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Journal of Macromolecular Science Part A-Pure and Applied Chemistry · 2024 · IF 2.1

pH-responsive and mechanical strong chitosan-based hydrogel reinforced with rice straw cellulose micro-fibrils for efficient removal of cu(II)

Ping Jiang,Wan Liu,Jing Li,Yuan Gao

Straw and chitosan are underutilized raw materials, which could make a significant contribution to sustainable development. Herein, a novel chitosan-based hydrogel incorporating rice straw cellulose micro-fibrils (SCMF) was prepared to effectively remove Cu(II). FTIR and SEM showed that straw cellulose-g-poly (acrylic acid)/chitosan-g-poly (acrylic acid) interpenetrating polymer networks were prepared and the hydrogel SCCH had a 3D porous structure after cross-linking with AA. The swelling properties of SCCH were studied and compared in various pH solution. The results indicated that SCCH replayed pH responsibility, which had the largest and smallest swelling capacity at pH9.18 and pH4.00 respectively. The pseudo-second-order kinetic model can be effectively used to evaluate swelling kinetics of hydrogels. The effects of contact time and initial concentration on Cu(II) ion removal were investigated. The equilibrium adsorption capacity (Qe) was 209.2 mg/g and the obtained results indicated that the adsorption kinetics conformed to the pseudo-second-order. Chemical adsorption combined with porous physical adsorption endowed SCCH excellent swelling and adsorption properties. Tensile, compression, bending and twisting test convinced that SCMF played a significant role on the improvement of mechanical strength. This novel 3D porous chitosan-based hydrogel was identified to be a promising sorbent with advantages of excellent sorption and mechanical properties.

研究领域: 环境科学 · 高分子科学 · 材料工程 · 化学工程 · 可持续发展
✓ 已验证 DOI 高影响因子
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Lateral growth of Lithium dendrite enforced by 3D porous Core@Shell-Cu@Li3N protective layer toward Long-Life Lithium metal anode

Zhen Li,Kailin Luo,Geng Zhang,Lingxuan Qian,Xiaodong Huang

Li metal is promising as the anode for next-generation Li-ion batteries; however, uncontrollable dendrite growth and severe side reactions between the Li metal and electrolyte greatly restrict its commercialization. Here, a 3D porous protective layer constructed by core@shell-Cu@Li 3 N particles is developed to solve the above issues. This protective layer is easily prepared just by one-step dip coating in Cu(NO 3 ) 2 /N-methyl-2-pyrrolidone (NMP) solution. Due to rapid Li + transport and good wettability of the protective layer, it effectively modulates Li + flux and thus homogenizes Li deposition. More importantly, as confirmed by both the experimental results and phase-field simulations, the 3D porous protective layer enforces the Li dendrite to laterally grow to form an interconnected network, which causes that the subsequent Li deposition is constrained and filled in the inner space rather than savage growth. Therefore, both the symmetric battery and full cell constructed by the protected Li electrode displays much longer lifespan than the one with bare Li even in unstable liquid carbonate electrolyte. Also, this protective layer is demonstrated to be compatible with Li 1+x Al x Ti 2−x (PO 4 ) 3 (LATP) solid-state electrolyte by suppressing the side reactions. This work paves a new and facile strategy for developing high-performance Li metal anode.

研究领域: 材料科学 · 电化学 · 电池技术
✓ 已验证 DOI 高影响因子
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RSC Advances · 2023 ·Vol. 13 ·期 20 ·13902-13910 · IF 3.9

Synthesis of methanol over highly dispersed Cu–Fe based catalysts derived from layered double hydroxides

Jing Tian,Weixin Qian,Haitao Zhang,Hongfang Ma,Weiyong Ying

In this paper, catalysts with different aluminum contents were prepared by a co-precipitation method using LDHs (layered double hydroxides) as the precursors through the adjustment of Cu2+ : Fe2+, and the catalysts were named LDO catalysts. The effect of aluminum on CO2 hydrogenation to methanol was investigated by evaluating the characterization. With the addition of Al, Ar physisorption results showed an increase in BET-specific surface area, TEM demonstrated a decrease in catalyst particle diameter, XRD showed that Cu and Fe existed in the catalyst mainly in the form of CuFe2O4 and CuO, XPS demonstrated a decrease in electron cloud density and an increase in base sites and oxygen vacancies, and CO2-TPD and H2-TPD results indicated that Al promoted the dissociation and adsorption of CO2 and H2. When the reaction temperature was 230 °C, the pressure was 4 MPa, H2/CO2 = 2.5 and the space velocity was 2000 ml (h gcat)−1, the best conversion (14.87%) and the highest methanol selectivity (39.53%) of the catalyst were obtained at 30% aluminum content.

