摘要:
Based on rigid poly (vinyl benzyl chloride) (PVB) and flexible ethylene vinyl alcohol (EVOH) main chains, anion exchange membranes (AEMs) are prepared using the acetal reaction and the Menshutkin reaction. The crosslinking of rigid and flexible backbones, along with the regulation of hydrophilicity/hydrophobicity by fluorinated side chains on EVOH, endows the resulting AEMs with good mechanical properties. The high ionic conductivity of AEMs originates from the effective ionic aggregation morphology, which is generated from the differences between the two main chains and the fluorinated side chains. Their non-polar main chains with stable acetal groups and β-H-free cations contribute to high alkaline stability of AEMs. Specifically, c IM25-TFBA75-EVOH-PVB possesses an ionic conductivity of 148.5 mS cm −1 at 80 °C, with a swelling degree of 12.3 %. The tensile strength and elongation at break of the sample in a fully hydrated state at 25 °C are 7.0 MPa and 12.2 %, respectively. After immersion in 1 M KOH at 80 °C for 1080 h, it almost retains 90 % of its mass, ion exchange capacity, and conductivity. In fuel cells, it achieves peak power densities of 895 mW cm −2 with H 2 /O 2 and 692 mW cm −2 with H 2 /CO 2 -free air at 80 °C.
Based on rigid poly (vinyl benzyl chloride) (PVB) and flexible ethylene vinyl alcohol (EVOH) main chains, anion exchange membranes (AEMs) are prepared using the acetal reaction and the Menshutkin reaction. The crosslinking of rigid and flexible backbones, along with the regulation of hydrophilicity/hydrophobicity by fluorinated side chains on EVOH, endows the resulting AEMs with good mechanical properties. The high ionic conductivity of AEMs originates from the effective ionic aggregation morphology, which is generated from the differences between the two main chains and the fluorinated side chains. Their non-polar main chains with stable acetal groups and β-H-free cations contribute to high alkaline stability of AEMs. Specifically, c IM25-TFBA75-EVOH-PVB possesses an ionic conductivity of 148.5 mS cm −1 at 80 °C, with a swelling degree of 12.3 %. The tensile strength and elongation at break of the sample in a fully hydrated state at 25 °C are 7.0 MPa and 12.2 %, respectively. After immersion in 1 M KOH at 80 °C for 1080 h, it almost retains 90 % of its mass, ion exchange capacity, and conductivity. In fuel cells, it achieves peak power densities of 895 mW cm −2 with H 2 /O 2 and 692 mW cm −2 with H 2 /CO 2 -free air at 80 °C.
摘要:
The metal-organic framework materials ZIF-8 and UiO-66-NH2, synthesized by hydrothermal methods, were characterized in detail and combined to catalyze the transfer hydrogenation of 5-hydroxymethylfurfural (5-HMF) to 2,5-di(hydroxymethyl)furan (2,5-DHMF) using isopropanol as the hydrogen source. The ZIF-8/UiO-66-NH2 catalyst mixture exhibited abundant Lewis acid-base sites and a hierarchical multiporous structure with a large specific surface area (564.0 m2/g). The conversion of 5-HMF reached 98.2 %, and the selectivity and yield of 2,5-DHMF were 96.2 % and 94.5 %, respectively. The recycling performance of ZIF-8/UiO-66-NH2 was also investigated, and the conversion of 5-HMF and selectivity of 2,5-DHMF significantly decreased to 78.4 % and 79.1 % in the second run, respectively. The loss of −NH2 groups was found to be the main reason for the decrease in activity. However, the catalytic activity of the recovered catalyst can be almost completely restored by the addition of a small amount of fresh UiO-66-NH2 and ZIF-8, and the conversion of 5-HMF and selectivity of 2,5-DHMF were increased to 89.4 % and 95.5 %, respectively. In the proposed reaction mechanism, Lewis acid-base sites play important roles and exhibit a synergistic catalytic effect in the selective conversion of 5-HMF to 2,5-DHMF.
The metal-organic framework materials ZIF-8 and UiO-66-NH2, synthesized by hydrothermal methods, were characterized in detail and combined to catalyze the transfer hydrogenation of 5-hydroxymethylfurfural (5-HMF) to 2,5-di(hydroxymethyl)furan (2,5-DHMF) using isopropanol as the hydrogen source. The ZIF-8/UiO-66-NH2 catalyst mixture exhibited abundant Lewis acid-base sites and a hierarchical multiporous structure with a large specific surface area (564.0 m2/g). The conversion of 5-HMF reached 98.2 %, and the selectivity and yield of 2,5-DHMF were 96.2 % and 94.5 %, respectively. The recycling performance of ZIF-8/UiO-66-NH2 was also investigated, and the conversion of 5-HMF and selectivity of 2,5-DHMF significantly decreased to 78.4 % and 79.1 % in the second run, respectively. The loss of −NH2 groups was found to be the main reason for the decrease in activity. However, the catalytic activity of the recovered catalyst can be almost completely restored by the addition of a small amount of fresh UiO-66-NH2 and ZIF-8, and the conversion of 5-HMF and selectivity of 2,5-DHMF were increased to 89.4 % and 95.5 %, respectively. In the proposed reaction mechanism, Lewis acid-base sites play important roles and exhibit a synergistic catalytic effect in the selective conversion of 5-HMF to 2,5-DHMF.
通讯机构:
[Liu, P ; Liu, Y ; Liu, P] T;TianGong Univ, Sch Mat Sci & Engn, State Key Lab Separat Membranes & Membrane Proc, Tianjin 300387, Peoples R China.;Tiangong Univ, Sch Chem, Tianjin 300387, Peoples R China.;Wuhan Polytech Univ, Sch Chem & Environm Engn, Wuhan 430023, Peoples R China.;Tiangong Univ, Cangzhou Inst, Cangzhou 061000, Peoples R China.
