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Chem · 2019 · IF 18.205

High-Concentration Single Atomic Pt Sites on Hollow CuSx for Selective O2 Reduction to H2O2 in Acid Solution

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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ACS Applied Materials & Interfaces · 2018 · IF 8.097

Binary Mixtures of Highly Concentrated Tetraglyme and Hydrofluoroether as a Stable and Nonflammable Electrolyte for Li–O2 Batteries

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 · 电化学 · 材料科学 · 电池技术
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Journal of Materials Chemistry A · 2016 ·Vol. 4 ·期 25 ·10008-10013 · IF 8.262

Optimized nitrogen-doped carbon with a hierarchically porous structure as a highly efficient cathode for Na–O2 batteries

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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CHEMICAL ENGINEERING JOURNAL · 2026 · IF 12.5

Base-promoted O2 relay activation for the efficient HMF oxidation to FDCA at low temperature and ambient pressure

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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Journal of Environmental Chemical Engineering · 2025 ·Vol. 13 ·期 6 ·120354 · IF 7.2

Synergistic •OH/•O2⁻/1O2 radical cycling driven by H2O2 photolysis for base-free glycolic acid production from glycerol

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.

CAS / MDL: 64-18-6
研究领域: 催化化学 · 绿色化学 · 可再生能源 · 环境科学 · 化学工程
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MATERIALS LETTERS · 2018 · IF 2.687

CNTs-grafted cotton fabrics as binder-free, free-standing and cost-efficient cathodes for flexible Li-O2 batteries

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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Journal of Materials Chemistry C · 2020 ·Vol. 9 ·期 5 ·1593-1603 · IF 7.059

Synergy of surface fluorine and oxygen vacancy of TiO2 nanosheets for O2 activation in selective photocatalytic organic transformations

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 · 环境科学 · 化学工程
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Small · 2018 ·Vol. 14 ·期 34 ·1801798 · IF 9.598

Flexible, Flame-Resistant, and Dendrite-Impermeable Gel-Polymer Electrolyte for Li–O2/Air Batteries Workable Under Hurdle Conditions

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 · 先进电池技术 · 固态离子学
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JOURNAL OF HAZARDOUS MATERIALS · 2026 · IF 10.6

Harnessing pollutant complexation for self-accelerated remediation: Glyphosate oxidation and toxicity mitigation in a Fe(II)/O2 system

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.

✓ 已验证 DOI PubMed 高影响因子
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Biomaterials Science · 2021 ·Vol. 9 ·期 20 ·6772-6786 · IF 6.843

Microneedle-mediated delivery of MIL-100(Fe) as a tumor microenvironment-responsive biodegradable nanoplatform for O2-evolving chemophototherapy

Sulan Luo,Yiting Zhao,Kewei Pan,Yixian Zhou,Guilan Quan,Xinguo Wen,Xin Pan,Chuanbin Wu

The low oxygen level in tumors significantly reduces the antitumor efficacy of photodynamic therapy (PDT). The provision of O2 and monomeric hydrophobic photosensitizers (PSs) under physiological conditions would greatly help to shrink malignant tumors. We take advantage of the high porosity and multifunctionality of metal–organic frameworks (MOFs) to fabricate a simple all-in-one nanoplatform mediated by microneedle delivery to achieve synergistic O2 evolution and chemophototherapy. An iron(III)-based MOF (MIL-100(Fe)) acted not only as a vehicle for the concurrent delivery of zinc phthalocyanine (ZnPc) and doxorubicin hydrochloride (Dox), but also to supply O2 by decomposing hydrogen peroxide (H2O2) in the tumor microenvironment via a Fenton-like reaction. In vitro and in vivo experiments indicated that the nanoplatform had excellent biocompatibility and exerted enhanced anticancer effects. The encapsulated drug was sustainably released from the nanoplatform skeleton in response to acidic tumor microenvironments. Moreover, upon 660 nm light irradiation, ZnPc effectively produced reactive oxygen species (ROS) due to the reduction of hypoxia by MIL-100(Fe). A microneedle technique was adopted to directly deliver the nanoplatform into superficial tumors rather than via systemic circulation. Hence, this study provides a new strategy for more efficient chemophototherapy of hypoxic superficial tumors.

研究领域: 癌症治疗 · 纳米技术 · 生物医学工程 · 药学
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SOLID STATE IONICS · 2016 · IF 2.38

Understanding the enhanced electrochemical performance of samarium substituted Li[Li0.2Mn0.54 − xSmxCo0.13Ni0.13]O2 cathode material for lithium ion batteries

Guofeng Xu,Qingrui Xue,Jianling Li,Zhanyu Li,Xinping Li,Tianheng Yu,Jiguang Li,Xindong Wang,Feiyu Kang

Lithium-excess layered cathode materials Li[Li 0.2 Mn 0.54   −   x Sm x Co 0.13 Ni 0.13 ]O 2 (x   =   0, 0.01, 0.03, 0.05) with different quantities of Sm were synthesized by the coprecipitation-calcination method. The rare earth element samarium (Sm) was introduced into the structure of Li[Li 0.2 Mn 0.54 Co 0.13 Ni 0.13 ]O 2 as the replacement at Mn sites. The refinement unit cell parameters from the X-ray powder diffraction patterns illustrate the doping of Sm facilitates enlarging the lithium ions diffusion passageway space of the Li[Li 0 . 2 Mn 0.54 Co 0 . 13 Ni 0.13 ]O 2 structure. The Li[Li 0.2 Mn 0.51 Sm 0.03 Co 0.13 Ni 0.13 ]O 2 electrode presented the best electrochemistry properties. The initial discharge capacity is 287.5   mAh   g −   1 and the initial coulombic efficiency increases from 81.31% to 85.34% with a constant current density of 12.5   mA   g −   1 , which can be attributed to the suppression of the oxygen release from the structure at the initial charge-discharge process. The Li[Li 0·2 Mn 0.51 Sm 0.03 Co 0.13 Ni 0.13 ]O 2 electrode delivers 236.1   mAh   g −   1 after 40   cycles and the capacity retention ratio is 82.12% while only 206.8   mAh   g −   1 and 70.85% are obtained after 40 times of cycling for the pristine electrode. The Nyquist plots indicate that the electrical conductivity and interfacial electrochemical reaction activity increase as well.

CAS / MDL: 12060-58-1
研究领域: 材料科学 · 电化学
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MATERIALS LETTERS · 2014 · IF 2.269

Ni2+ doped InVO4 nanocrystals: One-pot microwave-assisted synthesis and enhanced photocatalytic O2 production activity under visible-light

Ming Yan,Yan Yan,Chao Wang,Wei Lu,Weidong Shi

In this letter, Ni 2+ doped InVO 4 nanocrystals were successfully synthesized by a simple one-pot microwave-assisted method. The energy bandgap of obtained samples can be precisely controlled by varying the Ni 2+ doping amount. The O 2 production rate of obtained Ni–InVO 4 nanocrystals is higher than that of pure InVO 4 nanocrystals under visible-light, which can be ascribed to the narrowed band gaps. The corresponding 1% doped sample N1 has the highest O 2 production rate (394   μmol/h) in all samples, which is 66% higher than the undoped sample N0.

研究领域: 材料科学 · 环境科学 · 化学工程
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