ACTA PHYSICO-CHIMICA SINICA
·
2025
·
IF 13.5
Yi Yang,Xin Zhou,Miaoli Gu,Bei Cheng,Zhen Wu,Jianjun Zhang
Photocatalytic hydrogen peroxide (H 2 O 2 ) production is a crucial process for clean energy conversion, involving the reduction of O 2 through two electrons. However, this process is often hampered by the sluggish water oxidation involving the photogenerated holes. To address this challenge, we have constructed a dual-functional S-scheme ZnO/CdIn 2 S 4 heterojunction systerm coupling the H 2 O 2 generation with a value-added benzylamine (BA) oxidation reaction. In this dual-functional photocatalytic system, photogenerated electrons in CdIn 2 S 4 efficiently reduce O 2 to produce H 2 O 2 , while photogenerated holes in ZnO selectively oxidize BA to N-benzylidenebenzylamine. Leveraging the advantages of the S-scheme heterojunction, the optimized ZnO/CdIn 2 S 4 photocatalyst displays an enhanced H 2 O 2 production rate (386 μmol·L −1 ·h −1 ) and BA oxidation fraction (81%) than pure ZnO or CdIn 2 S 4 . Femtosecond transient absorption (fs-TA) spectroscopy confirm the ultrafast S-scheme electron transfer from the ZnO conduction band (CB) to the CdIn 2 S 4 valence band (VB) upon photoexcitation of the ZnO/CdIn 2 S 4 composite. Besides, timely depletion of VB holes in ZnO and CB electrons in CdIn 2 S 4 can accelerate the interfacial electron transfer in the ZnO/CdIn 2 S 4 S-scheme heterojunction. The innovative design of the ZnO/CdIn 2 S 4 S-scheme photocatalyst provides new insights for developing efficient dual-functional heterojunction photocatalytic systems and introduces a novel method for studying S-scheme heterojunctions using fs-TA spectroscopy.
研究领域:
光催化
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材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Songyu Ren,Aimin Wang,Yanyu Zhang,Yongjun Song,Zhenjun Wen,Zhongguo Zhang
Electrocatalytic H 2 O 2 production via the two-electron oxygen reduction reaction on the cathode surface plays a crucial role in the electro-peroxidation (EO-H 2 O 2 ). In this work, the H 2 O 2 generation potential of the EO-H 2 O 2 process using an activated carbon fiber attached RuO 2 /Ti cathode (ACF@RuO 2 /Ti) was evaluated by simulation experiments with a high-precision syringe pump. Results shown that the actual average H 2 O 2 accumulation rate reached up to 4.92 mg h −1 cm −2 , while more than 95 % of the electrogenerated H 2 O 2 was decomposed quickly. Electron paramagnetic resonance and quenching tests confirmed that the primary oxidant • OH was produced from H 2 O 2 activation by ACF, RuO 2 catalyst and their synergistic effect, while RuO 2 played dominant role. The production of • OH in the EO-H 2 O 2 process was also confirmed by the degradation and mineralization of antibiotic ciprofloxacin. The characterization results indicated that heterogeneous catalysis of cathode was due to both the pyridinic nitrogen and oxygen-containing groups of ACF, along with RuO 2 catalyst on the RuO 2 /Ti surface. This study provides new insights into the mechanisms of the in situ H 2 O 2 generation and activation in the EO-H 2 O 2 process.
