Journal of Materials Chemistry A
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2024
·Vol. 12
·期 48
·33917-33925
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IF 10.7
Yi Ma,Luming Li,Jialing Tang,Zongkun Hu,Yong Zhang,Huan Ge,Ning Jian,Jun Zhao,Andreu Cabot,Junshan Li
Plastics have become an integral part of modern society due to their excellent mechanical properties, light weight, chemical stability and low cost. However, their continuous production and use worldwide have resulted in a major environmental problem. In this context, the green degradation and upcycling of waste plastics using electrochemical oxidation present a promising solution. To make this solution practical, the development of cost-effective catalysts optimized for this reaction is essential. In this study, we propose a new catalyst for the electrocatalytic reforming of ethylene glycol (EG) derived from polyethylene terephthalate (PET) to formic acid. The catalyst comprises layered Ni–Co9S8 nanosheet arrays (NSAs) grown on nickel foam (NF) via the hydrothermal method. Under EG oxidation reaction (EGOR) conditions, the Ni–Co9S8 NSAs/NF catalyst achieves Faraday efficiencies (FEs) of up to 92%. Additionally, the direct use of commercial PET plastic powder hydrolysate still enables formate FEs to exceed 90%. These outstanding results are rationalized using density functional theory (DFT) calculations providing insights into the role of the different elements in the EGOR. Overall, this study demonstrates both a synthetic strategy for transition metal sulfides and an efficient and sustainable strategy for the upgraded recycling of PET plastics.
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Energy Advances
·
2024
·
IF 3.2
Kunpeng Liu,Xu Wang,Nan Wang,Ruiyong Zhang,Meinan Yang,Baorong Hou,Wolfgang Sand
Rationally designing high-efficiency catalysts for electrochemical two-electron water oxidation reaction (2e− WOR) to produce hydrogen peroxide (H2O2) is extremely important, while designing bimetallic metal–organic frameworks (MOFs) is of great significance for effective 2e− WOR. Herein, MIL-53(Fe) and different proportions of Co-doped MIL-53(Fe) were prepared by a hydrothermal method. The structural characterization and elemental analysis showed that the Co ions were successfully doped into MIL-53(Fe) to form a MIL-53(Fe/Co) bimetallic MOF, and the morphology of MIL-53(Fe/Co) became more regular after Co doping. We found that the optimized MIL-53(Fe/Co) exhibits remarkable 2e− WOR performance, which gave an overpotential of 150 mV at 1 mA cm−2. The overpotential of MIL-53(Fe/Co) was approximately 220 mV (at 1 mA cm−2) lower than that of MIL-53(Fe), which may be attributed to the change of microstructure of MIL-53(Fe) after Co doping and the synergistic effect between Fe/Co. Our work introduces a strategy for designing bimetallic MOF-based electrocatalysts, opening up new possibilities for efficient 2e− WOR systems.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Zhao-Xing Yan,Ling-Xi Zhao,Ning Liu,Na Li,Ru-Song Zhao
Non-steroidal anti-inflammatory drugs (NSAIDs) have gained significant attention as emerging pollutants and are increasingly detected in aquatic environments. Therefore, it is imperative to investigate the efficient removal of NSAIDs from water systems. In this study, a magnetic LDH with three-dimensional hollow structure (Fe 3 O 4 @ZIF-67@Co-Ni LDH) was synthesized using ZIF-67 as a template for the removal of carprofen (CPF) and flurbiprofen (FLU) from water environments. The adsorption process of CPF and FLU on Fe 3 O 4 @ZIF-67@Co-Ni LDH and the competitive adsorption between these two NSAIDs were investigated. The adsorption mechanism was explored by experimental analysis and theoretical calculation. Results demonstrated that the pseudo-second-order kinetic model and Liu isotherm model can better fit the kinetic and isotherm data, and according to the thermodynamic data analysis, the adsorption process was exothermic, spontaneous and stable. The adsorption capacity of CPF and FLU on Fe 3 O 4 @ZIF-67@Co-Ni LDH can reach 856.2 mg/g and 797.5 mg/g. Fe 3 O 4 @ZIF-67@Co-Ni LDH exhibited high adsorption capacity for CPF and FLU in actual environment water, with stronger affinity towards CPF when both NSAIDs coexisted simultaneously. The three-dimensional hollow structure enhanced the adsorption capacity of Fe 3 O 4 @ZIF-67@Co-Ni LDH, making it a promising adsorbent for NSAIDs.
