ACS Nano
·
2025
·
IF 16
Cuicui Li,Haocheng Li,Xiuyun Ren,Liang Hu,Jiaojiao Deng,Jinhan Mo,Xiaoqi Sun,Guohua Chen,Xiaoliang Yu
The multielectron conversion electrochemistry of I–/I0/I+ enables high specific capacity and voltage in zinc–iodine batteries. Unfortunately, the I+ ions are thermodynamically unstable and are highly susceptible to hydrolysis. Current endeavors primarily focus on exploring interhalogen chemistry to activate the I0/I+ couple. However, the practical working voltage is below the theoretical level. In this study, the I0/I+ redox couple is fully activated, and I+ is efficiently stabilized by a chelation agent of cost-effective urea in the conventional aqueous electrolyte. A record-high plateau voltage of 1.8 V vs Zn/Zn2+ has been realized. Theoretical calculations combined with spectroscopy studies and electrochemical tests reveal that the coordination between the electron-deficient I+ and the electron-rich O and N atoms in urea molecules is thermodynamically favorable for I0/I+ conversion and inhibits the self-disproportionation of I+, which in turn promotes rapid kinetics and excellent reversibility of I0/I+. Moreover, urea decreases the water activity in the electrolyte by forming hydrogen bonds to further suppress the hydrolysis of I+. Accordingly, a high specific capacity of 419 mAh g–1 is delivered at 1C, and 147 mAh g–1 capacity is retained after 10,000 cycles at 5C. This work offers effective insights into formulating halogen-free electrolytes for high-performance aqueous zinc–iodine batteries.
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
ACS Nano
·
2022
·
IF 18.027
Yang-feng Cui,Zhen-bang Zhuang,Zi-long Xie,Ren-fei Cao,Qi Hao,Ning Zhang,Wan-qiang Liu,Yun-hai Zhu,Gang Huang
Alkaline Zn–MnO2 batteries feature high security, low cost, and environmental friendliness while suffering from severe electrochemical irreversibility for both the Zn anode and MnO2 cathode. Although neutral electrolytes are supposed to improve the reversibility of the Zn anode, the MnO2 cathode indeed experiences a capacity degradation caused by the Jahn–Teller effect of the Mn3+ ion, thus shortening the lifespan of the neutral Zn–MnO2 batteries. Theoretically, the MnO2 cathode undergoes a highly reversible two-electron redox reaction of the MnO2/Mn2+ couple in strongly acidic electrolytes. However, acidic electrolytes would inevitably accelerate the corrosion of the Zn anode, making long-lived acidic Zn–MnO2 batteries impossible. Herein, to overcome the challenges faced by Zn–MnO2 batteries, we propose a hybrid Zn–MnO2 battery (HZMB) by coupling the neutral Zn anode with the acidic MnO2 cathode, wherein the neutral anode and acidic cathode are separated by a proton-shuttle-shielding and hydrophobic-ion-conducting membrane. Benefiting from the optimized reaction conditions for both the MnO2 cathode and Zn anode as well as the well-designed membrane, the HZMB exhibits a high working voltage of 2.05 V and a long lifespan of 2275 h (2000 cycles), breaking through the limitations of Zn–MnO2 batteries in terms of voltage and cycle life.
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
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Mengdi Liu,Sai Zhang,Min Chen,Limin Wu
While electrochemical nitrogen reduction reaction (NRR) stands as a promising technique for sustainable NH 3 fabrication due to its mild operation conditions, it has long been suffered from low efficiency and poor selectivity owing to the inertness of N 2 and competition hydrogen evolution reaction (HER). Herein, we report the use of oxygen vacancy rich TiO 2 loaded with Au nanoparticles as NRR catalyst in super concentrated lithium bis(trifluoromethane sulfonyl) imide (Li TFSI) “water-in-salt” system (20 M electrolyte) and obtain the Faradaic efficiency of 37.2 % with an NH 3 yield rate of 20.3 μg h −1 cm −2 at − 0.4 V vs RHE, accompanied by the significant decay of both current density and onset potential of hydrogen evolution reaction. Electrochemical experimental and theoretical calculation results indicate that the HER process can be greatly hindered both kinetically and energetically. The unique effect of this “water-in-salt” electrolyte would offer a new idea to improve the NRR selectivity via HER suppression.
