CHINESE JOURNAL OF CHEMICAL PHYSICS
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2023
·Vol. 36
·期 1
·113-124
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IF 1
Xiao He,Gao Jian-ru,Zhao Man,Cheng Xiao-ru,Xue Shou-feng,Wang Xiao-xia,Chen Wen-wen,Jia Jian-feng,Wu Hai-shun
Integration of non-noble transition metal oxides with graphene is known to construct high-activity electrocatalysts for oxygen evolution reduction (OER). In order to avoid the complexity of traditional synthesis process, a facile electrochemical method is elaborately designed to engineer efficient WO 3- x /graphene (photo-)electrocatalyst for OER by a two-electrode electrolysis system, where graphite cathode is exfoliated into graphene and tungsten wire anode evolves into VO-rich WO 3- x profiting from formed reductive electrolyte solution. Among as-prepared samples, WO 3- x /G-2 shows the best electrocatalytic performance for OER with an overpotential of 320 mV (without iR compensation) at 10 mA/cm 2 , superior to commercial RuO 2 (341 mV). With introduction of light illumination, the activity of WO 3- x /G-2 is greatly enhanced and its overpotential decreases to 290 mV, benefiting from additional reaction path produced by photocurrent effect and extra active sites generated by photogenerated carriers (h+). Characterization results indicate that both VO-rich WO 3- x and graphene contribute to the efficient OER performance. The activity of WO 3- x for OER is decided by the synergistic effect between VO concentration and particle size. The graphene could not only disperse WO 3- x nanoparticles, but also improve the holistic conductivity and promote electron transmission. This work supports a novel method for engineering WO 3- x /graphene composite for highly efficient (photo-)electrocatalytic performance for OER.
研究领域:
材料科学
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电化学
·
可再生能源
✓ 已验证
DOI
高影响因子
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2024
·
IF 4.3
Qinli Ye,Miaomiao Wu,Qian Xu,Shuwen Zeng,Tao Jiang,Wei Xiong,Songyin Fu,Muhammad Danang Birowosuto,Chenjie Gu
The Surface-enhanced Raman scattering (SERS) is an attractive optical detecting method with high sensitivity and detectivity, however challenges on large-area signal uniformity and complex spectra analysis methods always retards its wide application. Herein, a highly sensitive and uniform SERS detection strategy supported by porous carbon film/WO 3-x nanosheets (PorC/WO 3-x ) based noble-metal-free SERS substrate and deep learning algorithm are reported. Experimentally, the PorC/WO 3-x substrate was prepared by high-temperature annealing the PorC/WO 3 films under the argon atmosphere. The defect density of the WO 3 was controlled by tuning the reducing reaction time during the annealing process. The SERS performance was evaluated by using R6G as the Raman reporter, it showed that the SERS intensity obtained on the substrate with the optimal annealing time of 3 h was about 8 times as high as that obtained on the PorC/WO 3 substrate without annealing treatment. And detection limit of 10 -7 M and Raman enhancement factor of 10 6 could be achieved. Moreover, the above optimal SERS substrate was utilized to detect flavonoids of quercetin, 3-hydroxyflavone and flavone, and a deep learning algorithms was incorporated to identify the quercetin. It revealed that quercetin can be accurately detected within the above flavonoids, and lowest detectable concentration of 10 -5 M can be achieved.
研究领域:
材料科学
·
分析化学
·
光学
·
机器学习
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Surfaces and Interfaces
·
2024
·
IF 5.7
Fengyun Su,Mengzhen Tian,Hailong Cao,Zhishuai Wang,Qiang Zhao,Haiquan Xie,Yezhen Zhang,Xiaoli Jin,Xin Li,Zhengdao Li
Semiconductor-based photocatalytic water splitting enables the conversion of abundant solar energy to green and renewable hydrogen energy. Graphitic carbon nitride (g-C 3 N 4 ) is synthesized using a straightforward method, demonstrating stable physicochemical properties and possessing an optimal bandgap, thus positioning it as a promising photocatalyst in the realm of environmental sustainability. Oxygen vacancies are extensively employed to modulate light absorption and surface properties of metal-oxide semiconductors. In this study, g-C 3 N 4 nanosheets were coupled with oxygen-deficient tungsten trioxide (WO 3-x ) to form heterojunction photocatalysts ( X -WOCN). Comprehensive material characterization results demonstrated that the constructed heterojunction extended the visible light absorption range, improved photogenerated electron-hole separation efficiency, and thus augmented photocatalytic activity . Notably, the optimum hydrogen evolution rate of 6 %-WOCN was enhanced by 5.4-fold compared to that of g-C 3 N 4 . Furthermore, we propose a Z-scheme heterojunction charge separation mechanism mediated by oxygen defects and support this mechanism through detection of surface-active substances •O 2 − and •OH. This study offers novel propositions into the function of oxygen defects in facilitating charge separation within Z-scheme heterojunction.
