APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Ruiyang Zhang,Penghui Li,Fang Wang,Liqun Ye,Abhijeet Gaur,Zeai Huang,Ziyan Zhao,Yang Bai,Ying Zhou
Atomically dispersed atom catalysts with atomically distributed active metal centers have attracted great attention owing to the maximum atom efficiency and excellent selectivity. Herein, for the first time, we found atomically dispersed Mo atoms can be formed on g-C 3 N 4 , and induce its amorphous transformation. This amorphous transformation leads to the formation of strong band tails with remarkably enhancing the absorbance edge of Mo-C 3 N 4 up to 750 nm, resulting in almost whole visible-light range absorption. The formation of new Mo-C and Mo-N bonds due to strong interfacial interaction between atomically dispersed Mo atoms and g-C 3 N 4 provide new electron and hole transport pathways to accelerate the separation of charge carriers. As a result, amorphous Mo/C 3 N 4 (a-Mo/C 3 N 4 ) reveals excellent photoreduction of CO 2 , yielding CO and H 2 productions of 18 and 37 μmol g −1 h −1 under visible-light illumination (λ > 420 nm), which manifest a remarkable 10.6- and 4-folds enhancement of that over crystalline g-C 3 N 4 . This finding provides a conceptually different approach to fabricate high-efficient photocatalyst through the strong interfacial interaction between atomically dispersed metal atoms and host.
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CERAMICS INTERNATIONAL
·
2019
·
IF 3.45
Liang Cheng,Biaojie Yan,Rui Gao,Xiangdong Liu,Zhenliang Yang,Bingqing Li,Yi Zhong,Pengchuang Liu,Yun Wang,Mingfu Chu,Bin Bai,Pengcheng Zhang
UO 2 /Mo composite pellets with enhanced thermal conductivity have been considered for the novel construction of high-safety fuel systems. UO 2 /Mo core-shell composite pellets with a reasonable porosity of 4–5% were fabricated by spark plasma sintering (SPS). In the SPS UO 2 /Mo composite, the majority of pores remained homogeneous in the UO 2 matrix, while it had a dense morphology in the continuous Mo channel for the heat conduction . The sintering behaviour of the UO 2 /Mo composite indicated that the incorporating Mo impeded densification of UO 2 , and the primary densification temperature ranged from 903 K to 1270 K. To introduce 2 vol% Mo to UO 2 , the thermal conductivity (TC) was enhanced to 4.02 W/m·K at 1073 K. The above result represented a 23.31% improvement over the value of 3.26 W/m·K (Fink) for a pure UO 2 pellet, which was approximated by the revised Hasselman-Johnson model. In particular, the coefficient of thermal expansion (CTE) was reduced to 10.0 × 10 −6 /K from 298 K to 1673 K, representing an 8.83% reduction from the value of 10.98 × 10 −6 /K (Martin) for a pure UO 2 pellet. The reduction effect on the CTE was superior to that of other UO 2 matrix composites fuel systems and, hence, offers an external safety aspect for reactors at the elevated temperatures close to accident conditions. These results provide a feasible method for the fabrication of a UO 2 /Mo core-shell pellet as an accident tolerant fuel.
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JOURNAL OF HAZARDOUS MATERIALS
·
2019
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IF 7.65
Bo Sheng,Xin Zhou,Zhun Shi,Zhaohui Wang,Yaoguang Guo,Xiaoyi Lou,Jianshe Liu
The interaction of reductive metal ions and peroxymonosulfate (PMS) is necessary for the generation of sulfate radials (SO 4 − ), however, this process is greatly restrained by the sluggish reduction of high-valent metal ions. Here we report that commercially available reductive metal (Mo or W) powders are capable of unlocking this kinetic constraint. The reduction of Fe(III) to Fe(II), decomposition of PMS, and degradation/mineralization of 4-chlorophenol (4-CP) are all accelerated in the Mo/Fe 2+ /PMS process at a very low Fe 2+ /PMS ratio (Fe 2+ /PMS = 1/10). In such an accelerated system, common adverse effects of natural water constituents such as chloride and humic acid are largely mitigated. According to the fluorescence measurement and scavenging tests, sulfate and hydroxyl radicals dominate in Mo/Fe 2+ /PMS process. The addition of Mo or W is further confirmed to favor Cu 2+ /PMS process, but this is not the case for other metal ions (Mn 2+ , Ni 2+ , Ce 3+ and Co 2+ ). Reductive zero-valence and four-valence active sites (Mo 0 and Mo 4+ ; W 0 and W 4+ ) play key roles in overall redox reaction. Overall, our present work provides an alternative route for expediting redox cycling of transition metals in advanced oxidation processes, without useless consumption of PMS and increase of total organic carbon.
