CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Zhiliang Jin,Tian Wang,Entian Cui,Xiuli Yang
The construction of heterojunctions is often considered an effective strategy for achieving solar driven photocatalytic decomposition of water. Graphdiyne has unique properties such as highly π conjugated structure, ideal direct bandgap, and high charge carrier mobility, making it a candidate for ideal photocatalysts. In this work, a graphdiyne based composite catalyst GDY-Cu with ohmic contact interface was prepared through organic synthesis. Subsequently, a S-scheme heterojunction was constructed between the contact interface of WO 3 nanorods with surface defects and GDY-Cu samples to promote electron transfer. The hydrogen evolution ability of GDY-Cu/WO 3 samples with different ratios was studied by adjusting the addition amount of GDY-Cu. In addition, GDY-Cu/WO 3 samples exhibits the highest photocatalytic hydrogen evolution activity, reaching 12.2 times that of pure GDY. In fact, the joint construction of Ohmic junctions and S-scheme heterojunctions provides a unique transport pathway for electron transfer. The built-in electric field between interfaces provides power for electron migration. Importantly, in-depth research on in-situ XPS and density functional theory calculations has confirmed the charge transfer pathway. Thorough charge dynamics analysis of the migration ability of photo generated charge carriers. This work not only enriches the photocatalytic system by integrating Ohmic junctions and S-scheme heterojunctions, but also provides a new design strategy for constructing graphdiyne based materials.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Linlin Fan,Yimin Wang,Xin Guo,Zhiliang Jin
Photocatalytic hydrogen production technology has great challenges in designing and synthesizing stable photocatalyst and inhibiting high recombination rate of carriers. In this paper, CoMoO 4 /GDY type-II heterojunctions were successfully constructed by coupling a new two-dimensional layered carbon material graphdiyne (GDY) with molybdate (CoMoO 4 ), and the positive effect of GDY on photocatalytic hydrogen production system was studied. The introduction of GDY provides a large number of reaction sites for the reaction. Moreover, due to the strong light absorption and excellent electrical conductivity of GDY, the photoelectrochemical properties of molybdate (CoMoO 4 ) are enhanced. The construction of type-II heterojunctions effectively promotes the spatial separation of photogenerated electrons and holes. The electron transfer mechanism of the photocatalyst was verified based on DFT and in-situ irradiation X-ray photoelectron spectroscopy. The experimental results show that the photocatalytic performance of CoMoO 4 /GDY photocatalyst is the best (121 μmol), which is 2 times and 45 times that of CoMoO 4 and GDY, respectively. This study provides a unique idea for the application of GDY in the field of photocatalysis.
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OPTICS EXPRESS
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2023
·Vol. 31
·期 25
·42637-42650
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IF 3.8
Jinjian Yu,Jinjian Yu,Piliang Liu,Piliang Liu,Yaxun Zhang,Yaxun Zhang,Qianran Sun,Qianran Sun,Yu Zhang,Zhihai Liu,Libo Yuan,Xiaoyun Tang,Xiaoyun Tang,Xiaoyun Tang
In the context of optical fiber humidity sensing, the long-term stability of sensors in high humidity and dew environments such as bathrooms or marine climates remains a challenge, especially since many humidity sensitive materials are water soluble. In this study, we use methyldiethanolamine, pentaerythritol triacrylate and Eosin Y to form a liquid-solid structure humidity sensitive component, the outermost layer is coated with PDMS passivating layer to ensure the stability and durability of the humidity sensor under the conditions of dew and high humidity. The liquid microcavity of the sensor consists of methyldiethanolamine-pentaerythritol triacrylate composite solution, and the sensitivity is several times higher than that of the liquid-free cavity sensor. The sensitivity of the sensor to temperature is verified (0.43 nm/°C and 0.30 nm/°C, respectively) and temperature crosstalk is compensated using a matrix. The compact structure allows for ultra-fast response (602 ms) and recovery time (349 ms). Our work provides a promising platform for efficient and practical humidity and other gas monitoring systems.