研究领域: 催化 · 化学工程 · 材料科学
✓ 已验证 DOI PubMed 高影响因子
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BIOSENSORS & BIOELECTRONICS · 2022 · IF 12.545

Nanozyme-mediated signal amplification for ultrasensitive photoelectrochemical sensing of Staphylococcus aureus based on Cu–C3N4–TiO2 heterostructure

Siyu Luo,Fanglei Liu,Siyu Gu,Ke Chen,Guohai Yang,Yingqiu Gu,Juntao Cao,Lu-Lu Qu

Food-borne pathogens are one of the leading causes of food poisoning, which vigorously affect food safety and human health. Therefore, the development of early and rapid detection methods for food pollution evaluation is the key to food safety and quality control. Herein, a simple and inexpensive photoelectrochemical (PEC) sensor is developed for highly selective and ultrasensitive detection of Staphylococcus aureus (S. aureus). The technique is based on “signal-off” that employs Cu–C 3 N 4 –TiO 2 heterostructures as photoactive materials and monolayer Cu–C 3 N 4 nanozyme as a signal amplifier. In the presence of S. aureus , the aptamer-modified Cu–C 3 N 4 (Cu–C 3 N 4 @Apt, a signal amplifier) and S. aureus were specifically anchored on the surface of the ligand-modified photoelectrode . The Cu–C 3 N 4 @Apt nanozyme acted as a peroxidase to catalyze the oxidation of 4-chloro-1-naphthol (4-CN) to produce insoluble precipitate on the electrode surface and resulted in a significant decrease in photocurrent . Based on the signal-amplification by the Cu–C 3 N 4 @Apt nanozyme, the constructed PEC sensor demonstrated a wide linear range between 10–10 8  CFU/mL for the S. aureus detection with the detection limit (LOD) as low as 3.40 CFU/mL. Furthermore, the PEC sensor was capable of determining S. aureus in spiked orange juice and milk, with the recovery of 91%–113%, indicating the reliability of the sensor for S. aureus detection in real samples. This investigation provides a feasible strategy for the design of highly selective and ultrasensitive PEC sensors to determine analytes in complex systems.

研究领域: 分析化学 · 生物传感器 · 食品安全 · 纳米技术 · 光电化学
✓ 已验证 DOI PubMed 高影响因子
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CHEMICAL ENGINEERING JOURNAL · 2018 · IF 6.735

Sulfur-doped copper-cobalt bimetallic oxides with abundant Cu(I): A novel peroxymonosulfate activator for chloramphenicol degradation

Cheng Chen,Li Liu,Jing Guo,Lixiang Zhou,Yeqing Lan

Sulfur-doped copper-cobalt bimetallic oxides (S-CuYO) with abundant Cu(I) were successfully synthesized by a co-precipitation method and were for the first time utilized to activate peroxymonosulfate (PMS) for the degradation of chloramphenicol (CAP). For comparison purposes, sulfur-doped monometallic oxides (S-CuO and S-CoO) and non-doped copper-cobalt bimetallic oxide (CuCoO-1) were also prepared via the same processes. The results demonstrated that S-CuCoO had the highest catalytic activity among the catalysts. The sulfur-doped catalyst significantly improved the catalytic performance and stability. More than 98% of CAP (20 mg/L) was removed within 15 min at the initial pH = 5. The superior catalytic activity of S-CuCoO mainly resulted from the synergy of Cu(I) and Co(II). The presence of Cu(I) improved the conversion of Co(III) to Co(II), which maintained the high catalytic performance of S-CuCoO. In addition, the produced Cu(II) was further converted to Cu(I) by lattice oxygen (O 2− ), ensuring an adequate supply of Cu(I) in the catalyst. Radical quenching experiments revealed that both the SO 4 − and OH radicals were generated by the interaction of S-CuCoO with PMS, thereby contributing to the efficient degradation of CAP and the OH radicals played a larger role. The main intermediates of the CAP degradation were identified by high-performance liquid chromatography–mass spectrometry (HPLC-MS/MS). Theoretical calculations of the frontier electron densities (FEDs) were performed to determine the possible degradation pathways of CAP.

