Journal of the Iranian Chemical Society
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2024
·Vol. 21
·期 12
·2943-2953
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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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NANO
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2015
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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
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2015
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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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APPLIED CATALYSIS A-GENERAL
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2024
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IF 4.7
Qingyang Li,Junxiang Jiang,Zhengting Xiao,Hongchuan Xin,Guangci Li,Da Wang,Yanpeng Li,Chao Feng,Xuebing Li,Song Chen,Keng H. Chung
CoMo 6 heteropolyacids were modified by cationic surfactants with different alkyl chain lengths to obtain oil-soluble Co–Mo complexes, which were subsequently employed to synthesize highly dispersed hydrodesulfurization catalysts. The surfactants, as structure-directing agents, markedly affected the morphology, specific surface area, and sulfurization degree of the Co-Mo sulfides at the sulfurization stage, resulting in more accessible edge active sites and Brønsted acid sites. Among the various Co-Mo sulfides, the one derived from dodecyl trimethyl ammonium bromide (DTAB)-modified CoMo 6 heteropolyacid (DTA-CoMo-S) exhibited the highest hydrodesulfurization (HDS) reaction rate (1.1×10 −5 mol/(g cat ·s)) for 4,6-dimethylbenzothiophene (4,6-DMDBT) at 330 °C and an initial H 2 pressure of 7.0 MPa. DFT confirmed that H 2 S adsorption and S-O exchange were more likely to occur on the surface of DTA-CoMo 6 during at the sulfurization stage, which was conducive to the sulfurization of the precursor and generated more CoMoS active phases and SO 4 2- groups. These species promoted both the HDS of 4,6-DMDBT and low-temperature cracking reactions of the intermediate products. In addition, the oil-soluble DTA-CoMo 6 complex showed better hydrocracking, HDS and hydrodemetallization performance in the hydrotreatment of vacuum residue.
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SENSORS AND ACTUATORS B-CHEMICAL
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2024
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IF 8
Weining Liu,Hairong Li,Dandan Huang,Xi Tan,Mingyang Zhao,Qionglin Cheng,Ming Yi,Qi Ding,Yaqian Ren,Guohan Liu
Triethylamine (TEA) poses severe safety hazards to industrial production and human health. To accurately detect TEA concentrations and rapidly warn of leakage, a simple reflux condensation method was deployed to successfully incorporate Zn 2+ in situ into Mo-MOFs precursor in a green, safe, and time-efficient synthesis condition. Subsequently, through calcination, MoO 3 /ZnMoO 4 -X (MMZ-X) were prepared, which exhibited an increased number of defects and enriched porosity, facilitating the access and interaction of TEA with adsorption sites. Simultaneously, rationally built in situ MoO 3 /ZnMoO 4 heterostructures accelerated carrier migration and induced a drastic resistive change. MMZ-2 demonstrated outstanding TEA sensing performance, exhibiting extremely high sensitivity ( R = 572.3, 100 ppm), along with superior selectivity, repeatability and stability, rapid response and recovery times, and a low detection limit. Moreover, the key intrinsic parameters of the heterostructure on the atomic scale were determined by density functional theory (DFT) calculations, providing a detailed elucidation of the sensing enhancement mechanism of the MoO 3 /ZnMoO 4 heterostructure. The simple and efficient synthesis method and the related mechanistic analysis pave a new path for designing high-performance TEA gas sensors with practical applications.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
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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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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
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IF 4.9
Worku Lakew Kebede,Dong-Hau Kuo,Xiaoyun Chen
Environment and energy are presently some of the highest priority topics for mankind that need to be addressed. Organic pollutants are toxic and carcinogenic for human and aquatic life hence their presence in water even in low concentrations can cause serious health problems. Photodegradation of organic pollutants by utilizing oxide-based heterostructure photocatalysts is the promising approach to carry out remediation efficiently ascribed to the advanced optoelectronic and structural superiority of oxide photocatalysts. The Zn(O,S)/Mo(O,S) 2 composites were synthesized via a facile solvothermal method at low temperatures. Several methods were used to characterize the composite morphology, structure, electrical conductivity, chemical composition, and optical characteristics. The heterostructured Zn(O,S)/Mo(O,S) 2 oxysulfide was employed successfully in the photocatalytic degradation of organic pollutants. Among the as-prepared samples, the 30-ZnMoOS composite catalyst was found to have the highest photodegradation performance on various organic dye pollutants. The photocatalytic activity of the as-synthesized Zn(O,S)/Mo(O,S) 2 samples was assessed on the photodegradation of different kinds of organic dyes under visible light irradiation. The photocatalytic degradation efficiency of 30-ZnMoOS composite over 10 ppm neutral red (NR), methylene blue (MB), rhodamine B (Rh B), and methyl orange (MO) was found to be 99.6 %, 99.9 %, 99.5 %, and 98.8 % within 40, 45, 180, and 180 min, respectively, under visible light illumination. In the present photocatalytic system, the superoxide ( . O 2 - ) anions, hydroxyl ( . OH) radicals, and holes (h + ) are proposed to be the direct reactive species causing the photodegradation of organic dyes.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2024
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IF 3.8
Da Sheng,Qing He,Zhong-Hua Cao,Lun-Bo Chen,Song-Hai Wu,Yong Liu,Hai-Tao Ren,Xu Han
Although photooxidation of benzyl alcohol to benzaldehyde in aqueous solution is an important chemical process, its selectivity cannot be readily controlled due to the overoxidation of benzaldehyde. In this study, a series of Bi–Mo/CN photocatalysts are synthesized, and their reactivity in photooxidation of benzyl alcohol under visible light is compared. Bi–Mo/CN-2 exhibits high photocatalytic reactivity in the conversion of benzyl alcohol (51%) with a high selectivity toward benzaldehyde of 99.9%. In this process, the formed ≡Bi–OO• and ≡Bi–OOH selectively oxidize benzyl alcohol to benzaldehyde via the H-abstraction pathway after O2 is photoreduced on Bi–Mo/CN, accompanied by the formation of H2O2. Meanwhile, the doped Mo utilizes the produced H2O2 or ≡Bi–OOH to produce ≡Mo–O2 peroxo, which not only contributes to the selective oxidation of benzyl alcohol to benzaldehyde but also effectively prevents overoxidation of benzaldehyde. This work provides new insight into designing novel photocatalysts for selective oxidation of organic substrates.
