Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Zehui Fan,Zhisen Li,Dan Mo,Jingyang Zhang,Shuyi Yang,Yun Li,Changlong Bi,Chong Peng,E Tao
Modulation of nano electrocatalysts for targeted excitation of different reactive oxygen species (ROS) is a key challenge to achieve environmentally catalyzed efficient pollutant degradation. In this study, multivalent copper catalysts (Cu (0)/Cu (I)/Cu (II)) load on the surface of biochar (CBX) are prepared by the hydrothermal-impregnation method, and the modulation effect of different valences of copper on the pathway of reactive oxygen species (ROS) generation is investigated. X-ray diffraction (XRD) analysis shows the coexistence of three copper valence states. Radical scavenging experiment and DFT calculations indicate that Cu (I) dominates the adsorption and activation of peroxodisulfate (PS) to efficiently generate ·SO 4 - and ·OH. Cu (II) selectively generates 1 O 2 by modulating the dissolve oxygen conversion pathway; whereas Cu (0) acts as an activation center for bound oxygen and significantly promotes ·O 2 - generation. The nano-electrocatalytic system prepared at 600°C (CB6-PS) degraded 98.3% of enrofloxacin (ENR) over a period of time (60 min). Mechanistic studies indicate that the catalytic system realizes the coupling reaction between the radical pathway (·SO 4 - /·OH /·O 2 - ) and the nonradical pathway ( 1 O 2 ) by the synergistic action of multivalent copper, which providing a new theoretical basis and technical strategy for the development of targeted ROS generation function.
研究领域:
环境催化
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材料化学
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污染控制
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纳米催化
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环境功能材料
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高级氧化技术
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Qiming Song,Zifan Li,Qun Peng,Xinwen Ou,Kun Zhao,Zhimin Dong,Liqun Ye,Chenchen Liu,Yunhai Liu,Jun He,Lai-Hon Chung,Bin Han
Photocatalytic O 2 activation, which produces miscellaneous reactive oxygen species (ROSs) via electron or energy transfer, is crucial for various chemical and biological processes. Unfortunately, controlling the exciton behaviors to flexibly regulate the generation of ROSs has rarely been explored and the underlying regulatory mechanisms remain poorly understood. Here, via linkage orientation engineering of covalent organic frameworks (COFs), we showcase a facile strategy for the flexible regulation between 1 O 2 and H 2 O 2 generation in photocatalytic O 2 activation. Imine-based COFs equipped with donor (D)-N=C-acceptor (A) chain (TFPT COFs) exerts effective H 2 O 2 production via electron transfer, while its structurally isomeric COFs with reversed imine orientation (TAPT COFs) tends to singlet oxygen ( 1 O 2 ) photosynthesis via energy transfer, attaining high efficiency for pollutant removal. Based on the results from ultrafast spectroscopy and theoretical calculations, when the N atom of the imine linkage is close to the electron acceptor, it diminishes the surface potential difference and increases the exciton binding energy; this favors the activation of the spin-triplet state excitons via an energy transfer process. Conversely, a strong built-in electric field is created when this N atom is adjacent to the electron donor, which encourages the dissociation of excitons into carriers and their subsequent separation.
研究领域:
化学
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材料科学
·
生物学
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产品关联
DOI
高影响因子
ADVANCED MATERIALS
·
2024
·Vol. 36
·期 31
·2404319
·
IF 27.4
Zongqiang Sun,Xiaodong Lin,Chutao Wang,Yanyan Tan,Wenjie Dou,Ajuan Hu,Jiaqing Cui,Jingmin Fan,Ruming Yuan,Mingsen Zheng,Quanfeng Dong
Lithium–oxygen (Li–O 2 ) batteries, renowned for their high theoretical energy density, have garnered significant interest as prime candidates for future electric device development. However, their actual capacity is often unsatisfactory due to the passivation of active sites by solid-phase discharge products. Optimizing the growth and storage of these products is a crucial step in advancing Li–O 2 batteries. Here, a fluorine-doped bimetallic cobalt-nickel oxide (CoNiO 2– x F x /CC) with an interlaced catalytic surface (ICS) and a corncob-like structure is proposed as an oxygen electrode. Unlike conventional oxide electrodes with a “single adsorption catalytic mechanism,” the ICS of CoNiO 2− x F x /CC offers a “competitive adsorption catalytic mechanism,” where oxygen sites facilitate oxygen conversion while fluorine sites contribute to the growth of Li 2 O 2 . This results in a change in Li 2 O 2 morphology from a surface film to toroidal particles, effectively preventing the burial of active sites. Additionally, the unique open architecture aids in the capture and release of oxygen and the formation of well-contacted Li 2 O 2 /electrode interfaces, which benefits the complete decomposition of Li 2 O 2 products. Consequently, the Li–O 2 battery with a CoNiO 2− x F x /CC cathode demonstrates a high specific capacity of up to 30923 mAh g −1 and a lifespan exceeding 580 cycles, surpassing most reported metal oxide-based cathodes.
