Journal of Environmental Chemical Engineering
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2025
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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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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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DOI
高影响因子
Chem
·
2019
·
IF 18.205
Rongan Shen,Wenxing Chen,Qing Peng,Siqi Lu,Lirong Zheng,Xing Cao,Yu Wang,Wei Zhu,Juntao Zhang,Zhongbin Zhuang,Chen Chen,Dingsheng Wang,Yadong Li
Summary The electrochemical direct synthesis of hydrogen peroxide (H 2 O 2 ) is significant but still challenging because of the lack of highly selective and active catalysts. Here, we report the synthesis of hollow nanospheres constructed by atomically dispersing platinum in amorphous CuS x support (h-Pt 1 -CuS x ) with a high concentration of single atomic Pt sites (24.8 at%), and this catalyst can consistently reduce O 2 into H 2 O 2 with selectivity of 92%–96% over a wide potential range of 0.05–0.7 V versus RHE in HClO 4 electrolyte. Scanning transmission electron microscopy and X-ray absorption fine structure spectroscopy confirmed the atomically isolated form of Pt with a low valance of +0.75. An electrochemical device that can synthesize H 2 O 2 directly from H 2 and O 2 is fabricated with H 2 O 2 productivity as high as 546 ± 30 mol kg cat − 1 h −1 . The well-defined and high-concentration single atomic Pt sites result in ultrahigh productivity of H 2 O 2 .
研究领域:
材料科学
·
电化学
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2018
·
IF 8.097
Qin Zhao,Yuhang Zhang,Guiru Sun,Lina Cong,Liqun Sun,Haiming Xie,Jia Liu
Developing a long-term stable electrolyte is one of the most enormous challenges for Li–O2 batteries. Equally, the high flammability of frequently used solvents seriously weakens the electrolyte safety in Li–O2 batteries, which inevitably restricts their commercial applications. Here, a binary mixture of highly concentrated tetraglyme electrolyte (HCG4) and 1,1,2,2-tetrafluoroethyl 2,2,3,3-tetrafluoropropyl ether (TTE) was used for a novel electrolyte (HCG4/TTE) in Li–O2 batteries, which exhibit good wettability, enhanced ionic conductivity, considerable nonflammability, and high electrochemical stability. Being a co-solvent, TTE can contribute to increasing ionic conductivity and to improving flame retardance of the as-prepared electrolyte. The cell with this novel electrolyte displays an enhanced cycling stability, resulting from the high electrochemical stability during cycling and the formation of electrochemically stable interfaces prevents parasitic reactions occurring on the Li anode. These results presented here demonstrate a novel electrolyte with a high electrochemical stability and considerable safety for Li–O2 batteries.
研究领域:
储能
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电化学
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材料科学
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电池技术
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DOI
高影响因子
Journal of Materials Chemistry A
·
2016
·Vol. 4
·期 25
·10008-10013
·
IF 8.262
Jin-ling Ma,Xin-bo Zhang
Development of an efficient air cathode for metal–air batteries composed of an element that is abundant on earth is a scientific and technical challenge. Here, nitrogen (N)-doped carbon cathodes were prepared using two conventional doping methods, namely ammonia activation (ammoxidation) and introduction of an N-containing precursor. Interestingly, the introduction of N-containing precursors to prepare the N-doped carbon material not only gave a different pore distribution with increased surface area but also maintained considerable N content, unlike the use of the ammoxidation method – thus greatly enhancing the catalytic activity (low overpotential) and improving the discharge capacity (6905 mA h g−1) and cycle life (from 8 to 66 cycles) in sodium–oxygen batteries compared with the pure carbon material. This study also stresses the importance of adopting the optimized synthesis method to prepare the N-doped carbon cathode.