摘要:
Correction for ‘Potentiating light-harvesting tactics through an A–D–A structure: repolarization of tumor-associated macrophages through phototherapy’ by Pai Liu et al. , J. Mater. Chem. B , 2024, 12 , 7870–7878, https://doi.org/10.1039/D4TB00814F.
摘要:
Lignin is the only natural polymer compound containing a benzene ring on earth, and its conversion to monophenolic compounds is attracting more attention. Cu-dopped CuCo 2 O 4 is synthesized and further used to catalyze the oxidative conversion of lignin to monophenolic compounds. It is found that the conversion of lignin is affected by the molar ratio of Cu to Co, the amounts of catalyst and H 2 O 2 , reaction temperature and time, and CuCo 2 O 4 exhibits excellent catalytic performance. Under the optimized reaction conditions, the total yield of monophenolic compounds reaches 21.7%. CuCo 2 O 4 also possesses good recyclable performance, and the total yield of monophenolic compounds slightly drops to 17.6% after four cycles. A plausible mechanism for the conversion of lignin to monophenolic compounds is proposed. During the depolymerization of lignin, C O and C C bonds are broken to form monophenols. This work provides an effective catalyst for the conversion of lignin to monophenol and expands the way of high-value utilization of biomass.
摘要:
Dual-co-catalyst-modified photocatalysts enhance charge separation efficiency, but the traditional dual co-catalyst is still difficult to get a high separation efficiency due to size and aggregation. Herein, we report bimetallic MIL-53(Fe/Mn) as dual co-catalysts with separate electron and hole mediators. CdS NPs were in-situ grown into MIL-53(Fe/Mn) at varying ratios. 20 %CdS/MIL-53(Fe/Mn) composites shown optimum photocatalytic CO 2 reduction activity. The XPS results shown the strong interaction between CdS and MIL-53(Fe/Mn). The EPR measure proved the carriers of CdS can be transferred to MIL-53(Fe/Mn) oxidation cluster by the oxo-Fe(III)/Fe(II) and oxo-Mn(II)/Mn(III) redox cycling, and the results also suggest the oxo-Fe(III) and oxo-Mn(II) were redox active sites. We believe the approach that bimetallic MOFs act as dual cocatalyst to improve the photocatalytic activity would open a new avenue for the separation efficiency of photo-generated charge carriers.
Dual-co-catalyst-modified photocatalysts enhance charge separation efficiency, but the traditional dual co-catalyst is still difficult to get a high separation efficiency due to size and aggregation. Herein, we report bimetallic MIL-53(Fe/Mn) as dual co-catalysts with separate electron and hole mediators. CdS NPs were in-situ grown into MIL-53(Fe/Mn) at varying ratios. 20 %CdS/MIL-53(Fe/Mn) composites shown optimum photocatalytic CO 2 reduction activity. The XPS results shown the strong interaction between CdS and MIL-53(Fe/Mn). The EPR measure proved the carriers of CdS can be transferred to MIL-53(Fe/Mn) oxidation cluster by the oxo-Fe(III)/Fe(II) and oxo-Mn(II)/Mn(III) redox cycling, and the results also suggest the oxo-Fe(III) and oxo-Mn(II) were redox active sites. We believe the approach that bimetallic MOFs act as dual cocatalyst to improve the photocatalytic activity would open a new avenue for the separation efficiency of photo-generated charge carriers.
作者机构:
[Quan, Fengjiao; Li, Jianfen; He, Yun; Shen, Wenjuan; Xu, Pengfei; Chen, Xiaolan] College of Chemical and Environmental Engineering, Wuhan Polytechnic University, Wuhan 430023, China;[Zhan, Guangming] School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, China;[Jia, Falong] College of Chemistry, Central China Normal University, Wuhan 430079, China. Electronic address: fljia@ccnu.edu.cn
通讯机构:
[Falong Jia] C;College of Chemistry, Central China Normal University, Wuhan 430079, China
作者机构:
[Wenjing Xiong; Yuxin Zhang; Guozhi Fan; Cheng Pan; Yifei Long] School of Chemical and Environmental Engineering, Wuhan Polytechnic University, Wuhan 430023, PR China;[Jia Meng; Canduo Shen] Systems Engineering Institute, Academy of Military Sciences of the People's Liberation Army, Beijing 100010, PR China
通讯机构:
[Canduo Shen; Yifei Long] S;Systems Engineering Institute, Academy of Military Sciences of the People's Liberation Army, Beijing 100010, PR China<&wdkj&>School of Chemical and Environmental Engineering, Wuhan Polytechnic University, Wuhan 430023, PR China
摘要:
As the increasing demand for food safety, it is crucial to find a safer and more effective method to replace traditional preservation of fruits and vegetables. Electric field preservation, as a novel preservation technology, not only prevents contamination of fresh vegetables, but also mitigates adverse effects on human health. In this paper, comparing conventional refrigeration as a benchmark, the impact of an alternating current electric field (ACEF) on the storage quality of fresh-cut Chinese cabbage and spinach was investigated. The differences in preservation effectiveness were determined by analyzing the changes of quality indicators, nutrients and four microbial indicators (Total Microbiological Numbers, E. coli , Molds, S. aureus ) within 30 days at a storage temperature of 4 °C. The spoilage rates of two fresh-cut vegetables with ACEF were lower compared with those without ACEF, reduced by 30 % and 25 %, respectively. In addition, the weight loss rate of the Chinese cabbage and spinach with ACEF was reduced by 0.10 % and 0.40 %, respectively. Between the two groups, the soluble solids content (SSC) of the Chinese cabbage with ACEF was about 4.93 % higher than without ACEF. On the contrary the SSC of the spinach with ACEF was consistently lower than without ACEF. Meanwhile, vitamin C content of the Chinese cabbage and spinach with ACEF was 4.58 % and 3.95 % higher than that without ACEF, respectively. Moreover, ACEF treatment inhibited microbial growth, resulting in lower levels of total microbiological numbers (9.19 %, 8.96 %), E. coli (12.72 %, 7.55 %), molds (7.88 %, 17.28 %), and S. aureus (10.16 %, 11.50 %) in the Chinese cabbage and spinach compared with those without ACEF treatment. All these results indicated that ACEF could represent an interesting preservation technique, which maintains the freshness of fresh-cut vegetables for a longer period of time.
