INORGANIC CHEMISTRY
·
2025
·
IF 4.7
Qing-Shuai Zhang,Yu-Le Wang,Li Yue,Yu-Dong Shan,Song-Hai Wu,Yong Liu,Xu Han
Although selective oxidation of benzene to phenol (SOBP) by H2O2 is an important chemical process, overoxidation of benzene by the produced nonselective •OH during the activation of H2O2 inevitably reduces the oxidation selectivity. We, therefore, attempt to mediate the oxidation selectively by using electrophilic KHCO3 in the oxidation system. In this study, Mo–Cu/NC has been successfully synthesized via ball-milling bimetallic Mo–Cu and N-doped carbon, which exhibits high reactivity in SOBP by H2O2 and KHCO3 with a desirable phenol yield of 25.1% and selectivity of 100%. A series of characterizations and DFT calculations reveal that the reaction between H2O2 and KHCO3 produces HCO4–, which is then moderately activated on Mo1Cu2/NC via the nonradical pathway with the formation of Mo-(η2-O2) peroxo. Meanwhile, Ov at Mo1Cu2/NC facilitates the adsorption of benzene, which is then selectively oxidized by Mo-(η2-O2) peroxo to phenol via the oxygen atom transfer pathway. This study provides new insights on the importance of Mo-(η2-O2) peroxo mediated by H2O2–KHCO3 in selective oxidation of aromatic C–H bond via the nonradical pathway.
研究领域:
化学
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材料科学
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DOI
PubMed
高影响因子
TALANTA
·
2024
·
IF 5.6
Xiupei Yang,Xiaoyi Xie,Ling Jiang,Yuxiu Fan,Chenglin Zhang,Ya Wang
Most conventional nanozymes have poor specificity and low activity, and designing high-performance nanozymes remains a challenge. In contrast, single-atom nanozymes have high atom utilization and high reactivity. Here, we prepared Cu single-atom nanozymes (Cu-NC) with excellent peroxidase-like activity by high-temperature pyrolysis using Cu as a transition metal source. The introduction of Cu formed the Cu-N x active site, which accelerated charge transfer between the reactants and the active site and was the key for improving the activity. With Cu-NC as a catalyst, H 2 O 2 rapidly oxidized 3,3′,5,5′-tetramethylbenzidine (TMB) to oxTMB, and the solution turned blue with strong absorption at 652 nm. Because d -penicillamine (D-PA) can reduce oxTMB or react with reactive oxygen species radicals to inhibit the color reaction, we built a colorimetric sensing platform around Cu-NC for the determination of D-PA and successfully used it for the determination of D-PA in urine samples. This work provides new ideas for the design of high-performance nanozymes and the detection of D-PA in real environments.
研究领域:
生物化学
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医学诊断
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材料科学
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DOI
PubMed
高影响因子
INORGANIC CHEMISTRY COMMUNICATIONS
·
2025
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IF 5.4
Wei Zhao,Mengyuan Qiu,Yajun Liu,Yingrui Dong,Xiaojing Huang,Siyue Li,Feifei Lin,Yongzhi Xiong,Changzhou Chen
The lack of high-performance, low-cost electrocatalysts is the key challenge for the production of 2,5 furandicarboxylic acid via electrocatalytic oxidation of 5-hydroxymethylfurfural. In this work, we report a novel approach for the preparation of highly dispersible transition metal catalysts loaded by carbon aerogel-loaded via a chitosan-transition-metal-ion coordination. The experimental results demonstrated that all of Ni 2+ , Co 2+ and Cu 2+ were able to coordinate with chitosan to form stable gels, which were then pyrolyzed to obtain highly dispersed transition metal-based catalysts (Co@NC, Ni@NC and Cu@NC) The Cu@NC exhibited the best HMFOR activity with high HMF conversion (nearly 100 %), FDCA selectivity (98.1 %), and Faraday efficiency (95.3 %). Mechanistic studies showed that Cu@NC was able to accumulate more effective oxidatively active species and thus achieve higher HMFOR current density compared to Co@NC and Ni@NC, and that the electrooxidation of HMF at the Cu@NC electrode followed the HMFCA oxidation pathway. This study provides a general and facile strategy for macropreparation of highly dispersible carbon aerogel-loaded transition metal catalysts for efficient electrocatalytic valorization of HMF.