研究领域:
材料科学
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电化学
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能源存储与转换
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产品关联
DOI
PubMed
高影响因子
ChemistrySelect
·
2024
·Vol. 9
·期 13
·e202303633
·
IF 1.9
Mingyan Chen,Wentao Wang,Xinkai Feng,Dehua Zhang,Yao Zhang,Yucheng Liu
Graphical This work describes the application of a highly efficient catalyst (NH 2 -UiO-66-Mo) to the catalytic oxidation desulfurization process. NH 2 -UiO-66-Mo can greatly improve the efficiency of oxidative desulfurization The optimum operating conditions of NH 2 -UiO-66-Mo are investigated through experiments, which prove the excellent performance of the catalyst, and the reaction mechanism is further studied through a series of characterizations. A highly efficient oxidative desulfurization composite catalyst NH 2 -Uio-66-Mo has been prepared and applied in the catalytic oxidative desulfurization. It was elucidated that Mo 6+ could increase the oxygen vacancies and active sites on the catalyst and increase the pore size of UiO-66. Meanwhile, the removal rate of dibenzothiophene (DBT) reached 99.2 % after 60 min under optimal conditions and remained above 90 % after 5 cycles, showing the composite catalyst's remarkable catalytic performance and satisfactory reusability NH 2 -UiO-66-Mo. In addition, kinetic studies revealed that the desulfurization process can present a pseudo-first-order kinetic process. The apparent activation energy was 10.6 kJ/mol. Finally, in combination with oxides, possible oxidation pathways were identified.
研究领域:
化学工程
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材料科学
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催化反应
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产品关联
DOI
高影响因子
Catalysts
·
2025
·Vol. 15
·期 6
·544
·
IF 4
Tingting Hu,Baozeng Ren,Liang Zhao
Hydrogen peroxide (H2O2) is an important industrial chemical that is widely applied in many areas. The direct synthesis of H2O2from H2and O2has proved to be a green and economic pathway. Pd-based bimetallic catalysts, due to their superior catalytic performances in this reaction, have attracted intensive attention. Herein, Tetrakis(hydroxymethyl)phosphonium chloride (THPC) was adopted as the protective ligand to immobilize Pd-Au alloy nanoparticles onto activated carbon (AC). The varied Pd/Au molar ratios demonstrated homogeneously distributed Pd-Au nanoalloys with average particle sizes ranging from 3.51 to 5.75 nm. The optimal ratio was observed over the Pd3Au1/AC-THPC catalyst with a maximum H2O2productivity of 165 mol/(kgPd·h) and selectivity of 82.3% under ambient pressure. The relationship between the electronic structure and catalytic activity indicated Pd0was the active site, while the presence of Au inhibited H2O2degradation rate. This research could help in the design efficient bimetallic catalysts for the direct synthesis of H2O2.
研究领域:
化学
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催化材料科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Cleaner Production
·
2025
·
IF 10
Mingjie Huang,Bingyuan Xu,Ke Feng,Wei Xiang,Xiaohui Wu,Yiliang Lv,Tao Zhou
Microscale zero valent iron (ZVI) is a promising material for in situ water purification through O 2 activation, but its activity is hindered by the slow electron transfer rate caused by the shielding effect of the surface passivation layer. Herein, we introduce a synergistic strategy that combines an inorganic ligand, i.e., tetrapolyphosphate (TPP), with magnetic field (MF) to boost the O 2 activation efficiency of ZVI under neutral conditions. This approach has resulted in a 4.7-fold increase in the degradation rate of diclofenac (DCF) compared to the MF-unassisted system and a remarkable 22.0-fold improvement over an analogous system with MF and EDTA. Multiphysics simulations, batch experiments, and characterizations revealed that the enhanced degradation rate was not only attributed to the elevated magnetic gradient on the ZVI surface to enrich the paramagnetic O 2 and Fe ions, but also to the functions of TPP to suppress the annihilation of •OH and reduce the redox potential of Fe 2+ /Fe 3+ . Furthermore, a synergistic mechanism between MF and TPP that facilitates the detachment of the surface-bound Fe 3+ -TPP complex into the aqueous phase, thereby regenerating the surface active sites was elucidated. This study underscores the potential of the MF-TPP synergy as an effective strategy to enhance ZVI-based Fenton-like catalysis for pollutant remediation.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF NUCLEAR MATERIALS
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2025
·
IF 3.2
Chengyu Wang,Xiaorui Xu,Yang Tong,Wentao Zhou,Yafei Wang