As the increasing demand for food safety, it is crucial to find a safer and more effective method to replace traditional preservation of fruits and vegetables. Electric field preservation, as a novel preservation technology, not only prevents contamination of fresh vegetables, but also mitigates adverse effects on human health. In this paper, comparing conventional refrigeration as a benchmark, the impact of an alternating current electric field (ACEF) on the storage quality of fresh-cut Chinese cabbage and spinach was investigated. The differences in preservation effectiveness were determined by analyzing the changes of quality indicators, nutrients and four microbial indicators (Total Microbiological Numbers, E. coli , Molds, S. aureus ) within 30 days at a storage temperature of 4 °C. The spoilage rates of two fresh-cut vegetables with ACEF were lower compared with those without ACEF, reduced by 30 % and 25 %, respectively. In addition, the weight loss rate of the Chinese cabbage and spinach with ACEF was reduced by 0.10 % and 0.40 %, respectively. Between the two groups, the soluble solids content (SSC) of the Chinese cabbage with ACEF was about 4.93 % higher than without ACEF. On the contrary the SSC of the spinach with ACEF was consistently lower than without ACEF. Meanwhile, vitamin C content of the Chinese cabbage and spinach with ACEF was 4.58 % and 3.95 % higher than that without ACEF, respectively. Moreover, ACEF treatment inhibited microbial growth, resulting in lower levels of total microbiological numbers (9.19 %, 8.96 %), E. coli (12.72 %, 7.55 %), molds (7.88 %, 17.28 %), and S. aureus (10.16 %, 11.50 %) in the Chinese cabbage and spinach compared with those without ACEF treatment. All these results indicated that ACEF could represent an interesting preservation technique, which maintains the freshness of fresh-cut vegetables for a longer period of time.
通讯机构:
[Hu, C ] W;Wuhan Polytech Univ, Sch Chem & Environm Engn, Wuhan 430023, Peoples R China.
关键词:
Agricultural carbon emissions;Spatial spillover effect;Super-SBM model;Yangtze River economic belt
摘要:
Researching the agricultural carbon emission efficiency (ACEE) of the Yangtze River Economic Belt (YEB) has significant theoretical and policy implications for promoting high− quality agricultural development and achieving China’s “dual carbon” goals. Based on the agricultural generation panel data from the YEB spanning 2001 to 2021, the Super-SBM model for undesirable outputs is employed to calculate the ACEE for 11 provinces and cities. Additionally, kernel density estimation and Moran’s I index are utilized to analyze the temporal and spatial evolution characteristics of ACEE. Furthermore, a spatial Durbin model is applied to investigate the key factors influencing ACEE in the YEB and their spatial spillover effects. Empirical results indicate that from 2001 to 2021, the ACEE within the YEB has demonstrated a fluctuating upward trend, with significant geographical disparities among the provinces and cities along the route. In terms of spatial distribution, ACEE is characterized by a pattern of downstream > midstream > upstream, reflecting an overall trend of “higher in the east and lower in the west, and the ACEE in the YEB exhibits characteristics of spatial aggregation. ACEE exhibits a significant positive spatial spillover effect in theYEB. Key factors influencing the enhancement of ACEE include the level of mechanization and the agricultural industrial structure. Conversely, the use of pesticides serves as the primary constraint hindering the improvement of ACEE. Based on the research findings, policy recommendations have been proposed to promote green, low-carbon agriculture and enhance high-quality agricultural development in the YEB.
通讯机构:
[Zhang, L ] W;Wuhan Polytech Univ, Sch Chem & Environm Engn, Wuhan 430023, Peoples R China.
摘要:
Diffusion dialysis (DD) with anion exchange membranes (AEMs) as the core component is an ideal technology for acid recovery from acidic wastewater. Herein, a series of TEA–BPPO AEMs were prepared from triethanolamine (TEA) and brominated polyphenylene ether (BPPO) using the solution casting method. The structures of the prepared membranes were characterized and analyzed through nuclear magnetic resonance hydrogen spectroscopy ( 1 H NMR), X-ray photoelectron spectroscopy (XPS), Fourier transform infrared (FTIR) spectroscopy, and scanning electron microscopy (SEM). In addition, the properties of the membranes, such as ion exchange capacity (IEC), linear swelling rate (LSR), water uptake ( W U ), chemical stability, thermal stability and mechanical stability, were explored. In DD experiments, the optimal AEM ( i.e. , TEA–BPPO–M80) applied to simulate acid recovery from a mixed HCl (1 mol L −1 )/FeCl 2 (0.2 mol L −1 ) solution exhibited an acid dialysis coefficient ( U H + ) of 0.0629 m h −1 and separation factor ( S ) of 97.78, which were significantly better than those of the commercial membrane DF-120. In addition, the TEA–BPPO–M80 AEM exhibited excellent thermal stability and acid resistance. In summary, the prepared membranes possess great potential for application in DD acid recovery.
通讯机构:
[Peng, H ] W;Wuhan Polytech Univ, Sch Civil Engn & Architecture, Wuhan 430023, Hubei, Peoples R China.
