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电化学工程
Small Methods · 2024 ·Vol. 8 ·期 7 ·2301233 · IF 10.7

Tin Hybrid Flow Batteries with Ultrahigh Areal Capacities Enabled by Double Gradients

Xiaolin Ye,Ningxin Xiong,Shaopei Huang,Qixing Wu,Hongning Chen,Xuelong Zhou

Tin-based hybrid flow batteries have demonstrated dendrite-free morphology and superior performance in terms of cycle life and energy density. However, the quick accumulation of electrodeposits near the electrode/membrane interface blocks the ion transport pathway during the charging of the battery, resulting to a very limited areal capacity (especially at high current density) that significantly hinders its deployment in long-duration storage applications. Herein, a conductivity-activity dual-gradient design is disclosed by electrically passivating the carbon felt near the membrane/electrode interface and chemically activating the carbon felt near the electrode/current collector interface. In consequence, the tin metals are preferentially plated at the region near electrode/current collector, preventing the ion transport pathway from being easily blocked. The resultant gradient electrode demonstrated an unprecedentedly high areal capacity of 268 mAh cm −2 at a current density of as high as 80 mA cm −2 . Numerical modeling and experimental characterizations show that the dual-gradient electrode differs from conventional electrodes with regard to their reaction current density distribution and electrodeposit distribution during charging. This work demonstrates a new design strategy of 3D electrodes for hybrid flow batteries to induce a desirable distribution of electrodeposits and achieve a high areal capacity at commercially relevant current densities.

研究领域: 电化学储能 · 材料科学 · 能源化学 · 电池技术 · 功能材料 · 电化学工程
✓ 已验证 DOI 高影响因子
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Desalination and Water Treatment · 2024 · IF 1

Surface coating of a side-chain type polyelectrolyte for endowing perm-selectivity between specific anions to an anion-exchange membrane with a small loss of membrane conductivity

Yan-zhen Shen,Xun-liang Wang,Yu-xiang Jia,Meng Wang

The endowment of perm-selectivity for specific ions will further extend the applications of heterogeneous membrane. In this work, a side-chain type weak cationic polyelectrolyte, PVDF-g-PVP, was synthesized for surface hydrophobilization of heterogeneous anion-exchange membrane (AEM) in order to impart perm-selectivity between specific anions with different Gibbs hydration energy. After microstructure observation and chemical composition analyses by SEM, AFM, EA and FTIR, the perm-selectivity between specific anions, electrical resistance, transport number, limiting current density, surface homogeneity, as well as salt permeability of the modified AEMs were investigated. Series of electrodialysis experiments in SO 4 2– /Cl – system indicated that a significant perm-selectivity was indeed achieved by the attachment of PVDF-g-PVP coating. In particular, it was worth noting that only a small loss of membrane conductivity was observed after the functionalization. This should be closely related to the micro-phase separation morphology of the coating layer which was induced by the polarity difference between the main chains and side chains of PVDF-g-PVP. Besides, the chronopotentiometric analyses indicated surface homogeneity of the heterogeneous AEM was significantly enhanced and then effectively ameliorated concentration polarization behaviors at the membrane-solution interface. Meanwhile, the perm-selectivity for co-ions was also improved and suppressed back diffusion behaviors of salt driven by concentration gradient. In brief, the modifying scheme proposed in this work can effectively improve comprehensive transport properties of conventional heterogeneous AEM.

