SURFACE & COATINGS TECHNOLOGY
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2023
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IF 5.4
Duoli Wu,Yi Li,Ziyi Yuan,Liao Xiang,Xinlong Wei,Chao Zhang
The study examined the impact of varying molybdenum content (0 %, 5 %, and 10 % wt) on the high-temperature corrosion resistance of APS-sprayed Ni-clad Al coatings. The coatings were exposed to a simulated biomass-firing environment with pure KCl deposition at 600 °C for 168 h, and a mixed gas containing 15 % water vapor was passed through. The findings revealed that increasing Mo content improved the coating's high-temperature corrosion resistance. The coating with 10 % Mo displayed a continuous layer of Ni and Al oxides on its surface, while KCl was concentrated in the Mo region. Based on the experimental results, a mechanism for how the presence of Mo element contributes to the high-temperature corrosion resistance of NiAl coatings was proposed.
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PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
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2023
·Vol. 120
·期 39
·e2305883120
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IF 11.1
Chencheng Dong,Zhi-qiang Wang,Chao Yang,Xiaomeng Hu,Pei Wang,Xue-qing Gong,Lin Lin,Xiao-yan Li
Inspired by the development of single-atom catalysts (SACs), the fabrication of multimetallic SACs can be a promising technical approach for the in situ electro-Fenton (EF) process. Herein, dual-functional atomically dispersed Mo–Fe sites embedded in carbon nitride (C3N5) (i.e., MoFe/C3N5) were synthesized via a facile SiO2 template method. The atomically isolated bimetallic configuration in MoFe/C3N5 was identified by combining the microscopic and spectroscopic techniques. The MoFe/C3N5 catalyst on the cathode exhibited a remarkable catalytic activity toward the three electron-dominated oxygen reduction reaction in sodium sulfate, leading to a highly effective EF reaction with a low overpotential for the removal of organic contaminants from wastewater. The new catalyst showed a superior performance over its conventional counterparts, owing to the dual functions of the dual-metal active sites. Density functional theory (DFT) analysis revealed that the dual-functional 50-MoFe/C3N5 catalyst enabled a synergistic action of the Mo–Fe dual single atomic centers, which can alter the adsorption/dissociation behavior and decrease the overall reaction barriers for effective organic oxidation during the EF process. This study not only sheds light on the controlled synthesis of atomically isolated catalyst materials but also provides deeper understanding of the structure–performance relationship of the nanocatalysts with dual active sites for the catalytic EF process. Additionally, the findings will promote the advanced catalysis for the treatment of emerging organic contaminants in water and wastewater.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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IF 5.2
Shihao Miao,Yuanguang Zhang,Hongyu Xia,Hongcheng Gao,Weihao Tao,Zhenzhu Zhang,Chenyu Huang,Lin Huang
In the study, highly N-doped metal organic framework (MOFs) derived CoFeN photocatalysts (CoFeN-N) were successfully prepared by using carbon nitride (g-C 3 N 4 ) nanosheets as the support with simultaneous additional N source. CoFeN-N activated hydrogen peroxide (H 2 O 2 ) was used to remove Methyl orange (MO) and Tetracycline hydrochloride (TC-HCl) in water under simulated visible light . N doping improves the photo-Fenton degradation ability of CoFeN to varying degrees, and the photocatalyst with the best performance is CoFeN-N2. The degradation rate constants (K) of MO and TC-HCl are 1.8 and 5.1 times of CoFeN, respectively. CoFeN-N2 did not significantly inhibit the degradation efficiency of organic pollutants under acidic, neutral and alkaline conditions. Meanwhile, the presence of coexisting anions (Cl − 、HCO 3 - and HPO 4 2- ) in water similarly does not obviously reduce the degradation ability of CoFeN-N2 for MO and TC-HCl, which indicates the excellent anti-interference ability of the prepared photocatalyst. The TOC test results indicate that CoFeN-N2 has excellent mineralization ability for organic contaminants. In addition, hydroxyl radicals , superoxide radicals, and holes (·OH, ·O 2 - and h + ) were demonstrated to be the primary active species for the degradation of organic pollutants by CoFeN-N2 through free radical trapping experiments and EPR tests. This work provides an attractive strategy for the preparation of highly N-doped photocatalysts and the efficient removal of organic pollutants from water by photo-Fenton coupling.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Feiyu Gao,Chaowen Tan,Yang You,Yong Hou,Hongyan Yan,Xuewei Lv,Jie Dang