关键词:
Magnetic chitosan microspheres;Coking wastewater;Regeneration;Adsorption
摘要:
As a new type of polymer functional material, magnetic chitosan has been widely used in wastewater treatment. In this study, magnetic chitosan microspheres (MCMs) were prepared by reversed-phase microemulsion cross-linking technology, and the adsorption capacity of MCMs to organic pollutants with high chemical oxygen demand (COD) in coking wastewater was studied. Fourier transform infrared spectroscopy (FTIR), scanning electron microscope (SEM) and energy dispersive spectrometer (EDS), brunauer - emmett - teller (BET), vibrating sample magnetometer (VSM) were characterized. The effects of Fe 3 O 4 magnetic nanoparticles (MNPs), pH and the amount of adsorbent on the adsorption properties of MCMs were investigated. The following conclusions are obtained: the MCMs prepared in this study are successfully encapsulated, and the MCMs have good magnetic properties; Meanwhile, the removal performance of COD is higher. When the addition amount of Fe 3 O 4 is 10 % of the mass fraction of chitosan, the maximum adsorption amount of COD by MCMs can reach 261.82 mg/g under the conditions of pH 7.5, reaction temperature 298 K and adsorption time 42 h. The adsorption kinetics can be described by a quasi-second-order kinetic model. In addition, after 4 times of adsorption-desorption processes, the adsorbent still has more than 40 % COD adsorption, and has good adsorption performance. In general, because of the high adsorption efficiency, strong regeneration and excellent magnetic separation performance, MCMs have practical application potential in sewage treatment, biomedicine and other fields.
As a new type of polymer functional material, magnetic chitosan has been widely used in wastewater treatment. In this study, magnetic chitosan microspheres (MCMs) were prepared by reversed-phase microemulsion cross-linking technology, and the adsorption capacity of MCMs to organic pollutants with high chemical oxygen demand (COD) in coking wastewater was studied. Fourier transform infrared spectroscopy (FTIR), scanning electron microscope (SEM) and energy dispersive spectrometer (EDS), brunauer - emmett - teller (BET), vibrating sample magnetometer (VSM) were characterized. The effects of Fe 3 O 4 magnetic nanoparticles (MNPs), pH and the amount of adsorbent on the adsorption properties of MCMs were investigated. The following conclusions are obtained: the MCMs prepared in this study are successfully encapsulated, and the MCMs have good magnetic properties; Meanwhile, the removal performance of COD is higher. When the addition amount of Fe 3 O 4 is 10 % of the mass fraction of chitosan, the maximum adsorption amount of COD by MCMs can reach 261.82 mg/g under the conditions of pH 7.5, reaction temperature 298 K and adsorption time 42 h. The adsorption kinetics can be described by a quasi-second-order kinetic model. In addition, after 4 times of adsorption-desorption processes, the adsorbent still has more than 40 % COD adsorption, and has good adsorption performance. In general, because of the high adsorption efficiency, strong regeneration and excellent magnetic separation performance, MCMs have practical application potential in sewage treatment, biomedicine and other fields.
摘要:
Self-supporting carbon fibers are extensively employed as active components in energy storage systems due to their tunable microstructures, large specific surface area, affordability, and excellent electrical conductivity. Nevertheless, conventional methods for producing carbon fibers typically involve complicated synthesis processes, environmental pollution, and high energy consumption. In this study, lignin-based carbon nanofibers (LCNFs) were prepared through electrospinning and subsequent heat treatment. The morphologies, crystal structures, and specific surface area of the as-prepared LCNFs were characterized using scanning electron microscopy, X-ray diffraction and nitrogen sorption isotherms. The influence of lignin content on the on the structural, morphological, and electrochemical properties of the carbon nanofibers were examined, particularly in their applications as supercapacitor and lithium-ion battery anode materials. The as-prepared LCNF-2 possess the highest specific surface area of 468.3 m2 g−1. As a self-supporting electrode in supercapacitors (SCs), the LCNF-2 delivered 256.3 F g−1 at 0.2 A g−1, and capacitance retention of 62.0 % at the current density raised from 0.5 to 10 A g−1. The assembled LCNF-2//LCNF-2 symmetric supercapacitor demonstrated a specific capacitance of 168 F g−1 at 5 A g−1, maintaining 100 % capacitance retention after 10,000 cycles. Additionally, it achieved an energy density of 5.6 Wh kg−1 at a power density of 1250.0 W kg−1. As a lithium-ion batteries (LIBs) anode, the LCNF-2 showed a discharge specific capacity of 1108.3 mAh g−1 and a discharge specific capacity of 377.3 mAh g−1 in the first cycle, with a capacity retention rate of 84.6 % after 100 cycles at 1C. This work offers a novel approach for the high-value utilization of agricultural waste straw lignin in energy storage devices.
Self-supporting carbon fibers are extensively employed as active components in energy storage systems due to their tunable microstructures, large specific surface area, affordability, and excellent electrical conductivity. Nevertheless, conventional methods for producing carbon fibers typically involve complicated synthesis processes, environmental pollution, and high energy consumption. In this study, lignin-based carbon nanofibers (LCNFs) were prepared through electrospinning and subsequent heat treatment. The morphologies, crystal structures, and specific surface area of the as-prepared LCNFs were characterized using scanning electron microscopy, X-ray diffraction and nitrogen sorption isotherms. The influence of lignin content on the on the structural, morphological, and electrochemical properties of the carbon nanofibers were examined, particularly in their applications as supercapacitor and lithium-ion battery anode materials. The as-prepared LCNF-2 possess the highest specific surface area of 468.3 m2 g−1. As a self-supporting electrode in supercapacitors (SCs), the LCNF-2 delivered 256.3 F g−1 at 0.2 A g−1, and capacitance retention of 62.0 % at the current density raised from 0.5 to 10 A g−1. The assembled LCNF-2//LCNF-2 symmetric supercapacitor demonstrated a specific capacitance of 168 F g−1 at 5 A g−1, maintaining 100 % capacitance retention after 10,000 cycles. Additionally, it achieved an energy density of 5.6 Wh kg−1 at a power density of 1250.0 W kg−1. As a lithium-ion batteries (LIBs) anode, the LCNF-2 showed a discharge specific capacity of 1108.3 mAh g−1 and a discharge specific capacity of 377.3 mAh g−1 in the first cycle, with a capacity retention rate of 84.6 % after 100 cycles at 1C. This work offers a novel approach for the high-value utilization of agricultural waste straw lignin in energy storage devices.