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JOURNAL OF ETHNOPHARMACOLOGY
·
2025
·
IF 5.4
Shasha Han,Zichen Luo,Shihang Bao,Zihan Xiao,Weichen Xu,Tong Xie,Chen Shi,Jin Wang,Jinjun Shan
Ethnopharmacological relevance Platycodon grandiflorus root, is a widely used herb in East Asia for treating respiratory diseases, but research on its oral safety is limited. Aim of the study This study examines the potential adverse gastrointestinal reactions resulting from excessive consumption of Platycodon grandiflorus root (PR) and its effects on gut microbiota and host co-metabolism. Materials and methods This study evaluated the effects of different doses (1.5, 4.5, and 7.5 g/kg/day) of PR on ICR mice through gavage. Select the 7.5 g/kg/day dosage group and the control group to assess intestinal morphology and conduct histopathological studies. Examine inflammation-related factors and tight junction proteins using WB, qPCR, and ELISA. Additionally, perform 16S rDNA sequencing and metabolomic analyses to evaluate changes in gut microbiota and endogenous metabolites. Finally, the clearance of gut microbiota with antibiotics, the effects of excessive PR on mice were investigated. Results Excessive intake of PR can lead to mortality in mice, as well as symptoms such as intestinal flatulence and slowed intestinal transit, suggesting the occurrence of chronic intestinal pseudo-obstruction accompanied by endotoxemia. It altered both α-diversity and β-diversity in the gut microbiota of mice, with increased relative abundances of Pseudomonadota, Verrucomicrobiota, Escherichia-Shigella , Akkermansia , Bacteroides , and Klebsiella , closely linked to intestinal obstruction and bacterial overgrowth. Excessive intake of PR also resulted in metabolic disturbances in mice, particularly in the levels of metabolites such as bate-hydroxybutyrate, 5,6-dihydrouracil, uridine, isoleucine, mannitol, bate-alanine, L-cysteine, L-tyrosine, and orotic acid, which may provide insights into the side effects associated with excessive consumption of PR. Clearing the gut microbiota significantly mitigated adverse effects on the intestines and restored metabolite levels. Conclusions This study demonstrates that excessive PR induces gut microbiota and metabolic disruption in normal mice, with the overgrowth of Gram-negative bacteria releasing LPS that impair smooth muscle contraction, leading to adverse effects such as chronic intestinal pseudo-obstruction.
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ChemistrySelect
·
2025
·Vol. 10
·期 8
·e202406007
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IF 2
Chenxi Li,Kang Li,Shina Li,Ruixin Ma
Graphical In this study, copper hexacyanoferrate (CsRb–CuHCF) was used as a precipitant. Results demonstrated that CsRb–CuHCF can efficiently separate Rb + and Cs + from the high-salty solutions. The enrichment factor was up to 384 before and after precipitation. The precipitant reacts first with Cs + and then gradually with Rb + and can be used for the separation of Cs + and Rb + from each other. Cesium (Cs) and rubidium (Rb) are important rare alkali metal elements that are scarce and dispersed in nature. They often coexist with high amounts of Na + and K + . In this study, copper hexacyanoferrate (CuHCF) was used as a co-precipitant to enrich Cs + and Rb + in a high-salt solution. The effect of parameters, such as type and dose of divalent metal ions, solution pH, material dropping speed, reaction time, and temperature, was investigated for the recovery rate of Cs + and Rb + . Results showed that the recovery rates of Cs + and Rb + were 99.78% and 88.84% at the optimal Cu 2+ /(Cs + +Rb + ) molar ratio of 0.5, respectively. The reaction could be completed within 10 min in pH 3–8. The detailed characterization of the Cs + and Rb + containing co-precipitants, CsRb–CuHCF, confirm a general formula of Cs 1.09 Rb 0.81 K 0.16 Cu 0.97 Fe(CN) 6 . The (Cs + +Rb + )/(Na + +K + ) increased significantly from 0.074 to 28.47 before and after precipitation, which realized the effective enrichment of Cs + and Rb + . Studies of the precipitation reaction mechanism showed that the precipitant reacted first with Cs + and then with Rb + . This process offers a promising avenue for the enrichment and separation of Cs + and Rb + from high-salty solutions.
