Molecular Catalysis
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2024
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IF 3.9
Mengyao Yun,Tao Chen,Ning Zhao,Zhenhua Li
Energy is of great importance for the development of modern society, which is mostly dependent on crude oil. Due to the severe pollution caused by using crude oil and the diminishing of crude oil reserves, it is urgent to look for clean oil from alternative resource other than crude oil. Currently, Coal-to-Liquid (CTL) or Biomass-to-Liquid (BTL) technology is an important way to produce clean liquid fuels through Fischer-Tropsch Synthesis (FTS) of syngas. For FTS process, catalyst is a main factor for affecting on syngas conversion and product distribution. For traditional oxides-supported catalysts, the mutual constraint between active metal loading and dispersion at high metal loading is hard to overcome, which will hinder the synthesis of high-performance FTS catalysts. In this paper, a new type of Co@SiO 2 -T (CS-T) and Co@SiO 2 -X (CS-X) catalysts with core-shell structure were prepared by using polyvinyl pyrrolidone (PVP) as the structural stabilizer, hexadecyl trimethyl ammonium Bromide (CTAB) as the templating agent and tetraethyl orthosilicate (TEOS) as the silica source. The effects of hydrothermal temperature and pyrolysis temperature on the catalyst physical-chemical properties and FTS performance were investigated. The results showed that increasing the hydrothermal temperature favored the formation of the core-shell structure of the catalysts. With the increase of pyrolysis temperature, the catalyst particle size decreased from 0.54 μm to 0.23 μm. The FTS activities of the catalysts showed a volcano trend with hydrothermal and pyrolysis temperatures.
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Desalination and Water Treatment
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2024
·
IF 1
Chao Wang,Su Xu,WenChao Liao,TsingHai Wang
Manganese oxide-based catalysts have been frequently adopted to activate peroxymonosulfate (PMS) for the degradation of refractory contaminants such as sulfamethoxazole (SMX). In this study, the Co-doped ɑ-MnO 2 catalyst was prepared to validate the concept that the introduction of additional oxidation states and structural defects due to the doping process would significantly enhance the efficiency of PMS activation. Among all Co@ ɑ-MnO 2 catalysts prepared, the activator with the mole ratio of Co/Mn 0.05:1 exhibited the highest SMX degradation. A near 100% removal of SMX (1000 μ g / L ) was achieved within 1 min in a condition with 10.0 mmol/L PMS and 0.5 g/L Co 0.05 @ ɑ - MnO 2 at 25 ℃ . The effects of catalyst dose, PMS concentration, initial SMX concentration, solution pH, temperature, and coexisting cations, anions, and humic acid (HA) on SMX degradation were studied. The impressive sustainability of the Co 0.05 @ ɑ-MnO 2 /PMS system was confirmed by its capability of operating over a wide pH range, its stability after multiple cycles, and its insensitivity to the coexisting of cations. The presence of high electrophilic anions, such as NO 2 ¯ and HCO 3 ¯ , on the other hand, would compromise the SMX degradation. Furthermore, reactive oxygen species (ROS) generated in the Co@ ɑ-MnO 2 /PMS system were identified by scavenger tests and electron paramagnetic resonance (EPR). Singlet oxygen ( 1 O 2 ) was verified to be the major route contributing to the degradation of SMX. In addition, sulfate radicals ( SO4 •¯ ), superoxide radicals (O 2 •¯ ), and hydroxyl radicals (ּ • OH) were also generated in the Co@ ɑ-MnO 2 /PMS system and participated in SMX degradation. Therefore, the Co@ ɑ-MnO 2 is a promising catalyst for PMS activation in the degradation of SMX.
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Muhammad Sabir,Mahmoud Sayed,Zhuofan Zeng,Bei Cheng,Wang Wang,Chuanbin Wang,Jingsan Xu,Shaowen Cao
The photocatalytic conversion of carbon dioxide (CO 2 ) into valuable products holds great promise from environmental and economic perspectives. However, current photocatalytic materials still exhibit unsatisfactory efficiency. In this study, a notably efficient step-scheme (S-scheme) heterojunction was developed by combining the Co-MOFs with carbon nitride nanosheets (g-C 3 N 4 ). The electrostatic interaction between these components not only facilitates the exfoliation of g-C 3 N 4 layers but also enhances the stability of the photocatalyst structure. The optimal heterojunction Co-CN4 photocatalyst achieved a significantly enhanced CO production rate of 16.1 µmol g −1 h −1 , which is 4.7 times higher than that of pure g-C 3 N 4 . This improved activity is ascribed to the enhanced light absorption and mitigated charge carrier recombination. Density functional theory (DFT) computations in conjunction with experimental observations elucidate the establishment of a close contact interface. Additionally, electron paramagnetic resonance (EPR) and in situ X-ray photoelectron spectroscopy (XPS) characterization unveil the electron transfer pathway of Co-CN4 during photocatalytic CO 2 conversion. This study offers valuable insights into the design of S-scheme photocatalysts for enhancement of CO 2 photoreduction.