摘要:
In this study, bovine collagen peptide (BCP) decorated selenium nanoparticles (BCP-SeNPs) were prepared using BCP as a protective and reducing agent, and their structure, hypolipidemic and antitumor activities were investigated. The results of the various techniques including dynamic light scattering (DLS), transmission electron microscopy (TEM), energy dispersive x-ray (EDX) spectroscopy, x-ray photoelectron spectroscopy (XPS), circular dichroism (CD) spectroscopy, Fourier transform infrared (FT-IR) spectroscopy confirmed the successful synthesis of BCP-SeNP. The polydispersity index (PDI) and zeta-potential analysis displayed that the PDI of BCP-SeNPs was about 0.12, smaller than BCP. The zeta-potential absolute value of BCP-SeNPs was found to be 34.2 mV, higher than BCP, suggesting that the stability of the BCP-SeNPs was better than BCP. Hypolipidemic performance evaluation indicated that binding capacity of BCP-SeNPs to bile salts was the highest when its concentration was 0.3 mM, and significantly higher than bare SeNPs, bovine serum albumin decorated SeNPs (BSA-SeNPs), and hyaluronic acid decorated SeNPs (HA-SeNPs). Moreover, the viability of HepG2 cells after BCP-SeNPs treatment was only 22.95%, which was considerably lower than that of bare SeNPs, BSA-SeNPs, and HA-SeNPs, showing better antitumor activity. These findings are expected to provide novel active ingredients that can be employed as functional foods and drugs.
通讯机构:
[Liu, Y; Li, SL ] T;Tiangong Univ, State Key Lab Separat Membranes & Membrane Proc, Tianjin 300387, Peoples R China.;Tiangong Univ, Sch Elect & Informat Engn, Key Lab Hollow Fiber Membrane Mat & Membrane Proc, MOE, Tianjin 300387, Peoples R China.;Tiangong Univ, Sch Chem, Tianjin 300387, Peoples R China.
关键词:
S -Scheme heterojunction;Cuproptosis;Nanocatalytic therapy;Chemodynamic therapy;Apoptosis
摘要:
Nanocatalysts show great promise in nanomedicine due to their unique catalytic activities. However, the rapid recombination of excited electrons and holes leads to low efficacy of nanocatalytic therapy. Herein, ultrasmall S-Scheme heterojunction MoC/CuFeO x nanoparticles (MCFO NPs) with specific charge transport route are rationally designed and engineered for efficient apoptosis/cuproptosis co-activated nanocatalytic therapy. Thermal analysis revealed two steps of S-Scheme heterojunction formation: adsorption and internal structure change. In this structure, the staggered energy levels and band bending enhance the separation of photogenerated electrons and holes, improving redox capacity and catalytic activity, mediating O 2 production, regulating the hypoxic tumor microenvironment, increasing reactive oxygen species, and inducing apoptosis. Additionally, due to excessive copper, the oligomerization of lipoylated dihydrolipoamide S-acetyltransferase and disruption of tricarboxylic acid cycle are caused to evoke cuproptosis. This work proposes a feasible strategy to enhance the nanocatalytic therapeutic efficacy through charge transport engineering, thereby mediating apoptosis/cuproptosis co-activated synergistic anti-tumor therapy.
Nanocatalysts show great promise in nanomedicine due to their unique catalytic activities. However, the rapid recombination of excited electrons and holes leads to low efficacy of nanocatalytic therapy. Herein, ultrasmall S-Scheme heterojunction MoC/CuFeO x nanoparticles (MCFO NPs) with specific charge transport route are rationally designed and engineered for efficient apoptosis/cuproptosis co-activated nanocatalytic therapy. Thermal analysis revealed two steps of S-Scheme heterojunction formation: adsorption and internal structure change. In this structure, the staggered energy levels and band bending enhance the separation of photogenerated electrons and holes, improving redox capacity and catalytic activity, mediating O 2 production, regulating the hypoxic tumor microenvironment, increasing reactive oxygen species, and inducing apoptosis. Additionally, due to excessive copper, the oligomerization of lipoylated dihydrolipoamide S-acetyltransferase and disruption of tricarboxylic acid cycle are caused to evoke cuproptosis. This work proposes a feasible strategy to enhance the nanocatalytic therapeutic efficacy through charge transport engineering, thereby mediating apoptosis/cuproptosis co-activated synergistic anti-tumor therapy.
摘要:
Microplastics (MPs) carry and spread environmental pollutants far and wide. The surface structure of MPs changes when MPs are exposed to light, and which influences the adhesion of MPs to pollutants. In this study, ultraviolet (UV) irradiation (1000 W mercury lamp, 80W/cm2) was utilized to simulate the aging of PVC MPs in natural environments. The adsorption and desorption behaviors of PVC MPs on tildipirosin were investigated. Furthermore, Escherichia coli was used for antibiotic stress experiments. The results revealed that aged PVC MPs exhibited a new oxygen-containing absorption peak at 1736 cm−1, attributing to the stretching of a C = O. Notably, tildipirosin adsorption by the pristine PVC MPs conformed to the pseudo-first-order kinetic model (R2 = 0.975), while the aged PVC MPs followed the pseudo-second-order kinetic model. The adsorption process followed the Langmuir thermodynamic equation. Furthermore, the desorption rates of the pristine, 6-day-aged, and 12-day-aged PVC MPs were determined to be 24.2%, 24.3%, and 30.7%, respectively. Thus, the data indicated that tildipirosin was more easily desorbed from the aged PVC MPs. pH studies showed that electrostatic forces significantly impacted tildipirosin adsorption. The antibiotics stress experiments demonstrated that Escherichia coli K12 could tolerate a higher concentration (40 mg/L) of tildipirosin undergoing the domestication with low concentration (12.8 mg/L tildipirosin) sequential stress. The findings of this study are expected to contribute to the understanding of the synergistic behavior of MPs and antibiotics in the environment and the ecological risks involved.