研究领域:
电化学
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能源材料
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纳米材料
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电池技术
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多孔材料科学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Wangjie Chu,Shengkai Ke,Kexin Feng,Weizhen Xie,Zecui Sheng,Lu Lin,Xing Tang
Base-regulated ROS strategy enables mild HMF-to-FDCA oxidation. • NaHCO 3 stabilizes ·O 2 − ; NaOH promotes ·O 2 − /·OH synergy. • NaOH system drives O 2 relay: O 2 → ·O 2 − → H 2 O 2 → ·OH for FDCA synthesis. The sustainable conversion of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) via aerobic oxidation is a cornerstone of future biorefinery, yet its practical implementation under mild conditions is constrained by the spin-forbidden activation of triplet O 2 . In this work, we report a base-regulated reactive oxygen species (ROS) strategy that enables efficient HMF oxidation to FDCA at low temperatures (30–60 °C) under ambient oxygen pressure. We find that weak base NaHCO 3 selectively stabilizes ·O 2 − , directing a selective oxidation pathway, whereas strong base NaOH promotes a synergistic ·O 2 − /·OH mechanism that substantially accelerates the overall reaction. Through careful optimization, a 95.8% FDCA yield is obtained under ambient O 2 flow. Kinetic analysis, including reaction order determination and kinetic isotope effect measurements, demonstrates that O 2 activation is the rate-limiting step in the NaOH system, following a relay activation pathway of O 2 → ·O 2 − → H 2 O 2 → ·OH. This work not only elucidates the mechanistic role of bases in regulating ROS during HMF oxidation but also provides a practical and green route for synthesizing FDCA under mild, ambient-pressure conditions, advancing the field of sustainable biomass conversion. This work demonstrates a base-regulated reactive oxygen species (ROS) strategy for the mild oxidation of HMF to FDCA. The weak base NaHCO 3 selectively stabilizes ·O 2 − , directing a selective oxidation pathway, whereas the strong base NaOH promotes synergistic ·O 2 − /·OH participation, substantially accelerating the reaction. Mechanistic studies reveal that O 2 activation follows a relay pathway: O 2 → ·O 2 − → H 2 O 2 → ·OH in the NaOH system. Under ambient oxygen pressure and at 30–60 °C, a 95.8% FDCA yield is achieved, offering a new route for green biomass conversion. Download: Download high-res image (47KB) Download: Download full-size image
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DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·Vol. 13
·期 6
·120354
·
IF 7.2
Dan Dang,Xinyi Jiang,Juncheng Zhang,Yichao Wu,Baoxin Zha,Yingying Zhao
The valorization of crude glycerol, a major byproduct of biodiesel production, into high-value chemicals is critical for sustainable biorefineries. Herein, we report a novel alkali-free and homogeneous photocatalytic strategy for selectively converting glycerol to glycolic acid (GLYA) and formic acid (FA) using H 2 O 2 as a radical initiator under 365 nm UV irradiation. By optimizing volume fraction of H 2 O 2 (3.18％), light intensity (10 W), and temperature (35 °C), 99.3 % glycerol conversion with 23.47 % GLYA yield and 22.66 % FA yield was achieved within 2 h at ambient pressure. Crucially, scavenging experiments, post-illumination reactivity studies and the electron paramagnetic resonance (EPR) spectra revealed a synergistic •OH /•O 2 ⁻/ 1 O 2 radical cycle triggered by H 2 O 2 photolysis: (1) •OH initiates glycerol oxidation to glyceraldehyde; (2) •O 2 ⁻ (generated from O 2 reduction or H 2 O 2 decomposition) produces 1 O 2, which drives selective C-C cleavage to GLYA; (3) •OH/•O 2 ⁻/ 1 O 2 cycle enables mutual regeneration of active species, sustaining oxidation even after light cessation. This autocatalytic cycle eliminates the need for strong bases or noble metals, offering a green, energy-efficient route for glycerol upcycling.
研究领域:
催化化学
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绿色化学
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可再生能源
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环境科学
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化学工程
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产品关联
DOI
高影响因子
MATERIALS LETTERS
·
2018
·
IF 2.687
Yu Wang,Xingbao Zhu,Yingzhang Yan,Weihua Wan,Yuanguo Wu,Xin Ji,Zhe Lü
Actually, Li-O 2 batteries can be served as flexible power sources with extremely high specific energy densities to meet the rising demand for flexible and wearable electronic devices. In this work, the electrochemical performance and flexibility of a Li-O 2 battery are demonstrated to be significantly enhanced by introducing a KH550–NH 4 Cl-treated, KOH-activated, CNTs-grafted cotton fabrics cathode. The as-fabricated flexible cathode exhibits superior electrochemical performance, including a high specific capacity (22.4 mAh cm −2 at 0.15 mA cm −2 ), an excellent rate capability, and a good cyclic performance for more than 250 cycles.
研究领域:
材料科学
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电化学
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能源存储
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纳米材料
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柔性电子器件
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DOI
高影响因子
Journal of Materials Chemistry C
·
2020
·Vol. 9
·期 5
·1593-1603
·
IF 7.059
Guoming Gao,Ximeng Wang,Qifeng Chen,Caibo Xie,Jie Zheng,Huailin Fan,Lulu Ma,Ruifang Guan,Yanfen Fang,Xun Hu
Surface fluorinated TiO2 has received extensive attention in recent years due to the improved photocatalytic reactivity compared with that of pure TiO2. However, the synergy of surface fluorine (FS) and oxygen vacancy (VO) is not clear and needs further study. Here we systematically studied the effect of FS, VO and acidic sites of TiO2 nanosheets on the selective photocatalytic oxidation of benzylamine to imine. The photocatalytic activity first increased and then decreased as the content of FS decreased and VO increased. The photocatalytic activity reached a summit with the imine yield of 92.1% over TiO2-B-6 h, which is mainly due to the synergy between FS and adjacent VO, forming the frustrated Lewis pair that boosts the activation of O2. The varied contents of FS and VO not only cause an evident change in the amount of acidic sites, but also affect the band structure and separation efficiency of charge carriers. The experimental and calculation results demonstrate that the coexistence of FS and VO boosted the separation efficiency, density and mobility of photogenerated charge carriers, resulting in the improved photocatalytic activity. The improved photocatalytic activity can be attributed to the combined effects of FS, VO and acidic sites. This work provides a strategy for the explicit regulation of surface species on TiO2 nanosheets for improved photocatalytic activity.
