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.
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ELECTROCHIMICA ACTA
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2018
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IF 5.116
Yihui Li,Kun Chang,Hongwei Tang,Bao Li,Yalei Qin,Yan Hou,Zhaorong Chang
To address the large structural and volume changes of commercial WO 3 during charge/discharge, which make this material unsuitable for use in Li-ion batteries (LIBs), we herein prepared oxygen deficient WO 3- x nanosheets on a large scale by thermal treatment of ammonium paratungstate in a reducing atmosphere followed by sonication and freeze-drying. The above nanosheets were employed as LIB anode materials and exhibited a specific capacity and cycling stability significantly exceeding those of oxygen-deficient WO 3- x nanoparticles and commercial WO 3 . In addition, we investigated the effect of nanosheet loading on electrode performance, demonstrating that the best results (Li storage capacity of ∼628 mAh g −1 after 100 cycles at 100 mA g −1 ) were obtained at a nanosheet content of 20 wt%. This excellent performance was ascribe to the good exposure of defects caused by the comparatively small size of WO 3- x nanosheets , which resulted in an increased number of sites and diffusion paths available for Li-ion storage and transfer. The novel electrode-optimized strategy may be extended to the fabrication of other electrodes that use nanomaterials as active substances due to its superior comprehensive performance and low cost.
研究领域:
材料科学
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电化学
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纳米材料
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能源存储
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电池技术
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Baoting Tan,Jia Yan,Yiwen You,Xujie Cao,Zhilong Song
Environmental residues of fluoroquinolone antibiotics have become a major threat to both ecosystems and human health, necessitating the development of highly efficient adsorbents with molecular recognition capabilities. This study presents a novel class of WO 3− x quantum wire (QWs) designed to address the limitations of traditional adsorbents, particularly poor selectivity and difficult regeneration processes. We successfully fabricated sub-2 nm ultrathin WO 3− x QWs with enriched with W 5 + /W 6+ active sites and surface functional groups through a precise solvothermal method. The resulting WO 3−x QWs demonstrated exceptional selectivity for fluoroquinolone antibiotics, achieving > 90 % removal efficiency for ciprofloxacin, norfloxacin, and ofloxacin, in contrast to much lower removal rates for common dyes like rhodamine B and methylene blue, as well as other antibiotics like tetracycline hydrochloride. Comprehensive characterizations, including thermodynamic and kinetic models, revealed three key molecular recognition mechanisms driving this high performance. Furthermore, when incorporated into a composite membrane, the QWs demonstrated outstanding performance in continuous filtration, showing high removal efficiency, rapid adsorption, and long-term stability. This study not only provides a new class of efficient adsorbent materials for antibiotic treatment, but also offers fresh insights into the development of functional materials with molecular recognition properties for broader applications.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Wei Wen,Jianru Gao,Man Zhao,Qinyun Yan,Liwu Qiang,Shuai He,Peipei Zhao,Chunmei Liu,Jiamin Ma,Li Zhang,Junming Zhang,He Xiao,Jianfeng Jia
To enhance the kinetic rate of oxygen evolution reaction (OER) in water splitting, a composite (WO 3-x /CNT) of multivalent WO 3-x coupling with carbon nanotube (CNT) is successfully synthesized by a facile electric field-assisted synthesis method. The characterization data indicate that an oxygen bridge structure of W– O –C is formed in WO 3-x /CNT due to strong interaction between WO 3-x and carbon nanotubes. Benefitting from this unique interfacial W– O –C structure, the electronic structure of tungsten sites is regulated through electron-transfer from tungsten atoms to carbon atoms. This obtained electronic structure promotes the intrinsic activity of WO 3-x /CNT and optimizes the adsorption of active OH∗ species. Moreover, the CNT support improves the overall conductivity. The optimal WO 3-x /CNT-2h sample exhibits an overpotential of only 326 mV (without iR compensation) at 10 mA cm −2 , much lower than that of commercial RuO 2 (341 mV). With the introduction of illumination, OER activity on WO 3-x /CNT-2h is tremendously enhanced and the overpotential is reduced to 276 mV at 10 mA cm −2 . This improvement is attributed to photo-generated holes, which creates additional active sites for OER. This work not only encourages the application of novel electrosynthesis methods for designing multivalent metal-based OER electrocatalysts but also highlights the synergistic effect of photoelectricity in enhancing OER performance.
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Surfaces and Interfaces
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2024
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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.
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ACS Applied Materials & Interfaces
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2017
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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.
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PubMed
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CHEMICAL ENGINEERING JOURNAL
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2025
·
IF 13.2
Renzhi Xiong,Yiting Sun,Jiahao Huang,Fangde Liu,Yanhe Xiao,Baochang Cheng,Shuijin Lei
Photocatalytic production of H 2 O 2 faces challenges such as low charge separation efficiency, narrow light absorption, and sluggish reaction kinetics. This study developed a WO 3− x @Zn 3 In 2 S 6− x S-scheme heterojunction and designed atomic-level W S interface chemical bonds through a defect-induced strategy to address these challenges. Oxygen/sulfur vacancies not only promote the formation of chemical bonds but also trigger a local surface plasmon resonance effect (LSPR) in WO 3− x , enabling full-spectrum light harvesting and photothermal heating. The S-scheme charge transfer retains the high-energy electrons in Zn 3 In 2 S 6− x and holes in WO 3− x to realize dual H 2 O 2 generation pathways. Coupled with LSPR-induced thermal activation, this multidimensional strategy achieved an unprecedented H 2 O 2 yield (3891.2 μmol g −1 h −1 ) under simulated sunlight, which is 9.2 times and 161.5 times higher than that of the non-thermally activated pristine Zn 3 In 2 S 6− x and WO 3− x , respectively. In situ X-ray photoelectron spectroscopy and a series of photoelectrochemical measurements confirmed the S-scheme charge dynamics, and electron spin resonance verified the thermally enhanced reactive oxygen species generation. This work establishes defect-mediated heterointerfacial engineering as a universal paradigm for solar-to-chemical energy conversion and provides feasible insights for designing photothermal-assisted photocatalytic systems.