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Journal of Materials Chemistry A
·
2024
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IF 10.7
Jin-Long Fan,Sheng-Bo Liu,Ming-Liang Chen,Zhangxiong Wu,Sheng-Peng Sun,Yao-Yin Lou
Electrocatalytic reduction of nitrate (NO3−) to ammonia (NH3) is garnering increasing interest due to its potential to reduce CO2 emissions as a substitute for the Haber-Bosch process, while also mitigating NO3− pollution. However, it remains a challenge to achieve a current density exceeding 300 mA cm−2 while maintaining the stability of catalysts. Additionally, the anodic oxygen evolution reaction, characterized by slow kinetics and high energy barriers, severely impedes the widespread adoption of NH3 formation from NO3− reduction. Therefore, in this study, we introduce amorphous phosphorus-doped cobalt catalysts (Co–P@NF) prepared via a facile electrodeposition process for efficient NO3− reduction and hydrazine oxidation. The incorporation of phosphorus in Co–P@NF facilitates electron migration from phosphorus to cobalt, enhancing *H provision for efficient hydrogenation of the intermediate *NO2−. This results in a current density of 2 A cm−2 at −0.3 V, with a faradaic efficiency for NH3 of 91% in an electrolyte containing 1 M NO3−. Moreover, the Co–P@NF catalyst exhibits remarkable long-term stability, maintaining an NH3 faradaic efficiency exceeding 90% and a current density of 799 mA cm−2 after 82 hours of electrolysis. Furthermore, Co–P@NF displays high catalytic activity in promoting the rate-determining step of hydrazine oxidation, from *N2H2 to *N2H. The incorporation of the HzOR (hydrazine oxidation reaction)-assisted NO3−RR (nitrate reduction reaction) unit significantly reduces the cell voltage to 0.34 V at 300 mA cm−2.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Bin Liu,Haonan Chen,Changrong Zhao,Heng Liang
As a 2D nanomaterial with high hydrophilic and co-catalytic properties, MXene has been widely studied in the field of membrane separation and advanced oxidation. However, its susceptibility to oxidation in catalytic environments poses a significant challenge to its long-term stability and performance. Therefore, constructing an oxidation-resistant MXene catalytic membrane technology and ensuring its excellent flux and catalytic performance are important for the practical application of MXene membranes. Herein, we prepared a cobalt monoatomic intercalated M/E0.1-Co catalytic separation membrane by mild reduction of epigallocatechin-3-gallate (EGCG). EGCG not only connects the MXene lamellae during filtration through strong hydrogen bonding, but also protects the chemical stability of the MXene substrate through its antioxidant ability. Furthermore, the trace amount of EGCG in the confined domain space also promotes the rate-limiting step of the transition from the high-valent state to the low-valent state in Co single-atom catalysis. The stability of the catalytic separation layer was ensured along with a 100% degradation performance of sulfamethoxazole. This study establishes a bridge between the catalytic oxidation and chemical stability of a wide range of MXene-based materials nowadays and provides a viable proposal for the practical application of long-term utilized MXene materials in catalysis.