Pyroprocessing of spent nuclear fuel is an important step in nuclear fuel cycle with the purpose of minimizing the radiation impact on environment and recycling useful elements. One major concern in the development of pyroprocessing is the structural material corrosion in LiCl-KCl molten salt electrolyte, which is the core component of the spent nuclear fuel reprocessing. To understand the influence of O 2- impurity on the structural material corrosion in LiCl-KCl molten salt, the study investigates the corrosion behavior of Inconel 600 alloy in LiCl-KCl molten salt containing different amounts of O 2- impurities at 500 °C by immersion corrosion experiments and electrochemical analyses.The results indicate that O 2- could accelerate the high-temperature corrosion behavior. The alloy surface developed a bilayer oxide structure following 500-hour exposure to molten salt with 3 mol% O 2- , identified as a 3.36-μm-thick outer Li 2 NiO 2 layer and a 1.11-μm-thick inner LiCrO 2 layer. Based on the corrosion behaviors of Inconel 600 alloy in LiCl-KCl molten salt with different amounts of O 2- impurities, a new O 2- affected corrosion mechanism involving the formation of dual-layer oxide films and nickel-rich particles was proposed, which could provide new insights for the corrosion study in the applications of pyroprocessing of spent nuclear fuel.
研究领域:
核能工程
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of the American Chemical Society
·
2023
·
IF 15
Shang Shi,Zhenzhen Shen,Shanshan Li,Qian Wang,Rui Wen,Bing Liu
The use of carbon materials in porous electrodes has impressive advantages. However, precisely tailoring the multilevel pore structure of carbon electrodes remains an unsolved challenge. Here, we report a highly efficient site-selective growth strategy to synthesize colloidal carbon rings by templating patchy droplets. Carbon rings are used for the direct fabrication of self-standing porous electrodes with hierarchical pores for lithium–oxygen batteries (LOBs). In situ atomic force microscopy reveals that during discharge the discharge products densely nucleate and grow on carbon rings, demonstrating that such rings are a very potential electrode material in LOBs. The hollow carbon ring electrode (HCRE) possesses micrometer-scale channels formed by random packing of rings and nanochannels consisting of ring-shaped hollow cavities connected by nanosized pores in the wall. Both channels contribute to ion transportation and gas diffusion, but the storage of the discharge products mainly lies in micrometer-scale channels, leading to a high discharge capacity of LOBs (20 658 mAh/g). Our work paves a new way to construct hierarchically porous electrodes for application in electrocatalysis and electrochemical energy storage.
研究领域:
材料科学
·
电化学能源存储
✓ 已验证
DOI
高影响因子
FREE RADICAL BIOLOGY AND MEDICINE
·
2018
·
IF 6.02
Qing Li,Jie Su,Shi-Jie Jin,Wei Wei,Xiao-dong Cong,Xiao-Xue Li,Ming Xu
Background Insulin resistance in endothelial cells contributes to the development of cardiovascular disease in type 2 diabetes mellitus (T2DM). Therefore, there are great potential clinical implications in developing pharmacological interventions targeting endothelial insulin resistance. Our previous studies indicated that argirein which was developed by combining rhein with L -arginine by a hydrogen bond , could substantially relieved stress related exacerbation of cardiac failure and alleviated cardiac dysfunction in T2DM, which was associated with suppressing NADPH oxidase activity. However, it is unclear whether argirein treatment attenuates the vascular lesion and dysfunction in T2DM and its underlying mechanisms. Methods and results The rat aortic endothelial cells (RAECs) were used to treat with palmitic acid (PA), a most common saturated free fatty acid , which could induce insulin resistance. It was showed that argirein increased glucose uptake and glucose transporter-4 (Glut4) expression and reversed the phosphorylation of IRS-1-ser307 and AKT-ser473, consequently resulting in the increase of the production of eNOS and NO in PA-induced RAECs. We further found that argirein blocked the Nox4-dependent superoxide (O 2 -. ) generation, which regulated glucose metabolism in RAECs during PA stimulation. In vitro, argirein increased the release of endothelial NO to relieve the vasodilatory response to acetylcholine and insulin, and restored the expression of Nox4 and pIRS-1-ser307 in the aorta endothelium of high-fat diet (HFD)-fed rats following an injection of streptozocin (STZ). Conclusion These results suggested that argirein could improve endothelial insulin resistance which was attributed to inhibiting Nox4-dependent redox signaling in RAECs. These studies thus revealed the novel effect of argirein to prevent the vascular complication in T2DM.
