Materials Advances
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2024
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IF 5.2
Catherine Afriyie,Xingwang Zhang
Photocatalytic methane conversion is a sustainable approach to transform methane under mild conditions into its value-added derivatives for the petrochemical industry. However, obtaining high productivity and selectivity of desired products still remains a great challenge. In this work, high-efficiency Fe-doped two-dimensional BiVO4 nanosheets have been synthesized and evaluated for photocatalytic methane conversion with H2O, O2 or H2O2 as the oxidizer. The Fe-doped and undoped samples were obtained by hydrothermal synthesis using 3-dodecylbenzenesulfonate (SDBS) as the morphology-directing agent, and examined by XRD, SEM, EDS, TEM, XPS, UV-DRS and BET characterization techniques. The replacement of some Bi3+ with Fe3+ was a successful approach to enhance the photoexcitation process and the adsorption properties of BiVO4, resulting in an improvement in the yield of methyl oxygenates. Complete selectivity of methyl oxygenates (CH3OH and CH3OOH) was achieved, and the yield reached 217.6 μmol gcat−1 h−1 in 2 h under visible light irradiation under mild conditions over 1.0 wt% Fe-doped BiVO4 nanosheets in the presence of H2O2, outperforming most reported studies on this reaction. This work provides new insight into the choice of a suitable oxidizer for methane conversion in the BiVO4 photocatalyst system by projecting H2O2 as the relevant oxidant.
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Journal of Materials Chemistry C
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2024
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IF 5.7
Yuedan Wang,Tao Yang,Panpan Hao,Changhui Li,Mufang Li,Yan Tan,Dong Wang
The Fe-MOF@PANI/Carbon fiber was prepared by solvothermal method and used as the gate of organic photoelectrochemical transistor (OPECT). The ratio of Fe-MOF to PANI was optimized to enhance the photoelectric signal transduction. In addition, the vertical configuration of devices was adopted to improve the sensor property. Under light illumination, the device shows good photoelectric conversion ability, periodic stability and duration stability. The uric acid biosensor was prepared by modifying the gate with urate oxidase. The sensitivity of sensors in the absence of light and under illumination is compared. The results show that the sensitivity of the sensor is significantly improved to 91.65 mV/decade under light. The linear relationship is good in the range of 1 nM-5 mM, with a correlation coefficient of R2=0.9506. The sensor can also be used under bending conditions and has been successfully applied to the detection of uric acid in human sweat samples, providing a viable solution for wearable electronic devices.
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ACS Applied Materials & Interfaces
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2018
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IF 8.097
Yuxue Ding,Jiaxun Wan,Zihao Zhang,Fang Wang,Jia Guo,Changchun Wang
The anticancer therapy on the basis of reactive oxygen species (ROS)-mediated cellular apoptosis has achieved great progress. However, this kind of theraputic strategy still faces some challenges such as light, photosensitizer and oxygen (O2) dependence. In this article, a ROS-mediated anticancer therapy independent of light, photosensitizer and oxygen was established based on a Fe2+-induced ROS-generating nanosystem. First, artemisinin (ART) was loaded in porous magnetic supraparticles (MSP) by a nanodeposition method. Then, the poly(aspartic acid)-based polymer, which consisted of dopamine, indocyanine green, and polyethylene glycol side chain, was coated onto the surface of ART-loaded MSP. When the nanoparticles entered into cancer cells, a reaction of Fe2+-mediated cleavage of the endoperoxide bridge contained in ART occurred and subsequent a large amount of ROS was generated. Moreover, a NIR light was used to effectively increase the local temperature of tumor in virtue of the superior photothermal effects of MSP, which enabled us to accelerate the ROS generation and achieved an enhanced ROS yield. The newly developed nanodrug system displayed a high level of intracellular ROS generation, leading to the desired killing efficacy against malignant cells and solid tumor. This smart nanosystem holds great potential to overcome the existing barrier in PDT and opens a promising avenue for anticancer therapy.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Qingchen Bai,Miao Wang,Kai Wang,Jingwei Liu,Fengyu Qu,Huiming Lin
