeated zinc plating/stripping processes through the reversible dissociation/reassociation of hierarchical hydrogen bonds (H-bonds) formed by the polar groups of urea and urethane moieties. Meanwhile, the coordination of Zn2+ with soft polypropylene glycol (PPG) segments contributes to fast ion transport. This hydrophobic elastomer can also effectively inhibit water-induced corrosion by shielding the active Zn metal from the aqueous electrolyte. Based on the above synergies, the surface-modified anode shows excellent cycling stability above 550 h at a high current density of 5 mA cm–2 and a capacity of 2.5 mAh cm–2. Moreover, the assembled Zn//MnO2 full cell also displayed an enhanced electrochemical performance. This work provides inspiration for the design of solid electrolyte interphase (SEI) layers in aqueous battery chemistry to accelerate the application of RAZBs.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Polymers
·
2023
·Vol. 15
·期 16
·3490
·
IF 5
Yujie Wang,Mengmeng Zhao,Yazhou Chen,Haifeng Bao,Chen Li
Dendrite growth and parasitic reactions with liquid electrolyte are the two key factors that restrict the practical application of the lithium metal anode. Herein, a bis(benzene sulfonyl)imide based single-ion polymer artificial layer for a lithium metal anode is successfully constructed, which is prepared via blending the as-prepared copolymer of lithiated 4, 4′-dicarboxyl bis(benzene sulfonyl)imide and 4,4′-diaminodiphenyl ether on the surface of lithium foil. This single-ion polymer artificial layer enables compact structure with unique continuous aggregated Li+clusters, thus reducing the direct contact between lithium metal and electrolyte simultaneously, ensuring Li+transport is fast and homogeneous. Based on which, the coulombic efficiency of the Li|Cu half-cell is effectively improved, and the cycle stability of the Li|Li symmetric cell can be prolonged from 160 h to 240 h. Surficial morphology and elemental valence analysis confirm that the bis(benzene sulfonyl)imide based single-ion polymer artificial layer effectively facilitates the Li+uniform deposition and suppresses parasitic reactions between lithium metal anode and liquid electrolyte in the LFP|Li full-cell. This strategy provides a new perspective to achieve a steady lithium metal anode, which can be a promising candidate in practical applications.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Advanced Energy Materials
·
2025
·
IF 26
Jia-Xin Guo,Chang Gao,Yun-Fei Du,Feng Jiang,Nai-Lu Shen,Wen-Bo Tang,Xin Shen,Xin-Bing Cheng,Yuping Wu
Solvents in liquid and gel polymer electrolytes are recognized for contributing to high ionic conductivity in high-energy-density lithium metal batteries. However, parasitic reactions involving solvents and lithium metal induce safety risks under thermal abuse conditions and poor lifespan during room-temperature cycles, which are rarely investigated. This study introduces a thermoresponsive mono-solvent electrolyte as a built-in safety switch. The mono-solvent electrolyte polymerizes at elevated temperatures, creating a passivate polymer network without residue solvents. The polymer exhibits high thermal stability with 91% mass retention at 200 °C and significantly suppresses side reactions between lithium metal and the electrolyte, reducing thermal runaway risks. Ah-level Li||LiNi 0.8 Co 0.1 Mn 0.1 O 2 pouch batteries employing this electrolyte can efficiently improve the critical temperature of thermal runaway by 75 °C compared to the thermoresponsive gel polymer electrolyte. At ambient temperatures, the electrolyte promotes the formation of a stable solid electrolyte interphase (SEI) rich in LiF and Li 2 O, effectively reducing side reactions and dendrite growth on the lithium anode. Consequently, Li||LiNi 0.5 Co 0.2 Mn 0.3 O 2 cells retain 91% capacity after 152 cycles, even under high-loading cathodes (19.7 mg cm −2 , 3 mAh cm −2 ). This research offers valuable insights into inhibiting parasitic reactions during the electrochemical cycle and thermal runaway, enhancing the lifespan and safety of high-energy-density batteries.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
Chem
·
2022
·
IF 25.832
Li-Peng Hou,Xue-Qiang Zhang,Nan Yao,Xiang Chen,Bo-Quan Li,Peng Shi,Cheng-Bin Jin,Jia-Qi Huang,Qiang Zhang
Practical lithium–sulfur batteries are severely hindered by parasitic reactions between lithium metal anodes and soluble lithium polysulfide (LiPS) intermediates. The solvation structure of LiPSs is pivotal in dictating the reaction kinetics. Herein, an encapsulating LiPS electrolyte (EPSE) is proposed to suppress parasitic reactions based on a nano-heterogeneous solvation structure design of LiPSs. In EPSE, with di-isopropyl sulfide (DIPS) as a co-solvent, soluble LiPSs are encapsulated into two concentric solvent shells with different solvating power and reduction stability. Reduction-stable DIPS in the outer solvent shell significantly suppresses the parasitic reactions between encapsulated LiPSs and lithium metal. A 1.2 Ah pouch cell under demanding conditions undergoes 103 cycles in the EPSE. This work provides two crucial criteria for constructing EPSE, that is, poor solvating power and high reduction stability of the solvent in outer solvent shell, and it opens up new frontiers in modulating the solvation structure of LiPSs toward long-cycling lithium–sulfur batteries.