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Journal of Environmental Chemical Engineering
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2023
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IF 7.7
Baiyu Chen,Man Zhang,Kaili Yao,Churu Zhang,Qi Wu,Tianding Hu,Shaoyun Shan
Metal-organic frameworks (MOFs) have attracted exciting application prospects in photocatalytic hydrogen (H 2 ) evolution due to the diversity of organic ligands and metal ions . However, the inappropriate conduction band position of pristine MOFs and corresponding large overpotential for H 2 evolution restrict the H 2 production under visible light. Herein, a dye-sensitized NH 2 -UiO-66 anchored with copper ions (EY-6Cu-NU-66) was synthesized by in-situ Cu anchoring followed by Eosin Y sensitization. The H 2 production activity showed that EY-6Cu-NU-66 reached 3579.82 μmol·g −1 ·h −1 under visible light, which was four times higher than that of dye-sensitized pristine NU-66 (EY-NU-66) and 99-fold higher than that of 6Cu-NU-66 free of dye sensitization. A series of characterizations and theoretical computations indicated that photo-generated electrons first transfer from the excited Eosin Y to the lowest unoccupied molecular orbital (LUMO) of the NU-66, then further transfer to the transition Cu II /Cu I metal center that is formed by Cu anchored on -NH 2 . This tandem mechanism not only improves the visible-light absorption ability of NU-66 but also promotes its separation efficiency of photo-generated carriers, thus greatly reducing the overpotential for H 2 evolution. This work provides a new strategy for visible-light-driven H 2 production by dye-sensitized MOF-based materials without noble metal loading.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Jiayi Wu,Qin Liu,Yan Wang
Thin film composite (TFC) membranes are commonly used for organic solvent nanofiltration (OSN) application. However, these membranes normally suffer from the layer delamination under harsh conditions. Chemically integral crosslinking is a common method to address this problem, but the resultant tightened polymeric chains and denser microstructure will inevitably bring the reduced solvent permeance. In this work, a facile metal integral crosslinking strategy, which has minimal adverse effect on the solvent permeance, was developed to improve the tolerance to the majority of organic solvents as well as enhance the adhesions of upper selective layers and underlying substrates simultaneously for the first time. The as-developed Cu 2+ integrally-crosslinked membranes demonstrated a high permeance for organic solvents and a high rejection towards rose bengal. In comparison to the Cu 2+ partially-crosslinked membranes (with substrate crosslinked only), the integrally-crosslinked ones exhibited superior solvent resistance and OSN performance. This improvement was attributed to the enhanced interactions and a defect-free PA layer. Additionally, the effects of solvent activation, crosslinking solution concentration as well as crosslinking time were also studied. It is believed that metal integral crosslinking strategy will offer a novel approach to develop promising TFC membranes with satisfactory OSN performance for practical applications.
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JOURNAL OF RARE EARTHS
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2023
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IF 4.9
Shiyong Xu,Mei Li,Yijun Wang,Caiyun Gao,Rongsheng Xu,Zhiliang Jin
A novel composite photocatalyst for photocatalytic decomposition of water for hydrogen evolution was successfully synthesized by in-situ growth of nitrogen and sulfur co-doped coal-based carbon quantum dots (NSCQDs) nanoparticles on the surface of sheet cobalt-based metal-organic framework (Co-MOF) and graphitic carbon nitride (g-C 3 N 4 , CN). The structure and properties of the obtained catalysts were systematically analyzed. NSCQDs effectively broaden the absorption of Co-MOF and CN in the visible region. The new composite photocatalyst has high hydrogen production activity and the hydrogen production rate reaches 6254 μmol/(g·h) at pH = 9. At the same time, NSCQDs synergy Co-MOF/CN composites have good stability. After four cycles of hydrogen production, the performance remains relatively stable. The transient photocurrent response and Nyquist plot experimental results further demonstrate the improvement of carrier separation efficiency in composite catalysts. The semiconductor type (n-type semiconductor) of the single-phase catalyst was determined by the Mott-Schottky test, and the band structure was analyzed. The conductive and valence bands of CN are −0.99 and 1.72 eV, respectively, and the conduction and valence bands of Co-MOF are −1.85 and 1.33 eV, respectively. The mechanism of the photocatalytic reaction can be inferred, that is, Z-type heterojunction is formed between CN and Co-MOF, and NSCQDs was used as cocatalyst.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-13
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IF 16.6
Xie Yifan,Feng Shuo,Deng Linxiao,Cai Aoran,Gan Liyu,Jiang Zifan,Yang Peng,Ye Guilin,Liu Zaiqing,Wen Li,Zhu Qing,Zhang Wanjun,Zhang Zhanpeng,Li Jiahe,Feng Zeyu,Zhang Chutian,Du Wenjie,Xu Lixin,Jiang Jun,Chen Xin,Zou Gang