研究领域: 膜科学与技术 · 高分子材料化学 · 分离科学 · 电化学工程 · 功能材料
✓ 已验证 DOI 高影响因子
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY · 2022 · IF 4.598

A coupling technology of capacitive deionization and carbon-supported petal-like VS2 composite for effective and selective adsorption of lead (II) ions

Dexi Liu,Shichang Xu,Yanmeng Cai,Yue Wang,Jiaqi Guo,Youlin Li

The conventional separation technologies, like chemical precipitation and adsorption processes, cannot quickly and selectively separate and recycle heavy metal ions from waste. Due to its rich sulfur content and excellent electrical conductivity, vanadium disulfide is a potential material for effectively removing lead from wastewater. The vanadium disulfide material with selective adsorption ability was introduced into CDI technology to construct a coupling technology with both advantages. The N -doped modified ZIF@vanadium disulfide (ZAC@VS 2 ) composites were successfully synthesized by hydrothermal method. Electrosorption experiments show that ZAC@VS 2 material presents the remarkable saturated adsorption capacity to lead(II) ions (239.52 mg/g) in the 500 mg/L PbCl 2 solution. In the triplex blend system (Fe 3+ /Pb 2+ /Na + ) with each solute density of 100 mg/L, the saturated adsorption efficiency of 85.4% to Pb 2+ can still be maintained. In addition, compared with the Langmuir(R 2 =0.873) adsorption isotherm model, the Freundlich model (R 2 =0.922) can be better used to fit the adsorption process, which proves that the adsorption process is multilayered and heterogeneous. XPS tests and competitive adsorption experiments show that the electric double layer (EDL) and complexation together promote the selective adsorption of heavy metal ions by ZAC@VS 2 . ZAC@VS 2 composite electrode shows excellent performance in the removal of lead ions in battery waste liquid, indicating the potential of introducing ZAC@VS 2 into CDI to remove lead ions.

研究领域: 环境科学 · 材料科学 · 水处理技术 · 重金属污染控制 · 电化学工程
✓ 已验证 DOI 高影响因子
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RSC Advances · 2015 ·Vol. 5 ·期 60 ·48946-48953 · IF 3.84

Catalytic and filterable polyester-filter membrane electrode with a high performance carbon foam–Fe–Co catalyst improved electricity generation and waste-water treatment in MBR–MFC

Tingting Yu,Lifen Liu,Qiao Yang,Jing Song,Fenglin Yang

Using the flat module membrane electrodes based on polyester filter modified with polyaniline (PANI)–phytic acid (PA), a new type of membrane bio-reactor (MBR) system is developed for both bio-electrochemical electricity generation and effluent filtration. A specifically prepared carbon foam–Fe–Co catalyst was coated on the conductive, filterable cathode membrane which makes it catalytic for enhancing cathodic oxygen reduction reaction and electricity generation. The cell voltage (with carbon foam–Fe–Co, 0.5–0.4 V) is superior to control test 1 (without any catalyst, 0.2 V), moreover, it is even better than control test 2 (with Pt–C catalyst, 0.5–0.3 V). The corresponding maximum power density of carbon foam–Fe–Co is 38.5 and 2.4 times higher than control test 1 and 2, respectively. More importantly, the base electrode materials and catalyst were both low-cost. The overall removal efficiency of COD and NH4+–N are satisfactory, at 95% ± 2.5% and 85% ± 2.5%, respectively. This integrated system is easy to scale up for practical application in waste-water treatment and offers a better option in operating and coupling MBR with bio-electricity generation.

研究领域: 环境工程 · 环境微生物学 · 电化学工程 · 水处理技术 · 生物电化学系统
✓ 已验证 DOI 高影响因子
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Chemical Engineering and Processing-Process Intensification · 2018 · IF 2.826

Electrogeneration of H2O2 using a porous hydrophobic acetylene black cathode for electro-Fenton process

Linchao Li,Huili Hu,Xiangguo Teng,Yuanchun Yu,Yongming Zhu,Xiaoqiang Su

The aim of this work is to prepare a hydrophobic cathode equipped with quite a few cracks for gas transfer, which can prepare H 2 O 2 in the course of electro-Fenton process. Scanning electron microscopy (SEM) and optical digital microscope are used to characterize the morphology of electrode, and an electrochemical workstation (CHI660e) is used to carry out all electrochemical studies with a conventional three-electrode system. The results demonstrate that the porous electrode is conducive to gas transmission with these cracks which can avoid the formation of bubbles. Additionally, the reaction is almost not affected by the content of dissolved oxygen and the gas flow with this structure. Under the conditions of 300 mA/cm 2 (current density), the H 2 O 2 concentration is up to 14.4 mmol/L after 30 min electrolysis with current efficiency beyond 90%. Furthermore, the cathode is successfully applied to electro-Fenton process which reduced catalyst loading. The results indicate that total degradation of MO is observed at the first 10 min, and 81% of TOC can be removed when the dosage of catalyst is 0.4 mmol/L within 60 min.