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Catalysis Science & Technology
·
2022
·Vol. 12
·期 22
·6827-6837
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IF 6.177
Penghui Li,Junhua Gao,Jing Shi,Huixiang Wang,Xiangying Xing,Jingzhao Ren,Yu Meng,Liancheng Wang,Baoliang Lv
Linear terminal olefin epoxidation is a significant oxidation reaction for the synthesis of valuable industrial intermediates. As typical olefin epoxidation catalysts, supported tungsten oxides are rich in oxygen vacancies, which have been investigated for improving catalytic performance in other reactions, but the influence on olefin epoxidation is rarely studied. Herein, a series of WO3−x/SBA-15 catalysts with different oxygen vacancy concentrations were obtained by impregnation and sequent hydrogen reduction at 300–600 °C. Their catalytic performances for 1-hexene epoxidation with hydrogen peroxide at 70 °C were studied. It was found that an appropriate concentration of oxygen vacancies could improve epoxidation (the epoxide productivity increased from 135 to 196 μmolepoxide gW−1 min−1) and reduce the apparent activation energy (from 51.6 to 46.9 kJ mol−1). The oxygen vacancies are also beneficial for cycloolefin and other linear olefin epoxidation. In particular, the productivity of cyclooctene oxide was promoted from 4161 to 5744 μmolepoxide gW−1 min−1. This promotion effect was attributed to the increase in the number of Lewis acid sites caused by introducing moderate oxygen vacancies, which could improve the activation of hydrogen peroxide and facilitate epoxidation. In situ FT-IR spectroscopy and density functional theory calculations further indicated that increasing the oxygen vacancies contributes to reducing the energy barrier of the transfer of electrophilic oxygen atoms in active intermediate W–OOH to 1-hexene, thereby promoting epoxidation.
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ENERGY CONVERSION AND MANAGEMENT
·
2021
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IF 9.709
Juan Yang,Pengyu Chen,Jun Dai,Yumei Chen,Liqing Rong,Dazhao Wang
Sunlight-driven photocatalysis is regarded as a promising strategy for direct conversion of methane in low concentration coal mine methane (LC-CMM) to value-added methanol, yet remains a grand challenge to efficiently activate and convert methane. Herein, WO 3−x nanosheets with gradient concentration of oxygen vacancy were synthesized and firstly served as full-spectrum responsive catalysts for transformation of LC-CMM to methanol at ambient conditions. Defect-rich WO 3−x -N2.0 shows a methanol yield of 1475 μmol·g −1 , roughly 4.5 times higher than WO 3 -A2.0 under simulated solar light irradiation. The selectivity of CH 3 OH on the optimal WO 3−x -N2.0 is up to 76%. More importantly, WO 3−x -N2.0 exhibits a methanol yield of 396 μmol·g −1 with the selectivity of 82% even under near infrared light irradiation while almost no CH 3 OH is detected over WO 3 -A2.0. Based on the results of energy-band structure, photoelectrochemical characterization, PLs and EPR tests, the significantly enhanced photocatalytic performance over WO 3−x -N2.0 is ascribed to the synergistic effect caused by the formation of oxygen vacancies, including extending light absorption into NIR region, improving separation of photoinduced electron-hole pairs and boosting production of hydroxyl radicals (key active species that drive CH 3 OH production). This work will offer a sustainable pathway to broaden the utilization of LC-CMM via efficient coupling of solar energy.
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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.
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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.
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DIAMOND AND RELATED MATERIALS
·
2024
·
IF 4.3
Lei Ge,Yingjie Ding,Chaoyang Zhu,Zezhong Xu,Hongdian Lu,Kunhong Hu,Ping Chen,Jinsong Xie
The electrochemical two-electron water oxidation reaction (2e-WOR) offers a promising avenue for hydrogen peroxide (H 2 O 2 ) production. It is crucial to design electrocatalysts with high selectivity, yield, resource abundance, and environmental friendliness. In this paper, as a new generation 2e-WOR electrocatalyst, the WO 3-X /CNTs@carbon fiber membrane nanostructure with abundant oxygen-rich vacancy (O V ) has been discovered by a series of test techniques including XRD, FE-SEM, TEM, FT-IR, Raman and XPS, comprising interconnected carbon nanotubes and carbon fibers enveloped in WO 3 nanorods with oxygen-rich vacancies. By comparing the specific surface area of WO 3-x /CNTs@carbon fiber membrane at different temperatures, it was observed that the maximum value is 44.09 m 2 /g when the mass ratio of AMT to PAN was 3:2 at 600 °C. Furthermore, the WO 3-X /CNTs@carbon fiber membrane can be directly utilized as an independent electrode. The electrochemical performance test revealed that the Faraday efficiency of the WO 3-X /CNTs @CF-600-2 can reach 54 % (2.48 V vs RHE (reversible hydrogen electrode)), while the H 2 O 2 yield can achieve 10.3 μmol· min −1 ·cm −2 , nearly ten times higher than that of pure WO 3 . Furthermore, the stability testing demonstrated that after 12 h, the WO 3-X /CNTs @CF-600-2 exhibited excellent stability with minimal change in its Faraday efficiency. This enhancement is attributed to the improved selectivity of WO 3 , excellent electrical conductivity, and mass transfer performance of carbon fiber. Finally, we proposed a mechanism for 2e-WOR and provided some perspectives on this reaction along with summarizing recent discoveries.
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