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
·
能源材料
·
纳米材料
·
电池技术
·
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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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
·
绿色化学
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可再生能源
·
环境科学
·
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
·
电化学
·
能源存储
·
纳米材料
·
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
·
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
·
材料科学
·
纳米复合材料
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先进电池技术
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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
Journal of Physical Chemistry C
·
2014
·
IF 4.835
Sujie Chang,Shigang Ruan,Erlong Wu,Weixin Huang
Oxide-on-metal particles with exposed interfaces exhibit wealthy structures and functions, but their facile synthesis remains as a challenge. Herein we report a facile O2-assisted hydrothermal method to synthesize CeO2-on-Ag particles with different CeO2 thicknesses. In this novel approach Ag particles catalyze the O2 + H2O reaction to form surface hydroxyls that induce the preferential nucleation of Ce(OH)3 on the surfaces of Ag particles, eventually forming CeO2 adlayers on Ag particles. CeO2-on-Ag particles exhibit the CeO2 thickness-dependent SERS effect in which their best SERS effect is 2 orders stronger than that of Ag particles. They also exhibit CeO2 thickness-dependent catalytic performance in CO oxidation in which the best one is as active as traditional CeO2-supported Ag catalyst. These results open up new opportunities to synthesize oxide-on-metal particles and explore their functions by tuning the oxide adlayer thickness.
研究领域:
材料科学
·
催化化学
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产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2014
·Vol. 17
·期 1
·335-342
·
IF 6.852
Muge Niu,Yucui Hou,Shuhang Ren,Wenhua Wang,Qitian Zheng,Weize Wu
Conversion of cellulose, the most abundant biomass, shows a high selectivity to yield formic acid (FA), when oxidized by O2 in NaVO3–H2SO4 aqueous solution. This conversion involves various reactions including hydrolysis and oxidation. In this work, the relationships between these reactions were studied. There are mainly two hydrolyses and two oxidations occurring in the conversion: initial hydrolysis (from cellulose to monosaccharides) and deep hydrolysis (from monosaccharides to levulinic acid); catalytic oxidation (from monosaccharides to FA) and ordinary oxidation (from levulinic acid to acetic acid). Among these four reactions, catalytic oxidation to FA and deep hydrolysis to byproducts are competitive. The increasing rate of deep hydrolysis is faster than that of catalytic oxidation, when temperature is increased. Catalytic oxidation is promoted and deep hydrolysis is suppressed, when the O2 pressure is increased. Moreover, deep hydrolysis is promoted and catalytic oxidation is suppressed, when H2SO4 concentration is increased. The hydrolysis–oxidation pathway of this conversion was proposed. Thus, the byproducts could be inhibited, and FA-oriented transformation could be realized.
研究领域:
生物化学
·
可再生能源
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产品关联
DOI
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
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产品关联
DOI
PubMed
高影响因子
ACS Applied Energy Materials
·
2018
·
IF 0
Huanhuan Guo,Guangmei Hou,Jianguang Guo,Xiaohua Ren,Xiaoxin Ma,Linna Dai,Shirui Guo,Jun Lou,Jinkui Feng,Lin Zhang,Pengchao Si,Lijie Ci
Lithium–oxygen batteries (LOBs) have attracted increasing interest because of their superior theoretical specific energy. However, the stability of lithium metal anode is one of the obstacles limiting their practical applications. Here, we introduce an artificial Li3PO4 solid electrolyte interphase (SEI) film to protect the lithium anode in LOB with LiI/LiNO3/DMSO (dimethyl sulfoxide) electrolyte. The Li3PO4-protected Li anode exhibits excellent electrochemical stability during the Li stripping/plating process and leads to a relatively uniform and featureless surface in LOB after cycling. Our research demonstrates that superior electrochemical performance can be achieved in the Li–O2 battery with the synergistic combination of the DMSO-based electrolyte, the LiI redox mediator, and the Li3PO4-protected Li anode. The LOB with a Li3PO4-protected Li anode exhibits a prolonged cycling life span of 152 cycles with a fixed capacity of 1000 mA h g–1 at 2 A g–1. The results in this work provide knowledge for the development of a robust strategy for protecting the Li anode in the applications of Li–O2 batteries.
研究领域:
材料科学
·
电化学
·
能源存储技术
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产品关联
DOI
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2018
·Vol. 26
·期 2
·1445-1454
·
IF 2.8
Wang Daiyao,Zou Jing,Cai Huahua,Huang Yixin,Li Fei,Cheng Qingfeng
Advanced oxidation processes offer effective solutions in treating wastewater from various industries. The process of alkali-activated hydrogen peroxide (H 2 O 2 ) was superior for the treatment of alkaline dye wastewater because no additional reagents were required except H 2 O 2 . However, an important and interesting phenomenon had been observed that the primary reactive species were found different for degrading organic pollutants with the process of alkali-activated H 2 O 2 . Azo dye of Orange G (OG) and triphenylmethane dye of Rhodamine B (RhB) were chosen as the target organic pollutants. The influences of various parameters on OG and RhB degradation by alkali-activated H 2 O 2 were evaluated. Furthermore, different scavengers, including ascorbic acid, methanol, t -butanol, isopropyl alcohol, furfuryl alcohol, and nitro blue tetrazolium, have been tested to identify the active species involved in dye degradation, and it was found that O 2 ·− was mainly responsible for degrading OG, while HO 2 − anion was the primary oxidant for degrading RhB.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子