DIAMOND AND RELATED MATERIALS
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2023
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IF 4.1
Ying Quan,Qinfu Liu,Kuo Li,Hao Zhang,Yakui Li,Jing Zhang
Preparation of cost-effective fluorinated graphene (FG) has been a great challenge due to the expensive starting materials. In this article, natural coaly graphite (NCG) samples, collected at various distances from the intrusion, were used as starting materials to synthesis FG via a one-step hydrothermal process in hydrofluoric acid. The influence of NCG precursors on the resultant FG was investigated systematically. Not only the poorly ordered graphite layer with large interlayer distance and the structural defects , but also the organic oxygen and pyridinic groups in NCG promote the fluorination. For well crystallized NCG samples, the parameters of organic oxygen ratio (O/C), graphitization degree (DOG) or defect level (I D /I G ) of the NCG were reliable indicators of fluorination ability. For poorly crystallized NCG, the maximum fluorination of the resultant FG is as high as 34.50 % benefitting from the rich carbonyl groups of poorly crystallized NCG. In addition, the ash content is reduced to 0.04–2.41 % in FG samples from 13.58 to 28.05 % in NCG samples, and bulk NCG samples could be stripped into nanosheets of a few layers thickness simultaneously, which are respectively controlled by the ash content and crystalline order of NCG. Such findings provide crucial guidance for industry to design FG with a predicable fluorination level through selection of a specific NCG material. Most importantly, FG synthesized from NCG is facile, low-cost and highly scalable, which will drastically improve the value of currently ignored NCG.
研究领域:
材料科学
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化学工程
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DOI
高影响因子
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES
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2025
·Vol. 130
·期 5
·e2024JD041920
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IF 3.4
Chun Xiong,Binyu Kuang,Xueyan Chen,Xiaolei Ding,Huichao Liu,Xiangyu Pei,Zhengning Xu,Fei Zhang,Shikuan Yang,Huan Hu,Zhibin Wang
Organic oxidized sulfur (OOS) compounds, particularly surface-active ones like organosulfates and organosulfonates, constitute a significant atmospheric sulfur reservoir and play a crucial role in cloud formation. Due to limited measurements, the physical characteristics of OOS aerosols under high relative humidity (RH) and subsequent cloud activation potential remain unclear. In this study, we measured phase state, surface tension and morphology of mixtures containing inorganic salts (sodium chloride (NaCl) and ammonium salfate (AS)) and OOS under high RH (>99.5%), and investigated their cloud condensation nuclei (CCN) activity. We found that the κ CCN of the studied OOS ranged from 0.15 to 0.37, showing a negative relationship with molar volume. κ CCN and chemistry-derived κ Chem agreed well for mixtures containing OOS with short carbon chain length (≤4), which could be explained by the ideal solution because of the liquid phase and slight surface tension reduction compared to that of water. However, κ Chem overpredicted κ CCN by 35% and 17% on average for NaCl–OOS and AS–OOS with long carbon chain length (seven and eight), respectively, which was the opposite of results from inorganic–dicarboxylic acid mixtures we previously reported. Although surface tension notably decreased by 25%–44%, inorganic–OOS mixtures exhibited core-shell morphology and the OOS shell suppressed water uptake, whereas inorganic–dicarboxylic acid particles exhibited homogeneous state thus not inhibiting water uptake. Based on the results, we emphasize the pivotal role of surfactant in determining aerosol morphology and thereby CCN activations. Key Points Inorganic–OOS mixtures exhibited liquid phase at high relative humidity and surface tension was affected by organic carbon chain length Slightly reduced surface tension in short carbon chain systems could explain the closure between predicted and measured cloud condensation nuclei (CCN) activity CCN ability of the mixtures with long carbon chain length was mainly affected by initial morphology rather than surface tension Plain Language Summary Ubiquitous surface-active organic oxidized sulfur (OOS) compounds significantly influence the aerosol physical properties and subsequent cloud droplet activation. In this study, phase state, surface tension, morphology, and cloud condensation nuclei (CCN) activity of submicron particles containing inorganic salt and OOS were investigated. For mixtures containing OOS with short organic carbon chain length (≤4), the liquid phase and slight reduction in surface tension compared to that of water under nearly saturated conditions indicate ideal solution, leading to good closure between predicted and measured CCN activity. Inorganic-OOS mixtures exhibited core-shell morphology and water uptake suppression by the outer OOS shell contributed to the overprediction of CCN ability, whereas inorganic-dicarboxylic acid particles were homogeneous and water uptake was not inhibited. This study sheds light on the significance of OOS compounds in influencing submicron aerosol morphology and subsequent cloud formation.