The imperative need for efficient and selective adsorption of Ni(II) and Mo(VI) is crucial for resource utilization and environmental protection. However, this process faces a challenge due to the scarcity of adsorbents that can adeptly adsorb both metal ions simultaneously. To address this, this study introduces a novel composite adsorbent material, denoted as BECZN, achieved through composite cross-linking of waste orange peel biochar with in situ aminated cobalt/zinc-zeolitic imidazolate frameworks (Co/Zn-ZIF-NH 2 ). The incorporation of Co/Zn-ZIF-NH 2 enhances the availability of active groups within BECZN. The aerogel structure of BECZN prevents ZIF material collapse and agglomeration, thereby improving active site exposure. BECZN exhibits notable adsorption capacities, reaching 151.84 mg/g for Ni(II) at pH = 7 and 842.54 mg/g for Mo(VI) at pH = 3. Further investigations indicated that the adsorption of Ni(II) and Mo(VI) obeys the Langmuir isotherm model, while exhibiting pseudo-second-order kinetics and intraparticle diffusion characteristics. Notably, BECZN selectively adsorbs Ni(II) and Mo(VI) efficiently under acidic and neutral conditions, respectively. It can maintain high capacity under the interference of various cations and anions. Meanwhile, this excellent selective adsorption of Ni(II) and Mo(VI) by Co/Zn-ZIF-NH 2 is revealed at the atomic level using density functional theory (DFT) calculations. This study offers a theoretical basis and experimental reference for the design and synthesis of ZIF and biomass-based composite adsorbents.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Weishan Qin,Ting Su,Guodong Chai,Xinhong Wang,Weichao Qin,Hongbin Yu
Photoelectrocatalysis is a promising method for removing biorefractory organic pollutants. However, the inefficient utilization of light and electricity by photoanodes and the failure to effectively execute cathode functions typically lead to poor degradation performance. Therefore, in this study, a photoelectrocatalytic (PEC) system coupled with electro-activated persulfate (E-PS) was constructed using a 3D nanostructured PbO 2 /Sb-SnO 2 //blue-TiO 2 //WO 3 bifacial anode and a Mo-CuFeO 2 -modified carbon felt cathode. The results indicate that the bifacial anode could effectively implement electro-assisted photocatalysis on the irradiating side and electrocatalysis on the back side. This significantly accelerated acetaminophen degradation with a synergy index of 48.98 %. Additionally, the PEC/E-PS system was established by combining a bifacial anode with a persulfate-activated cathode, which promoted the efficient utilization of photogenerated electrons and increased the number of active species in the coupled system. Density functional theory calculations confirmed that Mo tended to dope the Fe sites and promote the adsorption of PS on Mo-CuFeO 2 , facilitating the continuous activation of persulfate. In the coupled system, the contribution order of different active species to acetaminophen degradation was h + > OH > SO 4 − > 1 O 2 > O 2 − . Their mutual conversion enabled the PEC/E-PS system to efficiently remove acetaminophen with a relatively high current efficiency (22.69 %) and low energy consumption (0.06 kWh⋅gCOD −1 ). The proposed PEC/E-PS system is an efficient and sustainable method for treating organic contaminants in wastewater.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Hui Lu,Hongbo Wang,Changfei Gao,Lifen Liu,Tingting Yu,Yihua Li,Shaoying Lin
Lanthanum and cerium are widely used as important raw materials for energy storage batteries due to excellent natural electrical, magnetic, and optical properties. However, with the explosive growth of new energy generation and the environmental degradation-resistant of lanthanum and cerium, it is difficult to balance environmental sustainability and resource scarcity to achieve lanthanum-cerium removal by conventional chelate salt precipitation. Herein, a laboratory-scale self-powered electro-membrane bioreactor (SPEMBR), integrating high-active nitrogen-doped carbon nanotube-loaded iron and molybdenum bimetallic conductive composite electrode membrane (M−N−CNTs@Fe/Mo) by hydrothermal and phase inversion processes was successfully constructed and evaluated for removing lanthanum cerium from industrial wastewater. The prepared bi-functional M−N−CNTs@Fe/Mo5% electrode membrane exhibited a uniform morphology and excellent hydrophilicity, with nano pore lattice spacing only 0.2637 nm. Electrochemical test results demonstrated that the novel electrode indicated excellent redox properties (i 0 = 8.35 × 10 −3 A cm −2 , C dl = 1.13 mF cm −2 ) and efficient electron transfer efficiency (R ct = 4.69 Ω, n = 3.9). Based on optimized conditions (5)% doping ratio, pH = 10, C = 20 mg/L), the SPEMBR assisted by M−N−CNTs@Fe/Mo catalytic electrode membrane achieved approximately complete removal efficiency of lanthanum and cerium (>99.2 %), superior to most publicly available related studies (86.3 %-99.0 %), but with a calculation cost of only $8.54. Identification of membrane interface products and system precipitates demonstrated that the outstanding removal efficiency was attributed to the combined reaction mechanism of electroreduction, electrocoagulation and electromembrane filtration. This work provides a bright application prospect for low-cost and effective removal of lanthanum cerium metal based on electrode membranes.
