ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Wenqing Hou,Chen Chen,Diya Xie,Yiming Xu
Metal–organic frameworks (MOFs) as photocatalysts have received increasing attention. In this work, a dual metal-substituted UiO-66-NH2 (Ti/Ce-MOF) containing different Ti/Ce mole ratios (x = 0–2.46) has been prepared via post-synthetic exchange between Ce-UiO-66 and TiCl4, followed by amination. The solid had a high surface area (828–937 m2/g) and a large pore volume (0.451–0.507 m3/g). Under visible light, Ti/Ce-MOF showed x-dependent activity for H2O reduction and oxidation on a film electrode, respectively. However, such a change for H2 evolution in a Na2S/Na2SO3 aqueous solution was observed only after CdS loading. In combination with the photoluminescence and band parameters, we propose that the photoactivity of Ti/Ce-MOF for redox reaction is determined by its ability for electron transfer. Furthermore, there is an interfacial electron transfer from Ti/Ce-MOF to CdS and a hole transfer from CdS to Ti/Ce-MOF, respectively, significantly improving the efficiency of charge separation for redox reactions. This work offers a new insight that Ti substitution benefits the performance of Ce-based MOF.
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RSC Advances
·
2023
·Vol. 13
·期 37
·25681-25690
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IF 3.9
Jie Liang,Ting Fan,Jian-tao Lü,Tianjie Guan,Ting-ting Deng,Bangyun Xiong
NaGdF4:Ce,Eu,Tb nanocrystals were successfully prepared by a one-step hydrothermal method with Ce3+ ions as sensitizers, Eu3+ and Tb3+ ions as activators, and polyethylenimine (PEI) as surfactants. Color-adjustable fluorescence emission was achieved by the energy transfer effect between rare earth ions. Blue fluorescent carbon quantum dots (CDs) with a double UV response under 254 nm and 365 nm excitation were synthesized by a one-step hydrothermal method. A hydrophilic NaGdF4:Ce,Eu,Tb/CD composite ink was prepared by an easy physical mixing method. Because of the electrostatic self-assembly effect, the color adjustable luminescence was achieved in a few seconds, and the white light emission with color coordinates of (0.32, 0.32) was obtained. A dual-mode luminescence anti-counterfeiting pattern was designed and achieved by excitation with ultraviolet light at 254 nm and 365 nm.
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DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 32
·11076-11084
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IF 4
Zhuoyou Gao,Mengying Wang,Ningzhao Shang,Wei Gao,Xiang Cheng,Shutao Gao,Yongjun Gao,Chun Wang
Hydrodeoxygenation (HDO) is an indispensable approach to produce renewable biofuels and value-added chemicals using natural biomass and its derivatives. 2,5-Dimethylfuran (DMF) is considered to be a very promising liquid biofuel, and it can be fabricated by HDO of the biomass derivative 5-hydroxymethylfurfural (HMF). Herein, a highly efficient bifunctional catalyst, Co/HAP(Ce), was fabricated by anchoring highly dispersed Co on Ce-doped hydroxyapatite (HAP(Ce)). Co/HAP(Ce) displayed excellent HDO catalytic activity to convert HMF to DMF, and 99% HMF conversion and 96% DMF selectivity can be obtained under 150 °C, 2 MPa H2 conditions for 5 h. Density functional theory calculations revealed that H2 can be more easily activated by Co/HAP(Ce). Systematic studies confirmed that the high activity of Co/HAP(Ce) can be ascribed to the desired acid–alkali properties, highly dispersed cobalt species and strong metal–support interactions. This research provides a cost effective approach for designing efficient catalysts for HDO of biomass and its derivatives.