研究领域:
电化学
·
能源材料
·
纳米材料
·
电池化学
·
界面化学
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Hongjiao Wang,Lilin Wu,Bai Xue,Fang Wang,Zhongkuan Luo,Xianghua Zhang,Laurent Calvez,Ping Fan,Bo Fan
Controlling the composition and microstructure of the solid electrolyte interphase (SEI) layer is critical to improving the cycling stability of the high-energy-density lithium–metal electrode. It is a quite tricky task to control the properties of the SEI layer which is conventionally formed by the chemical reactions between a Li metal and the additives. Herein, we develop a new route to synthesize a lithium-compatible sol of the sulfide electrolyte Li3PS4, so that a Li3PS4 artificial SEI layer with a controllable nanoscale thickness and high phase purity can be prepared by spin-coating. The layer stabilizes the lithium/electrolyte interface by homogenizing the Li-ion flux, preventing the parasitic reactions, and alleviating concentration polarization. Consequently, a symmetrical cell with the Li3PS4-modified lithium electrodes can achieve stable lithium plating/stripping for 800 h at a current density of 1 mA cm–2. The Li–S batteries assembled with the Li3PS4-protected Li anodes show better capacity retention than their bare Li counterparts, whose average decay rate from the 240th cycle to the 800th cycle is only 0.004%/cycle. In addition, the Li3PS4 layer improves the rate capacity of the batteries, significantly enhancing the capacity from 175 to 682 mA h g–1 at a 2 C rate. The spin-coated Li3PS4 artificial SEI layer provides a new strategy to develop high-performance Li metal batteries.
研究领域:
材料科学
·
电化学
·
电池技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Zhen Zeng,Shang Wang,Jun Cheng,Guangmei Hou,Deping Li,Guifang Han,Lijie Ci
Solid polymer electrolytes (SPEs) are preferable in the pursuit for developing high-energy Li metal batteries due to their inherent flexibility and intimate contact with electrodes. However, continuous interfacial parasitic reactions and undesired Li dendrite growth caused by inhomogeneous plating/stripping of Li+ result in rapid deterioration of an SPE/Li interface. Herein, a novel Zn2+-containing SPE (SPE-xZn) with anionic groups partially tethered on the polymer chains is developed to meet these challenges. During cycling, Zn2+ cations inside the SPE-xZn will gradually migrate to the surface of a Li electrode and then evolve to a Li-Zn alloy layer, where Li+ can diffuse more efficiently. Meanwhile, owing to the electrostatic interaction, the immobilized anionic groups within SPE-xZn can alleviate local concentrated Li+ flux. The synergistic effects of an in situ formed alloy layer and unique macromolecular structure can promote uniform plating/stripping of Li, thus yielding a more stable SPE-xZn/Li interface. Therefore, steady cycling over 300 h at 0.2 mA cm–2 is achieved by Li/SPE-5Zn/Li, and an impressive capacity retention of 87.3% at 0.5 C after 800 cycles is realized by LFP/SPE-5Zn/Li with an average Coulombic efficiency of 99.90%.
研究领域:
材料科学
·
电化学
·
电池技术
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）