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Chem
·
2024
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IF 19.1
Yaolin Wang,Jiaqiang Yang,Yuhai Sun,Daiqi Ye,Bin Shan,Shik Chi Edman Tsang,Xin Tu
Plasma catalysis offers a flexible and decentralized solution for CO 2 hydrogenation to methanol under ambient conditions, avoiding the high temperatures and pressures required for thermal catalysis. However, the reaction mechanism, particularly plasma-assisted surface reactions, remains unclear, limiting the development of efficient catalysts for selective methanol synthesis. Here, we report a bimetallic Ni-Co catalyst effective in plasma-catalytic CO 2 hydrogenation to methanol at 35°C and 0.1 MPa, achieving 46% methanol selectivity and 24% CO 2 conversion. In situ plasma-coupled Fourier transform infrared characterization, along with density functional theory calculations, reveals that the engineered bimetallic sites act as primary active centers for methanol synthesis, promoting the rate-determining step in H-radical-induced reaction pathways by reducing steric hindrance effects. This work demonstrates the significant potential of bimetallic catalysts in plasma-catalytic CO 2 hydrogenation to methanol under ambient conditions, representing a major step toward sustainable CO 2 conversion and fuel production.
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Catalysts
·
2025
·Vol. 15
·期 3
·219
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IF 4
Xuan Han,Chao Guo,Hui Wang,Weijuan Xu,Qinlian Liu,Qingshan Zhao,Mingbo Wu
Hydrogen production from water electrolysis offers a highly promising and sustainable route to solve the energy crisis. However, it is severely limited by the sluggish kinetics of the oxygen evolution reaction (OER) occurring on the anode. Herein, employing carbon dots functionalized with benzene sulfonate groups (BS-CDs) as a distinctive inductor, a Co(OH)2catalyst featuring abundant defects was synthesized for an enhanced OER. The highly hydrophilic nature of BS-CDs exerts a significant interfacial induction effect on the growth dynamics of Co(OH)2, fostering the formation of elevated crystal defects and a substantial quantity of oxygen vacancies. The resulting BS-CDs/Co(OH)2catalyst requires an overpotential of only 340 mV to achieve a current density of 10 mA cm−2in alkaline media, demonstrating markedly improved OER activity compared to pristine Co(OH)2and N-CDs/Co(OH)2induced by amine-modified CDs. Furthermore, the structural integrity of the catalyst is maintained, with a current retention rate of 92% observed following a 20 h stability assessment. This work provides a novel approach for developing cost-effective transition metal catalysts that exhibit exceptional catalytic efficiency and excellent stability for the OER.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Wenchen Ren,Huanxi Wang,Qianlin Zhang,Mengchi Chen,Zhongrui Li,Huan Guo,Jing Bai,Xiaomin Dai,Santosh Kumar Verma,Yunhua Xu
In this paper, petal sheet layered Co-Al bimetallic hydroxides were prepared using the hydrothermal method using methanol as a solvent. Pt/Co-Al-O catalysts were produced after the impregnation method and H 2 reduction. This catalyst was applied to the dehydrogenation reaction process of methylcyclohexane to toluene. A fixed-bed reaction device carried out comparative tests of this series of catalysts, and the effect of Co addition on the performance of Pt/Co-Al-O catalysts was investigated in detail. Among them, the Pt/Co 3 -Al 1 -O catalyst showed the best performance with high toluene selectivity throughout the dehydrogenation process. The MCH conversion started to be greater than 90% at 330 °C, and the hydrogenolysis rate was 262.7 mmol/g Pt /min. The conversion gradually increased with the reaction temperature, and the conversion could reach 99.5% at 410 °C. The appropriate introduction of Co element can reduce the excessive strong acidic sites of Al 2 O 3 itself and retain a certain number of weak acidic sites, while the bimetallic hydroxide carrier improves the dispersibility of the active component, reduces its particle size, and forms a certain strong interaction between the carrier and Pt. The final conversion of the catalyst decreased by about 2% in the 100 h stability test at 380 °C, which indicated that the Pt/Co 3 –Al 1 –O catalyst had strong coking resistance and good stability. These results indicate that the Pt/Co–Al–O series catalysts have potential industrial applications in hydrogen energy utilization.
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POLYMER BULLETIN
·
2025
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IF 4
Wang Guoqiang,Wang Yueying,Wei Deyu,Hui Yunfeng,Yu Yiheng,Zhang Mengke,Shi Longqing,Hu Jing
Polylactic acid (PLA) is a kind of bio-based polyester with high tensile strength and poor ductility. Poly(butylene sebacate-co-terephthalate) (PBSeT) is a kind of biodegradable polyester with good ductility. To improve the ductility of PLA, PBSeT with high molecular weight was synthesized and melt blended with PLA to obtain PLA/PBSeT blends with high ductility in this study. Their structures and properties were characterized by differential scanning calorimetry, thermogravimetric analysis (TGA), dynamic mechanical analysis (DMA), and scanning electron microscopy (SEM). Although SEM, DMA, and TGA suggested poor compatibility between PBSeT and PLA, PBSeT can still improve the ductility of PLA. When the PBSeT content was 30 wt%, the elongation at break of the blend increased to 85.9%. PBSeT debonds with the PLA matrix to form internal cavitation and the shear band to absorb a large amount of energy to induce plastic deformation. Meanwhile, PBSeT can reduce the complex viscosity of PLA.