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2023
·
IF 10.9
Huijie Wang,Yang Wan,Binrong Li,Jian Ye,Jiahao Gan,Jiejing Liu,Xin Liu,Xianghai Song,Weiqiang Zhou,Xin Li,Pengwei Huo
The charge carrier separation efficiency and the adsorption capacity of the photocatalyst usually affect the degradation rate of antibiotics. Herein, Cerium-doped leaf-like CdS (Ce-CdS) modified with ultrathin N-doped rGO (N-rGO) composites were successfully constructed (Ce-CdS/N-rGO) to investigate the removal efficiency of tetracycline (TC). X-ray photoelectron spectroscopy (XPS) and photoelectrochemical results revealed that Ce ions doped in CdS acting as the electron capture sites facilitated the interfacial charge transfer. Theoretical calculation (DFT) results indicated that the interfacial effect between Ce-CdS and ultrathin N-rGO promoted the transfer of photogenerated electrons under the synergistic effect between the doping and interface modification strategy. The optimized Ce5-CdS/N-rGO20 composites had the maximum TC removal capability (94.5%) and maintained a stable cycling performance. In addition, the adsorption-driven photocatalytic degradation pathway of TC was studied through mass spectrometry (MS) and in-situ Fourier transform infrared spectroscopy ( in-situ FTIR). This study will provide an effective strategy for the construction of efficient photocatalytic composites for wastewater treatment.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 44
·99830-99841
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IF 5.8
Chen Yanzhu,Zeng Zheng,Liu Dongyang,Zhang Jing,Guo Yang,Zou Jianwu,Guan Juan,Xu Xiang,Li Liqing
Abstract The controllable preparation of efficient non-crystalline solid solution catalysts is a great challenge in the catalytic oxidation of volatile organic compounds. In this work, series non-crystalline solid solution structured Ce-Mn co-oxide nanofibers were creatively prepared by adjusting Ce/Mn molar ratios using electrospinning. 0.20CeMnO x (the ratio of Ce to Mn was 0.2) displayed an outstanding low-temperature toluene oxidation activity ( T 90 = 233 °C). The formation of the amorphous solid solution and the unique nanofiber structure both contributed to a large specific surface area ( S = 173 m 2 g -1 ) and high adsorbed oxygen content (O ads /O = 41.3%), which enhanced the number of active oxygen vacancies. The synergies between non-crystalline structure and active oxygen species markedly improved oxygen migration rate as well as redox ability of the catalysts. Additionally, in situ diffuse reflectance infrared Fourier transform spectra showed that the absorbed toluene could be completely oxidized to CO 2 and H 2 O with benzyl alcohol, benzaldehyde, benzoic acid, and maleic anhydride as intermediates. In summary, this study provided an alternative route for the synthesis of non-crystalline metal co-oxide nanofibers. Graphical abstract
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ANALYST
·
2022
·Vol. 147
·期 23
·5355-5362
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IF 5.227
Yi Xia,Jiaxin Zhou,Yanying Liu,Yutong Liu,Ke Huang,Huimin Yu,Xue Jiang,Xiaoli Xiong
Due to their high catalytic activity, stability and low cost, nanozymes with oxidase-like activity have attracted widespread interest in the fields of analytical detection and colorimetric sensing. To further promote the catalytic activity and the sensitivity of dopamine (DA) sensing, herein, a mixed valence Ce-MOF (MVCM) with enhanced oxidase-like activity was synthesized by the dielectric barrier discharge (DBD) microplasma method. Compared with hydrothermal synthesis, the prepared MVCM synthesized using a microplasma showed a higher catalytic activity, which benefits from a low Ce3+/Ce4+ ratio. Due to the spontaneous redox properties of Ce3+/Ce4+ in a MVCM, the MVCM-based colorimetric sensing of dopamine was established and showed a limit of detection of 0.74 μM over a linear range of 5–100 μM with high selectivity and stability and has been applied for the detection of dopamine in sweat. The proposed study provides an effective synthesis method for nanozymes with enhanced activity and shows great promise in widespread analytical and sensing applications.
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Royal Society Open Science
·
2022
·Vol. 9
·期 8
·
IF 3.653
Lin Li,Ting Yu,Zhenghua Qian,Xiaoling Wu,Hui He,Guoan Ye,Yanbo Qiao
Two new metal-organic frameworks (MOFs) (Th/ Ce -TCPE) based on 1,2,4,5-tetrakis(4-carboxyphenyl)ethylene were obtained using a straightforward reaction under moderate conditions. Th and Ce formed the central units of this MOF in the mononuclear and in the unusual trinuclear cluster configurations, respectively. The resulting MOFs were analysed by fluorescence spectroscopy to understand their luminescence. The obtained data revealed that benzene's electron cloud density and torsion angle on the ligand were affected by the acetic acid molecule and Th(IV), which caused Th-TCPE to irradiate stronger blue emission, but Ce-TCPE showed no fluorescence due to the self-quenching. Such a unique luminescence property could be used for fluorescence or radiopharmaceutical sensing.
