LANGMUIR
·
2026
·
IF 4.4
Chenxi Wu,Huaizhou Tong,Fangyong Shu,Tao Wu,Haining Cui,Han Zhu,Chan Wang,Qijun Song
Photocatalytic hydrogen peroxide (H2O2) production from water and molecular oxygen offers a sustainable alternative to the energy-intensive anthraquinone process; however, its practical advancement is limited by inefficient charge utilization, poor selectivity, product instability, and challenging separation. Herein, we report a quasi-homogeneous phase-transfer photocatalytic system enabled by rhodamine B-derived amphiphilic carbon dots that enables interfacial redox decoupling for high-efficiency H2O2 photosynthesis. The as-prepared carbon dots serve a trifunctional role as visible-light harvesters, interfacial stabilizers, and redox catalysts, facilitating the formation of a light-responsive water/benzyl alcohol emulsion. This biphasic architecture maximizes interfacial charge carrier flux while ensuring spontaneous phase separation postirradiation. In this configuration, the two-electron oxygen reduction reaction is localized within the aqueous phase, while the photogenerated holes drive the selective oxidation of benzyl alcohol to value-added benzaldehyde in the organic phase. Consequently, an exceptional H2O2 production rate of 13 250 μmol g–1 h–1 is achieved, accompanied by a benzyl alcohol conversion of 83.7% and a benzaldehyde yield of 82.6%. This strategy not only suppresses H2O2 decomposition through spatial segregation but also enables in situ product isolation and facile catalyst recycling. This work establishes interfacial phase-transfer photocatalysis as a robust and versatile platform for integrating solar-to-chemical energy conversion with selective organic transformations.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Hongfei Mei,Jinsong Peng,Haiyan Song,Chunxia Chen
Photocatalytic H2O2 production in seawater offers a novel and sustainable route for the substitution of freshwater consumption. However, this strategy is limited by the complexity and cost resulting from electron–proton donors and pure O2 dependency. Simultaneously, adsorption, a frequently used method to treat radionuclide wastewater, latently causes issues of adsorbent-caused waste and pollution. In this work, we designed a sustainable system based on recycling MXene Ti3C2 adsorbent after radioactive cesium (Cs+) uptake and further used it in photocatalytic H2O2 production from seawater. The adsorptive performance and behavior of Ti3C2 were evaluated for model nuclear wastewater with different Cs+ concentrations. Cs+ was uniformly adsorbed on the layer surface of Ti3C2 and promoted the delamination of Ti3C2. Cs+ uptake also improved e––h+ pair separation and photogenerated electron transfer on the Ti3C2 matrix. Without using an organic electron–proton donor and pure O2, Ti3C2 adsorbed Cs+ achieved 892.43 μmol·g–1·h–1 H2O2 productivity in real seawater, which was 1.84 times higher than that over pristine Ti3C2. It also obtained 12.44% apparent quantum yield (AQY) at 550 nm, and 6 cycles of reusability. Enhancement in photocatalytic performance was attributed to the regulation of the bandgap of Ti3C2 by the adsorbed Cs+ from 1.51 eV to a semiconductor range of 2.00 eV. Further, the conduction band (CB) of Ti3C2 was shifted to a more negative potential, facilitating the two-electron reduction of O2 to generate more H2O2. This study opened avenues for the sustainable use of spent adsorbents and resolved freshwater reliance.