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ELECTROCHIMICA ACTA
·
2024
·
IF 5.5
Mingyao Yang,Yanwei Li,Jinhuan Yao,Jiqiong Jiang,Xuejiao Chen,Wenhan Xu
Prussian blue (PB) and its analogs (PBAs) have become a research hotspot in the fields of electrochemical energy storage and electrochromism due to their good reversible redox activity, and reversible color change response in different redox states. Herein, a series of trimetallic PBAs (Co/NiHCF with Co to Ni molar ratios of 1:0, 3:1, 1:1, 1:3, and 0:1) are synthesized by a facile co-precipitation method. In particular, the impact of Co to Ni molar ratio on the lithium storage and electrochromic properties of Co/NiHCF materials are systemically investigated. All five samples possess good crystallinity but the particle size decreases with the reduction of Co/Ni molar ratio. The color change, redox reaction potential, and lithium storage activity of the samples can be readily controlled by adjusting the molar ratio of Co to Ni. The lithium storage activity of the samples strengthens with the increase of Ni content in Co/NiHCF, accompanied by a decrease in redox potentials. With the increase of Ni content, the color of the Co/NiHCF film in the oxidation state changes from purple-red to orange, and finally to yellow; in the reduction state, the color of the film changes from green to light green and then to colorless. All the samples exhibit superior rate capability, excellent cycling stability, and short switching time (in the range of 1.6 to 4.3 s). The present work demonstrates a facile strategy for readily tunning the lithium storage activity, redox reaction potentials, and realizing rich color changes of PBA-based bifunctional materials.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Linbo Yang,Yichao Lin,Yayun Zhao,Jiejie Li,Ziqi Tian,Yaqi Wu,Haitao Hu,Hao Wang,Liang Chen
Zeolites are promising materials for CO2 adsorption, yet they still face the challenges of low adsorption capacity and selectivity. Herein, we report a strategy of grafting ethylenediamine to a Co-exchanged Y zeolite to improve the CO2 adsorption capacity of Y zeolite via strong interactions between Co2+ and amine groups. Functionalization of zeolite Y with amines (Co-Y-EN) enables significant improvement in the CO2 adsorption capacity (4.36 mmol/g at 1 bar and 298 K), which is 1.73 times higher than that of pristine Na-Y zeolite. Moreover, Co-Y-EN demonstrates enhanced CO2 selectivity, as confirmed by both single-component gas adsorption experiments and breakthrough tests. The superior selectivity is attributed to the strong affinity between the amine sites and CO2 molecules, as well as the optimized pore sizes for CO2 adsorption. Overall, this study presents a straightforward approach to enhancing the CO2 adsorption performance of zeolite materials.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Siru He,Huimin Yuan,Peide Zhu,Xingzhu Wang,Baomin Xu
Enhancing the energy output of batteries in low temperatures is critical to broadening the application areas of advanced electronic devices, which can be accomplished by utilizing high-voltage cathodes to match lithium metal anode, optimizing electrolyte electrochemical windows and forming stable solid electrolyte interphases to provide facile ion-transmission kinetics at low temperature. Herein, we demonstrate a fluorinated ester co-solvent electrolyte, which applies 1 M LiPF 6 in an ethyl 4,4,4-trifluoro butyrate/fluoroethylene carbonate (FEC) (4/1 by volume ratio) that jointly satisfies high voltage cathode and lithium metal anode reversibility at required ambient. The performance of the battery is due to the rapid dissociation of Li + and the formation of a fluorine-rich inorganic electrolyte interface in the fluorinated solvent. Therefore, the fluorinated ester co-solvent electrolyte system can provide 209.9 mAh g −1 , 194.8 mAh g −1 , and 175.5 mAh g −1 when discharged at room temperature, −20 ℃ and −40 ℃, respectively, those far exceeds the performance of carbonate electrolytes. This work advances the development of low-temperature lithium metal batteries.
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