Artificial chiral materials and nanostructures with strong and tuneable chiroptical activities, including sign, magnitude, and wavelength distribution, are useful owing to their potential applications in chiral sensing, enantioselective catalysis, and chiroptical devices. Thus, the inverse design and customized manufacturing of these materials is highly desirable. Here, we use an artificial intelligence (AI) guided robotic chemist to accurately predict chiroptical activities from the experimental absorption spectra and structure/process parameters, and generate chiral films with targeted chiroptical activities across the full visible spectrum. The robotic AI-chemist carries out the entire process, including chiral film construction, characterization, and testing. A machine learned reverse design model using spectrum embedded descriptors is developed to predict optimal structure/process parameters for any targeted chiroptical property. A series of chiral films with a dissymmetry factor as high as 1.9 ( g abs ~ 1.9) are identified out of more than 100 million possible structures, and their feasible application in circular polarization-selective color filters for multiplex laser display and switchable circularly polarized (CP) luminescence is demonstrated. Our findings not only provide chiral films with the highest reported chiroptical activity, but also have great fundamental value for the inverse design of chiroptical materials.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2023
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IF 7.2
Shiyong Xu,Mei Li,Yijun Wang,Zhiliang Jin
In pursuit of exploring functional applications of coal, this study ultrasound-assisted hydrogen peroxide was used to transform cheap coal into environmentally friendly and high-value coal-based carbon quantum dots (CQDs). These CQDs are then harnessed to synergistically assist the photocatalytic water splitting for hydrogen evolution , in collaboration with CoMoO 4 (CM) and g-C 3 N 4 (CN). The results indicated that the novel composite photocatalyst , CMCN-11/8%SCQDs, exhibited high hydrogen evolution activity, reaching a maximum hydrogen production rate of 4916.63 μmol g −1 h −1 at pH 9. At a wavelength of 420 nm, the apparent quantum efficiency (AQE) was 1.78%. The conduction and valence band positions of CM were determined to be −1.03 eV and 1.65 eV, respectively, while those of CN were −0.83 eV and 1.72 eV, suggesting the formation of an S-type heterojunction between CM and CN. The significant role of SCQDs in enhancing the photocatalytic hydrogen evolution was extensively investigated, demonstrating that the synergistic effect between SCQDs, CM, and CN could enhance the hydrogen evolution activity. SCQDs exhibited excellent electron transfer capabilities, serving as bridges for electron transport, functioning both as electron acceptors and donors, effectively impeding the rapid recombination of electron-hole pairs and enhancing their separation efficiency. This study provides crucial insights into the utilization of coal-based CQDs for photocatalytic water splitting, offering an economically viable and sustainable option for the functional application of coal and opening new avenues for the rational design of efficient and cost-effective photocatalysts.
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Therapeutic Advances in Gastroenterology
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2021
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IF 4.409
Fenghua Xu,Yi Cheng,Guangcong Ruan,Liqin Fan,Yuting Tian,Zhifeng Xiao,Dongfeng Chen,Yanling Wei
Background: The community of gut microbes is a key factor controlling the intestinal barrier that communicates with the nervous system through the gut-brain axis. Based on our clinical data showing that populations of Roseburia intestinalis are dramatically decreased in the gut of patients with ulcerative colitis, we studied the efficacy of a strain belonging to this species in the context of colitis and stress using animal models. Methods: Dextran sulfate sodium was used to induce colitis in rats, which then underwent an enema with R. intestinalis as a treatment. The disease activity index, fecal changes and body weight of rats were recorded to evaluate colitis, while histological and immunohistochemical analyses were carried out to examine colon function, and 16S rRNA sequencing was performed to evaluate the gut microbiota change. Behavioral assays and immunohistochemical staining of brain were performed to assess the effect of R. intestinalis on the gut-brain axis. Results: Colitis-related symptoms in rats were significantly relieved after R. intestinalis enema, and the stool traits and colon length of rats were significantly recovered after treatment. The gut epithelial integrity and intestinal barrier were restored in treated rats, as evidenced by the higher expression of Zo-1 in colon tissues, accompanied by the restoration of gut microbiota. Meanwhile, depressive-like behaviors of rats were reduced after treatment, and laboratory experiments on neuronal cells also showed that IL-6, IL-7 and 5-HT were downregulated by R. intestinalis treatment in both serum and brain tissue, while Iba-1 expression was reduced in treated rats. Conclusions: The administration of R. intestinalis contributes to restoration of the gut microbiota, promoting colon repair and the recovery of gastrointestinal function. These alterations are accompanied by the relief of depressive-like behaviors through a process modulated by the neuronal network and the regulation of inflammation by the gut-brain axis.
