JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2022
·
IF 6.76
Jiaqi Zhang,Quanhui Hou,Yanbing Liu,Xinglin Yang
The design of catalysts with excellent catalytic activity plays an important role in the field of solid-state hydrogen storage of new energy sources. Herein, a novel hydrangea-like NiO@NiMoO 4 composite catalyst was prepared through a facile hydrothermal reaction. Subsequently, NiO@NiMoO 4 was doped into MgH 2 by ball milling to solve the problems of high dehydrogenation temperature and slow desorption kinetics of MgH 2 . It can be seen from the experimental results that the MgH 2 + 10 wt% NiO@NiMoO 4 composite starts to dehydrogenate at about 190 °C, which is about 170 °C lower than that of pure MgH 2 . Meanwhile, after complete dehydrogenation, the composites can start to absorb hydrogen below 40 °C. Compared with pure MgH 2 , the activation energy of hydrogen absorption and dehydrogenation of the composite decreased by 47.6 kJ/mol and 46.5 kJ/mol, respectively. In 10th cycle tests, the MgH 2 + 10 wt% NiO@NiMoO 4 composite still has good cycle stability. After adding a small amount of biomass charcoal, the hydrogen storage capacity can even be maintained above 97%. Furthermore, the characterization results show that the in situ generated new species Mo and Mg 2 Ni/Mg 2 NiH 4 synergistically promote the adsorption and dissociation of hydrogen. This new synergistic mechanism provides new comprehensive insights for improving reversible hydrogen storage in MgH 2 .
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Qianqian Xie,Xuxu Wang,Wenqian Chen,Chao Lei,Binbin Huang
Bimetallic sulfides have distinctive catalytic property in activating peroxymonosulfate (PMS) for water remediation . Polyoxometalates as potential precursors have rarely been reported for the catalytic degradation of refractory organic pollutants . Herein, a composite catalyst of Co-Mo bimetallic sulfides supported onto graphene oxide (O-CoMoS/GO) with a heterojunction architecture was synthesized through a hydrothermal strategy with polyoxometalates ((NH 4 ) 4 [Co II Mo 6 O 24 H 6 ]·6H 2 O) as the precursor and applied in the PMS activation . This material showed a superior performance for the catalytic degradation of the model organic pollutant, 4-chlorophenol (rapidly removed within 10 min with an apparent reaction rate constant of 0.5458 min −1 ). O-CoMoS/GO outperformed most of the reported catalysts in terms of activity and had a strong tolerance towards common organic and inorganic compounds in water, and could perform well in different real water systems. Experimental and theoretical results indicated that the introduction of GO could achieve the enrichment of electrons on the metals and reduce the d band center (ε d ) of Co close to the Fermi level (ε F ), thereby facilitating the interfacial electron transfer process. The activation mechanism was due to the as-prepared bimetallic sulfides and the formation of heterojunction structure with GO, where Co(II) as the active center could be regenerated by the adjacent Mo element (as co-catalyst) and by gathering electrons from GO through the Co/Mo-O-C coupling. This work provides insights into the design of bimetallic sulfide catalysts in activating PMS for water remediation.