研究领域: 环境化学 · 电化学工程 · 水处理技术 · 反应器设计 · 污染物降解
✓ 已验证 DOI 高影响因子
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Small · 2024 ·Vol. 21 ·期 4 ·2410657 · IF 13

2D MOF Structure Tuning Atomic Ru Sites for Efficient and Robust Proton Exchange Membrane Water Electrolysis

Jia Wang,De Wang,Zelin Zhao,Ganggang Chang,Wei Guo,Jun Xu,Yinyu Xiang,Junrui Li,Junsheng Li

Developing cost-effective ruthenium (Ru)-based HER electrocatalysts as alternatives to commercial Pt/C is crucial for the advancement of proton exchange membrane water electrolysis (PEMWE). However, the strong hydrogen adsorption of Ru-based catalysts restricts its activity. Herein, a strategy is reported to tune the electronic structure and improve mass transfer by implanting Ru atoms onto the (002) facet of two-dimensional zeolitic imidazolate framework-67 (Ru@ L ZIF (002) ) to optimize the d -band center ( ε d ) of Ru and the hydrogen spillover behavior. Benefiting from the ultrathin nanosheet structure and optimized ε d of Ru, the over-strong H adsorption energy is weakened and the electron/mass transfer is facilitated. Ru@ L ZIF (002) exhibits an overpotential of 9.2 mV at 10 mA cm −2 and a long-lasting stability of 35 days at 100 mA cm −2 . The mass activity and price activity of Ru@ L ZIF (002) is 2.9 and 14.7 times higher than Pt/C, respectively. More impressively, Ru@ L ZIF (002) delivers a cell voltage of 2.01 V at a high current density of 4 A cm −2 in PEMWE. The excellent long-term durability of 1200 hours operating at 4 A cm −2 with an ultralow decay rate of 7.5 × 10 −3 mV h −1 has been achieved, making it promising as a cost-effective alternative to Pt/C catalyst for PEMWE applications.

研究领域: 电催化 · 材料科学 · 能源化学 · 纳米材料 · 电化学工程 · 可持续能源技术
✓ 已验证 DOI 高影响因子
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Journal of Materials Chemistry A · 2018 ·Vol. 7 ·期 11 ·5991-6000 · IF 9.931

A bimetallic thermally regenerative ammonia-based battery for high power density and efficiently harvesting low-grade thermal energy

Weiguang Wang,Hua Tian,Gequn Shu,Dongxing Huo,Fang Zhang,Xiuping Zhu

A bimetallic thermally regenerative ammonia-based battery (B-TRAB) using inexpensive materials efficiently converts low-grade thermal energy into electricity with high power density. Through thermal regeneration of the anolyte, the B-TRAB system realized high-voltage discharge (1.38 V) with redox couples [Cu(II)/Cu and Zn(NH3)42+/Zn] and low-voltage charge (0.72 V) with Zn(II)/Zn and Cu(NH3)42+/Cu. Adding 2 M NH3 to the anolyte of a Cu/Zn-TRAB produced a peak discharge power density of 525 W m−2-electrode (120 W m−2-membrane), and the voltage (or current) and peak power could be doubled by connecting two cells in series (or parallel). In successive regeneration cycles, a maximum power density of 115 W m−2-electrode (26 W m−2-membrane) and a net energy density of 714 W h m−3 were produced at a constant current density of 100 A m−2. The power density was enhanced to 515 W m−2-electrode (118 W m−2-membrane) and maintained in successive cycles by adding acid to the regenerated catholytes, with a net energy density of 299 W h m−3 (discharged at a constant load of 12 Ω and charged at a constant current density of 100 A m−2). A thermal-electricity conversion efficiency of 0.95% (10.7% relative to the Carnot efficiency) was achieved.