研究领域:
环境科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2024
·
IF 11.2
Bo Zhang,Kang Li,Renfu Li,Shoufeng Wang,Longtian Kang
Here, 1D bis(N-carboxymethyl) peryleneimide (H 2 PDI), 0D 1,6,7,12-tetrachloro-bis(N-carboxymethyl) peryleneimide (4Cl-H 2 PDI), and 2D 4Cl-H 2 PDI/graphene quantum dot (4Cl-H 2 PDI/GQD) nanostructures are synthesized and carefully analyzed. The effect of bay-/end-substitution and S-scheme heterojunction of PDI-based materials as main catalysts on the photocatalytic H 2 O 2 evolution is first studied through the oxygen reduction reaction (ORR). Under the visible-light irradiation (> 420 nm), 4Cl-H 2 PDI and 4Cl-H 2 PDI/GQD as photocatalysts exhibit the ∼7 and ∼16 times H 2 O 2 evolution rate than H 2 PDI (1059.6 vs. 2484.0 vs. 160.0 µM g −1 h −1 ), respectively. The systematical experiments reveal that 4Cl-H 2 PDI and 4Cl-H 2 PDI/GQD should prefer a two-step single-electron ORR process, while H 2 PDI may involve a 4e ‒ water oxidation and one-step 2e ‒ ORR process. Further experiments confirm that the bay-substitution and GQD doping of H 2 PDI can promote the generation, transportation, and separation of photogenerated electrons and holes, and prolong the carrier lifetime. This work provides insight into PDI-based photocatalytic H 2 O 2 production.
研究领域:
材料科学
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光化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Tiantian Lu,Ying Liu,Youzeng Li,Jialei Chen,Shan Chen,Xuelong Liao,Wei Xia,Tong Zhou,Wei Wang,Zhuo Chen,Rong Huang,Huan Wang
Cobalt single atom catalysts (Co SACs) have been extensively explored in catalyzing the two-electron oxygen reduction reaction (2e – ORR) into hydrogen peroxide (H 2 O 2 ). However, the contribution of active sites for 2e – ORR in different media remains elusive. Here, we synthesized epoxy-modified Co SACs through a chemical vapor deposition approach followed by an oxidation treatment, which provides a model catalyst to identify the distinct role of Co sites and oxygen species for 2e – ORR. It is found that Co sites dominantly function in acidic media and barely works in neutral solution. Introduction of epoxy groups in the vicinity of Co sites can enlarge interlayer spacing and reinforce Co–N strength, which facilitates O 2 transport and weakens Co–*OOH interaction, collectively contributing to a superior selectivity for acidic H 2 O 2 generation. While for neutral 2e – ORR, the O-containing groups distant from Co sites serve as the dominant active sites. Encouragingly, the onsite production of H 2 O 2 in the acidic solution can be efficiently utilized for pollutant removal.
研究领域:
催化化学
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环境科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Junhao Cai,Yaru Peng,Po Hu,Yuan Zhou,Qiaoge Yao,Hao Lyu,Youtang Gao
The light absorption, active sites, and charge carriers separation of photocatalysts are extremely important factors in the field of photocatalysis. Near-perfect lattice-matched homojunction constructed using disorder engineering and doping strategies is an effective strategy to improve photocatalytic activity. Herein, we developed crystalline TiO 2 nanoparticles (NPs) and Ti 3 C 2 T x MXene-derived C-doped amorphous TiO x homojunction (TCT) at room temperature. In this homojunction, TiO 2 NPs are evenly distributed on the surface of the C-TiO x nanosheet to form a type-II structure, which promotes the separation of photogenerated carriers. The light absorption range of TCT extends to 550 nm due to the presence of intermediate energy levels in C-TiO x , which increases its photon absorption capacity. Moreover, TCT possesses a large number of oxygen vacancies, which are beneficial for improving the adsorption and degradation of pollutants. These characteristics of TCT could significantly improve its photodegradation performance for tetracycline. Interestingly, the precursor mass ratio of TCT with the best degradation efficiency is different under different illumination conditions, which is attributed to the different band gaps of C-TiO x and TiO 2 NPs resulting in different light absorption ranges. This work provides a new approach to rationally designing crystalline and amorphous homojunction for photocatalytic applications.