研究领域:
电化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
eScience
·
2021
·
IF 0
Mengke Peng,Li Wang,Longbin Li,Zhongyou Peng,Xiannong Tang,Ting Hu,Kai Yuan,Yiwang Chen
The development of low-cost and eco-friendly aqueous electrolytes with a wide voltage window is the key to achieving safe high energy density supercapacitors (SCs). In this work, a molecular crowding electrolyte is prepared by simulating the crowded environment in living cells. Ion transport in the molecular crowding electrolyte can be effectively improved via reducing the molecular weight of the crowding agent, polyethylene glycol (PEG). The results show that PEG with a molecular weight of 200 (PEG200) can significantly improve ionic conductivity while maintaining a wide voltage window. These advantages enable commercial activated carbon-based SCs to work at 2.5 V with high energy density, outstanding rate performance and good stability for more than 10,000 cycles. On this basis, three series of molecular crowding electrolytes using sodium perchlorate, lithium perchlorate, and sodium trifluoromethanesulfonate as salts are developed, demonstrating the versatility of PEG200 for wide-voltage aqueous electrolytes.
研究领域:
材料科学
·
能源技术
✓ 已验证
DOI
RSC Advances
·
2024
·Vol. 14
·期 54
·40247-40254
·
IF 3.9
Xin Zhang,Kai Zheng,Dingyi Hu,Si Liu,Zhifeng Lin
Aqueous zinc-ion batteries are highly praised for their cost-effectiveness, environmental friendliness, and high safety, making them an ideal choice for next-generation energy storage systems. However, the practical application of Zn metal anodes is constrained by well-known challenges such as dendrite growth and significant interfacial side reactions. This study introduces a trace amount of taurine (TAU) as a leveling additive into the electrolyte to optimize the microstructure of the electrolyte and the anode interface chemistry. On one hand, the preferential adsorption of TAU on the Zn surface promotes the in situ formation of a stable, protective molecular interfacial layer on the anode, which helps to refine the deposited grains and guide the uniform deposition of Zn2+. On the other hand, the introduction of TAU can regulate the hydrogen bond structure in the electrolyte, reduce the activity of water, thereby significantly inhibiting the occurrence of side reactions such as hydrogen evolution. Consequently, the Zn//Zn symmetric cell system demonstrates an extended cycle life of over 1150 cycles at a current density of 1 mA cm−2 and maintains stable cycling performance for over 600 cycles at 10 mA cm−2. Moreover, the Zn//Cu asymmetric cell system achieves over 1400 cycles of reversible deposition/dissolution at a current density of 1 mA cm−2, with a coulombic efficiency of 99.4%. The incorporation of TAU further enhances the cycle stability of the Zn//MnO2 full cell. These innovative achievements have laid a solid foundation for the broader industrial adoption of aqueous zinc-ion batteries.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
高影响因子
ChemSusChem
·
2022
·Vol. 15
·期 24
·e202201739
·
IF 9.14
Kang Zhou,Nan Wang,Xuan Qiu,Haijiao Xie,Peng Wei,Xiaoli Dong,Yonggang Wang
Graphical No water, no problem : The H 2 O activity in aqueous electrolyte is restrained by adding glycerol and acetonitrile into the electrolyte to form hydrogen bonds between organic solvents and H 2 O molecules, which facilities the smooth Zn deposition and alleviates Zn corrosion. Therefore, the Zn//Zn symmetrical cell cycles for over 1300 h and the Zn//FD28 full cell cycles for 9000 cycles. The advantages of low cost and high safety of zinc (Zn) metal have attracted much attention on its application in batteries, but H 2 O-induced issues of hydrogen evolution reaction (HER), Zn corrosion, and Zn dendrites formation limit the application. Here, a strategy of adjusting H 2 O activity was provided by adding glycerol (GL) and acetonitrile (AN) into aqueous electrolyte to form hydrogen bonds between organic solvents and H 2 O, which alleviated the Zn corrosion. Furthermore, molecular dynamics (MD) simulation indicated that GL could exclude H 2 O from the Zn 2+ solvation shell, thus preventing undesired HER and Zn dendrites formation. Therefore, the corresponding Zn//Zn symmetrical cell showed a ultralong lifespan (1300 h). Then, a Zn-organic battery with 3,7-dimorpholino-phenothiazin-5-ium iodide (FD28) cathode was fabricated by using such electrolyte. Interestingly, the reduced H 2 O activity also ensured the stable operation of organic cathode, and thus the full cell showed superior cycle stability for over 9000 cycles (≈1100 h), which is superior to previous reports. Moreover, such electrolyte owns novel properties of nonflammability, great weatherability, and low freezing point, thus boosting the practicality of the battery.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