Due to their rigid π-conjugated macrocyclic structure, organic sonosensitizers face significant aggregation in physiological conditions, hindering the production of reactive oxygen species (ROS). An acid-sensitive nanoassembly was developed to address this issue and enhance sonodynamic therapy (SDT) and emission. Initially, copper phthalocyanine (CuPc) was activated using a H 2 SO 4 -assisted hydrothermal method to introduce multiple functional groups (–COOH, –OH, and −SO 3 H), disrupting strong π–π stacking and promoting ROS generation and emission. Subsequently, negatively charged CuPc-SO 4 was incorporated into bovine serum albumin (BSA) to form CuPc-Fe@BSA nanoparticles (10 nm) with Fe 3+ ions serving as linkers. In acidic conditions, protonation of CuPc-SO 4 and BSA weakened the interactions, leading to Fe 3+ release and nanostructure dissociation. Protonated CuPc-SO 4 tended to self-aggregate into nanorods. This acidity-sensitive aggregation is vital for achieving specific accumulation within the tumor microenvironment (TME), thereby enhancing retention and SDT efficacy. Prior to this, the nanocomposites demonstrated cycling stability under neutral conditions. Additionally, the released Fe ions exhibited mimicry of glutathione peroxidase and peroxidase activity for chemotherapy (CDT). The synergistic effect of SDT and CDT increased intracellular oxidative stress, causing mitochondrial injury and ferroptosis. Furthermore, the combined therapy induced immunogenic cell death (ICD), effectively activating anticancer immune responses and suppressing metastasis and recurrence.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
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IF 4.9
Shuyu Chen,Zhengkai Wu,Xueying Cheng,Lu Chen,Yunning Chen,Yingna Guo,Changhua Wang,Qingkun Shang
In this work, we used a simple hydrothermal method to in-situ grow Zn 3 In 2 S 6 on MIL-100(Fe) octahedra, and obtained a MIL-100(Fe)@Zn 3 In 2 S 6 Z-scheme heterojunction photocatalyst. We systematically studied its performance in degrading phenol and p-nitrophenol (PNP) under visible light. MIL-ZIS 6 -2 can remove 89.1 % of phenol within 120 min and nearly 100 % of PNP within 60 min. Its photocatalytic activity to the degradation of phenol is 30.7 times and 1.7 times higher than that of MIL-100(Fe) and Zn 3 In 2 S 6 , respectively. And the photocatalytic activity to degrade PNP is 18.2 times and 1.4 times higher than MIL-100(Fe) and Zn 3 In 2 S 6 . Further research was conducted on its band structure and photocatalytic response mechanism through photoelectric performance, ultraviolet photo-electron spectroscopy, and electron spin resonance spectrometer testing. The results showed that the formation of Z-scheme heterojunction not only increased the specific surface area of the composite photocatalyst, enabling it to provide more reaction sites, but also effectively suppressed the recombination of photogenerated holes and electrons, improving the redox ability of the photocatalyst. This work provides a new perspective for constructing efficient Zn 3 In 2 S 6 -based composite photocatalysts and addressing environmental issues.
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Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Wenjin Ni,Sicheng Zhang,Lingling Cheng,Tiejun Luo,Hongyun Yang,Tengfei Duan,Dejian Yan
Developing efficient photoanodes for water oxidation is highly promising due to their critical role in producing green H 2 and harnessing solar energy. Herein, a metal-organic framework (MOF)/photoanode was successfully constructed by coating TiO 2 nanorods with MIL-88(Fe) MOF for photoelectrochemical (PEC) water splitting. The results demonstrated that MIL-88(Fe) was uniformly and tightly coated on TiO 2 and functioned as a cocatalyst. The MIL-88(Fe) MOF provides a large surface area and more Fe-O active sites, contributing to high PEC activity by reducing electron/hole recombination and enhancing light response capability. Moreover, the photoanode also exhibited an improved charge conductivity. As a result, the MIL-88(Fe)/TiO 2 photoanode exhibited an excellent photocurrent density of 1.06 mA cm −2 at 1.23 V RHE , which is approximately 2.6 times higher than the pristine TiO 2 . Charge transfer kinetics analyses and electrochemical tests were carried out and revealed that the improved PEC performance was attributed to the introduction of MIL-88(Fe), which promoted charge separation-transfer. This research provided new insights into the design of efficient semiconductor/MOF composite photoanodes for PEC water oxidation.