研究领域:
材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry B
·
2024
·Vol. 12
·期 25
·6164-6174
·
IF 6.1
Lihui Yuwen,Pei Lu,Qi Zhang,Kaili Yang,Zhaowei Yin,Bin Liang,Lianhui Wang
Catalytic therapy based on nanozymes is promising for the treatment of bacterial infections. However, its therapeutic efficacy is usually restricted by the limited amount of hydrogen peroxide and the weak acidic environment in infected tissues. To solve these issues, we prepared polyvinyl alcohol (PVA)–polyacrylic acid (PAA)–iron oxide (Fe3O4)/polyvinyl alcohol (PVA)–zinc peroxide (ZnO2) double-layer electrospun nanofibers (PPF/PZ NFs). In this design, PVA serves as the carrier for ZnO2 nanoparticles (NPs), Fe3O4 NPs, and PAA. The double-layer structure of nanofibers can spatially separate the PAA and ZnO2 to avoid their reaction with each other during preparation and storage, while in the wet wound bed, PVA can dissolve and PAA can provide H+ ions to promote the generation of hydrogen peroxide and subsequent conversion to hydroxyl radicals for bacteria killing. In vitro experimental results demonstrated that PPF/PZ NFs can reduce the methicillin-resistant Staphylococcus aureus by 3.1 log (99.92%). Moreover, PPF/PZ NFs can efficiently treat the bacterial infection in a mouse wound model and promote wound healing with negligible toxicity to animals, indicating their potential use as “plug-and-play” antibacterial wound dressings. This work provides a novel strategy for the construction of double-layer electrospun nanofibers as catalytic wound dressings with hydrogen peroxide/acid self-supplying properties for the efficient treatment of bacterial infections.
研究领域:
生物材料学
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医学
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纳米医学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Jingjing Wang,Ruonan Liu,Yuxin Qiao,Shuxin Liu,Chuanguang Qin
In this work, flower-like Bi 2 S 3 was prepared by hydrothermal method using different solvents, and materials with better performance were selected. Graphene quantum dots (GQD, which is rich in specific amino groups) was prepared by aqueous phase fusion technology. Ultimately, a straightforward one-step hydrothermal process was used to successfully manufacture composite materials in order to build GQD(4)/Bi 2 S 3 heterostructures. The study results have shown that the H 2 production efficiency of 2% GQD(4)/Bi 2 S 3 is the best, and its photocatalytic hydrogen production efficiency within 3 h is 5.92 times that of GQD(4) and 3.03 times that of Bi 2 S 3 . The H 2 O 2 production and tetracycline (TC) degradation efficiency of 2% GQD(4)/Bi 2 S 3 are the best, while the methylene blue (MB) degradation efficiency of 1% GQD(4)/Bi 2 S 3 is relatively better. The research results show that as a perfect combination of GQD(4)/Bi 2 S 3 heterostructures, it offers a productive plan for eliminating organic pollutants in water and producing clean oxidant and hydrogen energy.
研究领域:
材料科学
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环境科学
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
Food Science and Human Wellness
·
2024
·
IF 5.6
Xiaomei Du,Kexin Wang,Xiaoyan Sang,Xiangxing Meng,Jiao Xie,Tianxin Wang,Xiaozhi Liu,Qun Huang,Nan Zhang,Hao Wang
Naringin exists in a wide range of Chinese herbal medicine and has proven to possess several pharmacological properties. In this study, PC12, HepG2 cells, and female Drosophila melanogaster were used to investigate the antioxidative and anti-aging effects of naringin and explore the underlying mechanisms. The results showed that naringin inhibited H 2 O 2 -induced decline in cell viability and decreased the content of reactive oxygen species in cells. Meanwhile, naringin prolonged the lifespan of flies, enhanced the abilities of climbing and the resistance to stress, improved the activities of antioxidant enzymes, and decreased malondialdehyde content. Naringin also improved intestinal barrier dysfunction and reduced abnormal proliferation of intestinal stem cells. Moreover, naringin down-regulated the mRNA expressions of inr , chico , pi3k , and akt-1 , and up-regulated the mRNA expressions of dilp2 , dilp3 , dilp5 , and foxo , thereby activating autophagy-related genes and increasing the number of lysosomes. Furthermore, the mutant stocks assays and computer molecular simulation results further indicated that naringin delayed aging by inhibiting the insulin signaling (IIS) pathway and activating the autophagy pathway, which was consistent with the result of network pharmacological predictions.