摘要:
Collagen is one of the most important natural biopolymers, it plays its role as a load-bearing structure in tissues only after polymerizing into fibrils. DDR2 is a collagen-binding receptor tyrosine kinases, playing a role in the regulation of collagen-cell interactions. Here, we studied the recognition of collagen fibrils by DDR2 and the effect of fibrillogenesis on cell biological activity. Our results showed that for monomeric collagen, the binding affinity of DDR2 to mammalian porcine skin collagen is higher than that to fish collagen. When the assembly of collagen monomers into the collagen fibril, the binding affinity of DDR2 is enhanced. In contrast, the binding ability of the hybrid fibril is stronger than the corresponding black carp skin collagen fibrils, and slightly weaker than corresponding porcine skin collagen fibril. This indicates that the introduction of porcine skin collagen in the co-assembly system can regulate the binding of DDR2 to fish-sourced collagen. We also find that compared to monomers, the fibrillogenesis of collagen promotes cell interaction with the collagen substrate, and has an increased ability to induce cells spreading. Our results confirmed that the physical state of collagen impacts its binding with DDR2 and cell behavior. These findings provide new insights into cell-collagen interactions.
Collagen is one of the most important natural biopolymers, it plays its role as a load-bearing structure in tissues only after polymerizing into fibrils. DDR2 is a collagen-binding receptor tyrosine kinases, playing a role in the regulation of collagen-cell interactions. Here, we studied the recognition of collagen fibrils by DDR2 and the effect of fibrillogenesis on cell biological activity. Our results showed that for monomeric collagen, the binding affinity of DDR2 to mammalian porcine skin collagen is higher than that to fish collagen. When the assembly of collagen monomers into the collagen fibril, the binding affinity of DDR2 is enhanced. In contrast, the binding ability of the hybrid fibril is stronger than the corresponding black carp skin collagen fibrils, and slightly weaker than corresponding porcine skin collagen fibril. This indicates that the introduction of porcine skin collagen in the co-assembly system can regulate the binding of DDR2 to fish-sourced collagen. We also find that compared to monomers, the fibrillogenesis of collagen promotes cell interaction with the collagen substrate, and has an increased ability to induce cells spreading. Our results confirmed that the physical state of collagen impacts its binding with DDR2 and cell behavior. These findings provide new insights into cell-collagen interactions.
作者机构:
[Yun He; Hui Li; Jianfeng Li] School of Chemical and Environmental Engineering, Wuhan Polytechnic University, Wuhan, 430032, Hubei, China;School of Resource and Environmental Science, Wuhan University, Wuhan, 430079, Hubei, China;Center for Water and Ecology School of Environment Tsinghua University, Beijing 100084, China;College of Environment and Ecology, Hunan Agricultural University, Changsha 410128, China;School of Information and Engineering, WuHan University of Technology, Wuhan, 430070, Hubei, China
通讯机构:
[Yang sheng Tian] S;School of Chemical and Environmental Engineering, Wuhan Polytechnic University, Wuhan, 430032, Hubei, China<&wdkj&>School of Information and Engineering, WuHan University of Technology, Wuhan, 430070, Hubei, China
摘要:
Despite extensive studies on dibutyl phthalate (DBP) degradation in isolated bacterial cultures, the primary degraders, community dynamics, and metabolic pathways involved in its biotransformation within complex sediment microbial communities remain poorly understood. In this study, we aimed to investigate the biotransformation mechanism of DBP by microorganisms in a sediment–water system by employing gas chromatography-mass spectrometry, 16S rRNA gene sequencing, metagenomic analysis, and bacterial isolation techniques. We observed that DBP biotransformation has three distinct phases: lag, degradative, and stationary. During the degradative phase, DBP gets progressively degraded by microorganisms, resulting in a microbial community with reduced stability and ambiguous boundaries. DBP, primarily metabolised by key phylotypes into monobutyl phthalate (MBP), phthalic acid (PA), and protocatechuic acid, subsequently enters the tricarboxylic acid (TCA) cycle. Through metagenomic analysis, ten functional genes from five genera were identified as crucial for DBP metabolism. Firstly, Arthrobacter degrades DBP into MBP and PA using pheA. Subsequently, Acinetobacter , Massilia, and Arthrobacter convert PA into TCA cycle intermediates using phtBAaAbAcAd and pcaCH. Concurrently, Hydrogenophaga and Acidovorax degrade PA to TCA cycle intermediates through pht1234 and ligAB. Genes related to amino acid synthesis, ABC transporters, and two-component regulatory systems also contribute significantly. Thus, the listed key bacteria, along with their diverse functional genes, collectively exhibit a high capacity for DBP degradation. This study provides insights into the bacterial responses to DBP degradation and offers a theoretical basis for the prevention and control of this pollutant.
Despite extensive studies on dibutyl phthalate (DBP) degradation in isolated bacterial cultures, the primary degraders, community dynamics, and metabolic pathways involved in its biotransformation within complex sediment microbial communities remain poorly understood. In this study, we aimed to investigate the biotransformation mechanism of DBP by microorganisms in a sediment–water system by employing gas chromatography-mass spectrometry, 16S rRNA gene sequencing, metagenomic analysis, and bacterial isolation techniques. We observed that DBP biotransformation has three distinct phases: lag, degradative, and stationary. During the degradative phase, DBP gets progressively degraded by microorganisms, resulting in a microbial community with reduced stability and ambiguous boundaries. DBP, primarily metabolised by key phylotypes into monobutyl phthalate (MBP), phthalic acid (PA), and protocatechuic acid, subsequently enters the tricarboxylic acid (TCA) cycle. Through metagenomic analysis, ten functional genes from five genera were identified as crucial for DBP metabolism. Firstly, Arthrobacter degrades DBP into MBP and PA using pheA. Subsequently, Acinetobacter , Massilia, and Arthrobacter convert PA into TCA cycle intermediates using phtBAaAbAcAd and pcaCH. Concurrently, Hydrogenophaga and Acidovorax degrade PA to TCA cycle intermediates through pht1234 and ligAB. Genes related to amino acid synthesis, ABC transporters, and two-component regulatory systems also contribute significantly. Thus, the listed key bacteria, along with their diverse functional genes, collectively exhibit a high capacity for DBP degradation. This study provides insights into the bacterial responses to DBP degradation and offers a theoretical basis for the prevention and control of this pollutant.