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Catalysts
·
2022
·Vol. 12
·期 7
·775
·
IF 4.501
Yang Liu,Gongda Chen,Jianjun Chen,Hejingying Niu
Metal organic framework (MOF) is a type of porous organic material. In this work, three catalysts loaded with noble metal Pt were prepared by NaBH4reduction method with three different morphologies of Ce–MOF as carriers. Their physicochemical properties were characterized by XRD, Raman, FTIR, N2adsorption, SEM, XPS, and TGA. The catalytic performances of different catalysts were evaluated via toluene oxidation and CO2selectivity. Rod–shaped Pt/MOF–BTC exhibited best catalytic performance compared to Pt/MOF–808 and Pt/UiO–66, its T50and T90were 140 °C and 149 °C, respectively. After deducting the effect of specific surface, Pt/MOF–BTC still had the lowest apparent activation energy (62.8 kJ·mol−1), which is due to the abundant atomic Pt and oxygen vacancy content on its surface. After the reaction, the structure of Pt/MOF–BTC may become amorphous according to XRD results. Furthermore, the presence of amorphous structure had no effect on the catalytic activity of the catalyst. In the stability test of Pt/MOF–BTC to toluene oxidation, both toluene conversion and CO2selectivity remained at 100%, and remained stable for 11 h. Moreover, Pt/MOF–BTC also had better resistance to high weight hourly space velocity (WHSV) or water resistance. The catalyst maintained high catalytic activity for 3 times reusability. This study provides valuable experience for the future work of MOF in the field of VOC catalytic oxidation.Keywords:Ce–MOF;noble metal;oxygen vacancy;catalytic oxidation
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JOURNAL OF RARE EARTHS
·
2022
·
IF 4.632
Luyao Zhang,Fuli Tian,Huan Li,Jiangman Meng,Qi Liu,Xiaoqian Guo,Yun Qiu,Jun Zhang,Changyan Li
A series of non-enzymatic graphene functionalized biosensors was developed via deposition precipitation method for lactic acid (LA) detection, which were characterized by transmission electron microscopy (TEM), Raman spectroscopy , X-ray photoelectron spectroscopy (XPS), gas chromatography-mass spectrometry, liquid chromatography-mass spectrometry, and proton nuclear magnetic resonance ( 1 H NMR). The electrochemical performances of the non-enzymatic biosensors were measured by means of the electrochemical impedance spectroscopy (EIS) and cyclic voltammetry (CV) method. The comprehensive analysis of structures shows that Pt, CeO 2 , and GO components interact with each other. During the storing and releasing oxygen, the valence ratio of Ce 3+ /Ce 4+ and the number of oxygen vacancies in CeO 2 change accordingly, which can be conducive to increasing electronic transmission capacity and finally leads to the improvement of electrocatalytic performance. Among them, the Pt/CeO 2 /GO biosensor containing 0.47 at% platinum exhibits an excellent electrochemical detection performance with high sensitivity of 12.3 µA·L/ (mmol·cm 2 ) and a low limit of detection (LOD) of 5.12 μmol/L in a wide linear range from 10 to 900 μmol/L. In addition, the proposed biosensor possesses a promising anti-interference capability, as well as high stability and good reproducibility, which was assessed by testing the cyclic voltammogram in 0.1 mol/L lactic acid one year later. The underlying mechanism was proposed for electrochemical oxidation of LA to carbon dioxide and acetic acid with the synergistic effect among Pt, CeO 2 , and GO. Furthermore, the results of the standard addition method in real samples (human serum and urine samples) reveal that the lactic acid detection of the non-enzymatic Pt/CeO 2 /GO biosensor is accompanied by high reliability. Thus, it will be a valuable biosensor for in vitro detection of lactic acid level in clinical samples.
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ENERGY
·
2022
·
IF 8.857
Haifeng Jiang,Haipeng Liu,Jiaxin Dong,Jiaxing Song,Sunhua Deng,Jie Chen,Yu Zhang,Wenpeng Hong
Using cellulose to produce high-quality oxygenated fuels or chemicals is becoming an important way to replace chemical synthesis technology. In this work, the Ce–Co–Na ternary composite metal catalyst is synthesized and used for catalytic cracking of cellulose to prepare the ketone-rich bio-oil production. To construct an environment-friendly process, CO 2 is used as a pyrolysis reaction atmosphere to improve the enrichment of ketones. Strong synergistic effects among metal components effectively promote the thermal-cracking of cellulose to produce primary products (anhydrosugars), and further convert to oxygenates due to the excellent oxygen transferability of the catalyst. The introduction of CO 2 enhances the selectivity of ketones in the liquid product, especially 2,3-dimethyl-2-cyclopenten-1-one. The highest content of ketones in the liquid is 22.73%, which is about four times higher than that of the blank sample. In addition, the generation of CO in the syngas is promoted. This study provides an alternative way for the pyrolysis of biomass to prepare ketone platform compounds and syngas production .
