JOURNAL OF CHEMICAL THERMODYNAMICS
·
2018
·
IF 2.631
Qingnan Zhang,Aijie Yan,Zixiang Cui,Yongqiang Xue
As an electrode material, the many excellent properties of nano-Bi 2 O 3 have been researched. However, the influences of particle size on the electrode reaction thermodynamic properties of nano-Bi 2 O 3 electrode are not clear. In this paper, the effect of particle size on electrochemical thermodynamic functions of nano-Bi 2 O 3 electrode was analyzed theoretically. In experiment, the spherical nano-Bi 2 O 3 with different particle sizes and the corresponding nano-Bi 2 O 3 electrodes were prepared, then the temperature coefficients of nano-Bi 2 O 3 electrodes and the thermodynamic functions of the electrode reaction were obtained by measuring the electrode potentials of nano-Bi 2 O 3 electrodes with different particle sizes at different temperatures. The experimental results show that the particle size has significant influence on the thermodynamic properties of nano-Bi 2 O 3 electrode, the standard electrode potentials and the equilibrium constants increase with the particle size decreases, while the temperature coefficient, the mole Gibbs energy change, the mole enthalpy change and the mole entropy change reduce. In addition, these physical quantities are all linearly related with the reciprocal of average particle size when the radius exceeds 10 nm. The experimental regularities are consistent with the theoretical analysis.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Journal of Environmental Sciences
·
2019
·
IF 3.556
Kaiyuan Zheng,Yuqiao Song,Xu Wang,Xin Li,Xuhui Mao,Dihua Wang
Herein, with the exploitation of iron and nickel electrodes, the 2,4-dichlorophenol (2,4-DCP) dechlorinating processes at the anode and cathode, respectively, were separately studied via various electrochemical techniques (e.g., Tafel polarization, linear polarization , electrochemical impedance spectroscopy). With this in mind, Ni/Fe nanoparticles were prepared by chemical solution deposition, and utilized to test the dechlorination activities of 2,4-DCP over a bimetallic system. For the iron anode, the results showed that higher 2,4-DCP concentration and solution acidity aggravated the corrosion within the electrode. The charge transfer resistance ( R ct ) values of the iron electrode were 703, 473, 444, and 437 Ω ∙ cm 2 for the initial 2,4-DCP concentrations of 0, 20, 50, and 80 mg/L, respectively. When the bulk pH of the 2,4-DCP solution varied from 3.0, 5.0 to 7.0, the corresponding R ct values were 315, 376, and 444 Ω ∙ cm 2 , respectively. For the nickel cathode, the reduction current densities on the electrode at − 0.75 V (vs. saturated calomel electrode) were 80, 106, and 111 μA/cm 2 , for initial 2,4-DCP concentrations of 40, 80, and 125 mg/L. The dechlorination experiments demonstrated that when the initial pH of the solution was 7.0, 5.0, and 3.0, the dechlorination percentage of 2,4-DCP by Ni/Fe nanoparticles was 62%, 69%, and 74%, respectively, which was in line with the electrochemical experiments. 10 wt.% Ni loading into Ni/Fe bimetal was affordable and gave a good dechlorination efficiency of 2,4-DCP, and fortunately the Ni/Fe nanoparticles remained comparatively stable in the dechlorination processes at pH 3.0.
研究领域:
环境科学
·
电化学工程
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DOI
高影响因子
Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 40
·21645-21654
·
IF 11.9
Min Zhang,Zhihong Du,Zhipeng Sun,Hailei Zhao
Iron-based double perovskites, as mixed electronic and oxygen ionic conductors, are potential air electrodes for reversible solid fuel cells. However, their catalytic activity towards the oxygen reduction reaction/oxygen evolution reaction is inferior to that of cobalt-based perovskites. Herein, a BaCO3-infiltrated SmBaFe2O5+δ (SBF) electrode is proposed with significantly enhanced catalytic activity. The theoretical computation and experimental study demonstrate that BaCO3 can significantly accelerate the oxygen adsorption/dissociation kinetics, which is identified to be the rate-limiting step of the SBF electrode. The BaCO3 decoration decreases significantly the polarization resistance from 0.154 to 0.068 Ω cm2 at 700 °C in air, and enables superior electrochemical performance in both fuel cell (FC) and electrolysis cell (EC) modes. The single cell with BaCO3 infiltrated SBF as an air electrode exhibits good operational stability in a reversible FC/EC mode for 34 cycles at ±300 mA cm−2, manifesting the good structural stability of the BaCO3-infiltrated SBF composite electrode under redox conditions. This work highlights the importance of clarifying the rate-limiting step and finding an effective strategy to facilitate this specific process for the design of high performance electrode materials.