研究领域:
光催化
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材料化学
·
能源科学
·
半导体物理
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环境可持续性
·
纳米材料
✓ 已验证
DOI
高影响因子
Small
·
2025
·
IF 12.1
Qi Wu,Mingyang Liu,Hui Zhang,Guanghao Li,Ziqing Yang,Xiaodan Wu,Guanghui Tan,Chenfeng Ji,Yingxue Jin
At present, tumor immune escape is a major problem in the treatment of tumors. The complex network of tumor microenvironments significantly impairs the efficacy of immunotherapy. This paper reports the preparation and immunoantitumor activity of a novel multifunctional defect tungsten trioxide@ferrocene-folic acid composite (WO 3-x @Fe-FA) with a high Fenton reaction rate. Ferrocene is modified on the surface of defective trioxide by the covalent coupling method for the first time, and the reaction rate of Fenton is increased by 10 times. WO 3-x @Fe-FA induces immunogenic cell death (ICD) through the powerful synergistic anti-tumor effect of PTT/CDT and decomposes H 2 O 2 to produce oxygen through the Fenton reaction, thus down-regulating the expression of immune checkpoint PD-L1 induced by tumor hypoxia. In vitro and in vivo experiments proved that WO 3-x @Fe-FA reverses the immunosuppressive tumor microenvironment, transforms the immunosuppressive “cold tumor” into the immune “hot tumor”, and activates the immune activity of the system. In vitro and in vivo experiments show that WO 3-x @Fe-FA has excellent immunoantitumor activity, and it is expected to be a candidate drug for immunoantitumor therapy.
研究领域:
肿瘤学
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免疫学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
LANGMUIR
·
2023
·
IF 3.9
Xingrui Qi,Jiamin Gan,Zhidong Zhao,Nian Li,Yufang Chen,Tao Jin
One of the potential treatments for bacterial wound infections is photodynamic therapy. WO3–x semiconductor materials can generate reactive oxygen species when exposed to light, which can inactivate bacteria. In this work, we improved their photocatalytic performance by doping WO3–x with Cu. The wound dressing was prepared by loading Cu–WO3–x into a highly biocompatible chitosan sponge. The composite sponge dressing showed significant inactivation of Escherichia coli and Staphylococcus aureus, and in vitro toxicity assays on L929 cells demonstrated the biosafety of the dressing. Through in vivo wound healing trials, composite sponge dressings have been shown to accelerate wound healing, and this composite chitosan sponge can be possibly used for photodynamic therapy of bacterial wound infections.
研究领域:
材料科学
·
生物医学工程
·
光催化
·
伤口护理
✓ 已验证
产品关联
DOI
PubMed
高影响因子
NANOTECHNOLOGY
·
2019
·Vol. 30
·期 25
·255703
·
IF 3.399
Ning Li,Xun Cao,Tianci Chang,Shiwei Long,Ping Jin
Pursuing excellent photochromic (PC) properties is still a longstanding challenge for energy-efficient smart coatings. Herein, we have prepared a novel series of self-coated crystalline WO3-amorphous WO3−x homojunctions by a one-step hydrothermal process, in which oxalic acid was used as a capping agent to prevent polycondensation and the crystallization of [WO6]. The as-prepared nanopowders with tight interfaces have a large specific surface area and rich surface electrons, which leads to a dramatic PC property reaching up to ΔTsol = 64.74% at the near-infrared (NIR) range of 1000–2600 nm with high luminous transmittance (Tlum = 94.6% in the virgin state and Tlum = 32.47% in the colored state). Meanwhile, the as-prepared crystalline WO3-amorphous WO3−x homojunction reveals fast reversible PC circulation; most particularly, the self-bleaching rate increases at least three times—the self-bleaching time is less than 8 h. Moreover, as the microstructure of the homojunction is tuned, the solar modulation range can be selective and tuned, so that the solar modulation efficiency is up to the best energy-saving state by controlling the main absorption according to the solar energy distribution.