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Catalysis Science & Technology
·
2022
·Vol. 13
·期 2
·468-478
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IF 6.177
Xinyu Lu,Xiaoli Gu
The chemical demand for alkyl phenols (mainly extracted from fossil-derived resources) has been increasingly growing, which has accelerated global energy shortages. Due to the inherent aromaticity of lignin, its effective conversion into alkyl phenols is central to its adoption as a sustainable precursor to produce biochemicals. In this study, catalytic transfer hydrogenation (CTH) of alkali lignin was carried out in a mixed medium (isopropanol/formic acid) at 240 °C for 8 h over a series of bimetallic Ni based catalysts. The acidity and reducibility of the as-prepared catalysts are enhanced via WO3 introduction (to form a WO3–Al2O3 mixed support) and a bimetallic synergistic effect, respectively, leading to improved catalytic activity and selectivity towards alkyl phenols. Different kinds of phenolic compounds (e.g., those with substitutions of methoxyl, alkyl, alkenyl, carbonyl, carboxyl, or hydroxyl groups) were generated over these bimetallic Ni based catalysts with various combinations of Ni + Fe/Zn/Co/Mo/Cu, which was due to their own catalytic promotion of certain reactions (e.g., hydrogenation, deoxygenation, and/or hydrogenolysis). Reaction mechanisms of lignin depolymerization were proposed according to the distribution of phenolic compounds. This work provides a comprehensive investigation on yielding alkyl phenols from lignin CTH over a series of inexpensive bimetallic Ni based catalysts (Ni/(Fe/Zn/Co/Mo/Cu)–WO3/Al2O3), and undertook a catalytic evaluation of the bimetallic synergistic effects on improving the chemical selectivity towards alky phenols, which is beneficial for lignin valorization.
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CATALYSIS COMMUNICATIONS
·
2023
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IF 3.7
Xigang Du,Hongyu Liu,Mengfan Su,Yuping Tai,Bingli Pan,Ning Guo,Jun Zhang
Ru nanoparticles doped and supported by Mo oxide (Ru/Mo oxide NPs) were synthesized via an in situ co-precipitation strategy for hydrogen production via hydrolysis of ammonia borane (AB). The optimized Ru 0.9 Mo 0.1 catalyst composition exhibited a total turnover frequency (TOF) value of 514.8 mol H2 (mol Ru0.9Mo0.1 ) −1 min −1 at room temperature. Systematic characterization of the catalysts unveiled the dual role of Mo oxide in regulating the structure and catalytic performance of Ru NPs. This work provides a new approach for the design of Ru-based nanocatalysts toward hydrolysis of AB for H 2 harvest.
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ACS ES&T Water
·
2022
·
IF 0
Yibing Sun,Hongchao Li,Shengli Zhang,Ming Hua,Jieshu Qian,Bingcai Pan
Heterogeneous peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs) are under extensive investigation for their great potential in water remediation. The understanding of the PMS activation mechanism is crucial but still debatable. Here, we describe a thorough investigation of the mechanism involved in PMS activation by using molybdenum disulfide (MoS2) as a catalyst. This MoS2/PMS system exhibited intriguing target-dependent reactivity. Further comprehensive experimental results excluded the major contributions of various possible species, including HO•, SO4•–, O2•–, 1O2, homogeneous Mo(VI), and heterogeneous Mo(VI). We then proposed a surface ≡Mo–OOSO3– complex as the major reactive species, while SO4•– derived from the decomposition of ≡Mo–OOSO3– acted as the secondary reactive species for pollutant removal. This complex could oxidize pollutants through the oxygen-atom-transfer mechanism and perform both nucleophilic and electrophilic attacks. This work provides novel perspectives for the mechanistic understanding of heterogeneous PMS-based AOPs for water remediation.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Yunqing Liu,Xuefeng Wang,Yuanna Zhu,Haiqing Wang,Jinghua Yu,Hong Liu,Shenguang Ge