研究领域:
大气科学
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环境化学
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产品关联
DOI
高影响因子
ChemSusChem
·
2024
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IF 7.5
Wei Fang,Haoran Luo,Ibrahim Mwamburi Mwakitawa,Fang Yuan,Xiaoxue Lin,Yifan Wang,Hao Yang,Tatyana Shumilova,Lijun Hu,Yujie Zheng,Chen Li,Jianyong Ouyang,Kuan Sun
Graphical A high-performance liquid quinone/hydroquinone (Q/HQ) based thermogalvanic cell is demonstrated through the synergistic coupling of redox reactions and thermogalvanic corrosion. These two processes kinetically reinforce each other, resulting in a rapid kinetic rate. This synergistic coupling not only enhances the power output but also induces copper deposition at the cold electrode, demonstrating the reversibility of the entire reaction system. Thermogalvanic cells with organic redox couple (OTGCs) have received significant attention for low-grade heat harvesting due to their high thermopower, versatile molecular design, and tailorable physiochemical properties. However, their thermogalvanic conversion power output is largely hindered by slow kinetic rate, which limits practical applications. In this work, we demonstrate a high-performance liquid quinone/hydroquinone (Q/HQ) based OTGC by synergistic coupling redox reaction and thermogalvanic corrosion. By adding hydrochloric acid (HCl) into electrolyte solution, HCl not only boosts intrinsic redox kinetic rate of Q/HQ, but also induces rapid thermogalvanic corrosion of the copper electrode. Notably, these two processes reinforce each other kinetically. Consequently, the Q/HQ-based OTGC exhibits a rapid kinetic rate alongside an increased thermopower, leading to a significantly enhanced power output density. As a result, the Q/HQ-based OTGC achieves an enhanced effective conductivity σ eff of 4.22 S m −1 and a record high normalized power density P max (ΔT) −2 of 108.7 μW m −2 K −2 . This strategy provides a feasible and effective method for development of high-performance OTGCs.
研究领域:
材料科学
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能源工程
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化学工程
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF POWER SOURCES
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2023
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IF 9.2
Xi Liu,Haolong Du,Jiayi Gao,Ziyan Shen,Tengfei Sun,Zhan'ao Tan,Fengming Chu
The organic redox flow battery (ORFB) has garnered attention due to its environmentally friendly nature, safety features, and design flexibility, making it an ideal choice for large-scale energy storage. A novel cobweb bionic flow field is designed to significantly improve the battery performance of the ORFB. The battery performance including the charge-discharge voltage, overpotential, concentration distribution and uniformity factors of the cobweb bionic flow field were compared with those of the serpentine flow field and the parallel flow field by a three-dimensional (3D) numerical model. The results indicate that the discharging voltage of the cobweb flow field is 3.35 % higher than that of the serpentine flow field. The uniformity factor of the cobweb flow field is 15.55 % higher than that of the serpentine flow field. The average concentration value of the cobweb flow field is 13.86 % higher than that of the serpentine flow field. Therefore, the design of the cobweb bionic flow field enhances the mass transfer behaviors in the flow field and improves the battery performance. The impacts of the number of branches on the battery performance are studied, and the results show that the cobweb flow field achieves optimal performance with 6 branches.