研究领域:
药理学
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分子生物学
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衰老研究
✓ 已验证
产品关联
DOI
高影响因子
Journal of Breath Research
·
2019
·Vol. 13
·期 3
·036005
·
IF 3
Yuanling Liu,Wenwen Li,Yixiang Duan
Oxidative stress (OS) refers to the process of oxidative damage caused by reactive oxygen species (ROS) and reactive nitrogen species (RNS) accumulated by the organisms or cells during the process of generating and scavenging oxygen free radicals. In this study, an OS model of MCF-7 cells was constructed through H2O2-treatment, which for the first time combined volatile organic compounds (VOCs) and intracellular metabolic analysis for a comprehensive and in-depth study of the OS effect on cell metabolism. The VOCs produced by cells in H2O2-treated groups and control groups were extracted with solid-phase microextraction (SPME) and analyzed by gas chromatography-mass spectrometer (GC-MS). Meanwhile, the intracellular metabolites were extracted by methanol and analyzed by GC-MS coupled with silyl-derivatization. The results indicated 15 VOCs and 29 intracellular metabolites were statistically different (p < 0.05) between the H2O2-treated groups and the control groups. The VOC biomarkers were mainly linear chain alkanes and branched chain alkanes, and they were up-regulated in cells treated by H2O2. The intracellular metabolites with significant changes were mainly fatty acids, amino acids, and organic acids. Most of them, however, were down-regulated under OS state. This study revealed volatile and non-volatile metabolites that influenced by elevated OS in MCF-7 cells, and provided clues for mechanism exploration of exhaled biomarkers, thus promoting the non-invasive prediction of BC.
研究领域:
癌症研究
·
代谢组学
·
生物化学
✓ 已验证
DOI
PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2017
·Vol. 27
·期 43
·1700626
·
IF 12.124
Chi Zhang,Wei-Hai Chen,Li-Han Liu,Wen-Xiu Qiu,Wu-Yang Yu,Xian-Zheng Zhang
Conventional photodynamic therapy (PDT) has limited applications in clinical cancer therapy due to the insufficient O 2 supply, inefficient reactive oxygen species (ROS) generation, and low penetration depth of light. In this work, a multifunctional nanoplatform, upconversion nanoparticles (UCNPs)@TiO 2 @MnO 2 core/shell/sheet nanocomposites (UTMs), is designed and constructed to overcome these drawbacks by generating O 2 in situ, amplifying the content of singlet oxygen ( 1 O 2 ) and hydroxyl radical (•OH) via water-splitting, and utilizing 980 nm near-infrared (NIR) light to increase penetration depth. Once UTMs are accumulated at tumor site, intracellular H 2 O 2 is catalyzed by MnO 2 nanosheets to generate O 2 for improving oxygen-dependent PDT. Simultaneously, with the decomposition of MnO 2 nanosheets and 980 nm NIR irradiation, UCNPs can efficiently convert NIR to ultraviolet light to activate TiO 2 and generate toxic ROS for deep tumor therapy. In addition, UCNPs and decomposed Mn 2+ can be used for further upconversion luminescence and magnetic resonance imaging in tumor site. Both in vitro and in vivo experiments demonstrate that this nanoplatform can significantly improve PDT efficiency with tumor imaging capability, which will find great potential in the fight against tumor.