期刊:
Separation and Purification Technology,2025年354:129142 ISSN:1383-5866
通讯作者:
Tingting Zhang<&wdkj&>Zhenlei Wang
作者机构:
[Tan, Shuyang; Zhang, Tingting; Cheng, Cheng; Li, Haiyang] School of Chemical and Environmental Engineering, Wuhan Polytechnic University, Wuhan 430023, China;[Zhao, Yunliang] School of Resources and Environmental Engineering, Wuhan University of Technology, Wuhan 430070, China;Instituto de Geologia, Facultad de Ingeneria, Universidad Autonoma de San Luis Potosi, Av. Parque Chapultepec 1570, San Luis Potosi 78210, Mexico;[Wang, Zhenlei] School of Chemical and Environmental Engineering, Wuhan Polytechnic University, Wuhan 430023, China<&wdkj&>School of Resources and Environmental Engineering, Wuhan University of Technology, Wuhan 430070, China<&wdkj&>Instituto de Geologia, Facultad de Ingeneria, Universidad Autonoma de San Luis Potosi, Av. Parque Chapultepec 1570, San Luis Potosi 78210, Mexico
通讯机构:
[Tingting Zhang; Zhenlei Wang] S;School of Chemical and Environmental Engineering, Wuhan Polytechnic University, Wuhan 430023, China<&wdkj&>School of Chemical and Environmental Engineering, Wuhan Polytechnic University, Wuhan 430023, China<&wdkj&>School of Resources and Environmental Engineering, Wuhan University of Technology, Wuhan 430070, China<&wdkj&>Instituto de Geologia, Facultad de Ingeneria, Universidad Autonoma de San Luis Potosi, Av. Parque Chapultepec 1570, San Luis Potosi 78210, Mexico
摘要:
Heavy metals in wastewater have caused serious environmental contamination in the world. However, a key challenge with the most effective solution through chemical precipitation is the high pH of in the effluent by the use of lime. Herein, we propose a strategy using highly active calcium carbonate (HACC) for enhancing its slow-release activity, which efficiently removes heavy metal contamination while avoiding high pH of the effluent. The HACC demonstrate a removal of more than 99 % for Cd(II), Cu(II), Zn(II) and Pb(II) from the composite contaminated water within 50 min, while maintaining the pH of the effluent close to neutral. In addition, mechanistic analyses unveil that the free heavy metals in different solutions combine with OH – and CO 3 2– released from HACC in different precipitation behaviors to form their respective precipitates, thereby discovering the mechanism of regulating the precipitation rates of different heavy metals by controlling the activity of calcium carbonate. Based on it, the stepwise recovery of heavy metals was realized by adjusting the calcium carbonates with different activity. The present work provides guidance for gentle and efficient removal of heavy metal pollution in water bodies and inspires the future development of recovery of heavy metals.
Heavy metals in wastewater have caused serious environmental contamination in the world. However, a key challenge with the most effective solution through chemical precipitation is the high pH of in the effluent by the use of lime. Herein, we propose a strategy using highly active calcium carbonate (HACC) for enhancing its slow-release activity, which efficiently removes heavy metal contamination while avoiding high pH of the effluent. The HACC demonstrate a removal of more than 99 % for Cd(II), Cu(II), Zn(II) and Pb(II) from the composite contaminated water within 50 min, while maintaining the pH of the effluent close to neutral. In addition, mechanistic analyses unveil that the free heavy metals in different solutions combine with OH – and CO 3 2– released from HACC in different precipitation behaviors to form their respective precipitates, thereby discovering the mechanism of regulating the precipitation rates of different heavy metals by controlling the activity of calcium carbonate. Based on it, the stepwise recovery of heavy metals was realized by adjusting the calcium carbonates with different activity. The present work provides guidance for gentle and efficient removal of heavy metal pollution in water bodies and inspires the future development of recovery of heavy metals.
摘要:
Background Efficient separation of Re from molybdenum and uranium ores holds significant implications for resource utilization and environmental conservation.
Efficient separation of Re from molybdenum and uranium ores holds significant implications for resource utilization and environmental conservation.
Methods A novel quaternary phosphonium (PPh 3 ) modified cellulose (CMS-g-VBPPh 3 NO 3 ) was synthesized through the halogenation reaction between PPh 3 and the VBC grafted cellulose intermediate (CMS-g-VBC). The recovery of Re was evaluated by batch and dynamic adsorption experiments.
A novel quaternary phosphonium (PPh 3 ) modified cellulose (CMS-g-VBPPh 3 NO 3 ) was synthesized through the halogenation reaction between PPh 3 and the VBC grafted cellulose intermediate (CMS-g-VBC). The recovery of Re was evaluated by batch and dynamic adsorption experiments.
Significant Findings The adsorption performance of CMS-g-VBPPh 3 NO 3 for Re(VII) remains stable across a broad pH range. Even in the presence of various coexisting anions (NO 3 - , SO 4 2- and PO 4 3- ), CMS-g-VBPPh 3 NO 3 demonstrates exceptional adsorption efficiency towards Re(VII). In column experiments, the CMS-g-VBPPh 3 NO 3 selectively captured Re(VII) from both acidic and alkaline uranium ore leachate, with concentration factors reaching 600 and 1228, respectively. These results highlight the material's effective Re(VII) separation capabilities, indicating its potential as a promising candidate for practical applications involving Re(VII) recovery.