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CERAMICS INTERNATIONAL
·
2024
·
IF 5.1
Changhong Zhou,Rui Ling,Menglei Wang,Chao Yang,Wentao Qi
Syngas , a mixture of H 2 and CO with adjustable compositional ratios, can be directly produced via H 2 O/CO 2 co-electrolysis in solid oxide electrolysis cells (SOECs). In this study, We have developed a strategy to enhance the catalytic activity of titanate perovskite cathodes by constructing active metal-oxide interfaces through the in-situ growth of Ni x Cu 1-x alloy nanocatalysts (x = 0, 0.25, 0.5, 0.75 and 1) on LST matrix. The evenly distribution of Ni x Cu 1-x alloy nanoparticles (∼30 nm) on the LST substrate has been confirmed through a serious of characterization techniques, including XRD , XPS, SEM and TEM. Specifically, the LSTNi 0.75 Cu 0.25 cathode demonstrated an optimal synergistic effect , achieving high efficiency in the co-electrolysis of H 2 O/CO 2 to syngas. Under an applied voltage of 1.6 V at 800 °C, the syngas production rate reaches 5.43H 2 and 3.48 CO ml min −1 cm −2 with ∼96 % Faradaic efficiency. Furthermore, the composition of the produced syngas can be finely tuned in a broad range from 0.8 to 3.5 b y simply adjusting the inlet gas composition (H 2 O/CO 2 ratio) and the operating temperature. The LSTNi 0.75 Cu 0.25 cathode, when subjected to continuous H 2 O/CO 2 co-electrolysis for 100 h, exhibited remarkable stability, attributing to the robust and active nature of the metal-oxide interfaces.
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BIOMASS & BIOENERGY
·
2025
·
IF 5.8
Wenhao Zhang,Fei Wang,Junfeng Feng,Hui Pan
Hydrodeoxygenation is currently an effective strategy for upgrading bio-oils. In this study, Al 2 O 3 –TiO x composite metal oxide was synthesized using the sol–gel method and then impregnated with Ni–Co bimetals for the selective hydrodeoxygenation conversion of lignin-derived phenolic compounds into cyclohexanol. The impact of different carriers and Ni Co metal content was investigated in detail, with the optimal 10Ni–5Co/Al 2 O 3 –TiO x achieving 93.7 % cyclohexanol yield by completely converting guaiacol within 2 h under mild reaction conditions of 200 °C and 1 MPa H 2 with isopropanol as the solvent. XRD and HRTEM analyses confirmed the presence of Ni and Co in an alloy form. XPS results indicated that the Ti synthesized by the sol–gel method primarily existed in the form of Ti 3+ , with suitable oxygen vacancies that could enhance substrate adsorption and conversion. The reaction pathway for the selective conversion of guaiacol to cyclohexanol was inferred based on the results of GC-MS analysis of byproducts.
