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JOURNAL OF THE ELECTROCHEMICAL SOCIETY · 2017 ·Vol. 164 ·期 12 ·H828 · IF 3.259

The Size-Dependence of Electrochemical Thermodynamics of Metal Nanoparticles Electrodes in Theory and Experiment

Jianhua Zhang,Zongru Li,Qingshan Fu,Yongqiang Xue,Zixiang Cui

Metal nanoparticles electrodes present great difference in electrochemical thermodynamics compared with corresponding bulk electrodes, which depends on the size of nanoparticles that construct the electrodes. However, it remains unclear about the influences of particle size on electrochemical thermodynamics of the electrodes. Herein, the size-dependence of electrochemical thermodynamic functions of metal nanoparticles electrodes was deduced theoretically. Experimentally, taking copper nanoparticles electrode as an example, the standard electrode potentials, the temperature coefficients, and the thermodynamic functions of electrode reaction were obtained by determining the electrode potentials of the electrodes constructed by copper nanoparticles with different sizes at different temperatures. Both the theoretical and the experimental results indicate that with the particle size of metal nanoparticles decreasing, the standard electrode potential and surface tension decreases, while the temperature coefficient, the molar reaction Gibbs energy, enthalpy and entropy increase. Moreover, all these physical quantities are linearly related with the reciprocal of particle radius when the radius exceeds 10 nm. Meanwhile, we also found that the influence regularities of particle size on electrochemical thermodynamic functions of metal nanoparticles electrodes are quite opposite to those of oxide nanoparticles electrodes, which is attributed to the nanoparticles being reactant or product in an electrode reaction.

研究领域: 物理化学 · 材料科学
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Nano-Micro Letters · 2022 ·Vol. 14 ·期 1 ·1-12 · IF 23.655

Facet-Controlled LiMn2O4/C as Deionization Electrode with Enhanced Stability and High Desalination Performance

Jiang Yuxin,Chai Liyuan,Zhang Dehe,Ouyang Fangping,Zhou Xiangyuan,Alhassan Sikpaam I.,Liu Sailin,He Yingjie,Yan Lvji,Wang Haiying,Zhang Wenchao

AbstractSection Highlights First report of a lithium-ion battery cathode as a deionization electrode for desalination. A novel approach to suppress manganese dissolution by exposing the (111) facet is proposed. Excellent desalination performance by the LiMn 2 O 4 /C cathode. The material achieves an ultrahigh desalination capacity of 117.3 mg g −1 at 1.0 V and a longer cycle life (200 cycles without capacity decay) with minor manganese dissolution during the cycling test in 10 mM aqueous LiCl solution. AbstractSection Abstract Battery materials as emerging capacitive deionization electrodes for desalination have better salt removal capacities than traditional carbon-based materials. LiMn 2 O 4 , a widely used cathode material, is difficult to utilize as a deionization electrode due to its structural instability upon cycling and Mn dissolution in aqueous-based electrolytes. Herein, a facile and low-cost ball-milling routine was proposed to prepare a LiMn 2 O 4 material with highly exposed (111) facets. The prepared electrode exhibited relatively low dissolution of Mn during cycling, which shows its long cycle stability. In the hybrid capacitive deionization system, the LiMn 2 O 4 /C electrode delivered a high desalination capacity of 117.3 mg g −1 without obvious capacity decay at a voltage of 1.0 V with a 20 mM initial salt concentration. In addition, the exposed (111) facets significantly alleviated Mn ion dissolution, which also enhanced the structural steadiness.