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PubMed
高影响因子
TRANSACTIONS OF TIANJIN UNIVERSITY
·
2018
·Vol. 25
·期 1
·52-65
·
IF 0
Li Wang,Zhang Qingjun,Zeng Aiwu
In this study, liquid-phase aerobic oxidation of toluene catalyzed by Mn–Mo oxide was conducted in a 1.0 L batch reactor. The macroscopic kinetics of toluene consumption and benzaldehyde generation at 413–443 K were obtained from a combination of experimental observation and hypothetical models. The results clearly showed that both the oxidation rate of toluene and generation rate of the aromatic product were proportional to the concentration of the substrate, the partial pressure of oxygen and the surface area of the catalyst. The energy barrier of toluene oxidation to benzyl alcohol was the highest (≈ 81 kJ mol −1 ), while that of benzyl alcohol oxidation to benzaldehyde was the lowest (≈ 57 kJ mol −1 ). Moreover, the activation energy of further oxidation of benzaldehyde in an acetic acid solvent was only slightly lower (≈ 1.9 kJ mol −1 ) than that of toluene oxidation. Significantly, the transformation of benzyl alcohol indeed contributed to the generation of benzaldehyde and this step conformed to a first-order parallel-consecutive model. Increased reaction temperature and residence time favored the transformation of benzyl alcohol to benzaldehyde. In addition, doping with molybdenum at Mn/Mo = 3/1 enhanced the catalytic performance of the heterogeneous catalyst and was attributed to the presence of a synergetic effect between different metal cations. Regarding the microscopic kinetics, the LH-OS-ND mechanism (Langmuir–Hinshelwood adsorption of reagents on the same type of active sites and non-dissociative adsorption of oxygen) was verified as responsible for the heterogeneous oxidation of toluene. Oxygen and benzaldehyde were weakly adsorbed (Δ H ads,Oxy ≈ − 15 kJ mol −1 , Δ H ads,Bald ≈ − 30 kJ mol −1 ), but showed strong mobility (Δ S ads,Oxy ≈ − 22 J mol −1 K −1 ), Δ S ads,Bald ≈ − 39 J mol −1 K −1 ). The fundamental intrinsic rates were deduced based on the LH-OS-ND mechanism and showed great consistency with the macroscopic results.
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Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 19
·9228-9235
·
IF 9.931
Teng Wang,Rumei Jin,Xiuqi Wu,Jie Zheng,Xingguo Li,Kostya Ostrikov
A highly efficient Ni–Mo bimetallic catalyst for the hydrogen evolution reaction can be obtained from a molybdate incorporated Ni-MOF by thermal decomposition in NH3. The catalyst is composed of crystalline Ni nanoparticles doped with amorphous low valence Mo oxide encapsulated in thin N-doped carbon layers, showing excellent HER performance, featuring a very low overpotential for the HER (η20 = 58 mV), low Tafel slope (57 mV dec−1) and excellent long term stability. The catalyst apparently outperforms N-doped carbon encapsulated Ni catalysts without Mo doping, emphasizing the critical synergetic effect of Mo doping and the surface N-doped carbon thin layer on promoting the performance of Ni based HER catalysts.
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Small
·
2018
·Vol. 14
·期 27
·1800090
·
IF 9.598
Lianshan Sun,Chunli Wang,Xuxu Wang,Limin Wang
Controllable synthesis of functional materials is of widespread interest for particle engineering. Such a method has not been widely promoted due to the lack of recognition of the fundamental principle, especially for organic–inorganic hybrid materials. Here, as an entrance, the controllable synthesis of Mo-polydopamine coordination flowers is realized through a facile foaming method, and a 2D nanopetal as the building monomer of the flower is synthesized. Depending on the morphology evolution of Mo-dopamine complex under different conditions, and the surface iterative topology growth of the Mo-polydopamine petal, the reasons of why the Mo-polydopamine complex self-assembles into a flower structure can be attributed to the synergistic effect of multicore symbiosis and structural self-protective growth behaviors. Benefiting from the strong structure stability of the Mo-polydopamine nanopetal, a hybrid structure of MoO 2 quantum dot in situ anchoring in the N-doped 2D carbon framework is prepared by direct pyrolysis, which shows a highly reversible performance in application for lithium-ion secondary batteries (LIBs). This work enhances the possibility for the controllable synthesis of organic–inorganic hybrid materials by adjusting the multicore intergrowth and inhibiting the interfacial assembly.