研究领域: 能源材料 · 电化学工程 · 热电转换技术 · 可持续能源 · 功能材料
✓ 已验证 DOI 高影响因子
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2024 · IF 8.1

An engineering approach for active and stable dry methane reforming within solid oxide fuel cell stacks using La0.6Sr0.2Cr0.85Ni0.15O3-δ as a catalyst

Cheng Li,Guangyu Li,Yongtao Zhan,Chenzhao Liu,Yujie Tang,Dong Yan,Jian Li,Lichao Jia

A strategy of in-stack dry reforming of methane (DRM) is proposed by using La 0.6 Sr 0.2 Cr 0.85 Ni 0.15 O 3-δ -loaded Ni foam (LSCrN@NF) as a CH 4 –CO 2 reformer, fuel gas distributor, and anode current collector in a SOFC stack. The prepared LSCrN exists as a single phase in a perovskite structure ; its reduced form contains exsolved Ni nanoparticles embedded on the surface of the LSCrN substrate. Introduced into an NF, the reduced LSCrN@NF demonstrates high DRM activity that increases with the increase of LSCrN amount to an optimum of about 42%. With the LSCrN@NF in-stack DRM, the conversions of CH 4 and CO 2 into CO and H 2 increase. Thus, the electrode polarization resistance, including the cathode and anode , decreases to 0.62, 1.07, and 3.93 Ω cm 2 at 800 °C, 750 °C, and 700 °C, respectively. Consequently, the peak power density (PPD) of the cell using 45% CH 4 -45% CO 2 –10% N 2 as fuel is 1.17, 0.94, and 0.47 W cm −2 , significantly higher than that of the cell without LSCrN@NF in-stack DRM. In addition, the voltage of the cell with LSCrN@NF in-stack DRM is stable on a level between 0.81 and 0.82 V at 400 mA cm −2 and 750 °C for 270 h without detected carbon deposition in the Ni–Y 2 O 3 stabilized ZrO 2 anode. This LSCrN@NF in-stack DRM strategy is also adopted with a large-scale (13 × 13 cm 2 ) single cell, which shows an extrapolated PPD of 428.3 mW cm −2 at 750 °C and is operated for 40 h at 400 mA cm −2 without noticeable performance degradation .

研究领域: 能源材料 · 电化学工程 · 催化化学 · 燃料电池技术 · 高温材料科学 · 化学反应工程 · 清洁能源转化
✓ 已验证 DOI 高影响因子
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SEPARATION AND PURIFICATION TECHNOLOGY · 2020 · IF 5.774

Formic acid recovery from EDTA wastewater using coupled ozonation and flow-electrode capacitive deionization (Ozo/FCDI): Performance assessment at high cell voltage

Longqian Xu,Yu Xie,Yang Zong,Yunfeng Mao,Bing Zhang,Huaqiang Chu,Deli Wu

Carbon resource recovery from toxic organic wastewater to reduce unnecessary energy loss and greenhouse gas emissions is rarely pursued. In the present study, a promising approach for formic acid (FA) recovery from EDTA wastewater was proposed by coupling ozonation and flow-electrode capacitive deionization (Ozo/FCDI). In the ozonation process, a FA productivity of 25% was obtained with the complete degradation of EDTA. The FA recovery from wastewater was compared under electrodialysis (i.e., without the use of flowable carbon electrodes, 0 wt%) and FCDI (i.e. using 5 wt% flowable carbon electrodes) processes and the results demonstrated the superiority of the FCDI process. After 390 min of operation, the accumulated FA concentration in the anode chamber of the FCDI system had increased to 633.6 mg/L with a low energy consumption of 8.0 kWh/kg FA, which was 1.8 times of the FA concentration in the electrodialysis (ED) process and nearly 6.4 times in the feed stream. These findings suggest the effective acquisition of high value-added FA in the Ozo/FCDI system; may provide new opportunities and challenges for the recovery of organic compounds.