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NEW JOURNAL OF CHEMISTRY
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2024
·Vol. 48
·期 20
·9185-9195
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IF 2.7
Shikai Xue,Dongying Zhu,Qing Zuo,Shuangfeng Yang,Haiyan Wang,Qiujun Lu,Guoxing Yin,Guihua Ruan,Fuyou Du
A novel MIL-101(Fe)/ZnCrZr-LBMO heterojunction was successfully constructed and used for the removal of ciprofloxacin (CIP) in this work. The MIL-101(Fe)/ZnCrZr-LBMO composite exhibited significantly enhanced photocatalytic degradation activity, with reaction rates approximately 3.4 and 3.1 times faster than those observed with pristine MIL-101(Fe) and ZnCrZr-LBMO, respectively. The effect of different amounts of ZnCrZr-LBMO, sample pH, CIP concentration, inorganic cations, and anions on CIP removal was investigated, and the possible intermediates and degradation pathways of CIP were speculated. The·O2− radicals dominated CIP degradation, with minor contributions from 1O2, h+, and ·OH radicals. The composite exhibited high removal rates for CIP (94.7%), ofloxacin (86.8%), and tetracycline (96.3%), respectively, within 60 min of light irradiation, and excellent reusability, retaining over 85.1% CIP degradation rate after five cycles. Our work provides a new reference to construct highly efficient and easily recyclable MIL-101(Fe)/ZnCrZr-LBMO photocatalysts for the removal of antibiotic pollutants, promising advancements in real water treatment applications.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Haofan Jia,Liujing Yang,Hao Zhu,Yang Wang,Ying Chen,Kai Sun,Xinbao Li
In this study, a series of high-efficient catalyst, Co–Fe/Al 2 O 3 , were synthesized via the sol-gel method for low-temperature phenol steam reforming (PSR). The optimized catalyst, 15Co–2Fe/Al 2 O 3 , exhibited a remarkable phenol conversion of 95.3%, a H 2 yield of 92.1% at 450 °C, GHSV = 7500 h −1 and a steam-to-carbon (S/C) ratio of 10. Furthermore, the catalyst activity was maintained for 660 min before a gradual decline was observed. The NH 3 -TPD analysis revealed that the addition of Fe enhanced the surface acidity of the catalyst, providing more active sites for phenol adsorption and activation. This study aims to address the challenges associated with high reaction temperatures and poor catalyst stability in PSR. Various characterization techniques have been employed to investigate the reaction mechanisms of bimetallic catalysts in low-temperature PSR.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Chengcheng Qi,Yaqi Kong,Ziyin Yang
The regulation of the activity of single-atom nanozymes is crucial for the development of highly sensitive electrochemical sensors. The accessibility of single-atom nanozymes is an important factor limiting their activity. This study proposes a directional anchoring strategy to regulate the accessibility of single-atom nanozymes for boosting electrochemical nonenzymatic H 2 O 2 sensing. The directional anchoring of Fe single-atoms on the inner surface of nitrogen-doped carbon materials (In-Fe SAs/NC) and the outer surface of nitrogen-doped carbon materials (Out-Fe SAs/NC) was achieved via the hard template assisted method. The impact of the anchoring position of Fe SAs on the electrocatalytic reduction of H 2 O 2 was investigated. Density functional theory (DFT) calculations reveal that Fe SAs nanozymes are more likely to activate H 2 O 2 than the previously reported Fe 3 O 4 nanozymes. The anchoring of Fe SAs on the outer surface of NCs markedly enhances the accessibility of active sites in comparison to anchoring Fe SAs on the inner surface, thereby increasing the sensitivity for the detection of H 2 O 2 . The electrochemical sensor based on Out-Fe SAs/NC can be used to detect H 2 O 2 content in milk samples. The high accessibility and excellent intrinsic activity of Fe SAs render Out-Fe SAs/NC a highly effective sensing material.