研究领域:
能源科学
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仿生学
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电化学
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DOI
高影响因子
JOURNAL OF POWER SOURCES
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2020
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IF 8.247
Quanbing Liu,Xiangrong Li,Chuanwei Yan,Ao Tang
Organic redox flow batteries with many technological advantages over conventional metal-based flow batteries represent a new generation flow battery technology for electric grid storage applications. Herein, we report a dopamine-based catholyte with a high redox potential of 0.77 V for aqueous organic redox flow batteries . In sulfuric acid, the dopamine exhibits an excellent combination of good electrochemical reversibility and high solubility up to 0.7 M, and undergoes a fast two-electron transfer redox reaction with a rate constant of 1.82 × 10 −3 cm s −1 . Paired with V 3+ /V 2+ , the dopamine-vanadium full cell delivers an average round-trip efficiency of 65% at 20 mA cm −2 and achieves a capacity retention of 50% for 100 consecutive charge-discharge cycles. Moreover, an energy efficiency of 51.3% can be steadily realized at an increased current density of 60 mA cm −2 , while an enhanced capacity retention over extended 200 charge-discharge cycles is also observed by introducing saturated ammonium chloride into sulfuric acid. The proposed dopamine-based catholyte not only successfully offers a new alternative for aqueous organic redox flow batteries, but its performance can be also further promoted by rational molecule design and optimizations in mass transfer and electrode kinetics .
研究领域:
材料科学
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电化学
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产品关联
DOI
高影响因子
ACS Catalysis
·
2023
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IF 12.9
Yaming Hao,Jili Li,Xueting Cao,Lingshen Meng,Jianxiang Wu,Xuejing Yang,Yefei Li,Zhipan Liu,Ming Gong
The paired electrolysis via anodic organic oxidation and cathodic hydrogen evolution has been an emerging hydrogen production technology with high efficiency and high values. Nickel oxyhydroxide is a special electrocatalyst that is capable of selectively oxidizing various alcohols, aldehydes, and amines to the corresponding carboxylates and nitriles at more favorable potentials compared to the oxygen evolution reaction. However, its detailed molecular-level mechanism is still in debate, especially for the potential-dependent behavior of some organic substrates. In this study, we revealed that the nickel oxyhydroxide can be dissected into two functional regions with a more facilely oxidized surface for facilitated substrate adsorption and a relatively inert bulk phase for accelerated electron transfer via probe-assisted kinetics and in situ surface-enhanced Raman spectroscopy. The prerequisite of the two regions conceals a universal potential-dependent oxidation behavior for almost all organic substrates. Further combining with the computational investigation unravels the origin of this potential dependence from the exothermic O/N-centered adsorption process on the surface and the rate-limiting proton-coupled electron-transfer (PCET) steps for the C–H bond breaking that demands bulk electron conductivity. This provides a rationale for designing more conductive underlayers to break the intrinsic limitations of nickel oxyhydroxide toward more efficient organic electrooxidation processes.
研究领域:
化学
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材料科学
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催化反应
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DOI
高影响因子
JOURNAL OF POWER SOURCES
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2019
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IF 7.467
Jiashu Yuan,Cuijuan Zhang,Yihan Zhen,Yicheng Zhao,Yongdan Li
The non-aqueous redox flow battery (NARFB) is a promising device for grid-scale energy storage. However, its electrochemical performance and long-term stability still need to be improved. This work shows that the electrochemical performance of NARFB can be remarkably enhanced by optimizing the supporting electrolyte and separator. The battery with 2,1,3-benzothiadiazole (BzNSN) as anolyte, 2,5-di-tert-butyl-1-methoxy-4-[2′-methoxyethoxy]benzene (DBMMB) as catholyte, tetraethylammonium bis(trifluoromethylsulfonyl)imide (TEATFSI) as supporting electrolyte , and porous Daramic 250 separator delivers an average discharge capacity of 1.7 Ah L −1 , voltage efficiency of 87.8%, Coulombic efficiency of 89.1%, and energy efficiency of 78.3% over 100 cycles at the current density of 40 mA cm −2 with 0.1 M active materials. The reasons for the capacity decay over cycling in terms of electrolyte leakage, crossover, and chemical decomposition are discussed.