研究领域:
材料科学
·
能源科学
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DOI
高影响因子
DESALINATION
·
2024
·
IF 8.3
Changyuan Dong,Wenpeng Hong,Lei Zhang,Jingrui Lan,Yan Li,Haoran Li
Ion migration-based moisture-electric generator holds the open-circuit voltage to power portable electronics, the Internet of Things, and wireless transmission. However, most devices still encounter challenges with the attainment of high-density power generation in continuous mode. Here, we introduce a sustainable and high-power density ion-selective bipolar moisture-electric generator that relies on Au-Al electrodes, capillary water supply, and interfacial evaporation. The device generates electricity by exploiting the salinity gradient between the capillary waterways in the photothermal and waste heat layers. This process is synergized by electrochemical reactions of the electrodes, which propel the migration of cations and anions through ion-selective bipolar hydrogels toward the intermediate waterway. It demonstrates a short-circuit current density of 52.2 A m −2 and a power density of up to 33.8 W m −2 over 0.5 cm × 0.5 cm electrodes. Connecting 13 devices in series in darkness successfully illuminates an LED lamp with a rated power of 1 W together with an operating voltage of 2.0–2.8 V. This work offers an off-grid, environmentally friendly, and affordable solution for high-density moisture power generation.
研究领域:
能源科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2022
·
IF 7.336
Wenting Wei,Jiaxuan Li,Huiqin Yao,Hongyun Liu
Herein, by a one-step synthetization method, a viologen derivative diallyl viologen (DAV) was first polymerized with methacryloylglycine (MAG) into P(MAG-DAV) polymer films on the surface of ITO electrodes. DAV component in the P(MAG-DAV) films was used not only as a cross-linker and immobilized in the film phase for repetitive usages, but also demonstrated reversibly electrochromic and luminescent properties. When the electrode voltage was switched between −0.7 and −0.5 V (vs SCE), DAV could transfer from its purple reduction state (DAV •+ ) to colorless oxidation state (DAV 2+ ) through the electrode reactions , accompanied with the fluorescence signal switching between non-fluorescence (DAV •+ ) and green fluorescence (DAV 2+ ) states. The addition of KMnO 4 in the solution could oxidize DAV •+ to its DAV 2+ form in the films to generate electrocatalytic signals and change the optical signals at the same time. Based on various reversible stimulus-responsive behaviors of P(MAG-DAV) film electrodes, a logic system of 3-input/3-output was established using potential, KMnO 4 and ultraviolet excitation light as inputs, and cyclic voltammetry (CV), fluorescence (FL) and UV−vis signals as outputs. Including an encoder and a decoder, a unique resettable and reprogrammable keypad lock was built with 3 different outputs. The system used a single immobilized molecule as the core of computing, and applied only 3 stimuli as inputs to construct an integrated logic computing system with 3 different output signals, which greatly improved the complexity and diversity of the molecular computing system. This might provide a new idea for the subsequent development of multifunctional integrated logic devices.
研究领域:
材料科学
·
化学
·
生物医学工程
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产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2022
·Vol. 33
·期 5
·2210343
·
IF 19.924
Qiuchen Xu,Shitao Geng,Bin Yuan,Meng Liao,Lei Ye,Xiaoju Zhao,Yan Wang,Xiao Zhang,Shuo Wang,Zongtao Qu,Han Miao,Zhibin Yang,Yue Gao,Bingjie Wang,Yongfeng Zhou,Huisheng Peng,Hao Sun
Lithium/thionyl chloride (Li/SOCl 2 ) primary batteries are appealing power solutions because of their remarkable electrochemical performances. However, their mass applications are hindered by the challenges in sustainability, cost and safety concerns owing to the employed Li chemistry. Here, magnesium (Mg) chemistry is shown as a promising alternative through synergistic optimization of electrolyte solvation and electrode reaction kinetics. The first Mg/SOCl 2 primary battery yields surprisingly high specific capacities up to ≈14 000 mAh g −1 at a decent discharge voltage of ≈1.67 V, which outperforms the state-of-the-art Mg-based primary batteries. In addition, it retains almost 100% of the original capacity after 20-day reservation. The impressive battery performances are originated from the stabilized MgCl 2 formation on high-surface-area carbon cathode and suppressed Mg anode corrosion via the Mg-induced solvation effect. Mg/SOCl 2 primary batteries are promising candidates for low-cost and recyclable power supplies, and they thus open new avenues for the development of sustainable battery chemistries.