研究领域:
材料科学
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环境科学
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化学工程
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DOI
高影响因子
Small
·
2018
·Vol. 14
·期 34
·1801798
·
IF 9.598
Xiaohong Zou,Qian Lu,Yijun Zhong,Kaiming Liao,Wei Zhou,Zongping Shao
Gel-polymer electrolytes are considered as a promising candidate for replacing the liquid electrolytes to address the safety concerns in Li–O 2 /air batteries. In this work, by taking advantage of the hydrogen bond between thermoplastic polyurethane and aerogel SiO 2 in gel polymer, a highly crosslinked quasi-solid electrolyte (FST-GPE) with multifeatures of high ionic conductivity, high mechanical flexibility, favorable flame resistance, and excellent Li dendrite impermeability is developed. The resulting gel-polymer Li–O 2 /air batteries possess high reaction kinetics and stabilities due to the unique electrode–electrolyte interface and fast O 2 diffusion in cathode, which can achieve up to 250 discharge–charge cycles (over 1000 h) in oxygen gas. Under ambient air atmosphere, excellent performances are observed for coin-type cells over 20 days and for prototype cells working under extreme bending conditions. Moreover, the FST-GPE electrolyte also exhibits durability to protect against fire, dendritic Li, and H 2 O attack, demonstrating great potential for the design of practical Li–O 2 /air batteries.
研究领域:
电化学能源
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材料科学
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纳米复合材料
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先进电池技术
·
固态离子学
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DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2026
·
IF 10.6
Fen Liu,Wei Xiang,Chen Wang,Yongchun Zhao,Tao Zhou,Mingjie Huang,Xiaohui Wu
High-concentration glyphosate (Gly) wastewater presents a formidable remediation challenge due to its recalcitrance and the inherent risk of generating toxic intermediates like aminomethylphosphonic acid (AMPA). Herein, we report a facile “waste-treats-waste” strategy utilizing a self-accelerated Fe(II)/O 2 system that operates efficiently under neutral pH, effectively circumventing the acidic constraints of traditional Fenton processes. This system achieved a 57% Gly removal efficiency (initial concentration 0.5 g/L) within 60 min, with a kinetic rate constant ( k obs = 0.029 min −1 ) significantly outperforming conventional oxidation technologies. Mechanistic investigations reveal that Gly acts as a suicide ligand, forming an inner-sphere Fe(II)-Gly complex that lowers the Gibbs free energy barrier, thereby rendering O 2 activation thermodynamically favorable. The degradation proceeds via a dual-pathway mechanism, synergizing hydroxyl radical (•OH) attack (∼40%) with a dominant intramolecular ligand-to-metal charge transfer (LMCT) process (∼60%). Crucially, density functional theory (DFT) calculations elucidate that Fe(III) coordination induces a regioselective weakening of the C–N bond adjacent to the phosphonate group. This steric and electronic modulation steers the reaction pathway toward the preferential formation of benign glycine, successfully suppressing the generation of highly toxic AMPA. Bioassays using Tetrahymena thermophila confirmed that this glycine-selective pathway optimization significantly mitigates the acute toxicity of the effluent, validating the system as a sustainable and eco-safe solution for herbicide wastewater treatment.
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Xiangcheng Zhang,Jingzhen Zhang,Jie Miao,Xue Wen,Chao Chen,Baoxue Zhou,Mingce Long
Photocatalytic H 2 O 2 production is a promising strategy for decentralized applications, but to realize efficient H 2 O 2 production in the ambient conditions and absence of organic sacrifice remains challengeable. Herein, anthraquinone functionalized covalent organic frameworks (TpAQ-COFs) were fabricated by β-ketoenamines links of 2,6-diaminoanthraquinone (AQ) and 2, 4, 6-triformylphloroglucinol (Tp), and the structures and compositions were tuned by controlling the condensation time. The increase of time favors the assembly of TpAQ-COFs into more ordered lamellar stacking structure, and induces the increase of enol-imine form. The critical role of anthraquinone moieties as the active sites for oxygen reduction was proved, that is, facilitating charge separation and enhancing the activity and selectivity of H 2 O 2 production. Upon visible light irradiation, the TpAQ-COF synthesized after 12 h reaction has the highest content of anthraquinone moieties and the best performance for H 2 O 2 production (420 μmol h −1 g −1 ) in the absence of organic sacrificial agents. These findings bring insights to incorporate anthraquinone chemistry into photocatalysts at molecular levels for efficient H 2 O 2 production.
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DOI
高影响因子
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