研究领域:
材料科学
·
能源科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Ying Chen,Li Wang,Ruijie Gao,Yong-Chao Zhang,Lun Pan,Chenyu Huang,Kan Liu,Xin-Yuan Chang,Xiangwen Zhang,Ji-Jun Zou
Photosynthesis with Z-scheme charge transfer has been recognized as an efficient pathway to achieve solar-energy conversion. Herein, the all-solid-state direct Z-scheme ZnO-WO 3-x nanorod arrays were synthesized by in-situ solvothermal treatment for highly piezoelectric (PE)-photoelectrochemical (PEC) water splitting. The chemical bonding between WO 3-x and ZnO via W-O-Zn and the inherent band structures/Fermi levels drive the formation of direct Z-scheme charge-transfer pathway. Importantly, the optimized structure (Zn-W-5) shows higher PEC activities with high photocurrent density of 2.39 mA/cm 2 at 1.23 V vs. RHE, which is 2.13 times higher than pure ZnO. Surprisingly, the obvious PE polarization of ZnO increases its Fermi level toward conduction band and significantly enhances Z-scheme effect between ZnO and WO 3-x . Especially, the best sample (Zn-W-5-1000 rpm) shows a photocurrent of 3.38 mA/cm 2 at 1.23 V vs. RHE, which is 3.02 times higher than pure ZnO. This work provides a facile PE polarization approach for enhancement of Z-scheme charge-transfer process.
研究领域:
材料科学
·
纳米技术
·
电化学
·
可再生能源
·
光化学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Ling Cheng,Xianglong Yang,Xiaomei Chen,Chunling Lv,Jin Mao,Qi Zhang,Peiwu Li
A surface oxygen vacancy-engineered WO 3-x film with enhanced photoelectrocatalytic (PEC) activity for the detoxification of deoxynivalenol (DON) was successfully synthesized via an improved sol-gel method. The presence of oxygen vacancy was verified by high-resolution transmission electron microscopy, X-ray photoelectron spectroscopy, X-ray diffraction, Raman spectra and electron spin resonance spectroscopy. The introduction of oxygen vacancy into WO 3-x film substantially enhanced its absorption in visible region, and facilitated its transfer and separation of photogenerated charges. This made the WO 3-x film to have excellent PEC activity for the detoxification of DON under visible light illumination at a low bias of +0.3 V. The percentage of DON removed was up to 86.4 % after being treated with PEC for 2 h. When the bias potential applied was further increased, there were no obvious changes in the degradation efficiency of the film. The cell viabilities were dramatically enhanced with prolonged time, which were over 95 % after 2 h PEC treatment compared to the control. Through the analysis of eight intermediates that were separated and identified by high performance liquid chromatography-mass spectrometry, it can be concluded that the reduction of DON and the cleavage of double bond at C9 C10, epoxy group at C12 13 and hydroxyl group at C3 in DON could greatly reduce the toxicity, and the detoxification mechanism of this PEC system was proposed. This work can provide further insights into DON detoxification using PEC system with low bias.
研究领域:
环境科学
·
材料科学
·
毒理学
·
分析化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2017
·
IF 7.504
Jian Huang,Dayan Ma,Feng Chen,Dongzhen Chen,Min Bai,Kewei Xu,Yongxi Zhao
Surface-enhanced Raman scattering (SERS) has proven to be an effective technique for identifying and providing fingerprint structural information on various analytes in low concentration. However, this analytical technique has been plagued by the ubiquitous presence of organic contaminants on roughened SERS substrate surfaces, which not only often result in poorer detection sensitivity but also significantly affect the reproducibility and accuracy of SERS analysis. Herein, we developed a clean, stable, and recyclable three-dimensional (3D) chestnutlike Ag/WO3–x (0 < x < 0.28) SERS substrate by simple hydrothermal reaction and subsequent green in situ decoration of silver nanoparticles. None of the organic additives were used in synthesis, which ensures the substrate surfaces are completely clean and free of interferences from impurities. The innovative design combines the SERS enhancement effect and self-cleaning property, making it a multifunctional and reusable SERS platform for highly sensitive SERS detection. Using malachite green as a model target, the as-prepared SERS substrates exhibited good reproducibility (relative standard deviation of 7.5%) and pushed the detection limit down to 0.29 pM. The enhancement factor was found to be as high as 1.4 × 107 based on the analysis of 4-aminothiophenol. The excellent regeneration performance indicated that the 3D biomimetic SERS substrates can be reused many times. In addition, the fabricated substrate was successfully employed for detecting thiram in water with a detection limit of 0.32 nM, and a good linear relationship was obtained between the logarithmic intensities and the logarithmic concentrations of thiram ranging from 1 nM to 1 μM. More importantly, the resultant SERS-active colloid can be used for accurate and reliable determination of thiram in real fruit peels. These results predict that the proposed SERS system have great potential toward rapid, reliable, and on-site analysis, especially for food safety and environmental supervision.