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ENVIRONMENTAL POLLUTION
·
2016
·
IF 4.839
Dun Fu,Zheng Chen,Dong Xia,Liang Shen,Yuanpeng Wang,Qingbiao Li
Solid digestate, a by-product of anaerobic digestion systems, has led to a range of environmental issues . In the present study, a novel composite based on a solid digestate-biochar-Cu NP composite was synthesized for tetracycline removal from an aqueous medium. The removal efficiency values for tetracycline (200 mg L −1 ) were 31.5% and 97.8%, respectively, by the biochar-Cu NP composite (0.5 g L −1 ) in the absence and presence of hydrogen peroxide (H 2 O 2 , 20 mM) within 6 h of reaction time. The possible degradation pathway of tetracycline was investigated using liquid chromatography-mass spectrometry. The desorption experiment results suggested that no significant concentration of tetracycline was detected on the composite after the reaction, but a small amount of intermediates in terms of total organic carbon (TOC) accounting for 3.1%, and 23.3% of the end-product NH 4 + was adsorbed onto the biochar sheets. The dispersive Cu NPs on the biochar resulted in an increase in the surface area and pore volume of the biochar-Cu NP composite, which enhanced tetracycline adsorption as well as the degradation efficiency. Relative tetracycline removal mechanisms were dominantly ascribed to ·OH generation from the Cu(II)/Cu(I) redox reaction with H 2 O 2 and the electron-transfer process of free radicals (FRs) in biochar. The proposed approach serves dual purposes of waste digestate reuse and treatment of antibiotic pollutants. This study highlights the activation of H 2 O 2 by the dispersive Cu NPs coupling with biochar derived from a waste solid digestate for tetracycline treatment.
研究领域:
环境科学
·
微生物学
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JOURNAL OF POWER SOURCES
·
2025
·
IF 7.9
Yongyi Li,Wei Li,Zhigang Shao,Huiyang Xu,Shuanglong Li,Bo Wang,Xiaorui Huang,Shichao Jiao,Zhiwei Li
Photocatalytic production of hydrogen peroxide from water is regarded as an environmentally benign technology for energy storage and supply. Herein, a disordered K&Na-C 3 N 5 photocatalyst co-intercalated with K + &Na + and modified by cyano/hydroxyl groups is successfully fabricated via alkali-activated thermal-polymerization. Alkali activation effectively anchors cyano and hydroxyl active groups on the surface: hydroxyl groups enhance the material's hydrophilicity and promote proton transfer, while cyano groups exhibit electron-attracting characteristics to localize photogenerated electrons. Simultaneously, interlayer intercalation of K + &Na + forms electron transport channels, synergistically facilitating surface proton transfer and optimizing charge distribution. This multi-component modification strategy significantly enhances the adsorption capacity of O 2 , effectively modulates the 2e − ORR pathway, and improves the selectivity of H 2 O 2 , demonstrating its excellent bifunctional properties. Experimental data show that the optimally alkali-activated K 3 &Na 3 -C 3 N 5 achieves a remarkably high H 2 O 2 production rate of 26,920.49 μmol g −1 ·h −1 — a 90.3-fold increase over unmodified C 3 N 5 . This work pioneers alkali activation as a universal and scalable paradigm for engineering surface-active sites to enable performance amplification through functional group-metal ion cooperativity, and it provides a design blueprint for advanced carbon nitride-based photocatalysts to boost H 2 O 2 fuel cell performance.
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NPG Asia Materials
·
2022
·Vol. 14
·期 1
·1-13
·
IF 10.761
Peng Mengran,Ju Enguo,Xu Yanteng,Wang Yuqin,Lv Shixian,Shao Dan,Wang Haixia,Tao Yu,Zheng Yue,Li Mingqiang
Chemodynamic therapy holds great potential for cancer treatment due to its reliable curative effects, minimal invasiveness, and few systemic side effects. However, the limited amount of intracellular H 2 O 2 makes achieving high-performance chemodynamic therapy challenging. Herein, we report a core-shell nanoplatform with dual-responsive disassembly that self-supplies H 2 O 2 and undergoes an autocatalytic Fenton reaction for enhanced chemodynamic therapy. The platform was designed by coating glucose oxidase-mimicking nanozyme gold nanoparticles (AuNPs) with a metal-polyphenol network (Au@MPN). Both ATP and low pH can disassemble the Au@MPN to release Fe(III), which can then be reduced into Fe(II) by the simultaneously released tannic acid (TA). In particular, the exposed AuNPs can catalyze the oxidation of intracellular glucose to produce H 2 O 2 . Subsequently, Fe(II) and the self-supplied H 2 O 2 induce an efficient Fenton reaction for chemodynamic therapy by generating hydroxyl radicals (•OH) that are highly toxic to cancer cells. Moreover, tumor growth can be effectively suppressed after both intratumoral and intravenous Au@MPN administration. Additionally, metastatic melanoma lung tumors could be inhibited by intratracheal instillation of Au@MPN. Thus, this work not only reports a facile method to construct a chemodynamic agent with self-supplied H 2 O 2 and high therapeutic efficiency but also provides insight into the design of nanoplatforms with enhanced efficiency for chemodynamic therapy.