Engineering of robust nonprecious electrocatalysts toward anodic oxygen evolution reaction (OER) is of great significance for lowering the cost and energy consumption for renewable fuel production. Herein, we report NiFeMoO x nanosheets as high-performance OER electrocatalyst through promoting the thermodynamic-limiting oxidation cycle process in NiFe oxyhydroxide via high-valence Mo doping. The NiFeMoO x nanosheets are prepared by an elaborate in-situ solvothermal etching-depositing process with NiFe alloy framework as substrate and metal precursors. The resultant nanosheets exhibit outstanding alkaline OER activity, requires only 235/282/327 mV overpotentials to achieve current density of 10/100/300 mA cm −2 , respectively, with a good long-term stability at 20 mA cm −2 for 72 h. Besides, the Tafel slope low to 28.1 mV dec −1 indicates a favorable OER kinetics. The superior catalytic activity of NiFeMoO x nanosheets should be attributed to the lower oxidation states of Ni and Fe induced by high-valence dopant , leading to easier surface reconstruction at low charge oxidation cycling during OER, thereby effectively reducing the overpotential. The synergy between the electronic effect among multimetallic sites and the unique morphology is expected to inspire the development of robust OER electrocatalyst for industrial application.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Linwei Jiang,Yichen Pan,Jiancheng Zhang,Xin Chen,Xinwen Ye,Zhendong Li,Caicai Li,Qingfeng Sun
Replacing the sluggish oxygen evolution reaction (OER) with thermodynamically favorable urea oxidation reaction (UOR) is an appealing tactic in the energy-saving water splitting system. Herein, by a facile composite electrodeposition method, an electrocatalyst with Mo particles anchored on the Ni-P matrix (Mo/Ni-P) was fabricated and utilized for urea-assisted water electrolysis of hydrogen production. As expected, the urea-involved electrolytic cell with the as-obtained Mo/Ni-P served as both the anode and cathode merely needs a voltage of 1.55 V to sustain a current density of 50 mA cm −2 (0.16 V less than that of the conventional water splitting at 50 mA cm −2 ) and can maintain the stability for 12 h. Additionally, the solar-driven urea-assisted water electrolysis system was constructed under lab conditions and solar-hydrogen-electricity energy conversion processes were also simulated. Moreover, it was demonstrated that tungsten (W) particles can also serve as an accelerant for promotion both the hydrogen evolution reaction (HER) and UOR activity of pristine Ni-P. This work will present a facile method for rational integration of metal particles with Ni-P layer for highly efficient electrocatalysts applied in economic production of H 2 .
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Materials Today Chemistry
·
2022
·
IF 7.613
S. Yang,Y. Cheng,T. E,Y. Wang,L. Liu,Y. Li,D. Wang,J. Qian
The inert substrate surface of MoS 2 leads to unsatisfactory adsorption performance. Herein, an inert substrate surface activation strategy is proposed, and the resulted MoS 2 /montmorillonite (MMT) prepared via the hydrothermal method is immersed with NaF (F–Mt). The intercalation of Na + contributes to inducing the transformation of MoS 2 from 2H phase to 1 T phase, thereby providing a large number of S vacancies and exposing available Mo 4+ . Meanwhile, the surface of MMT is activated due to the fact that partially [Si 4 O 10 ] 4- are etched by F - , which facilitates forming Si–O–Mo bonds to promote the charge transfer. The improved charge transfer rate can make S 2- in MoS 2 accumulate more negative charges, greatly enhancing the adsorption capacity to Pb 2+ . Moreover, the natural negative potential on the surface of MMT solves the problem of easy stacking for nanosheets , improving the availability of active sites on the edge, which are also benefit from the etching effect on MoS 2 nanosheets with NaF. The maximum adsorption capacity achieves 97.09 mg/g. Additionally, density functional theory (DFT) calculations confirm the resulted S vacancies in MoS 2 are in favor of removing Pb 2+ , which is also contributed by the electrostatic and chemical adsorption with MMT. Therefore, it suggests that F–Mt is an excellent adsorbent for Pb 2+ .
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Shuisen He,Tingting Huang,Yu Fan
Novel alumina-supported Ni-Mo hydrodesulfurization (HDS) catalysts were prepared via assembly of Mo and Al precursors induced by tetradecylamine (TDA). Compared with conventional impregnation, this assembly method improves Mo dispersion, weakens metal-support interactions, enhances Ni modification at MoS 2 edge sites, and produces more NiMoS phases on Al 2 O 3 . The optimal NiMoS microstructure was obtained by modulating the TDA/Mo ratio in the assembly. A microstructure-activity correlation indicated that the S vacancies at the NiMoS corner sites favored σ-adsorption and direct desulfurization of 4,6-dimethylbenzothiophene (4,6-DMDBT), and those at the NiMoS edge sites promoted C-S breaking in hydrogenated derivatives of 4,6-DMDBT. Among these catalysts, NiTMo-2.0/Al 2 O 3 , which had the most corner and edge S vacancies, exhibited the highest reaction rate constant of 5.89 × 10 −7 mol·g −1 ·s −1 and the highest desulfurization ratio of 99.5% in HDS of 4,6-DMDBT.