研究领域: 环境工程 · 废水处理 · 资源回收 · 电化学工程 · 可持续化学 · 污染控制化学
✓ 已验证 DOI 高影响因子
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2020 ·Vol. 45 ·期 41 ·21816-21824 · IF 4.939

Towards continuous ammonia electro-oxidation reaction on Pt catalysts with weakened adsorption of atomic nitrogen

Yuanhui Wang,Zehui Yang,Jun Yang,Jingxiang Xu,Yaoping Xie,Jieyu Chen,Minghui Yang,Jianxin Wang,Wanbing Guan,Hiroki Muroyama,Toshiaki Matsui,Koichi Eguchi

One of the key challenges for ammonia-fed anion exchange membrane fuel cells is to the ammonia electro-oxidation reaction (AEOR) at anode, which has sluggish kinetics and generates atomic nitrogen (N ads ) poisoning the Pt catalyst. In this study, a comparative study on Pt/Ta 3 N 5 , Pt/Ta 2 O 5 , Pt/carbon black, and Pt plate are conducted in order to clarify the promoting effect of the support materials for Pt catalysts. X-ray photoelectron spectroscopy analysis and density functional theory calculations reveal that the support materials significantly affect the electron condition of the Pt, resulting in the tuned adsorption energy of N ads on Pt surface. The electrochemical analysis demonstrates that the weakened adsorption of N ads lowers the coverage of N ads on Pt surface, resulting in the enhanced performance and stability of Pt catalysts for AEOR. In particular, Pt/Ta 3 N 5 catalyst exhibits a current density of 5.92 mA cm −2 of AEOR at −0.34 V vs. SCE, which is higher than that of Pt/Ta 2 O 5 (2.56 mA cm −2 , −0.35 V vs. SCE) and Pt/C (4.45 mA cm −2 , −0.26 V vs. SCE). The achievements in this study demonstrate the importance of controlling the type of supports for the development of an active electrocatalyst for continuous AEOR.

研究领域: 电催化 · 能源材料 · 表面化学 · 燃料电池 · 电化学工程
✓ 已验证 DOI 高影响因子
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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

Cu-modified Ni foams as three-dimensional outer anodes for high-performance hybrid direct coal fuel cells

Heping Xie,Shuo Zhai,Tao Liu,Hailong Liao,Yuan Zhang,Wei Zhou,Zongping Shao,Meng Ni,Bin Chen

The hybrid direct coal fuel cell (HDCFC) is a promising technology for the generation of power using coal, which is abundant and cheap. However, restricted contact between the solid carbon in the coal and the anode of the cell not only limits the electrochemical oxidation sites, but also adversely affects the transport of electrons and ions. Herein, we demonstrate a new strategy of using Cu-modified Ni foams as the three-dimensional outer anode for a high-performance HDCFC with 3D structure, that is rich in electrochemical reaction sites and beneficial for electron and ion transport when filled with molten carbonates and anthracite coal. Moreover, the CuNi alloy layer formed on the surface of Ni foam is of excellent coking-resistance and capable of preventing ash-clogging, therefore effectively promoting the durability of an electrolyte-supported HDCFC. An excellent maximum power density of 378 mW cm −2 at 750 °C is achieved using the prepared 3D anode with anthracite coal as fuel. Besides, the cell exhibited stable operation for more than 13 h at 100 mA cm −2 , promising a new electrode design strategy for developing high-performance HDCFC anodes.

研究领域: 能源材料 · 燃料电池技术 · 电化学工程 · 洁净煤技术
✓ 已验证 DOI 高影响因子
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