研究领域:
材料科学
·
能源化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Rongrui Deng,Zhongting Wang,Shuangshuang Tan,Xueting Huang,Zhipeng Gao,Yongheng Fang,Chunfeng Chen,Ronghua Wang,Chaohe Xu,Guangsheng Huang,Jingfeng Wang,Fusheng Pan
Magnesium ion batteries (MIBs) hold immense potential for large-scale energy storage applications. However, serious polarization and sluggish reaction/diffusion kinetics resulting from high charge density of bivalent Mg 2+ significantly impeded the advancement of high-performance MIB cathodes. In this study, a coupling strategy of interlayer expansion and anionic vacancies is introduced into the cathode design of MIBs via PAN (polyacrylonitrile) intercalation, which can greatly enlarge the interlayer spacing of V 2 O 5 while induce cation reduction and generates abundant anion vacancies by facilitating electron transfer, thus expediting ion diffusion and electron transfer kinetics as demonstrated via combined GITT, EIS and CV analysis. Moreover, the PAN intercalation also endowed the electrode with ideal structural stability and electrochemical reversibility as proved via the systematic ex-situ investigations. Benefitting from this comprehensive strategy, PAN intercalated V 2 O 5 (V 2 O 5 -PAN) achieves remarkable electrochemical performance: a high discharge specific capacity of ∼ 180 mAh g −1 at 50 mA g −1 after stabilization, and an impressive life-span of 18,000 cycles at 2 A g −1 . This methodology offers valuable insights into enhancing the electrode kinetics performance of MIBs.
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 the American Chemical Society
·
2021
·
IF 15.419
Qing-Xia Chen,Ying-Huan Liu,Zhen He,Jin-Long Wang,Jian-Wei Liu,Hui-Jun Jiang,Wei-Ran Huang,Guan-Yin Gao,Zhong-Huai Hou,Shu-Hong Yu
The kinetics of electrode reactions including mass transfer and surface reaction is essential in electrocatalysis, as it strongly determines the apparent reaction rates, especially on nanostructured electrocatalysts. However, important challenges still remain in optimizing the kinetics of given catalysts with suitable constituents, morphology, and crystalline design to maximize the electrocatalytic performances. We propose a comprehensive kinetic model coupling mass transfer and surface reaction on the nanocatalyst-modified electrode surface to explore and shed light on the kinetic optimization in electrocatalysis. Moreover, a theory-guided microchemical engineering (MCE) strategy has been demonstrated to rationally redesign the catalysts with optimized kinetics. Experimental measurements for methanol oxidation reaction in a 3D ordered channel with tunable channel sizes confirm the calculation prediction. Under the optimized channel size, mass transfer and surface reaction in the channeled microreactor are both well regulated. This MCE strategy will bring about a significant leap forward in structured catalyst design and kinetic modulation.