研究领域:
材料科学
·
分析化学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nanoscale Advances
·
2019
·Vol. 1
·期 10
·3941-3947
·
IF 0
Xiao Li,Yucong Yan,Yi Jiang,Xingqiao Wu,Shi Li,Jingbo Huang,Junjie Li,Yangfan Lin,Deren Yang,Hui Zhang
Hydrolysis of ammonia borane (AB) is a safe and convenient means of H2 production when efficient catalysts are used. Here we report a facile one-pot solvothermal method to synthesize Rh/WO3−x hybrid nanowires. Ultra-small Rh nanoparticles with an average size of ∼1.7 nm were tightly anchored on WO3−x nanowires. Rh/WO3−x catalysts exhibited substantially enhanced activity for hydrolytic dehydrogenation of AB under both dark and visible light irradiation conditions relative to mixed Rh nanoparticles and WO3−x nanowires (Rh + WO3−x), and Rh/C and WO3−x nanowires. X-ray photoelectron spectroscopy (XPS) analysis indicated that the synergistic effect between Rh nanoparticles and WO3−x nanowires was responsible for such an enhancement in activity. Specifically, Rh/WO3−x achieved the highest turnover frequency (TOF) with a value of 805.0 molH2 molRh−1 min−1 at room temperature under visible light irradiation. The H2 release rate as a function of reaction time exhibited a volcano plot under visible light irradiation, indicating that a self-activation process occurred in the hydrolytic dehydrogenation of AB due to additional oxygen vacancies arising from in situ reduction of WO3−x nanowires by AB, and thus an enhanced localized surface plasmon resonance (LSPR). Such a self-activation process was responsible for the enhanced catalytic activity under visible light irradiation relative to that under dark conditions, which was supported by the lower activation energy (45.2 vs. 50.5 kJ mol−1). In addition, Rh/WO3−x catalysts were relatively stable with only little loss in activity after five cycles due to the tight attachment between two components.
研究领域:
催化
·
材料科学
·
纳米技术
·
化学工程
·
光化学
✓ 已验证
产品关联
DOI
PubMed
ANALYTICAL CHEMISTRY
·
2024
·
IF 6.7
Yanni Luo,Caiying Li,Fanggui Ye,Jianniao Tian,Xuecai Tan,Shengqiang Hu,Shulin Zhao
A disease-targeting nanoplatform that integrates imaging with therapeutic activity would facilitate early diagnosis, treatment, and therapeutic monitoring. To this end, a macrophage membrane-coated Cu–WO3–x-Hydro820 (CWHM) nanoreactor was prepared. This reactor was shown to target inflammatory tissues. The reactive oxygen species (ROS) such as H2O2 and ·OH in inflammatory tissues can react with Hydro820 in the reactor to form the NIR fluorophore IR820. This process allowed photoacoustic/fluorescence dual-mode imaging of H2O2 and ·OH, and it is expected to permit visual diagnosis of inflammatory diseases. The Cu–WO3–x nanoparticles within the nanoreactor shown catalase and superoxide enzyme mimetic activity, allowing the nanoreactor to catalyze the decomposition of H2O2 and ·O2– in inflammatory cells of hepatic tissues in a mouse model of liver injury, thus alleviating the oxidative stress of damaged liver tissue. This nanoreactor illustrates a new strategy for the diagnosis and treatment of hepatitis and inflammatory liver injury.
研究领域:
纳米技术
·
生物医学工程
·
医学成像
·
诊疗一体化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2025
·
IF 3.7
Hui Guo,Shaoshuang Zhu,Zhenghan Zhang,Lu Pan,Huimin Jiang,Nasir A. Siddiqui,Aslam Khan,Jianjian Lin
Constructing non-precious metal electrocatalysts with good hydrogen evolution activity is crucial for the hydrogen evolution reaction (HER) in acidic media. The synergistic optimization of the water dissociation and hydrogen desorption steps presents a challenge for the HER. Here, we have synthesized phosphorus-doped tungsten trioxide with oxygen vacancies (P-WO3-x) using a simple but effective hydrothermal reaction followed by calcination annealing. Interestingly, the P-WO3-x material exhibits unique characteristics that set it apart from conventional tungsten oxide-based electrocatalysts. The introduction of oxygen vacancies and phosphorus doping creates an optimal structure that significantly improves the electronic properties and the catalytic sites. The oxygen vacancies enhance the material’s ability to adsorb and activate water molecules, while phosphorus doping further modifies the electronic structure, facilitating more efficient hydrogen desorption. Meanwhile, the catalyst demonstrates a favorable urchin-like morphology with excellent supportability. Remarkably, the P-WO3-x electrocatalyst demonstrates excellent HER performance and excellent durability. We indicate that P-WO3-x exhibits a small overpotential (155.42 mV at -10 mA cm-2), a low Tafel slope (74.97 mV dec-1), and excellent durability over 12 hours. This work presents a significant advance for the development of tungsten oxide-based electrocatalysts with anion doping and oxygen vacancies for HER in acidic media.
研究领域:
材料科学
·
电催化
·
能源化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）