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JOURNAL OF MOLECULAR LIQUIDS
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2021
·
IF 6.165
Yue Sun,Minting Zou,Changyi Li,Xiaoran Li,Taoyan Mao,Cheng Zheng
Due to the benign features of biosurfactants such as their low toxicity and desirable biodegradability, there has been growing interest in developing these materials for environmental remediation applications. In this work, the relationship between the temperature and the solubilization of tea saponin was investigated via critical micelle concentration (CMC), particle size, and thermodynamics measurements. In addition, the aqueous solubility enhancements of naphthalene provided by micellar solutions of biosurfactants (tea saponin) and a synthetic surfactant (Tween 80) were measured and compared. Results indicated that the solubilization effect of tea saponin increased as the temperature was elevated from 298 to 313 K, which thus indicated that this effect had a strong dependence on temperature. An increase in the temperature also led to a lower CMC value, an increase of the particle diameter, and an enhancement of the molecular activity, which thus led to the enhanced solubilization effect of tea saponin. Moreover, the solubilization effect of tea saponin was better than that provided by Tween 80. The results confirmed the potential applicability of tea saponin for enhanced remediation of naphthalene.
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JOURNAL OF MEMBRANE SCIENCE
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2020
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IF 7.183
Yang Yang,Zhu Xiong,Zhu Wang,Yi Liu,Zijun He,Akun Cao,Li Zhou,Lijing Zhu,Shuaifei Zhao
Carbon nanotube (CNT) based adsorbents have attracted extensive research interest for aqueous pollutants removal. However, such adsorbents face the problems of limited adsorption capacities and costly regeneration. Here, we report a highly adsorptive photo-regenerable CNT based multifunctional membrane with excellent self-cleaning properties via the facile vacuum filtration method, followed by FeOOH in-situ anchoring and silver-amino reaction. Various dyes (Rhodamine B, methylene blue, eosin Y and acid orange 7) and emerging contaminants (bisphenol A, amoxicillin and p-nitrophenol) were tested with the CNT based membrane. Our membrane exhibited superior adsorption performance to dyes among CNT based adsorbents reported in literature. In particular, the CNT based composite membrane displayed even better adsorption performance to cationic dyes. The adsorption capacities of the membrane for Rhodamine B and methylene blue were up to 181 and 247 mg/g, respectively. The membrane also had excellent self-cleaning and photo-regenerable properties after severe organic fouling. Our multifunctional CNT based membrane combined the features of adsorption, membrane separation , and catalytic degradation into one system, showing great promise for dye polluted wastewater purification. This study also offers a new strategy to engineer robust adsorptive, self-cleaning and regenerable membranes for wastewater treatment .
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ChemSusChem
·
2020
·Vol. 13
·期 21
·5711-5721
·
IF 7.962
Fengliang Wang,Linghan Xiao,Jianmin Chen,Liyu Chen,Ruiqi Fang,Yingwei Li
Graphical Self-templated strategy : This work reports a self-templated strategy for the preparation of carbon-doped CuO hollow spheres (C−CuO HSs) featuring both modulated electronic structure and high water-adsorption capability through thermal transformation of a hierarchical MOF. The as-synthesized C−CuO HSs exhibits remarkable photocatalytic performance with a H 2 evolution rate of 67.3 mmol/g/h and an apparent quantum efficiency of 25.3 %. Copper(II) oxide featuring a narrow bandgap and low toxicity has been frequently applied in the visible-light-driven photocatalytic hydrogen evolution, but it suffers from large intrinsic overpotential and low water adsorption capacity. Herein, we report a self-templated strategy for the preparation of carbon-doped CuO hollow spheres (C−CuO HSs) through thermal transformation of a hierarchical MOF. The hierarchical Cu−MOFs not only act as a template to form interior voids during the thermal transformation, but also serve as precursors to dope C atoms into the CuO lattice. The as-synthesized C−CuO HSs exhibits remarkable photocatalytic performance with a H 2 evolution rate of 67.3 mmol/g/h and the apparent quantum efficiency of 25.3 % at 520 nm in the present of eosin-Y photosensitizer. The high performance of C−CuO HSs is attributed to the hierarchical porous structure and modulated electronic structure of CuO by C-doping with well exposed reactive sites, high water adsorption capability, and low water reduction reaction barrier. The results presented in this work might shed light on the design of high-performance photocatalysts for various energy-related applications.
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