研究领域:
能源存储技术
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电化学
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DOI
高影响因子
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
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2023
·Vol. 120
·期 20
·e2302407120
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IF 11.1
Ying-Jie Zhang,Jie-Jie Chen,Gui-Xiang Huang,Wen-Wei Li,Han-Qing Yu,Menachem Elimelech
Clarifying the reaction pathways at the solid–water interface and in bulk water solution is of great significance for the design of heterogeneous catalysts for selective oxidation of organic pollutants. However, achieving this goal is daunting because of the intricate interfacial reactions at the catalyst surface. Herein, we unravel the origin of the organic oxidation reactions with metal oxide catalysts, revealing that the radical-based advanced oxidation processes (AOPs) prevail in bulk water but not on the solid catalyst surfaces. We show that such differing reaction pathways widely exist in various chemical oxidation (e.g., high-valent Mn3+ and MnOX) and Fenton and Fenton-like catalytic oxidation (e.g., Fe2+ and FeOCl catalyzing H2O2, Co2+ and Co3O4 catalyzing persulfate) systems. Compared with the radical-based degradation and polymerization pathways of one-electron indirect AOP in homogeneous reactions, the heterogeneous catalysts provide unique surface properties to trigger surface-dependent coupling and polymerization pathways of a two-electron direct oxidative transfer process. These findings provide a fundamental understanding of catalytic organic oxidation processes at the solid–water interface, which could guide the design of heterogeneous nanocatalysts.
研究领域:
环境科学
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催化化学
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产品关联
DOI
PubMed
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
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2025
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IF 3.7
Jinghua Huang,Mingbao Huang,Jinan Li,Jie Zhang,Zhiyong Fu
Graphical A new thermoelectricity utilization system is established using tripyridinium–triazine compound for low-grade heat harvesting. The thermally induced potential shift arises from temperature-dependent interconversion between singlet and triplet states of the tripyridinium–triazine diradical. New energy technology is in urgent demand for waste heat harvesting and utilization for energy saving and renewable energy development. Herein, an aqueous organic redox flow battery (AORFB) with designed tripyridinium–triazine radicals ((TPyTz) ··4+ )/(TPyTz) ·5+ ) as the negative redox couple is constructed as a thermoelectricity utilization system. The electrochemical test indicates that the (TPyTz) ··4+ /(TPyTz) ·5+ couple shows an interesting potential change about 27 mV accompanied by system temperature varying from 298 K to 343 K. Nuclear magnetic resonance and electron paramagnetic resonance spectra approve that the population of high-energy (TPyTz) ··4+ triplet state increases with temperature rise. This shifts the potential of the (TPyTz) ··4+ /(TPyTz) ·5+ couple to a much more negative position. While the 2,2,6,6-tetramethylpiperidin-1-oxyl derivative (TPABPy)Cl 3 is used as the positive electrolyte with no temperature-dependent potential change, the AORFB established by these two couples displays a thermally induced potential change from 1.39 V to 1.42 V.