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ULTRASONICS SONOCHEMISTRY
·
2024
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IF 8.7
Xiaojie Hu,Ting Xiao,Qidong Huang,Shichen Liu,Hongxia Liu,Sili Ren,Dandan Gong,Wuhui Luo
The use of a resin to selectively separate thiomolybdate from a tungsten (W) feed solution is a well-known protocol for achieve high-purity W products; however, the regeneration of saturated resin is laborious. In this study, poly(diallyl dimethyl ammonium chloride) (PDADMA) was used to modify ultrasound-pretreated montmorillonite (Mt) for W and molybdenum (Mo) separation for the first time, and the resultant tetrathiomolybdate (MoS 4 2- )-loaded composite was further tested to remove heavy metals instead of regeneration. Among the three variables of ultrasound pretreatment, that is, Mt concentration, ultrasound power, and treatment time, the Mt concentration exhibited the most significant influence followed by ultrasound power on the separation performance of W and Mo. Compared to the distance of the interlayer space and the surface charge of the modified Mt, the PDADMA content showed a closer correlation with the W/Mo separation coefficient. Assisted by Box–Behnken design, with Mt concentration of 6.9 g/L, ultrasound power of 593.8 W, and treatment time of 13.8 min, the composite with the greatest separation coefficient was obtained. The adsorption of Cu(II) on the optimal W/Mo separation-derived composite was ascribed to the formation of Cu-S complexes, while that of Pb(II) was attributed to complexation and surface precipitation. In contrast, ion exchange with the initially loaded anions, reduction by sulfide to Cr(III), and formation of Cr(III)-S complexes accounted for Cr(VI) removal. The adsorption of Cu(II) and Pb(II) equilibrated faster and showed higher acid-resistance than that of Cr(VI). The adsorption capacities for Cu(II), Pb(II), and Cr(VI) were 0.535, 1.398, and 0.882 mmol/g, respectively. Applying PDADMA to modify Mt as a reagent for W/Mo separation was feasible, and the derived composite was capable of removing cationic and anionic heavy metals.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Xiaomei Xu,Bilu Yang,Zhaodi Xu,Qiaoling Mo,Xiaomei Shen,Hu Cai
In the pursuit of advancing the production of H 2 through hydrogen-evolution reaction (HER), the demand for the elaborate design of cost-effective and robust durability electrocatalysts has gained momentum, especially replacement of noble-metal counterparts like Pt. Herein, we introduce a facile one-pot hydrothermal approach to synthesize nickel foam-supported Ni 3 S 2 nanosheet arrays, which integrate with carbon-quantum-dot (CQDs) and Cu, Mo dual-metal doped. With the introduction of CQDs and Cu, Mo dual-metal doped site, the optimal CQDs-Cu-Mo-Ni 3 S 2 @NF exhibits superior HER catalytic activity with a low overpotential of 125 mV at 10 mA·cm −2 and strong durability for 30 h in alkaline medium. The exceptional electrocatalytic performance is ascribed to the synergistic effect of CQDs and Cu, Mo dual-metal site. This synergy encompasses optimization of water molecule adsorption/desorption energetics , elevated electrical conductivity , weakening of the strong S–H bond interaction on the Ni 3 S 2 surface, and providing ample active centers. Furthermore, an in-depth understanding of the electronic structure and adsorption energy during the HER process is probed by density functional theory (DFT) analysis. Our work provides a quintessential paradigm for the rational design of multi-component electrocatalysts for water splitting.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Fenglong Wu,Xiao Tian,Jin Song,Ying Zhang,Wei Li
The activation of the water molecule (H₂O) serves as the rate-determining step for hydrogen (H 2 ) evolution from the photo-assisted hydrolysis of ammonia borane (NH₃BH₃). Therefore, developing a low-cost efficient catalyst that can expedite the cleavage of O H bonds in H₂O is needed for improving hydrogen production efficiency in practical applications. Here, we prepared a supported non-noble metal catalyst (Co/Mo@MoO 2 –200) with a large number of active sites, comprising ultrathin low-crystalline cobalt (Co) nanosheets grown on amorphous molybdenum oxide (MoO 2 )-coated molybdenum (Mo) nanoparticles (Mo@MoO 2 –200), which serves as a high-performance non-noble metal catalyst to accelerate the activation of O H bonds in H 2 O. Notably, visible light irradiation facilitates the formation of ultrathin Co nanosheets by inducing the localized surface plasmon resonance of MoO 2 , as verified by transmission electron microscopy (TEM) images. Moreover, X-ray absorption near-edge structure (XANES) and X-ray photoelectron spectroscopy (XPS) spectra confirm the electron transfer from Co nanosheets to O sites in Mo@MoO 2 –200, establishing robust interfaces. Co/Mo@MoO 2 –200 exhibits high catalytic performance with the turnover frequency (TOF) value of 110.8 min −1 under visible light irradiation, which is greater than that of Co/Mo by 1.21 times and most of the reported Co-based catalysts. DFT calculations reveal that the Mo@MoO 2 –200 support in the catalyst can promote the Co-adsorption of NH 3 BH 3 and H 2 O, while facilitating H 2 desorption. Particularly, the Co/Mo@MoO 2 –200 can significantly decrease the activation energy barrier of the O H bond in H 2 O, compared with pristine Co and Mo@MoO 2 –200. This paper presents a flexible catalyst design strategy for NH 3 BH 3 hydrolysis and other H 2 O-associated catalytic reactions.
