Journal of Physical Chemistry C
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2024
·
IF 3.3
Caiyi Jiang,Ming Hou,Li Yang,Shenghui Guo,Guo Yang,Bo Xing,Yi Wang,Dongzheng Wang,Xiaolin Shi
Fe–N co-doped carbon catalyst has received increasing attention in the field of organic wastewater treatment because of its unique structure and outstanding activity. However, the reusability, catalytic activity, and pH working range are still a great challenge for future application. Herein, a novel αFe-HM@C-T catalyst was prepared by pyrolyzing a mixture of starch and heme and was analyzed by TEM, H2-TPR, XRD, BET, XPS, FTIR, and Raman spectrum. Meanwhile, αFe-HM@C-T catalysts show the highest catalytic performance due to abundant porous structure, higher redox property, and unique Fe–Nx configuration. The rhodamine B (RhB) could be almost completely degraded within 30 min on the 5Fe-HM@C-850, and recovery rates of catalytic activity of 96% and 91.8% were achieved in peroxydisulfate (PDS) and H2O2 systems with an extensive buffer pH range. Furthermore, mechanistic insights by quenching experiments and EPR verified the high removal efficiency of RhB mainly attributed to indirect oxidation of SO4•–, •OH, and 1O2 in both systems, and the potential mechanism was proposed.
研究领域:
环境科学
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催化材料科学
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高影响因子
JOURNAL OF POWER SOURCES
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2025
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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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Journal of Environmental Chemical Engineering
·
2025
·Vol. 14
·期 1
·120879
·
IF 7.2
Chengzhao Liu,Tao Liu,Suhua Liu,Xiufang Zhang,Guanlong Wang
Recently, it was reported photocatalytic H 2 O 2 generation performed in biphasic system could significantly increase the H 2 O 2 yield. Aiming to further improve the H 2 O 2 yield, hydrophobic heterojunction of α-S and vacancy-rich g-C 3 N 4 (CNN) was constructed. H 2 O 2 production performance tests demonstrated the 0.2α-S/CNN composite achieved H 2 O 2 yields 1.72 and 1.99 times higher than pristine CNN and α-S, respectively. N-(C) 3 bonded nitrogen(N 3 C ) promoted oxygen activation, and heterojunction facilitated the separation of photogenerated holes and electrons. These contributed more effective photocatalytic synthesis of H 2 O 2 . The optimal 0.2α-S/CNN achieved a production rate of 2218 μmol g −1 , with an impressive apparent quantum yield (AQE) of 6.92 % under 455 nm monochromatic light, outperforming the state-of-the-art catalysts. The proposed mechanism suggested that photogenerated electrons migrated from α-S to CNN, reducing adsorbed O 2 to form •O 2 − radicals. These radicals subsequently reacted with water in the aqueous phase to generate H 2 O 2 via 2e − ORR. Due to the strong hydrophobicity of the catalyst, most •O 2 − radicals were generated in benzyl alcohol (BA) phase, while H 2 O 2 predominantly formed in the aqueous phase. This spatial separation delayed H 2 O 2 decomposition, facilitating its accumulation and enhancing overall yield.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-11
·
IF 15.7
Xu Jing,Gu Kaiye,Wang Peifang,Cheng Pengfei,Che Huinan,Tang Chunmei,Zhang Kan,Ao Yanhui
Hydroxyl radicals (·OH) is one of the most important reactive oxygen species (ROSs) for organic pollution controlling in advanced oxidation processes, while its production suffers from numerous H 2 O 2 addition and narrow pH range in generally used Fenton reaction. Herein, we demonstrate a BiOIO 3 (BIO) piezo-catalyst loaded with γ-FeOOH nanoparticles (FNPs) (BF) that can convert O 2 to ·OH in a wide pH condition without external H 2 O 2 addition under ultrasonication. It is found that the robust interfacial interaction facilitates rapid electron migration from BIO to FNPs, enabling two-electron O 2 reduction into H 2 O 2 at the FNPs site, while the leaving behind piezo-holes to perform two-electron water oxidative H 2 O 2 generation on BIO. Because the electron-rich nature of FNPs favors the H + adsorption that contributes a surface acidic micro-environment, the produced H 2 O 2 can be in-situ catalyzed into ·OH in either neutral or even alkaline conditions with a great stability. Finally, the optimal BF can achieve either an impressive ·OH yield of 38.1 µM h −1 or a high H 2 O 2 yield of 522.0 µM h −1 by regulating the FNPs loading mass, which enables dual capabilities of rapid organic pollutants degradation and H 2 O 2 production in a wide pH condition.