研究领域:
癌症治疗
·
纳米技术
·
生物医学工程
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光化学
·
成像技术
✓ 已验证
DOI
高影响因子
Nanoscale
·
2020
·Vol. 12
·期 42
·21674-21686
·
IF 6.895
Jingjing Liu,Jiameng Gao,Amin Zhang,Yuliang Guo,Shanshan Fan,Yu He,Kai Yang,Jianbo Wang,Daxiang Cui,Yingsheng Cheng
Intelligent phototherapy by theranostic nanosystems that can be activated by a tumor microenvironment has high sensitivity and specificity. However, hypoxia and low drug accumulation in tumors greatly limit its clinical application. Herein, we have designed a cage-like carbon-manganese nanozyme, which effectively relieves tumor hypoxia and delivers numerous photosensitizers (PSs) to the tumor site, for real-time imaging and enhanced phototherapy of esophageal cancer. Specifically, bovine serum albumin (BSA) was used as a template and reducing agent for preparing a BSA-MnO2 nanozyme; then a BSA-MnO2/IR820@OCNC (BMIOC) nanosystem was successfully synthesized by crosslinking BSA-MnO2 on the surface of IR820-loaded carboxylated carbon nanocages (OCNCs). Abundant PSs were successfully delivered to tumor sites via hollow OCNCs, and the final loading rate of IR820 reached 42.8%. The intratumor BMIOC nanosystem can be initiated by a tumor microenvironment to switch on its magnetic resonance (MR) imaging signal, and photothermal therapy (PTT) and photodynamic therapy (PDT) functions. Notably, the BSA-MnO2 nanozyme, with intrinsic catalase (CAT)-like activity, catalyzed endogenous H2O2 for oxygen generation to overcome tumor hypoxia and enhance PDT, thereby leading to more efficient therapeutic effects in combination with OCNC-elevated PTT. In addition, the H2O2-activated and acid-enhanced properties enable our nanosystem to be specific to tumors, protecting normal tissues from damage. By integrating a high drug loading capacity, a hypoxia regulation function, an enlarged phototherapy effect, and bimodal imaging into a nanozyme-mediated nanoreactor, this work realizes a “one for all” system and represents promising clinical translation for efficient esophageal cancer theranostics.
研究领域:
纳米医学
·
癌症治疗
·
医学影像
·
生物医学工程
✓ 已验证
DOI
PubMed
高影响因子
Journal of Materials Chemistry B
·
2019
·Vol. 7
·期 29
·4568-4580
·
IF 5.047
Linfeng Bai,Wanquan Jiang,Min Sang,Mei Liu,Shouhu Xuan,Sheng Wang,Ken Cham-Fai Leung,Xinglong Gong
The exploitation of multifunctional nanocomposites as artificial mimetic enzymes has received significant attention. This study reports a novel sandwich-structural magnetic microsphere (Fe3O4@resorcinol/formaldehyde resin–metal@polydopamine), in which ultra-small noble metal nanocrystals can be sandwiched between the resorcinol/formaldehyde resin (RF) and polydopamine (PDA) layers. By changing the metal precursor, various microspheres decorated with mono- or bi-metallic nanocrystals (Pt, Pd, Au, PtAu, etc.) can be obtained. The dual-shelled magnetic microsphere not only provides abundant active sites for noble metal nanocrystals but also effectively restrains aggregation and leaching. The as-prepared Fe3O4@RF–Pt@PDA can efficiently catalyze the oxidation of 3,3,5,5-tetramethylbenzidine (TMB) in the presence of H2O2, which confirms that the as-prepared nanocatalyst shows good peroxidase-like activity. The catalytic activity of Fe3O4@RF–Pt@PDA is dependent on pH and temperature, and the relevant catalytic kinetics follow the Michaelis–Menten behaviors. Moreover, this kind of magnetic microsphere can be further applied for H2O2 and glucose detections and the limit of detection (LOD) is found to be as low as 3.1 μM and 1.36 μM, respectively. Benefiting from a facile preparation process, superior structure, and outstanding catalytic activity, these multifunctional microspheres possess high potential as artificial enzymes in clinical diagnosis, analytical chemistry and environmental fields.
研究领域:
生物化学
·
材料科学
·
分析化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）