研究领域:
纳米技术
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癌症治疗
·
生物医学工程
·
材料科学
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化学生物学
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Chemical Engineering Journal Advances
·
2021
·
IF 0
Kai Wei,Xiufan Liu,Shiyu Cao,Huijuan Cui,Yu Zhang,Zhihui Ai
In this study, we fabricated a micro-nano structured Fe 2 O 3 @FeB composites by treating commercial Fe 2 O 3 with sodium borohydride. The outside amorphous FeB alloy shell endowed the Fe 2 O 3 @FeB with remarkable Fenton-like performance in organic pollutants oxidation by efficient Fe(III)/Fe(II) cycle. For instance, the pseudo first-order rate constants of RhB degradation using Fe 2 O 3 @FeB as Fenton reagent was 74.6 times that of the Fe 2 O 3 counterpart, the hydroxyl radical generation rate of Fe 2 O 3 @FeB was 1-3 orders of magnitude larger than that of other heterogeneous Fenton reagent. Further mechanistic study unveiled that FeB was oxidized accompanying with Fe(0) and B(0) continuously donated electrons to Fe(III) to secure the efficient generation of surface Fe(II), which could generate additional H 2 O 2 by consecutive single-electron molecular oxygen activation (O 2 →•O 2 − →H 2 O 2 ), leading to enhance •OH production and Fenton-degradation toward typical pollutants. This study provides a facile route for efficient heterogeneous Fenton and strengthens the vital role of molecular oxygen activation on Fenton-like process.
研究领域:
环境科学
·
材料科学
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DOI
Catalysis Science & Technology
·
2024
·
IF 4.4
Pengken Li,Hui Zhao,Rong Ji,Wenwen Chi,Xinyu Sun,Yuming Dong,Yongfa Zhu
A one-step two-electron oxygen reduction pathway is crucial for the stable and efficient photosynthesis of hydrogen peroxide. However, the lower oxygen adsorption and activation capacity significantly restrict the ability of the one-step two-electron oxygen reduction pathway. In this work, a covalent organic framework containing a diacetylene unit (COF-Tfp-BDDA) as an efficient oxygen reduction active site was designed for the photosynthesis of hydrogen peroxide. This work demonstrates that the introduction of the diacetylene unit efficiently improved the oxygen adsorption and activation capacity of the COF. Additionally, the introduction of a diacetylene unit effectively promoted charge separation. COF-Tfp-BDDA exhibited a superior rate of H2O2 preparation (880 μmol g−1 h−1) under visible light irradiation from pure water and oxygen, better than most COF-based photocatalysts. The catalyst exhibited a stable hydrogen peroxide photosynthesis efficiency above 100 hours in cycling experiments. Based on the experimental and DFT calculation results, the introduction of a diacetylene unit not only enhances the adsorption and activation of oxygen but also alters the reduction pathway of oxygen, leading to effective charge separation. These factors contribute to the efficient photosynthesis of hydrogen peroxide in pure water. This work provides a novel idea regarding the application of COFs in the field of solar energy conversion.