研究领域:
化学工程
·
电化学
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产品关联
DOI
PubMed
高影响因子
Green Energy & Environment
·
2022
·
IF 12.781
Zhengshan Yang,Bowen Deng,Kaifa Du,Huayi Yin,Dihua Wang
Molten carbonate is an excellent electrolyte for the electrochemical reduction of CO 2 to carbonaceous materials. However, the electrolyte–electrode-reaction relationship has not been well understood. Herein, we propose a general descriptor, the CO 2 activity, to reveal the electrolyte–electrode-reaction relationship by thermodynamic calculations and experimental studies. Experimental studies agree well with theoretical predictions that both cations (Li + , Ca 2+ , Sr 2+ and Ba 2+ ) and anions (BO 2 − , Ti 5 O 14 8 − , Si O 3 2 − ) can modulate the CO 2 activity to control both cathode and anode reactions in a typical molten carbonate electrolyzer in terms of tuning reaction products and overpotentials. In this regard, the reduction of C O 3 2 − can be interpreted as the direct reduction of CO 2 generated from the dissociated C O 3 2 − , and the CO 2 activity can be used as a general descriptor to predict the electrode reaction in molten carbonate. Overall, the CO 2 activity descriptor unlocks the electrolyte–electrode-reaction relationship, thereby providing fundamental insights into guiding molten carbonate CO 2 electrolysis.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
RSC Advances
·
2018
·Vol. 8
·期 53
·30530-30538
·
IF 2.936
Wei Han,Wenjuan Wang,Yongchang Dong,Mei Li,Xiaoguang Yang,Milin Zhang
The electrode reaction of Pb(II) and co-reduction of Li(I) and Pb(II) were investigated on a tungsten electrode in LiCl–KCl eutectic melts by a range of electrochemical techniques. From cyclic voltammetry and square wave voltammetry measurements, the reduction of Pb(II) was found to be a one-step diffusion-controlled reversible process with the exchange of 2 electrons. The diffusion coefficients of Pb(II) were computed, and they obey the Arrhenius law. Using the linear polarization technique, the kinetic parameters, such as exchange current intensity (j0), standard rate constant (k0) and charge transfer resistance (Rct) for the Pb(II)/Pb(0) couple on a tungsten electrode were studied at different temperatures, and the activation energy is 27.32 kJ mol−1, smaller than the one for diffusion of Pb(II), which further confirmed that the reduction of Pb(II) was controlled by diffusion. A depolarisation effect for Li(I) reduction was observed from the results of cyclic voltammetry, square wave voltammetry and chronopotentiometry due to the formation of Li–Pb alloys by co-reduction of Li(I) and Pb(II). Furthermore, five Li–Pb intermetallic compounds, LiPb, Li8Pb3, Li3Pb, Li10Pb3 and Li17Pb4 characterized by scanning electronic microscopy and X-ray diffraction, were selectively prepared by potentiostatic electrolysis on a tungsten electrode and galvanostatic electrolysis on a liquid Pb electrode, respectively.
研究领域:
电化学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL PAPERS
·
2019
·Vol. 74
·期 3
·895-901
·
IF 1.246
Gao Ruo-Xuan,Gao Yuan-Yuan,Xie Rui-Jun,Han Li-Min
Ferrocenylcarboxylic acid Fe, Co, and Ni complexes were synthesized as model complexes to investigate how many ferrocene units of multi-ferrocenyl system can react with the electrode. The molecular structures of model complexes were characterized by X-ray single-crystal diffraction, the diffusion coefficient of the complexes and ferrocene was determined by the diffusion-ordered spectroscopy and Einstein–Stokes equation, the electrode reaction numbers of ferrocene units were determined by cyclic voltammetry and the Randles–Sevcik equation. A model of electrode reaction of multi-ferrocenyl system was proposed in this paper, which was used to explore how many ferrocene units of multi-ferrocenyl complexes can react with the electrode.
研究领域:
电化学
·
材料科学
·
分析化学
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2024
·Vol. 31
·期 17
·25952-25963
·
IF 0
Di Hongcheng,Jiang Zhuwu,Sun Fengyi,Yang Jiahan,Cheng Wei,Lu Jiahui,Zhang Hongyu,Bai Xue
Nitrogen-containing disinfection by-products (N-DBPs) produced in the process of drinking water disinfection are widely concerning due to the high cytotoxicity and genotoxicity. It is due to the difficulty of natural degradation of N-DBPs in water and the fact that conventional treatment systems do not effectively treat N-DBPs in drinking water. In this study, N-nitrosopyrrolidine (NPYR) in water was electrocatalytically degraded by a three-dimensional electrode reactor (3DER). This system applied graphite plates as anode and cathode. The granular activated carbon (GAC) was used as third electrode. The degradation of NPYR using a continuous flow three-dimensional electrode reactor was investigated by examining the effects of flow rate, current density, electrolyte concentration, and pollutant concentration on the degradation efficiency, energy consumption, and reaction kinetics of GAC particle electrodes. The results showed that the optimal operating conditions were flow rate = 0.45 mL/min, current density = 6 mA/cm 2 , Na 2 SO 4 concentration = 0.28 mol/L, and NPYR concentration = 20 mg/L. Under optimal conditions, the degradation of NPYR exceeded 58.84%. The main contributor of indirect oxidation was deduced from free radical quenching experiments. NPYR concentration was measured by GC–MS with DB-5 capillary column, operating in full scan monitoring mode for appropriate quantification of NPYR and intermediates. Based on the identification of reaction intermediates, a possible pathway for the electrochemical oxidation of NPYR on GAC particle electrodes was proposed.
研究领域:
环境科学
·
化学工程
·
饮用水处理
✓ 已验证
DOI
PubMed
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