PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
·
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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高影响因子
Journal of the Taiwan Institute of Chemical Engineers
·
2021
·
IF 5.876
Zichen Wang,Hongbin Li,Wei Ma,Yinglong Wang,Peizhe Cui,Jianguang Qi,Zhengrun Chen,Zhaoyou Zhu,Fanqing Meng
Peroxymonosulfate (PMS) activation have provided a new direction to eliminate the organic pollutant . Current challenges that must be solved include secondary pollution by the metal ions and limitation in the recyclability of the catalysts. The waste 1D-FeOOH adsorbent with adsorption of metal elements (As, Cr or Mo ions) has been reused as an efficient electro-catalyst for PMS activation and used to metronidazole (MTD) degradation for the first time. The effects of current density, initial reaction pH, stirring rate, PMS dosage and solution temperature on MTD degradation was studied. The used 1D-FeOOH with adsorption of Mo ions showed the highest PMS activation ability and 99.6% MTD could be removed after 30 min degradation. The •OH and Found that SO 4 •− is the main free radical for MTD degradation. DFT calculation and characterization results were demonstrated that the high PMS electro-catalysis activation ability of the 1D-FeOOH@Mo has resulted from the special composition-dependent interactions among FeOOH@Mo and PMS, including stable adsorption properties, easy electron transfer and weak O O bond. The possible PMS electro-catalysis activation mechanism and MTD degradation pathway have been proposed. (ECOSAR) was used to evaluate the toxicity of metronidazole during degradation. The results showed that the toxicity of MTD and its intermediates could be effectively reduced by prolonging the degradation time in 1D-FeOOH@Mo solution. This work provides new insights for waste adsorbent disposal and gives a new perspective for PMS activation to degradation of antibiotics in water.
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Journal of Materials Chemistry B
·
2020
·Vol. 8
·期 30
·6459-6468
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IF 5.344
Xiaodan Zhang,Yuwan Lu,Qiumeng Chen,Yuming Huang
A self-templated strategy was adopted to design hollow Co3O4/MO3 (M = Mo, W) mixed-metal oxides via the Mo or W doping of ZIF-67, and subsequent pyrolysis under an atmosphere of air at a low temperature of 450 °C. The hollow Co3O4/MO3 (M = Mo, W) mixed-metal oxides displayed tunable oxidase-like and peroxidase-like activities able to efficiently catalyze the oxidation of TMB to generate a deep blue color in the absence or presence of H2O2. Relative to that of the un-doped Co3O4, the oxidase mimic activity of the Mo-doped Co3O4 increased to 1.3 to 2.1-fold, while its peroxidase mimic activity increased to 7.1 to 19.9-fold, depending on different Mo doping amounts. The oxidase mimic activity of the W-doped Co3O4 increased to 2.1 to 2.3-fold, while its peroxidase mimic activity increased to 4.8 to 5.9-fold, depending on the different W doping amounts. The Mo- and W-doped Co3O4 nanohybrid exhibited both higher O2 and H2O2 activating capability, and their H2O2 activating capacity was superior to the O2 activating capability. Furthermore, the Mo- and W-doped Co3O4 nanohybrids exhibited similar O2 activating abilities, while the Mo-doped one displayed a higher H2O2 activating capability than the W-doped one. The discrepant peroxidase-like nature of Mo- and W-doped Co3O4 nanohybrids is likely attributed to their different catalytic mechanisms. The peroxidase-like activity of Mo-doped Co3O4 is highly related to the ˙OH free radical, while that of W-doped Co3O4 is likely ascribed to the electron transfer between TMB and H2O2. The Km values of Co3O4/MoO3 for TMB and H2O2 were 0.0352 mM and 0.134 mM, which were 3.2- and 1.9-fold lower than that of pure Co3O4, respectively. A Co3O4/MoO3-based colorimetric platform was developed for the determination of H2O2 in the 0.1–200 μM range, with a limit of detection of 0.08 μM (3σ). Based on the thiocholine (TCh) inhibition of the excellent peroxidase-like activity of Co3O4/MoO3 and the TCh generation via acetylcholinesterase (AChE) catalyzed hydrolysis of acetylthiocholine chloride (ATCh), the colorimetric platform was extended to screen AChE activity and its inhibitor.
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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
·
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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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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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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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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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Lumei Zhang,Chun Han,Zheng Ye,Dongzhe Cui,Junyuan Yang,Hao Xu,Haiyan Song,Zehua Guo,Xiaoliang Wu,Yunhe Zhao
The layered double hydroxides (LDHs) electrocatalysts have emerged as promising electrocatalysts for electrolytic water splitting due to their simple synthesis, high activity. However, traditional LDH-based catalysts face the low electrical conductivity and durability under electrolysis conditions. In this work, Mo–CoFe LDH was prepared by a two-step hydrothermal method, and the effect of different molybdenum content on its catalytic performance was studied. Among them, the OER and HER properties of Mo-CoFe LDH-1 are better than those of non-Mo doping. Mo–CoFe LDH-1 has the low HER and OER overpotentials are 192 mV and 134 mV, respectively at 10 mA cm −2 . In addition, using Mo–CoFe LDH-1 for water splitting can achieve a low voltage of 1.55 V at 10 mA cm −2 , and it also showed a good stability within 100 h. The excellent properties of Mo–CoFe LDH-1 is mainly due to the formation of 3D nanoflower structure and the doping of Mo element in CoFe LDH, significantly adjusting its electronic structure. This work is of great significance for the design of bifunctional LDHs-based electrocatalysts.
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