PubMed
高影响因子
Small
·
2024
·Vol. 20
·期 52
·2407961
·
IF 13
Meijing Wang,Jiaojiao Zhao,Yangyang Zhang,Yunyun Liu,Wei Ji,Xingde Xiang
Hydrogen evolution reactions that cause the alkalization of aqueous electrolytes generally frustrate the structural stability and cycling performance of NaTi 2 (PO 4 ) 3 /C anode material for rechargeable aqueous sodium-ion batteries (ASIBs). Herein, a novel highly concentrated electrolyte with a large hydrogen-evolution overpotential and hydroxide-capture ability is rationally established by incorporating a bifunctional Mg(Ac) 2 additive into a concentrated NaAc aqueous solution. The highly concentrated electrolyte salts (4 m NaAc+3 m Mg(Ac) 2 ) favor regulation on hydrogen-bonding configurations and kinetically shift the hydrogen evolution potential to a lower value of −1.37 V (vs Ag/AgCl). The Mg(Ac) 2 additive plays particular roles in spontaneously capturing hydroxide ions generated during hydrogen evolution reactions on anode surfaces and simultaneously forming a protective Mg(OH) 2 -like interphase. As a result, the unique electrolyte significantly improves the structural stability and cycling performance of NaTi 2 (PO 4 ) 3 /C anode (94.8% capacity retention after 100 cycles at 100 mA·g −1 ). The effect of salt concentration on hydrogen bonding configurations of aqueous electrolytes is investigated with Raman spectroscopy and FTIR spectroscopy. The interphase is identified by coupling EDS mapping, X-ray photoelectron spectroscopy, and X-ray diffraction. This work provides a new strategy for improving the cycling stability of aqueous sodium-ion batteries.
研究领域:
电化学
·
材料科学
✓ 已验证
DOI
高影响因子
ACS Nano
·
2025
·
IF 16
Shengxi Li,Yanxin Shang,Xuening Ren,Anqi Zhao,Nan Chen,Li Li,Feng Wu,Renjie Chen
Aqueous lithium-ion batteries (ALIBs) have attracted increasing attention for their inherent safety and environmental benefits. However, the narrow electrochemical stability window of water (1.23 V) imposed by hydrogen evolution reaction (HER) and high melting point (0 °C) critically limits the energy density and low-temperature operation. In this work, we report an electrolyte design principle that water activity can be suppressed by strengthening the O–H bonds between water molecules and regulating the pH. A strong polar solvent N,N-dimethylformamide (DMF) interacts with H2O through intermolecular hydrogen bonds, thereby reinforcing the covalent O–H bonds of water. Meanwhile, KOH renders the electrolyte alkaline, inhibiting water dissociation kinetics and consequently raising the HER overpotential. The designed LD1.7W0.6–KOH electrolyte exhibits a freezing point below −82 °C and expanded electrochemical stability window of 4.3 V. The 2.5 V aqueous LiMn2O4/Li4Ti5O12 full cell delivers 2000 cycles at a rate of 6 C with a Coulombic efficiency of 99% at 30 °C and over 1950 cycles at 0 °C. This work offers atomic-level insights into alkaline HER while providing guidance for advancing low-temperature aqueous batteries by tuning the electrolyte structures.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
PubMed
高影响因子
National Science Review
·
2022
·Vol. 9
·期 10
·
IF 23.178
Ma Yilin,Zhang Qiu,Liu Luojia,Li Yixin,Li Haixia,Yan Zhenhua,Chen Jun
Rechargeable aqueous Zn batteries are considered as promising energy-storage devices because of their high capacity, environmental friendliness and low cost. However, the hydrogen evolution reaction and growth of dendritic Zn in common aqueous electrolytes severely restrict the application of Zn batteries. Here, we develop a simple strategy to suppress side reactions and boost the reversibility of the Zn electrode. By introducing 30% (volume fractions) N,N-dimethylformamide (DMF) to the 2 M Zn(CF3SO3)2–H2O electrolyte (ZHD30), the preferential hydrogen-bonding effect between DMF and H2O effectively reduces the water activity and hinders deprotonation of the electrolyte. The ZHD30 electrolyte improves the Zn plating/stripping coulombic efficiency from ∼95.3% to ∼99.4% and enhances the cycles from 65 to 300. The Zn–polyaniline full battery employing the ZHD30 electrolyte can operate over a wide temperature range from –40°C to +25°C and deliver capacities of 161.6, 127.4 and 65.8 mAh g–1 at 25, –20 and –40°C, respectively. This work provides insights into the role of tuning solvent effects in designing low-cost and effective aqueous electrolytes.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2020