研究领域:
环境科学
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催化
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高级氧化工艺
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材料科学
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化学工程
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PubMed
高影响因子
ACS ES&T Engineering
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2025
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IF 6.7
Yaqiong Luo,Jiacheng Bao,Xin Yan,Lei Shi,Fei Wang,Xin Sun,Kai Li,Ping Ning
Wet flue gas denitrification offers a new route for converting industrial nitrogen oxides (NOx) into highly concentrated nitrate wastewater. This study presents a novel H2O2-based advanced oxidation process that utilizes the composite calcined phosphate rock to activate H2O2 for efficient NOx removal. The calcination treatment for composite phosphate rocks was found to enhance de-NOx efficiency and capacity by varying the CaMg(CO3)2 and Ca5(PO4)3OH contents and creating oxygen vacancies. A systematic investigation of the phase structural evolution under alkaline H2O2 conditions identified CaMg(CO3)2 and Ca5(PO4)3OH as the primary active components, with CaMg(CO3)2 preferentially participating in the reaction. Radical quenching experiments and time-resolved electron paramagnetic resonance (EPR) analysis confirmed the predominant roles of superoxide radicals (O2•–) and surface-bound hydroxyl radicals (•OHsurface) in NOx oxidation. A mechanistic pathway was proposed, highlighting the synergistic effects of reactive oxygen species (ROS) and mineral phase transitions on NOx removal. The proposed NOx purification method offers a promising option for nitrogen recovery and NOx pollution control.
研究领域:
环境科学
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化学工程
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高影响因子
WATER AIR AND SOIL POLLUTION
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2024
·Vol. 235
·期 5
·1-17
·
IF 3.8
Zhou Zhuyou,Ji Yufeng,Wang Yong,Liu Menghe,Xu Ying,Liu Ruijie,Yang Mingjie,Zou Congyang
In this study, the carbon-doped bimetallic organic framework C 60 /MIL-101(Fe,Cu) catalyst was prepared for the first time via solvothermal synthesis method. The catalysts were characterized using X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), and a series of other instruments. At the same time, methylene blue (MB) was used as the target degradation material to investigate the catalytic performance of H 2 O 2 for MB degradation under visible light. The degradation experiment showed that the removal rate of C 60 /MIL-101(Fe,Cu) to MB reached 99.2% within 80 min. Furthermore, cyclic experiments demonstrated good stability and reusability of the catalyst. Finally, the degradation mechanism of the reaction was deduced by quenching experiment, UV–vis diffuse reflection and mott-Schottky plots. The results show that hydroxyl radical (·OH) and superoxide radical (·O 2 − ) play a major role in the degradation of MB during photo-Fenton process.
研究领域:
环境科学
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材料科学
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高影响因子
CHEMISTRY OF MATERIALS
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2024
·
IF 7.2
Xiangjie Tian,Hui Xu,FangFang Zhou,Xiyu Gong,Songwen Tan,Yongju He
Cuproptosis is a newly identified copper-dependent cell death and holds great promise for cancer therapy. However, transporting enough copper into cancer cells is a challenge. Herein, an intelligent cupreous nanoplatform (denoted as CuO2-MSN@TA-Cu2+), consisting of in situ formation of CuO2 within mesoporous silica nanoparticles (MSN) and then deposition with a tannic acid (TA)-Cu2+ complex, is designed and developed to realize on-demand copper delivery for cuproptosis-based combination therapy. CuO2-MSN@TA-Cu2+ exhibits tumor microenvironment-triggered therapeutic activity, wherein the outer TA-Cu2+ complex is readily disassembled to release Cu2+ and liberate the internal CuO2 to produce Cu2+ and H2O2. The overloaded Cu2+ can not only directly convert endogenous H2O2 and self-supplied H2O2 into highly toxic hydroxyl radicals for chemodynamic therapy (CDT) via Cu-based Fenton-like reaction but also undergo glutathione-mediated reduction into Cu+ species to induce potent cellular cuproptosis and enhance CDT. The experimental results indicate that CuO2-MSN@TA-Cu2+ produces remarkable cytotoxicity against cancer cells and significantly suppresses tumor growth by 93.42% in mice-bearing 4T1 breast tumors. This work provides a new paradigm to boost cuproptosis-related therapy and may also inspire the design of advanced therapeutic nanoplatforms.
