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ACS Applied Energy Materials · 2024 · IF 5.4

Fish-Gill-Inspired Underwater Self-Breathing Zinc–Air Batteries

Fancheng Meng,Peng Chen,Shulin Li,Na Cao,Sheng Cheng,Xiangfeng Wei,Jiangtao Di,Jiehua Liu

Compared with the rapidly developing lithium- and sodium-ion batteries, zinc-air batteries (ZABs) offer the advantages of safety and high energy density. Nevertheless, their applications in underwater conditions are currently limited due to the low oxygen levels in such environments. Drawing inspiration from fish gills, we have successfully constructed a self-breathing zinc-air battery (ZAB) that can extract dissolved oxygen from water and convert it to electrical energy. By utilizing a Co2Fe-NC catalyst and a large-window cathode, the ZAB demonstrates a continuous discharge duration of 68.6 h in the underwater condition, thanks to its well-engineered architecture, optimized catalyst, and gas diffusion layer. Meanwhile, the underwater ZAB outperforms fish gills as it also operates efficiently in air, exhibiting a high capacity of 740 mA h g–1 and a high power density of 320 mW cm–2. Additionally, prolonged cycling tests indicate the ZAB’s capability for stable charging and discharging with minimal potential variation. This study introduces an innovative approach to the development of breathable underwater metal–air batteries.

CAS / MDL: 10026-22-9
研究领域: 材料科学 · 能源技术 · 仿生学
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Frontiers of Environmental Science & Engineering · 2020 ·Vol. 15 ·期 1 ·1-15 · IF 4.053

Evaluation of the technoeconomic feasibility of electrochemical hydrogen peroxide production for decentralized water treatment

Li Yang,Zhang Yixin,Xia Guangshen,Zhan Juhong,Yu Gang,Wang Yujue

This study evaluated the feasibility of electrochemical hydrogen peroxide (H 2 O 2 ) production with gas diffusion electrode (GDE) for decentralized water treatment. Carbon black-polytetrafluoroethylene GDEs were prepared and tested in a continuous flow electrochemical cell for H 2 O 2 production from oxygen reduction. Results showed that because of the effective oxygen transfer in GDEs, the electrode maintained high apparent current efficiencies (ACEs,>80%) for H 2 O 2 production over a wide current density range of 5–400 mA/cm 2 , and H 2 O 2 production rates as high as ∼202 mg/h/cm 2 could be obtained. Long-term stability test showed that the GDE maintained high ACEs (>85%) and low energy consumption (< 10 kWh/kg H 2 O 2 ) for H 2 O 2 production for 42 d (∼1000 h). However, the ACEs then decreased to ∼70% in the following 4 days because water flooding of GDE pores considerably impeded oxygen transport at the late stage of the trial. Based on an electrode lifetime of 46 days, the overall cost for H 2 O 2 production was estimated to be ∼0.88 $/kg H 2 O 2 including an electricity cost of 0.61 $/kg and an electrode capital cost of 0.27 $/kg. With a 9 cm 2 GDE and 40 mA/cm 2 current density, ∼2–4 mg/L of H 2 O 2 could be produced on site for the electro-peroxone treatment of a 1.2 m 3 /d groundwater flow, which considerably enhanced ibuprofen abatement compared with ozonation alone (∼43%–59% vs. 7%). These findings suggest that electrochemical H 2 O 2 production with GDEs holds great promise for the development of compact treatment technologies for decentralized water treatment at a household and community level.

研究领域: 环境科学 · 电化学工程
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JOURNAL OF MEMBRANE SCIENCE · 2025 · IF 9

A “grab-and-throw” access for monomer diffusion in interfacial polymerization process for high-efficiency polyamide membrane in water purification

Xiyue Cai,Yonggang li,Zhenyu Xi,Chen Yun,Lianghong Yin,Jing Guo,Yaohan Chen,Shenghai Li,Suobo Zhang