研究领域:
药理学
·
内分泌学
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心血管科学
·
糖尿病研究
✓ 已验证
DOI
PubMed
高影响因子
BIOMATERIALS
·
2021
·
IF 12.479
Hua Yu,Yue Cheng,Cong Wen,Yi-Qing Sun,Xue-Bo Yin
Nanozymes have been combined with glucose oxidase (GOx) for dual-enzyme cascade catalytic therapy. However, their catalysis efficiency is restricted because of the hypoxia tumor microenvironment (TME). Although many methods are developed for O 2 supply, the O 2 leakage and consumption of H 2 O 2 compromised their practical application. Herein, a biocompatible carbon nitride (C 3 N 4 )/nanozyme/GOx triple cascade nanocatalyst was designed with laser-activatable O 2 self-supply via water splitting to relieve tumor hypoxia and thus improve the catalysis efficiency. To this end, polydopamine (PDA) nanosphere was prepared and attached with C 3 N 4 nanosheet to improve water splitting efficiency and realize photothermal-enhanced catalysis, simultaneously. The [email protected] 3 N 4 composite was then coated with MIL-100 (Fe), where GOx was loaded, to form C 3 N 4 /MIL-100/GOx triple cascade nanocatalyst. The triple cascade catalysis was realized with laser-activatable O 2 supply from [email protected] 3 N 4 , H 2 O 2 generation with GOx, and •OH production from peroxidase-like MIL-100 (Fe) for tumor therapy. Upon 808 nm irradiation, PDA, as a photothermal agent, realized photothermal therapy and enhanced the catalytic therapy. Thus, the synergy of laser-activatable O 2 supply and photothermal enhancement in our triple cascade nanocatalyst improved the performance of catalytic therapy without drug resistance and toxicity to normal tissues.
研究领域:
纳米技术
·
癌症治疗
·
材料科学
·
生物医学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
RSC Advances
·
2018
·Vol. 8
·期 41
·23397-23403
·
IF 2.936
Zhuo-Liang Jiang,Jing Xie,Cong-Shan Luo,Meng-Yang Gao,Huan-Liang Guo,Mo-Han Wei,Hong-Jun Zhou,Hui Sun
The mechanism of Li–O2 batteries is based on the reactions of lithium ions and oxygen, which hold a theoretical higher energy density of approximately 3500 W h kg−1. In order to improve the practical specific capacity and cycling performance of Li–O2 batteries, a catalytically active mechanically robust air cathode is required. In this work, we synthesized a freestanding catalytic cathode with RuO2 decorated 3D web Co3O4 nanowires on nickel foam. When the specific capacity was limited at 500 mA h g−1, the RuO2–Co3O4/NiF had a stable cycling life of up to 122 times. The outstanding performance can be primarily attributed to the robust freestanding Co3O4 nanowires with RuO2 loading. The unique 3D web nanowire structure provides a large surface for Li2O2 growth and RuO2 nanoparticle loading, and the RuO2 nanoparticles help to promote the round trip deposition and decomposition of Li2O2, therefore enhancing the cycling behavior. This result indicates the superiority of RuO2–Co3O4/NiF as a freestanding highly efficient catalytic cathode for Li–O2 batteries.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Energy Storage Materials
·
2020
·
IF 16.28
Xiaohong Zou,Kaiming Liao,Di Wang,Qian Lu,Chuan Zhou,Ping He,Ran Ran,Wei Zhou,Wanqin Jin,Zongping Shao
Although aprotic Li-air batteries offer an attractive option for achieving ultrahigh energy density of electrochemical energy storage devices, the now-established system has so far fallen short of its potential due to a daunting challenge related to its open configuration, which results in not only the rapid corrosion of Li metal anodes but also the gradual evaporation of organic liquid electrolytes. Here, we show that these issues can be well addressed by protecting the Li-air battery with a new O 2 -permeable silica-aerogel-reinforced polydimethylsiloxane external membrane (OPSP). The highly flexible OPSP basically benefiting from hydrogen-bond cross-linking can be constructed in situ on any substrate with particularly desirable properties such as being water-/electrolyte-proof, O 2 -permeable, high thermotolerance, and transparent, which allows stable cycling of coin-type and flexible Li-air batteries under harsh conditions, such as a highly volatile DMSO electrolyte (over 660 h), a humid air (O 2 ) atmosphere (over 700 h) or circumstances in air (O 2 )-saturated liquid water (over 25 h). This work could potentially open a new research direction in developing O 2 -permeable membranes through hydrogen-bond cross-linking for the unfettered design of metal-air batteries.
研究领域:
材料科学
·
能源存储技术
✓ 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）