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NANO
·
2015
·
IF 1.09
Wen-Ting Li,Yu Wang,Fen-Fang Deng,Li-Li Liu,Hai-Jun Nan,He Li
A novel electrochemical immunosensor for determination of carcinoembryonic antigen (CEA) in human serum was fabricated by depositing Mo–Mn 3 O 4 /MWCNTs/Chits nanocomposite onto an indium-tin oxide (ITO) electrode. Mo-doped Mn 3 O 4 (MMO) was synthesized by sol–gel method and the presence of molybdenum improved its electrochemical properties. The MMO/MWCNTs/Chits nanocomposite could accelerate the electron transfer rate and enlarge the surface area to capture a large number of Carcinoembryonic Antigen (CEA). The factors influencing the performance of the immunosensor were investigated, such as incubation time, incubation temperature and pH. Under optimal conditions, the electrochemical immunosensor could detect CEA in a linear range from 0.1 ng ⋅ mL − 1 to 125 ng ⋅ mL − 1 with a detection limit of 4.9 pg ⋅ mL − 1 ( S ∕ N = 3 ). In addition, it exhibited high sensitivity and acceptable stability on a promising immobilization platform for signal amplification, which could be extended to other labeled recognition systems. This electrochemical immunosensor may provide potential applications for the clinical diagnosis.
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CHEMICAL ENGINEERING JOURNAL
·
2015
·
IF 4.321
Qizhou Dai,Jiazhong Zhou,Xiaoyang Meng,Daolun Feng,Chengqiang Wu,Jianmeng Chen
A novel molybdenum modified PbO 2 electrode was successfully prepared with the method of electrodeposition . The SEM and XRD were employed to study the surface morphology of electrodes, which indicated that the modified PbO 2 electrode had a larger effective area and more compact film. Electrochemical degradation of cinnamic acid (CA) in aqueous solution with Mo–PbO 2 electrode and PbO 2 electrode were investigated. The results showed that the Mo–PbO 2 electrode had a better effect of CA removal. The operational parameters influencing the electrochemical degradation of CA with Mo–PbO 2 electrode were optimized and the results revealed that the electrochemical degradation of CA followed the pseudo-first-order kinetics and the optimal removal of CA and COD were 85.51% and 25.79% after 120 min on condition of the electrolyte concentration, initial concentration of CA, current density and initial value of pH were 0.1 mol/L, 300 mg/L, 10 mA/cm 2 and 3.4, respectively. The degradation mechanism of CA in electrochemical oxidation with Mo–PbO 2 electrode was analyzed and the main degradation pathway of CA was proposed based on the intermediates identified by IC and GC–MS.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Jiabing Luo,Yongxiao Tuo,Jianchao Zhang,Wenle Li,Shutao Wang,Yanpeng Li,Yuan Pan,Yan Zhou,Jun Zhang
The development of efficient and low-cost overall water splitting electrocatalysts for an anion exchange membrane (AEM) electrolyzer is desirable for hydrogen production. The control of geometric and electronic structures of electrocatalysts can improve the catalytic efficiency of hydrogen evolution reaction (HER) and durability in oxygen evolution reaction (OER). Spatially confined growth and heteroatom doping can achieve this prospect of the target electrocatalysts. Herein, we prepared a carbon-shell confined Mo-doped CoP electrocatalyst (Mo-CoP@C) via an anion adsorption coupled pyrolytic phosphorization method. A Metal-Organic Framework (MOF) of Co was used to achieve Mo doping and carbon-shell encapsulation. Mo doping significantly altered the electronic structure of CoP, which produced a local polarized environment for water dissociation during alkali HER process. Meanwhile, carbon-shell confined growth and provided a protective layer for durable OER process. Consequently, Mo-CoP@C exhibits attractive alkali electrocatalytic HER and OER activities with the overpotentials of 122 and 280 mV at 0.01 A cm −2 . Finally, the assembled Mo-CoP@C-CP‖Mo-CoP@C-TFF AEM electrolyzer could operate for 500 h at 0.1 A cm −2 .