研究领域: 环境化学 · 材料科学 · 催化 · 水处理
✓ 已验证 DOI 高影响因子
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BIOSENSORS & BIOELECTRONICS · 2024 · IF 10.7

LTP-assisted fabrication of laccase-like Cu-MOF nanozyme-encoded array sensor for identification and intelligent sensing of bioactive components in food

Chao Liu,Qing Huang

Nanozymes are potential candidates for constructing sensors due to their adjustable activity, high stability, and high cost-effectiveness. However, due to the lack of reasonable means, designing and preparing efficient nanozymes remains challenging. Herein, inspired by the property of natural laccase, we applied the novel and facile low-temperature plasma (LTP) technology to fabricate a series of different base-ligand Cu metal organic framework (MOF) nanozymes (namely, A-Cu, G-Cu, C-Cu and T-Cu nanozymes) with laccase-like activity successfully. Owing to the different catalytic capacities of four types of base-Cu-MOF nanozymes in the response to five common effective bioactive substances, we constructed the nanozyme-encoded array sensor for the identification of different bioactive compounds. As a result, the four-channel colorimetric sensor array was constructed, in which four laccase-like nanozymes were utilized as the sensing units, achieving high-throughput, high-sensitivity and rapid detection/identification of five common bioactive compounds in the concentration range of 1.5–150 μg mL −1 through different color output patterns. It is worth noting that the as-prepared sensor array can successfully distinguish the natural bioactive compounds in a variety of real samples. Furthermore, with the assistance of smartphones, we also designed a portable smart sensing approach for detecting the bioactive compounds effectively in food. This study has therefore not only provided an effective way for preparation highly effectively nanozymes, but also established a new sensing platform for intelligent sensing of bioactive components in food.

研究领域: 材料科学 · 分析化学 · 生物技术 · 食品科学
✓ 已验证 DOI PubMed 高影响因子
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Science of Advanced Materials · 2022 ·Vol. 14 ·期 8 ·1410-1418 · IF 1.067

Visible and Ultraviolet Dual-Readout Detection of Cu(II) in Preserved Vegetables Based on Self-Assembly and Peroxidase Simulation Properties of Mb-AuNPs

Xin Jia-Ying,Li Yue,Liu Feng-Yuan,Sun Li-Rui,Wang Yan,Xia Chun-Gu

Cu(II) adulteration in preserved vegetables by unreliable producers to increase their visual appeal or compensate for natural colour changes is most common. Methanobactin (Mb) is a Cu(II)-coordinated peptide, which plays crucial role in Cu(II) capture and absorption and the catalysis of Cu(II)-containing methane monooxygenase in methanotrophs. In this study, Mb-functionalized gold nanoparticles (Mb-AuNPs) was applied to develop a dual readout colorimetric detection for Cu(II) adulteration in preserved vegetables. In the presence of Cu(II), Mb-AuNPs was assembled into nanocluster driven by Cu(II)/Mb coordination, and the assembly process was monitored by the visible spectrum on the variation of surface plasmon resonance peak. The results showed that, Mb-AuNPs possessed excellent peroxidase-like activity after Cu(II) coordination. In the presence of Mb-AuNPs, the amount of Cu(II) obviously affected the rate of hydroquinone oxidation by H2O2 and the change of A246. The visible and ultraviolet dual-readout detection system containing Mb-AuNPs, hydroquinone and H2O2 exhibited high sensitivity and selectivity for Cu(II). The linear range of visible and UV detection towards Cu(II) was 0.05–0.4 μmol/L, the limit of detection were 37.50 nmol/L and 4.48 nmol/L, respectively. In conclusion, the Cu(II) coordination driven Mb-AuNPs assembly makes it able to detect Cu(II) adulteration in preserved vegetables by dual channel methods to eliminate the occurrence of false positives and improve the accuracy of measurement results. Such non-spatially separated Mb-AuNPs assembly and it catalyzed hydroquinone oxidation dual channel readout was simple, fast, reliable and significantly facilitated the detection efficiency of Cu(II).