The surface structures of polyamide (PA) layer are closely related to the monomers diffusion during interfacial polymerization (IP) process and is one of the significant issues affecting nanofiltration separation performance. However, nanofiltration membrane prepared by the conventional interfacial polymerization method usually has a relatively smooth surface, which limits the effective filtration area leading to low water permeation. Effective strategies to control monomer diffusion also need to be developed. To solve these problems, carbon disulfide (CS 2 ) is inferred as an additive to form piperazine n-dithiocarbonate (PIP-CS 2 ) in aqueous phase, which can reversibly protonate piperazine (PIP) into PIP-CS 2 - anion and PIP-H + cation. Due to the amphiphilic piperazine part, PIP-CS 2 and PIP-CS 2 - /PIP-H + ion pair tend to gather at water-oil interface offering a special “grab-and-throw” access for free PIP monomer. In this way, the diffusion of PIP monomer is well-controlled to fabricate an ordered nanoscale hollow surface of polyamide layer. The exceptional surface structure significantly affects the properties of nanofiltration membrane. the pure water flux enlarged from 6.53 to 17.65 L m −1  h −1 bar −1 . Na 2 SO 4 rejection was maintained at more than 98 %. the separation coefficient of Cl − and SO 4 2− enhanced from 19.14 to 54.80. This work provided a novel and effective way to increase the flux and adjust the surface structure and cross-linking degree in nanofiltration membrane production.

研究领域: 材料科学 · 环境工程
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IONICS · 2022 ·Vol. 28 ·期 9 ·4321-4329 · IF 2.961

Design of gas diffusion electrode electrolyzer for CO2 reduction to CO with Cl2 and Na2CO3 produced as by-products

Zhang Jin-Zhong,Wu Shuai,Shen Fengxia,Song Wenkang,Hua Yaxin,Wu Zhenyu,Zhang Xiao-Gang,Shi Jin

A novel gas diffusion electrode (GDE) electrolyzer has been constructed to convert CO 2 into CO, with chlorine (Cl 2 ) and sodium carbonate (Na 2 CO 3 ) produced as the by-products. Using this method, the product value yielded from CO 2 electrolysis can be increased substantially. In contrast to the conventional GDE electrolyzer, we use a cation-exchange membrane as the diaphragm to separate the cathode from the anode compartment, and use NaCl aqueous solution as the anolyte. During the electrolysis process, CO 2 is reduced to CO on the cathode, with CO 3 2− generated accompanied with CO formation. On the anode, Cl − is oxidized to Cl 2 . Na + in the anode chamber transfers through the cation-exchange membrane, and migrates into the catholyte. Thus, Na 2 CO 3 can be obtained owing to the co-existing of Na + and CO 3 2− in the catholyte. Using this method, CO 3 2− penetrating through the anion-membrane can be avoided. This problem has been considered as the crucial obstacle that impedes the practical utilization of the conventional GDE electrolyzer. Our designed GDE electrolyzer has a promising application perspective in the phosgene chemical industry.

研究领域: 化学工程 · 环境科学
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CERAMICS INTERNATIONAL · 2020 · IF 3.83

Construction of pine-branch-like α-Fe2O3/TiO2 hierarchical heterostructure for gas sensing

Hui Mei,Shixiang Zhou,Mingyang Lu,Yong Zhao,Laifei Cheng

For real-time environmental monitoring and gas detection under harsh conditions, gas sensors with high reliability, sensitivity, and selectivity are in increasing demand. Therefore, pine-branch-like α-Fe 2 O 3 /TiO 2 with a core–shell hierarchical heterojunction structure was designed and fabricated for ethanol sensing. The heterojunction increased the O adsorption, resulting in the formation of more chemisorbed O species for reaction with the target gas. Moreover, the pine-branch-like morphology formed three-dimensional hollow holes as channels for molecule diffusion and adsorption. Compared with gas-proof structures, the hollow regions can realize gas diffusion in the inner and outer surfaces of materials simultaneously. Further, in contrast to aggregated structures, the fibers were separated from each other, and charge conduction between the fibers needed to pass through the surface sensing layer at the fiber boundary; thus, the overall resistance change of the sensors was significantly affected by the response of the heterojunction to the target gas. Consequently, the α-Fe 2 O 3 /TiO 2 sensor exhibited a high response value of 40.4 toward 500 ppm ethanol gas and had excellent selectivity to ethanol. The proposed strategy may facilitate the design and construction of effective heterojunctions and nanostructures for gas sensing.

CAS / MDL: 64-19-7 10025-77-1
研究领域: 材料科学 · 传感器技术 · 纳米科技
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY · 2021 · IF 4.464

Efficient degradation of ibuprofen by electro-Fenton with microtubular gas- diffusion electrodes synthesized by wet-spinning method

Kaiqiang Shi,Yi Wang,Anlin Xu,Xiezhen Zhou,Hongwei Zhu,Kajia Wei,Xiaodong Liu,Jinyou Shen,Weiqing Han