研究领域:
材料科学
·
光催化
·
太阳能转化
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高影响因子
ACS Applied Materials & Interfaces
·
2017
·
IF 7.504
Jinrong Peng,Qian Yang,Wenting Li,Liwei Tan,Yao Xiao,Lijuan Chen,Ying Hao,Zhiyong Qian
Because of the nontargeting release of anticancer drugs, conventional chemotherapy results in serious side effects and poor therapeutic outcomes. In addition, hypoxia situation in the tumor microenvironment also promotes the growth and metastasis of tumors. Multifunctional nanocarriers with stimuli-activation and hypoxia-relieving properties can help overcome some of these limitations. In this study, we have constructed a nanocarrier which is named PBMn–DOX@RBC. A Prussian blue/manganese dioxide (PBMn) nanoparticle is used as an oxygen precursor or catalyzer for H2O2 activation, and a red blood cell (RBC) membrane is used to increase the loading capacity of doxorubicin (DOX) and prolong the circulation time in vivo. H2O2 is overproduced in tumor tissues and tumor cells. It can be used as a stimulus to activate drug release. In the presence of H2O2, the hypoxia inside the tumors is relieved by the administration of PBMn–DOX@RBC. The generated oxygen disrupts the RBC coated on the surface of PBMn, which accelerates the release of DOX. RBCs also prolong the circulation time of the nanometer system in vivo. By combining the photothermal therapy (PTT) and chemotherapy, the tumor growth inhibition mediated by PBMn–DOX@RBC is further enhanced. PBMn–DOX@RBC fulfills the demands to relieve tumor hypoxia and enhance cancer chemotherapy/PTT.
研究领域:
生物医学工程
·
癌症治疗
·
纳米医学
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2020
·
IF 3.232
Guangxian Liu,Hongying Liu,Hanxiao Xu,Langlang Zhu,Chang Su,Chunchuan Gu,Lihua Li
In this paper, the composites of Fe 3 O 4 modified by sodium lignosulfonate and copper peroxide (Fe 3 O 4 @CP) were produced by a simple two-step method, and their morphology and composition were featured in Field emission scanning electron microscopy , X-ray powder diffraction, X-ray diffraction and Fourier transform infrared. Then, Fe 3 O 4 @CP catalyzed the oxidation of colorless 3,3′,5,5′-tetramethylbenzidine to blue oxide in the presence of H 2 O 2 , indicating that it had good catalytic performance. Further, the experimental conditions were optimized, including time, pH, temperature and material concentration. The kinetic analysis results showed that Fe 3 O 4 @CP exhibited excellent catalytic performance and its catalytic kinetic plot conformed to the Michaelis-Menten equation and the catalytic mechanism was consistent with the ping-pong mechanism. Finally, a H 2 O 2 colorimetric assay with a linear range of 0.2–300 μM and a detection limit of 0.11 μM was constructed. In addition, due to the decolorization reaction of ox-TMB with glutathione and the scavenging effect of GSH on hydroxyl radicals (·OH), a glutathione colorimetric assay was further constructed with a linear range of 0.2–40 μM and a detection limit of 0.05 μM. It also verified that the assay had excellent selectivity and stability and could be utilized to detect actual samples.
研究领域:
生物化学
·
分析化学
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Journal of Environmental Chemical Engineering
·
2020
·
IF 4.3
Sanping Zhao,Yongbing Zhu,Hailing Xi,Mengwei Han,Daxue Li,Yang Li,Hongjie Zhao
To overcome the insufficient understanding of the detoxification mechanisms of Chemical Warfare Agents (CWAs) and simulants by a molybdate-activated hydrogen peroxide solution (MoO 4 2− -H 2 O 2 ), detoxification performances toward CWAs and simulants were tested. The detoxification efficacy toward mustard gas (HD), nerve agent GD and VX by using MoO 4 2− -H 2 O 2 was higher than that by using H 2 O 2 activated/modified by sodium hydroxide , ammonia, bicarbonate , and borates, but the vesicant mustard sulfone (HDO 2 ) was only formed when using MoO 4 2− -H 2 O 2 to detoxify HD. Although Reactive Oxygen Species (ROS) such as singlet oxygen ( 1 O 2 ), superoxide anion (O 2 − ), H 2 O 2 and peroxide anion (OOH − ) were detected by electron spin resonance (ESR) and chemiluminescence (CL) in the 0.1 M MoO 4 2− -1.0 M H 2 O 2 solution, 95 Mo NMR indicated that Mo(O 2 ) 4 2− was the dominant oxidant for the oxidation of sulfide to sulfoxide and then to sulfone. Oxidation of HD by Mo(O 2 ) 4 2− occurred on the HD-drop/water interface through a direct oxygen transfer mechanism without the participation of H 2 O molecules, and further oxidation of HD to HDO 2 was inevitable in an aqueous MoO 4 2− -H 2 O 2 solution. 18 O tracer experiments confirmed that OOH − -based perhydrolysis dominated the detoxification reaction of nerve agents in an alkaline H 2 O 2 solution. Considering the balance of oxidation/nucleophilic reactivity for a practical decontaminant, pH 10.5–11 range was recommended as the ideal for the MoO 4 2− -H 2 O 2 system to detoxify CWAs.