研究领域: 材料科学 · 环境工程
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Carbon Letters · 2024 ·Vol. 34 ·期 7 ·1927-1939 · IF 5.5

The modification of nano-activated carbon used to construct particle electrodes and its application in degradation of nitrosodiethylamine

Ma Liyan,Sun Fengyi,Jiang Zhuwu,Di Hongcheng,Pan Chuntao,Zhang Fengying,Bai Xue,Zhang Hongyu

Activated carbon has broad application prospects for treating pollutants due to its easy availability, low cost and good adsorption. In our work, nano-activated carbons (NAC) with abundant functional groups are obtained by the oxidation modification of HNO 3 , (NH 4 ) 2 S 2 O 8 , and KMnO 4 , which are used to construct the particle electrodes to degrade NDEA in a continuous flow electrochemical reactor, and the influence of relevant factors on the performance of NDEA removal is discussed. The experimental data show that the optimal degradation efficiency is 42.55% at the conditions of 3 mL/min influent water flow, 0.21 M electrolyte concentration, 10 mA/cm 2 current density, and 10 μg/mL initial NDEA concentration. The degradation of NDEA conforms to a quasi second order kinetic equation. The electrocatalytic mechanism of NAC electrodes for removing NDEA is firstly discussed. The effects of different free radicals on the degradation of NDEA are also demonstrated through free radical quenching experiments, indicating that the degradation of NDEA is dominated by ⋅OH. The degradation pathway of NDEA and final products are obtained using GC–MS. NAC particle electrodes as the cheap and efficient electrocatalyst in continuous flow electrochemical reactor system provide a greener solution for the removal of disinfection by-products from drinking water.

CAS / MDL: 7757-82-6
研究领域: 环境科学 · 电化学工程
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY · 2022 ·Vol. 331 ·期 4 ·1585-1599 · IF 1.754

Efficient removal of uranium from aqueous solution in a modified three-dimensional electrokinetic system

He Guicheng,Wu Xueying,Zhang Shuwen,Huang Tao,Zhong Shijing

A modified electrokinetic system using activated carbon particles was proposed to quickly remove uranium (U). The influences of electrokinetic parameters such as voltage, length of particle electrode, particle electrode ration were studied through batch experiments. The results revealed that the three dimensional electrokinetic (3D-EK) treatment system showed a great potential for uranium removal. The uranium removal efficiency reached above 99% and the residual solution reached the discharge standard when pH = 2, voltage = 25 V,150 g/L of 4 mm particle electrode. The colloidal precipitates generated were detected as Fe(OH) 3 . Tthe probable removal mechanism is ascribed to the synergy of electromigration, electrocoagulation and adsorption.

研究领域: 环境科学 · 化学工程
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Frontiers in Chemistry · 2021 · IF 5.221

Preparation of Device-Level ZnO-Covered Silver Nanowires Films and Their Applications as Sub-Electrode for Polymer Solar Cells

Zhao Xin,Li Meng,Jiang Linping,Tang Hua,Guan Youwei

Silver nanowire films are good candidates to be used as transparent conductive films that could be widely utilized in organic photoelectronic devices such as polymer solar cells. However, their application is usually limited, as they are mainly used as top electrode materials; otherwise, they would be prone to complex transferring processes. In this study, we successfully prepared device-level ZnO-covered silver nanowire (AgNWs/ZnO) films. ZnO was prepared by a spray pyrolysis method using zinc-ammonia solution at a relatively low temperature (95°C). The films showed good adhesive properties to the glass substrate, considering it withstood the process of applying polyimide tapes on the surface and tearing them off more than 100 times. It also exhibited good conductivity (∼24 Ω/sq) with high transmittance in the visible range (>80%). After a simple polish and patterning, AgNWs/ZnO showed a good performance as a sub-electrode for polymer solar cells. The PM6:Y6 devices achieved a high power conversion efficiency of 8.37% with an open-circuit voltage of 0.81 V, a short-circuit current density of 18.18 mA/cm2, and a yield of 81.25%. This indicates that the technology has a good prospect of large-scale fabrication of organic photoelectronic devices.