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Frontiers in Chemistry
·
2022
·
IF 5.545
Hu Yanru,Zhang Gengrui,Liu Lele,Chi ZiXin,Wang Shuai,Lin Jingdong,Xiong Haifeng,Wan Shaolong
The thermocatalytic conversion of hexose into valuable chemicals such as methyl lactate under mild conditions is very appealing. Here, we report that Mo, Mg co-modified Sn-β catalyst can effectively catalyze the transformation of glucose and fructose into alkyl lactate at moderate temperatures. A maximum yield of around 35% of methyl lactate was achieved from the conversion of glucose in methanol at 100°C over Sn-β catalyst modified with 3 wt% Mo and 0.5 wt% Mg. However, up to 82.8% yield of ethyl lactate was obtained in the case of fructose in ethanol upon the same catalytic condition, suggesting a significant solvent effect. The Mo species plays a key role to enable the retro-aldol condensation of fructose, in which the competing side reactions are significantly suppressed with the assistance of neighboring Mg species probably through a synergetic effect of Lewis acid-base.
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Catalysis Science & Technology
·
2021
·Vol. 11
·期 22
·7445-7453
·
IF 6.119
Yijuan Wang,Ziyi Guo,Jianzhi Wang,Ningbo Yu,Yanan Xue,Faquan Yu
Crystal structure and morphology can be regulated by inducing the positioning growth of metal sulfide, which is an efficient strategy to improve the oxygen evolution activity of the anode. Herein, solid NiMoO4 nanoplate arrays were used as cages to immobilize the metal source, and Mo doped NiSx is obtained by in situ solvothermal sulfuration reaction with polysulfide as the sulfur source. The electronic structure, conductivity, crystallographic phase and microscopic morphology of oxygen evolution catalysts could be controlled simultaneously by polysulfide induced solid metal oxide sulfidation, thereby greatly improving their electrocatalytic oxygen evolution activity. Benefiting from these, the prepared Mo doped nickel-sulfur electrodes show great performance toward the oxygen evolution reaction with overpotentials of 184 mV and 240 mV at current densities of 50 and 100 mA cm−2 in alkaline electrolyte. This study provides a new pathway by polysulfide induced sulfidation based on solid metal oxide for developing metal sulfide electrode materials with high oxygen evolution reaction performance for overall water splitting.
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JOURNAL OF MOLECULAR LIQUIDS
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2021
·
IF 6.165
Bingqiao Yang,Pengliang Huang,Qing An
A small molecular triazole derivative called AMT (3-amino-5-mercapto-1,2,4-triazole) was explored as a novel and efficient chalcopyrite depressant in the preferential flotation of chalcopyrite from molybdenite. The flotation performances were comprehensively investigated via micro-flotation tests of singe and mixed minerals with and without Cu collector. The adsorption mechanisms were determined in terms of contact angle, adsorption capacity, and zeta potential, Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS) and DFT calculations. Single mineral flotation results illustrated that the AMT selectively depressed chalcopyrite over a wide range of pH values. Particularly, AMT was able to depress chalcopyrite even in the presence of sodium isobutyl xanthate (SIBX). The contact angle, adsorption capacity, zeta potential, and FTIR results suggested that AMT was preferentially adsorbed on chalcopyrite surface, but it barely interacted with molybdenite. XPS tests and DFT calculations demonstrated that AMT was chemically adsorbed on chalcopyrite surface through the hybridization of S (1) and N (1) 2p orbitals of AMT with the Cu (1) 3d orbital. The bonding between S (1) atom and Cu (1) was much stronger than that between N (1) and Cu (1). Thus, AMT exhibited good potential as a novel depressant due to its excellent selectivity and practicability.
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