Gas-diffusion electrodes (GDEs) are the efficient generator for the hydrogen peroxide, which plays an important role in the degradation of refractory organic contaminants by electro-Fenton processes. In this work, the microtubular gas-diffusion electrodes (MGDEs) were fabricated with the carbon nanotubes (CNTs) hollow fiber base by wet-spinning technology and then employed as gas-diffusion electrodes (GDEs). Characterized by FESEM, TEM, BET, XPS, the MGDEs were proved to be relatively compact and intact without fracture on the hollow fiber surface. Cyclic voltammetry test in three electrodes system was carried out to prove the catalysis effect of the surface functional groups in the electrochemical reactions. The time-course of H 2 O 2 production rate in the range of the different current density (10 ~ 25 mA cm −2 ), pH value (3.0 ~ 9.0) and electrolyte concentration (0.01 ~ 0.1 M Na 2 SO 4 ) were conducted to evaluated the electrochemical performance of MGDEs and explorer the optimal condition. The stability of electrocatalytic was also tested by repeated runs. Furthermore, several parallel-degradation process of the simulated wastewater with the 1.0 ~ 10.0 mg L -1 IBP were carried out in electro-Fenton system. Under the optimal conditions, the removal rate of IBP could reach 90.2% in 120 min with the pseudo first-order degradation rate constant of 0.01415 min −1 . It shows the potential of this system to degrade NSAIDs.

研究领域: 环境科学 · 化学工程
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2024 · IF 20.2

Stable H2O2 electrosynthesis at industrially-relevant currents by a membrane-based electrode with high oxygen accessibility

Zimou Liu,Kuiling Li,Lie Liu,Hang Song,Yong Zhang,Mike Tebyetekerwa,Xiwang Zhang,Ke Wang,Lili Xu,Jun Wang

Electrosynthesis of hydrogen peroxide (H 2 O 2 ) presents a sustainable alternative to the anthraquinone process, while the transition to applying this process at industrial-relevant currents remains a significant challenge. Most studies tried to solve it by catalysts modulations, whereas we found that the accessibility to the gaseous O 2 , might be the crux of this matter. Herein, we developed a series of membrane-based gas diffusion electrodes (Mem-GDEs) with varied O 2 accessibility. Their endurable currents were found to be well correlated with the O 2 mass transferability. By constructing high O 2 -accessible triphasic interfaces, Mem-GDE achieved a recorded current density , 1.4 A cm −2 , with the current efficiency higher than 80.6 %. It was also verified for the first time that the insufficient O 2 triggered a severe flooding problem and thus further deteriorate the O 2 mass transfer. This study highlights the importance of O 2 accessibility and provides new insights into triphasic interfaces construction for realizing industrial-used H 2 O 2 -generated electrodes.

研究领域: 化学工程 · 电化学 · 材料科学
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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

NH3 separation membranes with self-assembled gas highways induced by protic ionic liquids

Bingbing Yang,Lu Bai,Shaojuan Zeng,Shuangjiang Luo,Lei Liu,Jiuli Han,Yi Nie,Xiangping Zhang,Suojiang Zhang

As ecological pollution and resource waste caused by NH 3 emission become increasingly serious, thus the separation and recovery of NH 3 from exhausted gases is of great significance both for environment and economy. Herein, we present a kind of novel ionic liquids (ILs)-based hybrid membranes for efficient NH 3 separation. Protic ILs (PILs) are adopted to form self-assembled gas highways in the hybrid membranes with the nanostructures of a middle-sulfonated pentablock copolymer, exhibiting extremely high NH 3 affinity and gas diffusion. The highest NH 3 permeability and ideal NH 3 /N 2 selectivity is up to 2711 Barrer and 1407 at ambient temperature and 1 bar, much superior to the state-of-the-art membranes reported. The results indicated that the novel IL-based hybrid membranes are promising candidates for high-efficient NH 3 separation and purification.

研究领域: 环境科学 · 材料科学
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Separations · 2022 ·Vol. 9 ·期 5 ·130 · IF 3.344

Investigation of Molecular Mean Free Path, Molecular Kinetic Energy, and Molecular Polarity Affecting Knudsen Diffusivity along Pore Channels

Bin Xu,Haotian Qin,Lu Chen

The effective purification of corrosive gases at the cathode air stream side is essential for proton exchange membrane fuel cells’ performance in real-world applications. Gas molecular diffusion depth along the pore channel is a sufficient parameter that determines the effectiveness of the porous purification media. The collision between gas molecules and pore surfaces is the crucial determinant of the diffusion depth. An analytical model was developed to predict the gas molecular diffusion depth in the pore channels. Two different crystal sizes of UiO-66 were synthesized to validate against the model result and empirically determine the diffusion depths. The parametric effects of the mean free path, molecular kinetic energy, and molecular polarity on molecular diffusivity were assessed. A smaller molecular mean free path and greater molecular kinetic energy were favorable for larger diffusion depth, owing to the fewer collisions and enhanced bounces after collisions. Greater molecular polarity led to shorter diffusion depth due to the enhanced van der Waals force between molecules and pore surfaces.Keywords:gas diffusion;porous adsorption;mean free path;molecular kinetic energy;molecular polarity