The adsorption performance of CMS-g-VBPPh 3 NO 3 for Re(VII) remains stable across a broad pH range. Even in the presence of various coexisting anions (NO 3 - , SO 4 2- and PO 4 3- ), CMS-g-VBPPh 3 NO 3 demonstrates exceptional adsorption efficiency towards Re(VII). In column experiments, the CMS-g-VBPPh 3 NO 3 selectively captured Re(VII) from both acidic and alkaline uranium ore leachate, with concentration factors reaching 600 and 1228, respectively. These results highlight the material's effective Re(VII) separation capabilities, indicating its potential as a promising candidate for practical applications involving Re(VII) recovery.
作者机构:
[Xinguang Fang; Songdong Yuan; Haoran Yu; Jintao Xiao; Guodong Jiang; Jian Xiong] Institute of Energy Materials and Catalytic Technology, Hubei University of Technology, Wuhan, 430068, China;[Xiaobo Wang; Ya Sun; Deng Ding] College of Chemistry and Environmental Engineering, Wuhan Polytechnic University, Wuhan 430023, China;[Rui Liang] Sunwoda Electronic Co.,Ltd, Shenzhen 518108, China
通讯机构:
[Xiaobo Wang; Deng Ding] C;[Songdong Yuan] I;Institute of Energy Materials and Catalytic Technology, Hubei University of Technology, Wuhan, 430068, China<&wdkj&>College of Chemistry and Environmental Engineering, Wuhan Polytechnic University, Wuhan 430023, China
摘要:
In this study, polyacrylonitrile (PAN), lithium bisfluoromethanesulfonimide (LiTFSI) and carbon nanotubes (CNTs) with different addition amounts (LPC) were used as the host polymer, electrolyte salt and nano-filler to prepare high-performance solid polymer electrolyte (SPE). The introduction of CNTs not only enhanced mechanical strength but also improved electrical performance of SPE. The ionic conductivity of the 1.8wt% CNT-filled PAN-LiTFSI electrolyte at 25 °C was 2.93 × 10 –4 S cm -1 , which was much higher than that of the zero-filled electrolyte (2.52 × 10 –5 S cm -1 ). In addition, the anode potential and Li ion transfer number also increased to 4.84 V and 0.41, respectively. Subsequently, the electrical performance of LiFePO 4 /LPC/Li full cells assembled by using LPC-1.8 % as electrolyte was tested. The charge and discharge capacity in the first cycle were 135.8 mAh g -1 and 135.3 mAh g -1 at 0.1C, respectively. After 130 cycles, it still maintained 124.7 mAh g -1 and 119.4 mAh g -1 . The coulombic efficiency was about 95.8 %.
In this study, polyacrylonitrile (PAN), lithium bisfluoromethanesulfonimide (LiTFSI) and carbon nanotubes (CNTs) with different addition amounts (LPC) were used as the host polymer, electrolyte salt and nano-filler to prepare high-performance solid polymer electrolyte (SPE). The introduction of CNTs not only enhanced mechanical strength but also improved electrical performance of SPE. The ionic conductivity of the 1.8wt% CNT-filled PAN-LiTFSI electrolyte at 25 °C was 2.93 × 10 –4 S cm -1 , which was much higher than that of the zero-filled electrolyte (2.52 × 10 –5 S cm -1 ). In addition, the anode potential and Li ion transfer number also increased to 4.84 V and 0.41, respectively. Subsequently, the electrical performance of LiFePO 4 /LPC/Li full cells assembled by using LPC-1.8 % as electrolyte was tested. The charge and discharge capacity in the first cycle were 135.8 mAh g -1 and 135.3 mAh g -1 at 0.1C, respectively. After 130 cycles, it still maintained 124.7 mAh g -1 and 119.4 mAh g -1 . The coulombic efficiency was about 95.8 %.
摘要:
Two Ln-based Metal-Organic Frameworks (MOFs), Eu-BCTC and Tb-BCTC, were synthesized using the ligand [9,9′-bicarbazole]-3,3′,6,6′-tetracarboxylic acid (H 4 BCTC) via a solvothermal method. They emit green or red light, respectively. By adjusting the molar ratio of Eu 3+ /Tb 3+ of LMOFs, a single-phase white light emitter, Eu 0.075 Tb 0.925 -BCTC, was successfully synthesized. This compound exhibits an ideal CIE coordinate of (0.33, 0.33), internal quantum yield (IQY) at 8.37 % and a color temperature of 5623 K. Moreover, it has excellent performance in detecting Fe 3+ , Cr 2 O 7 2− and CrO 4 2− , with limit of detections (LODs) at 7.403 × 10 −5 M, 1.487 × 10 −5 M and 3.053 × 10 −5 M, respectively. This advancement marks a significant contribution to the field of MOF-based white-light-emitting phosphors and fluorescence probes.
Two Ln-based Metal-Organic Frameworks (MOFs), Eu-BCTC and Tb-BCTC, were synthesized using the ligand [9,9′-bicarbazole]-3,3′,6,6′-tetracarboxylic acid (H 4 BCTC) via a solvothermal method. They emit green or red light, respectively. By adjusting the molar ratio of Eu 3+ /Tb 3+ of LMOFs, a single-phase white light emitter, Eu 0.075 Tb 0.925 -BCTC, was successfully synthesized. This compound exhibits an ideal CIE coordinate of (0.33, 0.33), internal quantum yield (IQY) at 8.37 % and a color temperature of 5623 K. Moreover, it has excellent performance in detecting Fe 3+ , Cr 2 O 7 2− and CrO 4 2− , with limit of detections (LODs) at 7.403 × 10 −5 M, 1.487 × 10 −5 M and 3.053 × 10 −5 M, respectively. This advancement marks a significant contribution to the field of MOF-based white-light-emitting phosphors and fluorescence probes.