CAS / MDL: 1314-13-2 34819-78-8
研究领域: 材料科学 · 光电子器件
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Carbon-coating small-molecule organic bipolar electrodes for symmetric Li-dual-ion batteries

Chenbin Tang,Bangshuai Wei,Wu Tang,Yan Hong,Meichen Guo,Xuesong He,Jiahui Hu,Shan Jia,Cong Fan

A novel small organic molecule namely N,N’-bis(2-anthraquinone)-dihydrophenazine (DAQ-DPZ, 270 mAh/g) with n-p-n molecular heterojunction configuration is designed as the bipolar electrode material for Li-dual-ion batteries. To delay the dissolution for small-molecule organic electrodes, DAQ-DPZ is further coated by a protective carbon layer (DAQ-DPZ@C) through the process called surface self-carbonization. As expected, the resulting DAQ-DPZ@C can show the peak discharge capacity of 269 mAh/g and high median potential of 2.62 V in 1.6–4.4 V (vs. Li + /Li), corresponding to the peak energy density of 704 Wh kg −1 in Li-dual-ion half cells. Furthermore, DAQ-DPZ@C in the symmetric Li-dual-ion batteries can deliver the peak discharge capacity of 88 mAh/g cathode and the peak energy density of 113 Wh kg -1 cathode , stably running for over 5000 cycles. To the best of our knowledge, these results are the top ones for small-molecule organic bipolar electrodes in the symmetric Li-dual-ion batteries.

研究领域: 材料科学 · 电化学
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Journal of the American Chemical Society · 2020 · IF 14.612

Systematic Modulation of Charge Transport in Molecular Devices through Facile Control of Molecule–Electrode Coupling Using a Double Self-Assembled Monolayer Nanowire Junction

Bin Han,Yao Li,Xuan Ji,Xianneng Song,Shuaishuai Ding,Baili Li,Hira Khalid,Yaogang Zhang,Xiaona Xu,Lixian Tian,Huanli Dong,Xi Yu,Wenping Hu

We report a novel solid-state molecular device structure based on double self-assembled monolayers (D-SAM) incorporated into the suspended nanowire architecture to form a “Au|SAM-1||SAM-2|Au” junction. Using commercially available thiol molecules that are devoid of synthetic difficulty, we constructed a “Au|S-(CH2)6-ferrocene||SAM-2|Au” junction with various lengths and chemical structures of SAM-2 to tune the coupling between the ferrocene conductive molecular orbital and electrode of the junction. Combining low noise and a wide temperature range measurement, we demonstrated systematically modulated conduction depending on the length and chemical nature of SAM-2. Meanwhile, the transport mechanism transition from tunneling to hopping and the intermediate state accompanied by the current fluctuation due to the coexistence of the hopping and tunneling transport channels were observed. Considering the versatility of this solid-state D-SAM in modulating the electrode–molecule interface and electroactive groups, this strategy thus provides a novel facile strategy for tailorable nanoscale charge transport studies and functional molecular devices.

CAS / MDL: 109-79-5 143-10-2
研究领域: 材料科学 · 物理化学
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Journal of Energy Storage · 2024 · IF 8.9

Accurate prediction of redox potential and the rational design of organic molecular electrode with multi-electron active centers for supercapacitor

Congcong Meng,Ning An,Shengmiao Song,Ling Wang,Liangzhikun Xiao,Yi Zhou,Ruibin Qiang,Yuying Yang,Zhimin Li,Zhongai Hu