研究领域:
纳米技术
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癌症生物学
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治疗学
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材料科学
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高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2024
·
IF 10.8
Wen-Long Wang,Zi-Bo Jing,Yi-Lin Zhang,Qian-Yuan Wu,Jörg E. Drewes,Min-Yong Lee,Uwe Hübner
Low-pressure mercury lamps with high-purity quartz can emit both vacuum-UV (VUV, 185 nm) and UV (254 nm) and are commercially available and promising for eliminating recalcitrant organic pollutants. The feasibility of VUV/UV as a chemical-free oxidation process was verified and quantitatively assessed by the concept of H2O2 equivalence (EQH2O2), at which UV/H2O2 showed the same performance as VUV/UV for the degradation of trace organic contaminants (TOrCs). Although VUV showed superior H2O activation and oxidation performance, its performance highly varied as a function of light path length (Lp) in water, while that of UV/H2O2 proportionally decreased with decreasing H2O2 dose regardless of Lp. On increasing Lp from 1.0 to 3.0 cm, the EQH2O2 of VUV/UV decreased from 0.81 to 0.22 mM H2O2. Chloride and nitrate hardly influenced UV/H2O2, but they dramatically inhibited VUV/UV. The competitive absorbance of VUV by chloride and nitrate was verified as the main reason. The inhibitory effect was partially compensated by •OH formation from the propagation reactions of chloride or nitrate VUV photolysis, which was verified by kinetic modeling in Kintecus. In water with an Lp of 2.0 cm, the EQH2O2 of VUV/UV decreased from 0.43 to 0.17 mM (60.8% decrease) on increasing the chloride concentration from 0 to 15 mM and to 0.20 mM (53.5% decrease) at 4 mM nitrate. The results of this study provide a comprehensive understanding of VUV/UV oxidation in comparison to UV/H2O2, which underscores the suitability and efficiency of chemical-free oxidation with VUV/UV.
研究领域:
环境工程
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水处理
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化学工程
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PubMed
高影响因子
Journal of Water Process Engineering
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2025
·
IF 6.7
Zhou Shi,Chenxi He,Hao Huang,Xile Huang,Tong Hu,Yijia He,Dazhi Yang,Simeng Xia,Haojie Zhang,Lin Deng
The frequently detected antibiotics in aquatic environments can induce antibiotic-resistance genes, thereby posing significant risks to both ecosystems and human health. Thus, it is imperative to remove antibiotics from water environments. We constructed a novel polydopamine-loaded copper sulfide (CuS@PDA) through a simple hydrothermal method to activate H 2 O 2 to degrade tetracycline (TC). Compared to CuS/H 2 O 2 , the CuS@PDA/H 2 O 2 system not only achieved efficient TC removal with kinetic rate constant of 0.20 min −1 , but also showed much lower Cu 2+ ions leaching (3.81 mg/L from CuS vs. 0.21 mg/L from CuS@PDA). Besides, CuS@PDA exhibited remarkable recyclability with 93 % removal in the fifth consecutive cycle. Mechanisms analysis revealed that Cu and S contributed to the H 2 O 2 activation and S promoted the conversion of Cu(II) to Cu(I), beneficial for the production of reactive oxygen species. 1 O 2 was found to play the dominant role in the degradation of TC on the basis of quenching tests and electron paramagnetic resonance (EPR) analysis. PDA in CuS@PDA composites facilitated easier complexation with H 2 O 2 and conferred stronger oxidation capability. Lastly, the TC degradation pathway by CuS@PDA/H 2 O 2 was proposed, and the ecotoxicity of its degradation intermediates was estimated. In conclusion, this work demonstrates that the use of PDA can not only improve the catalytic activity and recyclability of CuS towards H 2 O 2 activation for organic pollutants degradation, but also greatly mitigate copper ions leaching.
研究领域:
环境科学
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材料科学
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生物化学
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高影响因子
WATER ENVIRONMENT RESEARCH
·
2025
·Vol. 97
·期 2
·e70022
·
IF 1.9
Guonan Zhao,Ke Feng
The Fenton-like process, utilizing zero-valent iron (Fe 0 ) and hydrogen peroxide (H 2 O 2 ), is employed to degrade refractory organic matter in membrane bioreactor (MBR) effluent derived from landfill leachate. However, the rate-limiting Fe 2+ /Fe 3+ redox step diminishes treatment efficacy and generates substantial iron sludge. This study elucidates the mechanism by which ultraviolet (UV) irradiation augments the Fe 0 /H 2 O 2 process for the removal of refractory organic matter in MBR effluent. The results show that the UV- enhanced H 2 O 2 process effectively disrupts the aromatic structure of organic compounds, reducing molecular weight, degree of polymerization, and humification. Compared with the Fe 0 /H 2 O 2 process, the removal efficiency of UV 254 , color number, and total organic carbon in the effluent treated by the UV/Fe 0 /H 2 O 2 process increased by 24.16%, 14.62%, and 57.46%, respectively. Concurrently, the generation of iron sludge was reduced by 21.6%. This enhancement is primarily attributed to UV's ability to intensify the Fe 2+ /Fe 3+ redox cycle and expedite the surface corrosion of Fe 0 , yielding more iron oxides. This accelerates the decomposition of H 2 O 2 , generating a higher quantity of • OH through both homogeneous and heterogeneous Fenton-like reactions. The refractory organic matter is removed through the oxidation by • OH, as well as the adsorption and precipitation facilitated by iron-based colloids. Practitioner Points UV promotes Fe 0 /H 2 O 2 process to degrade refractory organic matter in MBR effluent. UV promotes Fe 0 to dissolve more Fe 2+ and the redox cycle of Fe 2+ and Fe 3+ . The dosage of H 2 O 2 or Fe 0 influences the treatment effect of the process. Graphical UV can enhance the degradation of refractory organic matter in MBR effluent from landfill leachate by Fe 0 /H 2 O 2 process.