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ACS Catalysis
·
2025
·
IF 13.1
Shuo Cao,Ying Ma,Wei Chu,Bingsen Zhang,Bo Peng,Yuefeng Liu
Molybdenum carbides have received attention for the reverse water gas shift (RWGS) reaction. Normally, MoCx-based catalysts are synthesized via a high-temperature carbonization of 1100 K, leading to the agglomeration of the active phase. In order to minimize the atomic motion leading to single growth, insertion of heteroatoms has been attempted with the usage of components in the catalyst substrate. The current work applied the self-assembling strategy to prepare a Mo–O–Al composite instead of traditional impregnation before carburization. The dynamic structure evolution and detailed coordination environment of the active phase are investigated by in situ X-ray diffraction, quasi in situ X-ray photoelectron spectroscopy, in situ transmission electron microscopy, and temperature-programmed surface reaction techniques. Our findings reveal that Al doping enables carburization at a lower temperature (200 °C) via the topotactic pathway, yielding α-MoCx (fcc); even at a loading as high as 40 wt %, the catalyst maintains an ultrasmall particle size (1 nm). The optimized catalyst exhibits a RWGS reaction rate of 52.1 μmolCO2·gMo–1·s–1 at 400 °C, representing a 2.5-fold enhancement over bulk β-Mo2C. This work provides a possible solution for maintaining high dispersion at high metal loading for catalyst preparation, specially requiring a high temperature during either synthesis or reaction.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Conghan Zhang,Jiating Cheng,Fan Yang,Yang Sun,Xinyang Sun,Kexin Wei,Guang Ma,Junpu An,Meitong Zhao,Jiahui Liu,Yongfeng Li
Electrolytic water splitting using transition metal sulfide catalysts has garnered a lot of attention lately. Herein, a composite material consisting of Mo-doped Ni 3 S 2 nanoparticles supported on N-doped carbon layers with anchored Ni single atoms (Mo–Ni 3 S 2 /Ni–N–C) was synthesized using a two-step hydrothermal process. These features enable Mo–Ni 3 S 2 /Ni–N–C to achieve low overpotentials of 71, 58, and 89 mV for the hydrogen evolution reaction (HER) at 10 mA cm −2 in 1 M KOH, 0.5 M H 2 SO 4 , and 1 M PBS, respectively. After 20 h of durability testing, its current density retains over 95 % of the initial value across diverse pH electrolytes. Mo doping enhances structural stability, enabling wide pH applicability. Electron transfer from Ni 3 S 2 nanoparticles to Ni single atoms accelerates kinetics and boosts intrinsic activity, which improves HER performance. Theoretical calculations confirm that Ni single atoms possess ideal H∗ adsorption energy, which optimizes H∗ adsorption capability of Ni 3 S 2 . This work offers suggestions for creating excellent low-cost electrolytic water catalysts.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Tao Chen,Jiaxing Song,Menglei Xu,Zaifang Li
Urea-assisted hydrogen production can effectively improve the overall reaction rate, but achieving industrial-scale current density and long life is still a huge challenge. Herein, Vo-NiMoOOH/NF was prepared by hydrothermal-selenization-electrochemical reconstruction, which can achieve the industrial-grade current density of ∼860 mA cm −2 in an H-type reaction cell at 1.5 V (vs. RHE). A series of characterizations and DFT calculations reveal that the presence of oxygen vacancies and electrophilic-nucleophilic sites improves the D-band center of Ni, reduces the oxidation potential of Ni, accelerates the reconstruction of the catalyst, and inhibits the oxygen evolution reaction. Electrocatalytic urea oxidation coupled with hydrogen production was achieved in a two-electrode flow cell utilizing Vo-NiMoOOH/NF as a bifunctional catalyst. The current density of 1 A cm −2 at a cell voltage of 2.71 V and stable operation for more than 150 h at a current density of 500 mA cm −2 were realized, exhibiting excellent catalytic activity and stability.
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