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Materials Science and Engineering B-Advanced Functional Solid-State Materials
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2024
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IF 3.9
Boyu Du,Nan Jiang,Zengbin Chai,Chao Liu,Xing Zhu
DETA-Fe-BTC MOFs with an irregular porous structure is fabricated by a hydrothermal method combining with Diethylenetriamine (DETA) modification and investigated in batch adsorption experiments for arsenic removal from wastewater. DETA-Fe-BTC show high adsorption ability in wide pHs ranged from 2 to 12 and a wide arsenic concentration range from 1 mg/L to 1000 mg/L. The maximal arsenic adsorption capacity reaches 1748.50 mg/g at a pH of 10. Besides, the MOFs reveal a super-fast arsenic-removal rate. 90.58 % of arsenic was removed from wastewater with an initial arsenic concentration of 40 mg/L in 5 s. Arsenic adsorption kinetics and isotherms follow a chemical adsorption mode and a single-molecule adsorption mode that the MOFs offer abundant Fe 3+ active cites forming Fe-O-As coordination with arsenate or arsenite. Considering its strong recyclability and high efficiency, DETA-Fe-BTC will be used as a potential arsenic scavenger for the disposal of arsenic contaminated groundwater or industrial wastewater.
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ANALYTICAL CHEMISTRY
·
2025
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IF 6.7
Chengzhuo Yu,Jin Xu,Li Xiong,Yarui Wang,Silong Wang,Fanglan Geng,Zesen Shang,Huasheng Wu,Lixia Zhao,Yawei Wang
Luminol-based chemiluminescence (CL) systems, as a powerful tool for bioanalysis, are limited owing to their weak CL intensity and self-decomposition of the classic oxidant H2O2. Herein, we introduced a new luminol CL enhancer, the natural light-driven photocatalyst MIL-100(Fe)/TiO2, for the selective determination of dopamine (DA). By employing MIL-100(Fe)/TiO2 for the first time as an efficient enhancer, the MIL-100(Fe)/TiO2-luminol CL intensity was 100 times higher than that of the classical H2O2-luminol system. The CL spectrum, UV–vis absorption spectroscopy, radical scavenger experiments, and electron spin resonance spectroscopy were utilized to investigate the possible CL mechanism of the MIL-100(Fe)/TiO2-luminol system. All of the results indicated that MIL-100(Fe)/TiO2 can generate reactive oxygen species under mild natural light, which could react rapidly with the luminol anion radical and result in direct CL emission. The sensitive plate for DA was developed based on its inhibiting effect on CL intensity, and the linear range between CL intensity and DA concentration was 100 nM–1000 μM with a detection limit of 16.7 μM (S/N = 3). This study successfully achieved a stable reactant that can directly trigger the CL of luminol without the need for additional oxidizing agents under mild natural light and offers new possibilities for photoinduced amplification technology.
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Catalysis Science & Technology
·
2024
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IF 4.4
Xuewei Tu,Can Sun,Yang Hu,Yutong Chen,Shouxin Zhu,Jingyi Qu,Zhexiao Zhu,Xiang Zhang,Hui Zheng
Cycloaddition of CO2 and epoxides to synthesize cyclic carbonates via photothermal catalysis represents one of the effective strategies for achieving carbon neutrality. In this study, a facile one-step hydrothermal method was employed to synthesize a bimetallic photothermal catalyst FeCo@BPDC. This catalyst demonstrates remarkable efficiency in fixing CO2 to synthesize cyclic carbonates under atmospheric pressure and solvent-free conditions. Through comprehensive characterization and experimentation, the indispensability of bimetallic active sites has been convincingly demonstrated. Additionally, the incorporation of organic ligands significantly enhances the concentration of oxygen vacancies within the catalyst, thereby endowing it with excellent photocatalytic performance. This study presents a novel perspective for the design of photothermal catalysts that convert CO2 into value-added chemicals under mild conditions.
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