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JOM
·
2024
·
IF 2.1
Lei Shan,Wu Jiaxing,Miao Yu,Guo Bao
It is difficult to depress secondary copper sulfide minerals in the separative flotation of copper–molybdenum coexisting ores with a huge NaHS consumption, and causing serious safety and environmental problems. Galvanic interaction between active metallic granular (low consumption depressant; LCD) and secondary copper sulfide mineral particles can induce surface passivation, thereby depressing its floatability and achieving clean and efficient regulation of copper molybdenum separation. The use of 10% LCD was applied at the first stage and 5 kg/t NaHS at the second stage can recover 89.71% of Cu, while only 52.89% of Cu can be recovered for single stage flotation where 20 kg/t NaHS was used without any presence of LCD. To avoid the negative effect of Mg(OH) 2 colloids at higher pH at the second stage, sodium hexametaphosphate (SHMP) was added as a dispersant and Mo recovery could be pulled up to 89.63%.
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FUEL
·
2024
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IF 6.7
Han-Ming Zhang,Jiakang Li,Yuhang Gao,Jinfeng Sun,Shipeng Geng,Yongqiang Meng
Alkaline water/seawater electrolysis has drawn broad concern for green hydrogen production. Design and development of efficient, stable, and inexpensive bifunctional catalysts is one great bottleneck to overall alkaline water/seawater splitting. Herein, high-valence Mo, Mn co-doped amorphous bimetallic sulfide (MoMn-NiCoS) was prepared by facile pulse electrodeposition technology. High-valence Mo, Mn significantly enhanced the bifunctional catalytic performances for elevated reaction kinetics and rapid charge transfer with optimal electron structure modulation. Therefore, MoMn-NiCoS exhibited excellent bifunctional performances with low overpotentials of 70/69/73 mV and 247/226/282 mV at 10 mA cm −2 for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in alkaline water/simulated seawater/natural seawater , respectively. Besides, MoMn-NiCoS||MoMn-NiCoS electrolyzers required small cell voltages of 1.57/1.56/1.62 V to reach 10 mA cm −2 for overall alkaline water/simulated seawater/natural seawater splitting. Moreover, MoMn-NiCoS performed prominent stability during the 50 h-chronopotentiometry test at 50 mA cm −2 for the electrolyzer. Meanwhile, NiCo-based hydroxides/oxyhydroxides and sulfate ions were formed for electrocatalyst surface reconstruction during catalytic process, which were beneficial to the excellent bifunctional electrocatalytic activities and chloride repulsion. No hypochlorite formation verified the superior chloride oxidation inhibition of MoMn-NiCoS. The excellent catalytic performances of MoMn-NiCoS were attributed to the high-valence dual-cation doping, amorphous structure, electron structure modulation, synergetic effect, and surface reconstruction. This work provided an insightful strategy for the design and development of high-efficiency, stable, and cost-effective bifunctional electrocatalysts for overall alkaline water/seawater electrolysis.
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CHEMICAL ENGINEERING SCIENCE
·
2024
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IF 4.1
Yeshuang Wang,Zhelin Su,Mingxian Duan,Huiling Fan,Ju Shangguan,Chao Yang
Metal oxides-based adsorbents used for desulfurization encounter significant challenges during practical application owing to their inferior reusability and the nature of solid waste of their desulfurization products. This situation might be alleviated to some extent through a rational design of Ni–Mo composite, enabling them firstly to be used as adsorbents for H 2 S removal, and then being utilized as catalysts after desulfurization for C 4 H 4 S hydrogenation. The Ni–Mo composites before and after desulfurization were characterized using XRD, FT-IR, SEM, N 2 adsorption–desorption, XPS, CO 2 -TPD and H 2 -TPR techniques. The experimental findings suggested that Ni and Mo species function as primary active sites for H 2 S adsorption and C 4 H 4 S hydrogenation reactions, respectively. The Ni and Mo composite greatly facilitated the coupling of these two reactions due to the formation of NiMoO 4 phase. This novel active phase not only boosted the interaction between metal and H 2 S but also promoted the formation of weak and moderate alkaline sites, thereby significantly enhancing desulfurization performance. Importantly, this active phase fostered the sulfurization of Mo species and transforming into a Ni–Mo–S component, further favoring the subsequent catalytic reaction in C 4 H 4 S hydrogenation. Consequently, the prepared Ni–Mo composite oxides exhibited excellent properties in H 2 S adsorption and C 4 H 4 S hydrogenation activity, surpassing the capabilities of single metal adsorbents and commercial hydrogenation catalysts.
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ACS Sustainable Chemistry & Engineering
·
2024
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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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