研究领域:
化学
·
环境科学
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BIOSENSORS & BIOELECTRONICS
·
2020
·
IF 10.257
Hui Dong,Yanli Zhou,Yuanqiang Hao,Le Zhao,Shuo Sun,Yintang Zhang,Baoxian Ye,Maotian Xu
Oxidative stress plays an important role in the pathogenesis of many diseases, while the exact mechanism that hydrogen peroxide (H 2 O 2 ) as one of the most abundant reactive oxygen species (ROS) exerts its influence on oxidative stress remains unclear. We developed a novel turn-on ratiometric electrochemical sensor for the detection of H 2 O 2 in blood samples. The electrochemical probe 5-(1,2-dithiolan-3-yl)-N-(4-(4,4,5,5-tetramethyl-1,3,2-dioxaborolan-2-yl)phenyl)pent-anamide (BA) was designed and synthesized for the selective detection of H 2 O 2 via a one-step amide reaction. Meanwhile, Nile Blue A (NB) was optimized as an internal reference molecule, thus enabling accurate quantification of H 2 O 2 in a complex environment. BA and NB were then co-assembled onto a carbon fiber microelectrode (CFME) coated with Au cones. The oxidation peak current ratio between BA and NB demonstrated good linearity with the logarithm of the H 2 O 2 concentration values ranging from 0.5 μM to 400 μM with a low detection limit of 0.02 μM. The developed sensor showed remarkable selectivity against potential interferences in whole blood samples, especially for ascorbic acid , uric acid , and dopamine. In combination with the unique characteristics of CFME, such as a small size and good biocompatibility , the microsensor was used for rapid analysis of one drop of whole blood sample. This sensor not only creates a new platform for the detection of H 2 O 2 in whole blood samples, but also provides a new design strategy of other ROS analysis for early diagnosis of ROS-related diseases, drug discovery processes, and pathological mechanisms.
研究领域:
生物医学工程
·
分析化学
·
病理学
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Nano Research
·
2021
·Vol. 15
·期 1
·304-309
·
IF 8.897
Zhang Longcheng,Liang Jie,Yue Luchao,Xu Zhaoquan,Dong Kai,Liu Qian,Luo Yonglan,Li Tingshuai,Cheng Xiaohong,Cui Guanwei,Tang Bo,Alshehri Abdulmohsen Ali,Alzahrani Khalid Ahmed,Guo Xiaodong,Sun Xuping
Electrocatalytic oxygen reduction reaction (ORR) provides an attractive alternative to anthraquinone process for H 2 O 2 synthesis. Rational design of earth-abundant electrocatalysts for H 2 O 2 synthesis via a two-electron ORR process in acids is attractive but still very challenging. In this work, we report that nitrogen-doped carbon nanotubes as a multi-functional support for CoSe 2 nanoparticles not only keep CoSe 2 nanoparticles well dispersed but alter the crystal structure, which in turn improves the overall catalytic behaviors and thereby renders high O 2 -to-H 2 O 2 conversion efficiency. In 0.1 M HClO 4 , such CoSe 2 @NCNTs hybrid delivers a high H 2 O 2 selectivity of 93.2% and a large H 2 O 2 yield rate of 172 ppm·h −1 with excellent durability up to 24 h. Moreover, CoSe 2 @NCNTs performs effectively for organic dye degradation via electro-Fenton process.
研究领域:
材料科学
·
电化学
·
催化
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高影响因子
危险品化学品经营许可证（带存储）