研究领域: 分析化学 · 纳米技术 · 食品安全 · 环境科学
✓ 已验证 DOI 高影响因子
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SEPARATION AND PURIFICATION TECHNOLOGY · 2022 · IF 9.136

A novel Cu-BTC@PVA/PVDF Janus membrane with underwater-oleophobic/hydrophobic asymmetric wettability for anti-fouling membrane distillation

Libing Zheng,Min Tang,Yize Wang,Deyin Hou,Xiaoyu Li,Jun Wang

In this study, a novel Janus membrane was developed by constructing Cu-1,3,5-benzenetricarboxylic acid (Cu-BTC) metal–organic frameworks (MOFs) hydrophilic coating on polyvinylidene fluoride (PVDF) membrane. The Cu-BTC@PVA/PVDF Janus membrane showed a rougher surface with an in-air water contact angle of 27.4˚ and an underwater oil contact angle of 152.8°. The Cu-BTC had minimal impact on mass transfer efficiency in MD process, and the Janus membrane exhibited excellent anti-oil-fouling and anti-NOM-fouling properties. The formation of the hydration layer, the slip boundary effect, and the electrostatic repulsion by the hydrophilic serrated interface were the main antifouling mechanisms. The hydrophobic-hydrophobic interaction was the main fouling mechanism of PVDF membrane for both oil and NOM. Sodium alginate (SA) displayed severe fouling with a compacted fouling layer in PVDF membrane due to the concentration polarization (CP) and gel layer formation. Inorganic fouling was the predominant fouling for the high CP and inorganic–organic coupling. While humic acid (HA) surpassed SA in Cu-BTC@PVA/PVDF Janus membrane for the stronger hydrogen bond, hydrophobic-hydrophobic interaction was significantly alleviated. Inorganic fouling was also significantly alleviated due to the strong electrostatic repulsion effect. The prepared Janus membrane has great potential to promote MD dealing with hypersaline industrial wastewaters containing complex organic matters.

研究领域: 材料科学 · 环境工程 · 膜技术 · 水处理
✓ 已验证 DOI 高影响因子
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SENSORS AND ACTUATORS B-CHEMICAL · 2020 · IF 7.1

Electrosynthesized metal-organic framework: a dual-modality readout platform for Cu(II), coenzyme A and histone acetyltransferase analysis

Dandan Hu,Tianyu Zhan,Zhiyong Guo,Sui Wang,Yufang Hu

A novel dual-modality readout biosensing method is developed for Cu(II), coenzyme (CoA) and histone acetyltransferase (HAT) analysis based on an electrosynthesized tris(bipyridine)ruthenium(II)-functionalized metal-organic framework (Ru-MOF). In this protocol, the Ru-MOF with a delicate structure serves as both an electrochemiluminescent (ECL) and fluorescent (FL) probe. Interestingly, Cu(II) can hinder the two distinct processes favorably, thus realizing bidirectional detection of Cu(II) via an “on-off” method. Simultaneously, CoA, which contains a sulfhydryl group, can ignite a reverse “off-on” process due to the polymeric interaction of CoA and Cu(II) (2: 1). Similarly, abundant CoA molecules could also be generated regularly by a typical HAT p300-driven acetylation reaction, hence accomplishing HAT p300 activity analysis. Subsequently, an ingenious “on-off” route is exhibited again by the introduction of some small molecules (including anacardic acid and C646), which present an inhibiting effect on HAT p300 activity. Furthermore, quantitative analysis of Cu(II), CoA and HAT p300 (ECL/FL) is achieved brightly with detection limits of 0.19/0.76 nM, 1.3/6.5 nM and 1.5/8.8 nM, respectively. Ultimately, this two-channel biosensor with excellent analytical performance is applied successfully in real samples, demonstrating its potential use in bioanalysis.

研究领域: 分析化学 · 生物化学 · 分子生物学
✓ 已验证 DOI 高影响因子
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SENSORS AND ACTUATORS B-CHEMICAL · 2019 · IF 6.393

Electrochemical immunosensors with protease as the signal label for the generation of peptide-Cu(II) complexes as the electrocatalysts toward water oxidation

Ning Xia,Dehua Deng,Suling Yang,Yuanqiang Hao,Luyan Wang,Yuwei Liu,Cuixia An,Qiuyang Han,Lin Liu

This work reported that protease can be used as the signal label to amplify the signal of electrochemical immunosensors. Carbon nanotube (CNT) was used as the carrier of recognition antibody and signal label. The nanolabel was captured by sensor electrode via a sandwich-type immunoreaction. Protease on the surface of nanolabel can catalyze the hydrolysis of peptide substrate to liberate an amino terminal Cu(II)- and Ni(II)-binding (ATCUN) peptide. The released ATCUN peptide can bind with Cu(II) to generate an electrocatalyst which exhibits high electrocatalytic ability for water oxidation. Thus, the signal was amplified again by the redox cycling between ATCUN-Cu(II) and H 2 O. The immunosensor exhibits low background current because of the poor redox activity of peptide substrate and the high oxidation overpotential of H 2 O molecule. Based on the signal amplification of protease and redox cycling, the target concentration as low as 10 pg/mL can be readily measured with prostate-specific antigen (PSA) as the model analyte. The proposed immunosensor was applied to determine PSA in human serum samples with satisfactory results.