研究领域:
环境科学
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水处理工程
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
·
IF 8.1
Weikang Wang,Yadong Wu,Shahid Khan,Haopeng Jiang,Muhammad Adnan Qaiser,Xianzhi Chai,Chengzhang Zhu,Lele Wang,Qinqin Liu
Solar-driven hydrogen (H 2 ) and hydrogen peroxide (H 2 O 2 ) generation over visible-light responsive carbon nitride (CN) photocatalysts for in situ efficient sterilization is a promising and eco-friendly strategy. Herein, a colloidal potassium-ion (K + ) intercalated crystalline CN nanosheets (KCCN) photocatalyst was constructed for boosting synergetic H 2 O 2 synthesis with isopropanol (IPA) oxidation and in situ antibacterial effect . The surface hydroxyl (−OH) and cyano (−C N) groups induced by molten salt (KCl)-assisted thermal treatments contributed to the colloidal nature of CN, facilitating for high wettability of KCCN in aqueous solution to gain active hydrogen (H + ) from water sustainably. Meaningfully, the enhanced high-energy singlet oxygen species ( 1 O 2 ) produced by KCNN-2 were verified by electron paramagnetic resonance (EPR) and 9,10-anthracenediyl-bis(methylene)-dimalonic acid (ABDA)-fluorescent probe, significantly contributing to H 2 O 2 production and antibacterial effect. Consequently, the optimal KCCN-2 exhibited a much enhanced H 2 generation of 4.11 mmol g −1 h −1 , and H 2 O 2 production activity of 1.82 mmol L −1 h −1 with acetone yield rate of 47.3 mmol g −1 h −1 under visible-light (λ > 420 nm) irradiation in 10 vol% IPA solution. The in-situ generated H 2 O 2 can be activated to produce reactive oxygen species (ROS), especially 1 O 2 , to effectively kill the Escherichia coli , reaching an improved an antibacterial rate of 89.7% under stimulated sunlight irradiation in 1 h. This work could offer a new insight into the photoinduced ROS for aqueous H 2 O 2 photosynthesis and antibacterial application.
研究领域:
环境科学
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生物学
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材料科学
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2024
·
IF 12.2
Xiang Gao,Huanhuan Chen,Huimin Qiu,Yang Zhang,Jie Cheng,Yizhong Shen
Due to the typical volatility of gaseous pollutant methyl mercaptan (CH 3 SH), the development of a facile, reliable, and accurate onsite environmental surveillance of highly toxic CH 3 SH faces many challenges, but it is critical to environmental atmosphere assessment and safeguarding public health. Here, we prepared a novel bimetallic carbon dots (Fe&Cu@CDs) nanozyme with high peroxidase-mimicking activity to design a portable hydrogel kit for onsite visual H 2 O 2 -self-supplying enzymatic cascade catalytic colorimetric and photothermal signal synergistic amplification dual-modal monitoring of CH 3 SH in atmospheric environment. Assisted by alcohol oxidase (AOX), CH 3 SH could be specifically converted into H 2 O 2 for oxidizing chromogenic substrate 3,3′,5,5′-tetramethylbenzidine (TMB) catalyzed by Fe&Cu@CDs to produce dark blue ox-TMB with absorption at 652 nm and photothermal characters. Consequently, a CH 3 SH concentration-dependent change both in naked-eye color and photothermal effect-triggered temperature were observed. By hybridizing AOX-assisted Fe&Cu@CDs + TMB with agarose, a H 2 O 2 -self-supplying colorimetric and photothermal signal synergistic amplification sensory hydrogel kit integrated with Color Picker APP-installed smartphone and 660 nm laser-equipped handheld thermal imager for CH 3 SH was proposed with acceptable results in atmospheric environment around wastepile ( e.g. , solid waste and food waste piles), which exhibited great potentials to further develop commercial onsite monitoring platforms in warning-early abnormal atmospheric CH 3 SH for safeguarding environmental health.
研究领域:
环境科学
·
分析化学
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纳米技术
·
材料科学
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PubMed
高影响因子
危险品化学品经营许可证（带存储）