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ENVIRONMENTAL RESEARCH
·
2022
·
IF 8.431
Yuxin Zhu,Yue Zhao,Xun Sun,Fuhao An,Lanya Jiao,Xuan Sun
Antibacterial strategies based on reactive oxygen species (ROS) have opened up a new avenue for overcoming the great challenges of antibiotics topic including lack of broad-spectrum antibiotics and the emergence of super-resistant bacteria. Herein, we leveraged a strategy of constructing synergistic catalytic active sites to develop a simple yet efficient Fenton-like active nanocomposite, and investigated its catalysis mechanism and antibacterial performance thoroughly. This strategy provides a new direction for boosting the catalytic activity of nanocomposite catalysts for wide application. Specifically, by uniformly loading copper oxide and ceria onto the surface of silica nanocapsules (SiO 2 NCs), we fabricated a bimetallic oxide nanocomposite Cu 0.75 Ce 0.62 O 2 @SiO 2 NC, which performed superior Fenton-like capability in a wide pH range without additional exogenetic hydrogen peroxide (H 2 O 2 ). Such excellent catalytic activity was originated from the charge interaction between the two metal oxide components, where formation of Cu + and oxygen vacancies (OVs) was mutually reinforcing, resulting in a synergistic effect to produce H 2 O 2 and catalyze the generation of •OH under the slight acid condition (pH = 6.0). In view of the outstanding Fenton-like activity, the Cu 0.75 Ce 0.62 O 2 @SiO 2 NC was employed in antimicrobial testing, which demonstrated exceptional high in vitro antimicrobial efficacy against both the S. aureus and E. coli in a neutral environment (pH = 7.4). The excellent performance of the bimetallic nanocomposite Cu 0.75 Ce 0.62 O 2 @SiO 2 NC, including its facile and mild preparation, high water-solubility and stability, superior catalytic and antimicrobial performances, manifests a promising broad-spectrum antibiotic that can be anticipated to deal with the contamination of the environment by bacteria.
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ELECTROCHIMICA ACTA
·
2022
·
IF 7.336
Yongxiang Wang,Guocan Shen,Ting Tang,Jinming Zeng,Rizwan Ur Rehman Sagar,Xiaopeng Qi,Tongxiang Liang
Electrochromic capacitors are attracting a huge attention due to their dual functions in energy-saving and energy storage. Electrochromic and energy storage performance of the films could be effectively improved through regulating their physical phase and morphology. In the present work, the physical phase and morphology of the WO 3 nanofilms were regulated by doping RE ions (RE = Ce, Eu, Sm, Gd) using one-step hydrothermal technology. The three-dimensional (3D) urchin-like crystal WO 3 nanofilm would transfer into the 3D nest-like WO 3 (WO 3 -RE) nanofilms that consisted of crystal and amorphous phase by doping RE ions. Compared with the pure WO 3 nanofilm, the WO 3 -RE nanofilms exhibited higher optical contrast, faster switching speed, longer cyclic stability, and larger areal capacitance owing to faster ions transfer rate and more stable film structure. The optical contrast of WO 3 -Eu and WO 3 -Sm nanofilms were 76.3% and 73.8% at 633 nm, 75.5% and 74.6% at 900 nm wavelength, respectively. Notably, the WO 3 -Eu and WO 3 -Sm nanofilms could retain 99.6% and 99.1% of their original optical contrasts after 1000 cycles, respectively. Additionally, the areal capacitance of ECDs based on the WO 3 /PB, WO 3 -Ce/PB, WO 3 -Eu/PB, WO 3 -Sm/PB, and WO 3 -Gd/PB were 26.15, 49.27, 58.23, 71.46, and 79.52 mF/cm 2 at 0.3 mA/cm 2 , respectively. ECDs based on the WO 3 -RE/PB are promising for energy-saving and energy storage dual functional smart windows.
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