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ACS Sustainable Chemistry & Engineering
·
2024
·
IF 7.1
Xinyu Mao,Yu Chen,Shihao Li,Yang Yang,Chen Tao,Jiafu Shi,Zhongyi Jiang
Activation of the N≡N bond is of importance in photocatalytic nitrogen (N2) fixation, which strongly relies on the precise construction of catalytic active sites. Herein, we reported a dual-metal photocatalyst of Mo/UN(Zr) with a high proportion of Mo-coordinated Zr–O clusters (Zr–O–Mo dual-metal active sites) for photocatalytic N2 fixation, which was synthesized though post-modification to the defects of UN(Zr) by Mo. By contrast with the dual-metal photocatalyst of UN(Zr–Mo) synthesized via the co-mixing method, Mo/UN(Zr) possesses a higher proportion of Zr–O–Mo dual-metal active sites that is crucial for activating and polarizing N≡N bond as evidenced by in situ Fourier transform infrared (FTIR) spectroscopy combined with density functional theory (DFT) calculations. The synergistic effect of Zr–O–Mo dual-metal active sites resulted in a lower potential activation energy barrier for N2 activation which promoted the photocatalytic N2 fixation efficiency. The optimum photocatalytic N2 fixation rate of Mo/UN(Zr) was 255.7 μmol g–1 h–1 by adjusting the loading amount of Mo, which was enhanced about 2.5 times and 1.6 times compared with UN(Zr) and UN(Zr–Mo) photocatalyst, respectively. Our study will afford valuable guidance for designing efficient photocatalysts for photocatalytic N2 fixation.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
·
IF 4.9
Xiufeng Wang,Wenhui Ai,Ge Chen,Yao Jin,Jiayao Chen,Fang Wang,Ting Zhou,Guodong Zhang,Zhiqing Zhang
A novel Mo-MnO 2 nanoflowers (NFs) with oxidase-like (OXD-like) activity was performed by microwave-assisted hydrothermal synthesis, and the doping of Mo resulted in enhanced enzyme-like activity and stronger affinity for the chromogenic substrate 3,3′,5,5′-Tetramethylbenzidine (TMB) than single MnO 2 by the same synthesis method. In the presence of oxygen, Mo-MnO 2 NFs oxidized the colorless TMB to blue oxTMB, and the addition of isoniazid and ascorbic acid inhibited the color development reaction. Besides, it was further investigated that the inhibitory mechanism of INH and AA on the color development reaction of Mo-MnO 2 -TMB system, mainly due to the electrostatic interaction. The absorbance change of oxTMB at 652 nm could be used to quantitative detect isoniazid (INH) and ascorbic acid (AA). The linear ranges of colorimetric detection were 1–40 μM for INH and 1–30 μM for AA, and the limits of detection (LOD) were 0.436 μM for INH and 0.579 μM for AA, respectively. The successful application of this sensing platform in real samples further validated its practicality, demonstrating the broad potential in the field of colorimetric sensing.
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Journal of the Iranian Chemical Society
·
2024
·Vol. 21
·期 12
·2943-2953
·
IF 2.2
Pu Hongmei,Cui Yifan,Wang Haidan,Yu Lijuan,Yang Dezhi,Yang Yaling,Li Hong
Until now, there have been many reports on the regulation of inorganic metal ions on the catalytic activity of nanozymes, but few reports on the regulation of anions (such as NO 2 − ) on enzyme activity. In this work, a copper-molybdenum doped carbon dots (Cu, Mo-CDs) with peroxidase-like (POD) activity was synthesized by simple one-step microwave digestion method. The Cu, Mo-CDs + NO 2 − system can promote 3,3′,5,5′-tetramethylbenzidine (TMB) oxidizing to blue oxidative product (oxTMB) due to the formation of ∙NO 2 free radical. While Hg 2+ was introduced into the system, the POD-like activity of Cu, Mo-CDs + NO 2 − system was inhibited due to the strong interaction and the electron transfer between Cu, Mo-CDs and Hg 2+ . The formation of ∙NO 2 and the electron transfer capability of Cu, Mo-CDs + Hg 2+ were confirmed through ESR spectra and FMN experiments. The bioenzyme-free colorimetric assay based on Cu, Mo-CDs nanozyme is used for detection of NO 2 − and Hg 2+ , showing lower detection limit (LOD) of 1.63 µg/L for NO 2 − , 0.13 µg/L for Hg 2+ , respectively and good recovery from 90.79 to 108.90%. The work paves a new way to design a nanozyme-based colorimetric protocol for traces NO 2 − and Hg 2+ residues in food analysis.
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