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Journal of Energy Chemistry
·
2024
·
IF 14
Wenkang Miao,Ronghui Hao,Lu Gan,Wanyin Xu,Zihan Wang,Wenxin Lin,Heguang Liu,Yinchun Lyu,Qianqian Li,Jinyang Xi,Anmin Nie,Jinsong Wu,Hongtao Wang
Platinum-based (Pt) catalysts are notoriously susceptible to deactivation in industrial chemical processes due to carbon monoxide (CO) poisoning. Overcoming this poisoning deactivation of Pt-based catalysts while enhancing their catalytic activity, selectivity, and durability remains a major challenge. Herein, we propose a strategy to enhance the CO tolerance of Pt clusters (Pt n ) by introducing neighboring functionalized guest single atoms (such as Fe, Co, Ni, Cu, Sb, and Bi). Among them, antimony (Sb) single atoms (SAs) exhibit significant performance enhancement, achieving 99% CO selectivity and 33.6% CO 2 conversion at 450 °C. Experimental results and density functional theory (DFT) calculations indicate the optimization arises from the electronic interaction between neighboring functionalized Sb SAs and Pt clusters, leading to optimal 5 d electron redistribution in Pt clusters compared to other functionalized guest single atoms. The redistribution of 5 d electrons weaken both the σ donation and π backdonation interactions, resulting in a weakened bond strength with CO and enhancing catalyst activity and selectivity. In situ environmental transmission electron microscopy (ETEM) further demonstrates the exception thermal stability of the catalyst, even under H 2 at 700 °C. Notably, the functionalized Sb SAs also improve CO tolerance in various heterogenous catalysts, including Co/CeO 2 , Ni/CeO 2 , Pt/Al 2 O 3 , and Pt/CeO 2 -C. This finding provides an effective approach to overcome the primary challenge of CO poisoning in Pt-based catalysts, making their broader applications in various industrial catalysts.
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MOLECULES
·
2024
·Vol. 29
·期 21
·4994
·
IF 4.2
Fan Ma,Hong-Wei Lin,Zizi Li,Wen-Jing Li,Jia-Wei Wang,Gangfeng Ouyang
Noble-metal-free CO2reduction systems based on cobalt phthalocyanine (CoPc) and its derivatives have demonstrated remarkable photocatalytic performances; however, their structure-activity relationship with electronic tuning remains unexplored. Herein, we now provide a systematic study to investigate the electron effects of substituents on theCoPcfamily in photocatalytic CO2reduction, where a Cu(I) heteroleptic photosensitizer is utilized. The highest performance can be achieved using cobalt tetracarboxylphthalocyanine in light-driven CO2-to-CO reduction, with a maximum turnover number of 2950 at 450 nm and an outstanding apparent quantum yield of 63.5% at 425 nm, over ten times the activity with the tetra-dimethylamino-substitutedCoPcderivative. The favorable electron-withdrawing effects have been further verified by DFT calculations and cyclic voltammetry, which reduces the overpotential required for CO2reduction and decreases the Gibbs free energy of the catalyst active intermediates, particularly the CO-desorption energetics.
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DIAMOND AND RELATED MATERIALS
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2025
·
IF 5.1
Tengfei Wang,Boyu Liu,Qing Pang,Hongyu Wang
Three-dimensional graphene aerogels are emerging as promising materials for microwave absorption, due to their unique characteristics of low density and high porosity. Although lightweight electromagnetic wave (EMW) graphene-based aerogel absorbers have been developed, synergistically optimizing the EMW performance of these absorbers through structural design and simultaneously introducing multiple loss mechanisms remains challenging. This paper presents an innovative design strategy that modifies the hole structure of aerogel by controlling the content of Co ions while simultaneously introducing magnetic loss, thereby achieving ultra-light broadband absorption performance. Notably, when the added amount of Co ions is 0.3 mmol, the aerogel exhibits a minimum reflection loss (RL min ) of −44.9 dB, and an effective absorption bandwidth (EAB) of 5.68 GHz. The remarkable EMW absorption performance can be attributed to the enhancements of polarization loss and magnetic loss. Furthermore, the RCS simulation results indicate that the aerogel effectively reduces EMW scattering in practical applications. Thus, this research offers a highly effective strategy for the development of EMW absorption materials that are thin, lightweight, broadband, and high-performance.