CAS / MDL: 10026-11-6 100-21-0
研究领域: 材料科学 · 化学工程
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APPLIED SURFACE SCIENCE · 2020 · IF 6.182

Hydrophobic electrocatalyst for the enhanced activity of oxygen reduction reaction through controllable liquid/gas/solid interface

Jinmei He,Chen Yang,Xin Yang,Lulu Liu,Jiehui Li,Qian Liu,Lei Peng,Xiangrong Liu,Mengnan Qu

Slow gas consumption process has been considered as one of the main limiting factors to enhance the activity of oxygen reduction reaction (ORR). The superwettable materials can overcome the limitation of underliquid gas transport in electrocatalysis, however, most of the preparation process are complex and high cost. Herein, an electrocatalyst for ORR is synthesized by loading ZIF-67 on carbon black, then the hydrophobicity is bestowed on the catalyst and controlled by adjusting the amount of 1H,1H,2H,2H-perfluorodecyltriethoxysilane, aimed to preparing the carbon-based electrocatalyst with hydrophobic surface (Cal-CoZIF-XE2B/PFDS). Continuous and abundant cavitations on the catalyst surface ensure the rapid diffusion of oxygen to the three phase contact area of the reaction system. Compared with the unmodified catalyst, the hydrophobic catalyst has larger diffusion-limited current density (from 4.4 mA/cm 2 of the original catalyst to 5.2 mA/cm 2 of the modified catalyst) and higher half-wave potential (from 0.81 V of the original catalyst to 0.83 V of the modified catalyst). Furthermore, the as-prepared electrocatalysts which obtained with low cost and simple method, presenting durability and stability against alkaline and acidic electrolyte solutions and providing a general and reliable strategy for the study of ORR catalyst.

研究领域: 材料科学 · 电化学
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MATERIALS & DESIGN · 2022 · IF 9.417

Induced fast charge transport and gas release using 3D ordered vertical carbon nanotubes for high-performance electrocatalysis

Haifeng Zhang,Yang Liu,Xueya Xu,Ting Meng,Gangwen Fu,Yong Gao,Jie Pu,Yuxuan Wang

In the past decade, single-atom and nanocluster catalysts have emerged as promising materials for high efficiency electrocatalysis, while geometric morphologies and electronic properties of the supporting substrates dramatically affect the overall electrocatalytic performances. We have constructed highly oriented nitrogen-doped carbon nanotubes on carbon cloth (V-CNTs/CC) and demonstrated it can serve as superior substrate for Pt nanoclusters that are typical electrocatalysts for hydrogen evolution reactions. Compared with Pt@CNTs/CC, the Pt@V-CNTs/CC has significantly improved electron transport and charge transfer efficiency, as well as gas diffusion capability, leading to excellent catalytic activity and stability. The V-CNTs/CC designed in this work can serve as general support for various single-atom or nanocluster catalysts for high-performance electrocatalysis.

CAS / MDL: 62-31-7
研究领域: 材料科学 · 电化学
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JOURNAL OF THE EUROPEAN CERAMIC SOCIETY · 2021 · IF 5.302

Foaming mechanism of polishing porcelain stoneware tile residues via adding C, Al and Si powder

Hao Xiong,Anze Shui,Qingliang Shan,Shenghui Zeng,Xiuan Xi,Bin Du

Polishing porcelain stoneware tile residues (PPR) is used to prepare foamed ceramic to solve the problem of solid waste discharge in ceramic industry. In this study, C, Al and Si powder were added to the simulated PPR to control foaming, and the mechanism of silicon carbide foaming in the PPR was discussed in detail. After these powders were introduced into the simulated PPR, the phenomenon of alumina crystallization on the pore wall of the foamed ceramic and the diffusion of gas in the foamed ceramic were discovered to be exciting. The foaming mechanism of PPR is detailed as follows: the diffusion rate of oxygen in silicate liquid is faster than that of CO during sintering, so the CO generated by incomplete oxidation of silicon carbide in PPR accumulates in the liquid, which makes the volume of ceramics expand and causes foaming.

CAS / MDL: 1344-09-8
研究领域: 材料科学 · 环境工程
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