研究领域: 分析化学 · 生物化学 · 纳米技术 · 电化学 · 免疫学
✓ 已验证 DOI 高影响因子
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TRANSACTIONS OF NONFERROUS METALS SOCIETY OF CHINA · 2024 · IF 4.7

Improvement of ionic conductivity of solid polymer electrolyte based on Cu−Al bimetallic metal-organic framework fabricated through molecular grafting

Liu-bin SONG,Tian-yuan LONG,Min-zhi XIAO,Min LIU,Ting-ting ZHAO,Yin-jie KUANG,Lin JIANG,Zhong-liang XIAO

A composite solid electrolyte comprising a Cu−Al bimetallic metal-organic framework (CAB), lithium salt (LiTFSI) and polyethylene oxide (PEO) was fabricated through molecular grafting to enhance the ionic conductivity of the PEO-based electrolytes. Experimental and molecular dynamics simulation results indicated that the electrolyte with 10 wt.% CAB (PL-CAB-10%) exhibits high ionic conductivity (8.42×10 −4 S/cm at 60 °C), high Li + transference number (0.46), wide electrochemical window (4.91 V), good thermal stability, and outstanding mechanical properties. Furthermore, PL-CAB-10% exhibits excellent cycle stability in both Li−Li symmetric battery and Li/PL-CAB- 10%/LiFePO 4 asymmetric battery setups. These enhanced performances are primarily attributable to the introduction of the versatile CAB. The abundant metal sites in CAB can react with TFSI − and PEO through Lewis acid–base interactions, promoting LiTFSI dissociation and improving ionic conductivity. Additionally, regular pores in CAB provide uniformly distributed sites for cation plating during cycling.

研究领域: 材料科学 · 电化学 · 电池技术 · 聚合物科学
✓ 已验证 DOI 高影响因子
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CHEMICAL ENGINEERING SCIENCE · 2022 · IF 4.889

Highly active Mn-Cu bimetallic oxide catalyst assembled as 3D-printed monolithic agitating paddles for advanced oxidation process

Lu Long,Kaiji Xu,Kok Bing Tan,Dongren Cai,Yucheng Yang,Shu-Feng Zhou,Guowu Zhan

Catalytically agitating paddles are essential to perform liquid-solid heterogeneous catalytic reactions on an industrial scale due to the improved mass transfer and easy catalyst recovery. Herein, bimetallic oxides were formed after the calcination of nanomaterials derived from metal-organic frameworks (MOFs). Particularly, Mn(M)-BTC nanomaterials were synthesized by self-assembly of Mn 2+ ions (mixed with various dopants such as Cu 2+ , Ce 3+ , or Fe 2+ ) and H 3 BTC ligands in a mixed solvent of ethanol and water. It was found that in the powdery form, the Mn-Cu oxide derivate exhibited the highest degradation rate in the catalytic wet peroxide oxidation process (CWPO process), which was significantly higher than that of single metal oxide as well as Mn-Fe and Mn-Ce oxide derivates. The reason was caused by the synergistic effect between Mn-Cu promoted the formation of Mn 3+ and Cu + species to boost the CWPO reaction. Furthermore, the obtained Mn-Cu powdery catalysts were 3D-printed to obtain monolithic agitating paddles with different geometries, which were then mounted on a central shaft in the stirred reactor. An advanced oxidation process was used to investigate the effect of 3D patterns on the degradation efficiency of various organic dyes. It was discovered that the 3D-printed grid with higher cell density (484 cpsi) had better liquid mixing efficiency and thus better catalytic performance, which could be repeatedly used more than seven times. Additionally, the numerical simulation analysis (computational fluid dynamics) revealed a good mixing efficiency and improved mass transfer in the entire reactor equipped with the designed monolithic agitating impellers.

研究领域: 化学工程 · 材料科学 · 环境工程 · 催化
✓ 已验证 DOI 高影响因子
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