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Molecular Catalysis
·
2024
·
IF 3.9
Xingling Zhao,Xue Zhou,Wanyan Xing,Zhimin Yuan,Kaili Wang,Qihang Zhang,Yulong Shan,Jiani Liu,Lin Ju,Zaiyong Jiang,Hong He
CO is a ubiquitous air pollutant, frequently encountered in the fields of automotive exhaust purification, especial in the cold-start-emission stage. Pt based catalysts are widely used to purify CO into CO 2 owing to their exceptional performance. But they can be few excited to exhibit reasonable catalytic activity due to the low temperature at the cold-start-emission stage. In exhaust gas purification catalysts used by fossil fuel-based vehicles, Al 2 O 3 is used frequently. But there are rarely reports of Pt loaded Al 2 O 3 catalysts achieving feasible activity of CO oxidation at room temperature. Herein, we prepared Cu x Pt y alloy/Al 2 O 3 catalysts (with high penta-coordinated Al 3+ (Al V )), Al V centers as binding sites for Cu 3 Pt 1 alloys on Al 2 O 3 enable the high dispersion and stability of Cu 3 Pt 1 alloy. The adsorption capacity of O 2 and CO molecules on Cu 3 Pt 1 surface are stronger than the case on Pt surface, which may make O 2 and CO molecules more easily activated, making the CO oxidation reaction easier. In addition, the desorption of CO 2 from Cu x Pt y surface is easier compared to that on Pt surface, increasing the frequency of use of active sites there. Therefore, this Cu 3 Pt 1 /Al 2 O 3 catalyst exhibits 100 % conversion of CO with a GHSV of 6×10 3 mL·g −1 cat ·h −1 at room temperature. This work provides a feasible guideline for the design and synthesis of Pt loaded Al 2 O 3 catalysts toward room temperature CO oxidation.
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Scientific Reports
·
2024
·Vol. 14
·期 1
·1-15
·
IF 3.8
Yue Jiayuan,Zheng Qi,Ding Shushu,Yin Yujian,Zhang Xiaodan,Wang Liyun,Gu Yipeng,Li Jiejia,Zhang Yuhan,Shi Yurou,Dong Yuetan,Zhu Qing,Duo Huixiao
In this study, the removal effect of a new MOF-on MOF adsorbent based on Cu–Co bimetallic organic frameworks on tetracycline antibiotics (TCs) in water system was studied. The adsorbent (Cu-MOF@Co-MOF) were synthesized by solvothermal and self-assembly method at different concentrations of Co 2+ /Cu 2+ . The characterization results of SEM, XRD, XPS, FTIR and BET indicated that the MOF-on MOF structure of Cu-MOF@Co-MOF exhibited the best recombination and physicochemical properties when the molar ratio of Co 2+ : Cu 2+ is 5:1. In addition, the Cu-MOF@Co-MOF have a high specific surface area and bimetallic clusters, which can achieve multi-target synergistic adsorption of TCs. Based on above advantages, Cu-MOF@Co-MOF provided a strong affinity and could efficiently adsorb more than 80% of pollutants in just 5 to 15 min using only 10 mg of the adsorbent. The adsorption capacity of tetracycline and doxycycline was 434.78 and 476.19 mg/g, respectively, showing satisfactory adsorption performance. The fitting results of the experimental data were more consistent with the Langmuir isotherm model and pseudo-second-order kinetic model, indicating that the adsorption process of TC and DOX occurred at the homogeneous adsorption site and was mainly controlled by chemisorption. Thermodynamic experiments showed that Cu-MOF@Co-MOF was thermodynamically advantageous for the removal of TCs, and the whole process was spontaneous. The excellent adsorption capacity and rapid adsorption kinetics indicate the prepared MOF-on MOF adsorbent can adsorb TCs economically and quickly, and have satisfactory application prospects for removing TCs in practical environments. The results of the study pave a new way for preparing novel MOFs-based water treatment materials with great potential for efficient removal.
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