研究领域:
能源技术
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材料科学
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电化学
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产品关联
DOI
PubMed
高影响因子
Nature Communications
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2023
·Vol. 14
·期 1
·1-11
·
IF 16.6
Chen Zhe,Li Jili,Meng Lingshen,Li Jianan,Hao Yaming,Jiang Tao,Yang Xuejing,Li Yefei,Liu Zhi-Pan,Gong Ming
Simultaneously achieving abundant and well-defined active sites with high selectivity has been one of the ultimate goals for heterogeneous catalysis. Herein, we construct a class of Ni hydroxychloride-based inorganic-organic hybrid electrocatalysts with the inorganic Ni hydroxychloride chains pillared by the bidentate N-N ligands. The precise evacuation of N-N ligands under ultrahigh-vacuum forms ligand vacancies while partially retaining some ligands as structural pillars. The high density of ligand vacancies forms the active vacancy channel with abundant and highly-accessible undercoordinated Ni sites, exhibiting 5-25 fold and 20-400 fold activity enhancement compared to the hybrid pre-catalyst and standard β-Ni(OH) 2 for the electrochemical oxidation of 25 different organic substrates, respectively. The tunable N-N ligand can also tailor the sizes of the vacancy channels to significantly impact the substrate configuration leading to unprecedented substrate-dependent reactivities on hydroxide/oxide catalysts. This approach bridges heterogenous and homogeneous catalysis for creating efficient and functional catalysis with enzyme-like properties.
研究领域:
催化
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电化学
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材料科学
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化学工程
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Fei Qi,Zequan Zeng,Hongbin Lu,Wenhao Si,Yanbiao Liu,Zhanggen Huang,Yuting Niu
Herein, seleniSum and nitrogen (Se/N) co-doped carbon catalysts were prepared to improve the catalytic performance and degradation selectivity of periodate based advanced oxidation processes (PI-AOPs) for pollutant abatement. The additional Se/N doping in carbon resulted in a 183 % increase in the degradation efficiency of bisphenol A (BPA) compared to the exclusively N-doped carbon catalyst. The coupling effect of the dual dopants significantly enhanced the electron transfer process. DFT calculations revealed that the co-doping of Se and N induced electron rearrangement in the carbon lattice while simultaneously enhancing the adsorption energy for PI. Moreover, the dual-doping strategy narrowed the energy gap between the LUMO of the [SeNC-PI] complex and the HOMO of BPA, thereby offering an excellent electronic channel for facilitating the electron transfer process. Driven by the potential difference, selective degradation of different pollutants was dependent on the half-wave potential of organic compounds. Benefiting from the non-radical oxidation pathway, the SeNC800/PI system showed great resistance to interference from pH, coexisting ions and dissolved organic matter. This work provides a strategy for improving the oxidation performance and pathway selectivity of pollutants in PI-AOPs.
研究领域:
环境科学
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催化
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材料化学
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化学工程
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物理化学
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产品关联
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2021
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IF 7.46
You Dou,Ran Yang,Yue Xiao,Jiao Wu,Lingbo Qu,Yuanqiang Sun,Zhaohui Li
The development of light-driven organic nanozymes possessing photoactivity is of great significance in biomedical research and biosensing given that they exhibit prominent absorption and fascinating photo-controllability in the visible range. However, the number and availability of such nanozymes is quite low. In this work, N-arylpyridinium thiazolothiazole (N, N′-dichlorophenzyled dipyridinium thiazolo[5,4- d ]thiazole difluoride, TTz-Cl 2+ ), which exhibits inherent light-driven oxidase-mimicking activity, was synthesized and it was found that 3,3′,5,5′-tetramethylbenzidine (TMB) could be oxidized under visible light, and also underwent corresponding changes in color and absorption. Moreover, the enzymatic activity of TTz-Cl 2+ could be modulated precisely by switching the visible light on and off. Glutathione (GSH), an important biological antioxidation regulator, was shown to be capable of successfully impeding the catalytic functions of TTz-Cl 2+ . Thus, it proved possible to fabricate a facile photo-triggered colorimetric sensing system for detection of GSH based on the use of the TTz-Cl 2+ and TMB system. The sensor exhibited satisfactory analytical performance with a linear range of 1–17 μM and a detection limit of 0.47 μM and may be used to determine GSH in HeLa cell lysates with good selectivity and high sensitivity. This work not only extends the availability of organic nanozymes but also broadens the applications base of thiazolothiazole derivatives in biomedical analysis.
研究领域:
生物医学工程
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分析化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）