P-benzoquinone (BQ) and derivatives represent a novel class of supercapacitor electrode materials due to their environmental friendliness, design flexibility and significant potential for rapid multi-electron faradaic reactions. But at present, the progress in guiding the structure design of electrochemical organic molecules and understanding their redox properties is still limited in explaining certain experimental phenomena related to supercapacitors. In this study, we propose an effective strategy for accurately predicting the redox potential of the organic molecular electrode (OME) through first-principles density functional theory (DFT). Additionally, we systematically investigated the impact of different functional groups and quantities on the reduction potential of 14 type BQ derivatives. We have identified a key factor that significantly affects the redox potential of OME: the electron cloud density surrounding the quinone active site (C=O). The electron-donating group (-CH 3 ) and benzene ring structure can further increase the electron cloud density around the quinone group, reducing reactivity with protons (H + ), thereby leading to a decrease in redox potential. Conversely, electron-withdrawing groups (-NO 2 ) lead to decreased electron cloud density around C O resulting in an increase in electrode potential. Furthermore, calculation results using Pearson correlation coefficients show that electron affinity (EA) has best linear correlation with reduction potential. Finally, we employed four methyl-p-benzoquinone derivatives (MBQ) as the composite organic electrode materials and achieve rapid and continuous reactions among multi-electron active centers within the designated potential window. Due to the synergistic effect from multiple molecules, MBQ-4 demonstrates an impressive specific capacitance of 681 F g −1 in 1 M H 2 SO 4 electrolyte, which is comparable to the pseudocapacitive material RuO 2 but at one-twentieth cost only.

研究领域: 材料科学 · 电化学
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APPLIED SURFACE SCIENCE · 2019 · IF 5.155

Non-covalently self-assembled organic molecules graphene aerogels to enhance supercapacitive performance

Lijie Hou,Chao Kong,Zhongai Hu,Yuying Yang,Hongying Wu,Zhimin Li,Xiaotong Wang,Penji Yan,Xiaojuan Feng

Organic molecules electrodes with high electrochemical reversibility has enormous potential in energy storage. Here, benz[a]anthracene-7, 12-quinone (BAQ) and 2, 5-dihydroxy-p-benzoquinone (DHBQ) are anchored on reduced graphene oxide (rGO) [BAQ (DHBQ)/rGO] by non-convent method to form the porous 3D dry aerogels. The optimal BAQ (DHBQ)/rGO electrode materials display capacitance all in excess of 400 F g −1 at current density of 1 A g −1 and an excellent rate capability in 1 M H 2 SO 4 electrolyte. And BAQ/rGO and DHBQ/rGO are used respectively as the negative and positive electrode to fabricate the asymmetric supercapacitor (ASC), which achieves high energy density of 30.33 Wh kg −1 with power density of 802.9 W kg −1 . Finally, 47 light-emitting diode (LED) bulbs aligned in a ‘NWNU’ shape are lit by two ASCs device in series, demonstrating its outstanding energy storage performance. Moreover, density functional theory (DFT) calculations are employed to understand the adsorption orientations, binding interactions and charge storage mechanism of BAQ on rGO surface, elucidating the superior electrochemical performance of the tested organic molecule electrode. In short, quinones non-covalently modified graphene is a promising and effective strategy for energy storage devices in future.

CAS / MDL: 2498-66-0 615-94-1
研究领域: 材料科学 · 能源存储 · 电化学
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Journal of Materials Chemistry A · 2023 ·Vol. 11 ·期 7 ·3565-3574 · IF 11.9

A supramolecular electrode with high self-healing efficiency at room temperature, recyclability and durability for dielectric elastomer generators

Wenpeng Zang,Sijin Jin,Shuxiong Fu,Yuhao Wang,Yingjie Jiang,Xueying Liu,Nanying Ning,Ming Tian,Liqun Zhang

To achieve dielectric elastomer generators (DEGs) with excellent energy harvesting performance and long life, electrode materials with high compliance, high electrical conductivity (EC), high stability of EC under high strain, and high durability are key. Nevertheless, the compliance of previously reported electrodes for DEGs still needs to be improved, and they cannot be repaired at room temperature after being damaged, inducing the trouble of disassembling the DEG device. In this study, a highly conductive supermolecule-based electrode material for DEGs was designed and prepared by synthesizing a polyborosiloxane supermolecule network (PBS-SN) matrix with multiple dynamic bonds followed by introduction of highly conductive carbon black (CB) and carbon grease (CG) into the PBS-SN matrix. Benefiting from the multiple dynamic bonds of the PBS-SN matrix and the introduction of appropriate content of a silicone oligomer (SO) with high chain mobility and plasticizing effect, the as-prepared CB/CG/PBS-SN electrode exhibits a high elongation at break (>1000%), high compliance, high self-healing efficiency of EC at room temperature (93% for 3 h), good recyclability (at least five times without performance reduction) and high durability (up to 10 000 cycles). Compared with a DEG using the commonly used CG electrode, the DEG using the CB/CG/PBS-SN electrode exhibits higher energy density, which is 60.9% higher than that of the former, and much higher than that reported in many previous studies. The excellent room temperature self-healing ability of the electrode can help the in situ repair of the DEG device, reducing the trouble of disassembling the device and improving the convenience of usage.