·
IF 6.182
Ge Zhang,Zhengyi Qian,Ya Mao,Baoyu Sun,Pengjian Zuo,Yulin Ma,Chunyu Du,Geping Yin,Jingying Xie
Porous carbon materials are usually employed as cathode catalysts in Li-O 2 batteries. However, the poor catalytic performance of carbon cathode often results in low capacity and severe overpotential. Herein, we successfully prepared phosphorus doped carbon material by one-step pyrolyzation, effectively improving the performance of Li-O 2 batteries. The discharge capacity of Li-O 2 battery with P doped carbon reaches 3400 m Ah g −1 at 200 mA g −1 , which is increased by 52% compared to the un-doped sample. Besides, greatly decreased discharge overpotential and enhanced rate capability are also obtained after phosphorus doping. Furtherly, phosphorus doping was found to crucially affect the growth of discharge products, and the solution driven mechanism becomes more prominent, leading to larger sized discharge products and prolonged battery life. Our work provides a new way of improving the catalytic performance of carbon cathode for Li-O 2 batteries.
研究领域:
材料科学
·
能源存储与转换
✓ 已验证
产品关联
DOI
高影响因子
DESALINATION
·
2023
·
IF 9.9
Xi Wu,Zhiwei Chen,Yibo Lv,Youwen Zhang,Shiming Xu,Xiaojing Zhu
In order to simultaneously produce hydrogen and reduce the salinity of concentrated wastewater (brine) from the desalination plant , a lab-scale reverse electrodialysis (RED) hydrogen production system driven by salinity gradient energy is designed and its performance is experimentally studied. The energy conversion of the RED system is found affected by the ionic compositions of the desalination concentrated brine (DCB). The effects of ionic types (multivalent cation, anion, and phosphorous salt) and ionic concentration (from 0.01 to 0.05 M) and pH of DCB (from 5 to 11) on the hydrogen production are investigated. The results show that the existence of multivalent ions in brine significantly degrade the capability of output voltage and hydrogen production of the RED system. Compared to the control group, the additions of 0.05 mol·L −1 NaBr and 0.05 mol·L −1 FeCl 3 into the simulated brines lead to the output voltage drops of 29 % and 60 %, respectively, when the current is maintained at 0.2A. Additionally, the experiment yields an MHP of 128 mL·h −1 at the current of 0.3A. Generally, the performances of the RED stack can be improved as increasing the pH of an acidic DCB, but declined as the increasing the pH of an alkaline DCB.
研究领域:
环境科学
·
能源工程
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED MATERIALS
·
2024
·
IF 27.4
Yan Wang,Ting Ou,Yue Dong,Lu Chen,Yunjie Huang,Delong Sun,Wei Qiang,Xiaopeng Pei,Yiju Li,Ying Tan
Hybridizing aqueous electrolytes with organic co-solvents can effectively expand the voltage window of aqueous electrolytes while reducing salt usage, but most reported co-solvents are usually flammable and toxic, hardly achieving compatibility between safety and electrochemical performance. Here, a new non-flammable and non-toxic low-salt-concentration (1.85 m) aqueous electrolyte is reported using the green co-solvent isosorbide dimethyl ether (IDE). Owing to its unique 3D molecular structure, IDE can form a five-membered ring structure by binding the Li ion. The steric hindrance effect from IDE weakens its solvation ability, generating anion-participated solvation structures that produce a robust and uniform LiF-rich solid electrolyte interphase layer while containing elastic IDE-derived organics. Moreover, the multiple O atoms in IDE can effectively regulate the intermolecular hydrogen bonding networks, reducing H 2 O molecule activity and expanding the electrochemical window. Such unique solvation structures and optimized hydrogen bonding networks enabled by IDE effectively suppress electrode/electrolyte interfacial side reactions, achieving a 4.3 V voltage window. The as-developed Li 4 Ti 5 O 12 (LTO)||LiMn 2 O 4 (LMO) full cell delivers outstanding cycling performance over 450 cycles at 2 C. The proposed green hybrid aqueous electrolyte provides a new pathway for developing high-voltage aqueous lithium batteries.
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
危险品化学品经营许可证（带存储）