研究领域:
材料科学
·
电化学
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DOI
高影响因子
ELECTROCHIMICA ACTA
·
2026
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IF 5.6
Wei Lin,Yinghui Bian,Jintao Yao,Aocheng Yang,Lixin Yang,Hui Chen,Xuekui Xin,He Bian,Zichuan Lv
The composite material comprising copper phthalocyanine (CuPc) and graphene oxide (GO) is a novel functional material with broad application prospects in the field of electrochemistry. In this paper, a composite material consisting of copper coated with nitrogen-doped carbon supported on reduced graphene oxide (Cu@NC/rGO) was synthesized using CuPc/GO as the precursor through thermal treatment and carbonization processes. The porous Cu@NC/rGO composite not only provides abundant active sites but also constructs rapid ion transport pathways. Within the composite, Cu@NC nanoparticles act as effective electron transfer bridges, forming a continuous conductive network that reduces interfacial contact resistance. The hybrid dual-ion capacitor (HDIC) assembled with the Cu@NC/rGO composite material demonstrated outstanding cycling stability, achieving a discharge specific capacity of 328.6 mAh g -1 at a current density of 2.0 A g -1 after 4000 cycles. Density Functional Theory (DFT) calculations and electronic structure analysis revealed that the Cu@NC/rGO material exhibits the strongest adsorption capability toward EMIm + ions, with an adsorption energy as low as -299.02 kJ·mol -1 , accompanied by the most significant charge transfer. This work provides new design inspiration for the development of anode materials for HDIC.
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高影响因子
ChemistrySelect
·
2024
·Vol. 9
·期 18
·e202304772
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IF 1.9
Chenghao Tang,Chaoyang Song
Graphical Copper encapsulated N-rich carbon material derived from porous organic polymer was found to be highly active heterogeneous catalyst for solvent-free coupling of acyl chlorides with alkynes. Copper promoted Sonogashira coupling has recently emerged as an attractive route for synthesizing α, β-Acetylenic ketones (ynones). In this study, a porous organic polymer based on [2,6-Bis(1,2,3-triazol-4-yl)pyridine] (BTP) was prepared through oxidative coupling. By incorporating copper salt and subsequent pyrolysis, copper encapsulated N-doped carbon materials were obtained. The resulting copper/carbon materials exhibited excellent catalytic performance for the coupling of acyl chlorides and alkynes due to their large surface area, abundant mesopores, and uniformly distributed metal nanoparticles. The reaction proceeded efficiently, yielding ynones with good to excellent yields at room temperature within a short reaction time (4 h) using only 0.4 mol % catalyst. Compared to previously reported copper nanocatalysts, the N-doped carbon materials supported copper catalyst demonstrated higher catalytic activity and operated at lower reaction temperatures. Additionally, the catalyst displayed reliable recyclability without any significant loss in catalytic activity.
研究领域:
化学
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材料科学
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DOI
高影响因子
TALANTA
·
2025
·
IF 6.1
Chenyu Zhou,Jianxin Qiang,Wanyi Zhang,Yuntai Lv,Xingguang Su
The application of peroxidase-like nanozymes in on-site detection was often restricted due to the cumbersome operation caused by necessary step of adding H 2 O 2 . Herein, a novel composite peroxidase mimic CuO 2 @S/Cu-NC with self-supplying H 2 O 2 function was prepared by in situ synthesis of the copper peroxide nanodots (CuO 2 ) on the S/N co-doping carbon-based copper nanozyme (S/Cu-NC). The CuO 2 could produce H 2 O 2 in acidic environment, and the in situ formed H 2 O 2 could immediately bind to the active sites of S/Cu-NC, resulting in the greatly accelerated catalytic reaction efficiency. Because of the property of H + -induced H 2 O 2 production of CuO 2 @S/Cu-NC, the changes of pH value could affect its peroxidase-like activity. Therefore, a sensitive and convenient method for histamine sensing was established. Furthermore, a convenient test swab was designed for the portable histamine detection and visual monitoring the of seafood freshness, which showed great potential of multifunctional nanozyme in the field of food monitoring.
研究领域:
食品安全
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纳米技术
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生物传感器
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分析化学
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食品质量监控
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高影响因子
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