CAS / MDL: 10043-35-3 2530-85-0
研究领域: 材料科学 · 能源技术
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JOURNAL OF POWER SOURCES · 2024 · IF 8.1

A general separator modification tactic enables long-term stable cycling of small organic molecule electrodes in aqueous alkaline batteries

Rui Li,Mingsheng Yang,Liping Zheng,HaiPing Yu,Yan Wang,Huige Ma,Xinyu Wang,Qian Zhao,Hongwei Li,Mingjun Hu,Jun Yang

Rechargeable aqueous alkaline batteries based on small organic molecule anodes are a promising solution for large-scale energy storage due to their environmental friendliness and high energy efficiency. However, its development is limited by the poor cycling stability caused by the shuttling of soluble organic molecules between electrodes. Here, we propose a cell separator modified by metal organic framework (MOF) grown on the surface of graphene oxide (GO) to inhibit the shuttling of small organic molecules. It is demonstrated that the MOF@GO modified separator acts as an ion sieve in aqueous alkaline cells to effectively hold up small organic molecules without affecting the movement of metal ions. With the protection of the MOF@GO separator, soluble small molecules such as indanthrone (IDT) exhibit an amazing stability in alkaline electrolytes (a high reversible capacity of 137.0 mA h g −1 and a good capacity retention of 95.8% after 1000 cycles at 1 A g −1 ). It is the first report that employs carbonyl-containing small molecules as the electrodes for stable rechargeable aqueous alkaline batteries. Additionally, this strategy is also proved available to enhance the capacity and cycling stability of other active conjugated small molecules, such as PTCDI and 6CN-DQPZ, which will pave the way for the use of small organic molecules in aqueous alkaline batteries.

CAS / MDL: 7782-42-5
研究领域: 能源材料 · 电化学
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ACS Applied Energy Materials · 2021 · IF 6.024

Quinolinediol Molecule Electrode and MXene for Asymmetric Supercapacitors with Efficient Energy Storage

Long Jiao,Fuquan Ma,Xiaotong Wang,Zhimin Li,Zhongai Hu,Qing Yin

Asymmetric supercapacitors (ASCs) need positive and negative electrodes to produce a larger redox peak position difference to achieve a higher energy density. Here, 2,8-quinolinediol (QD) is adopted to modify reduced graphene oxide (rGO) and prepare an organic molecule electrode (OME), in which the Faraday reaction occurs in a more positive potential range. The electrochemical tests show that the optimized OME (QD/rGO-0.75) releases a high special capacitance (371 F g–1 at 5 mV s–1) and exhibits an excellent rate capability (86.8% of the initial value at a scanning rate multiple of nearly 20 times). Meanwhile, an MXene (Ti3C2Tx) with a relatively negative potential is prepared. QD/rGO-0.75 and Ti3C2Tx are, respectively, used as positive and negative electrodes to assemble an ASC. The measurements indicate that the assembled ASC is able to store charge within a wide voltage window of 1.6 V in the 1 M H2SO4 electrolyte and exhibit better energy storage performance. Furthermore, the device delivers an excellent cycling stability (83.5%, over 10,000 cycles). The two series-connected devices can light 37 red light-emitting diodes, indicating their potential application.

研究领域: 材料科学 · 电化学
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