Nature Communications
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2024
·Vol. 15
·期 1
·1-13
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IF 14.7
Li Yifan,Huang Aijian,Zhou Lingxi,Li Bohan,Zheng Muyun,Zhuang Zewen,Chen Chang,Chen Chen,Kang Feiyu,Lv Ruitao
Developing highly active and durable air cathode catalysts is crucial yet challenging for rechargeable zinc-air batteries. Herein, a size-adjustable, flexible, and self-standing carbon membrane catalyst encapsulating adjacent Cu/Na dual-atom sites is prepared using a solution blow spinning technique combined with a pyrolysis strategy. The intrinsic activity of the Cu-N 4 site is boosted by the neighboring Na-containing functional group, which enhances O 2 adsorption and optimizes the rate-determining step of O 2 activation (*O 2 → *OOH) during the oxygen reduction reaction process. Meanwhile, the Cu-N 4 sites are encapsulated within carbon nanofibers and anchored by the carbon matrix to form a C 2 -Cu-N 4 configuration, thereby reinforcing the stability of the Cu centers. Moreover, the introduction of Na-containing functional groups on the carbon atoms significantly reduces the positive charge on their outer shell C atoms, rendering the carbon skeletons less susceptible to corrosion by oxygen species and further preventing the dissolution of Cu centers. Under these multi-type regulations, the zinc-air battery with Cu/Na-carbon membrane catalyst as the air cathode demonstrates long-term discharge/charge cycle stability of over 5000 h. This considerable stability improvement represents a critical step towards developing Cu-N 4 active sites modified with the neighboring main-group metal-containing functional groups to overcome the durability barriers of zinc-air batteries for future practical applications.
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Journal of Materials Research and Technology-JMR&T
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2024
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IF 6.2
Luqiang Li,Hongqu Jiang,Yichun Liu,Qi Zhao,Jingmei Tao,Yunying Fan,Yanzhang Liu,Caiju Li,Jianhong Yi
The graphite-reinforced epoxy resin composite (Gr/EP) is considered one of the promising solid lubricating materials. However, the low thermal conductivity and correlated poor wear resistance cause limitations to its tribological applications. With the expectation to improve the thermal conductivity and wear property, carbon nanotube (CNT)-reinforced copper foams (CNTs/Cu f ) are introduced as 3-dimensional skeletons to reinforce Gr/EP composites. Herein, comprehensive testing was conducted to assess the wear resistance, thermal conductivity, microstructure, and wear morphology of the composites. The results revealed that incorporating Cu or CNTs/Cu foams into the Gr/EP matrix significantly enhanced thermal conductivity and wear resistance, with only minor elevation of the friction coefficients, which showed a consistent decline trend with increasing CNTs contents. Notably, with the CNT content of 0.159 wt%, the composites reached the favorable combination of a 25.4 % improvement in thermal conductivity and a 34 % reduction in wear rate compared to pure copper foam-reinforced Gr/EP composites.
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CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Haichuan He,Xiao Yu,Wei Wang,Liu Deng,Hao Zeng,Liqiang Wang,Ke Zeng,Jianhan Huang,Minghui Yang,You-Nian Liu
Bismuth-based materials have emerged as promising electrocatalysts for the electrochemical reduction of carbon dioxide (eCO 2 RR) to HCOOH. However, it remains challenges to meet the practical application requirements and identify the active sites of bismuth-based catalysts in eCO 2 RR. Herein, bismuthate (MBi 2 O 4 , M = Ca, Cu, Zn) derived nanosheet-like electrocatalysts with metal-modified edge defects are developed. During electrochemical processes, MBi 2 O 4 pre-catalyst undergoes surface reconstruction to expose more active Bi 0 sites and to form abundant metal-modified edge defects, which facilitate the modulation of charge state of adjacent Bi sites and improve the adsorption of *OCHO intermediate, thereby enhancing the selectivity of eCO 2 RR towards HCOOH. The Ca-modified defect-rich Bi catalyst exhibits a maximum HCOOH Faradaic efficiency of 94.3 % at an industrially relevant current density of 400 mA cm −2 , together with high stability/reproducibility of 55 h. This work proposes a new strategy for construction of Bi-based catalysts and explores its structural reconstruction mechanism during the electrocatalytic process, opening a new window for design of eCO 2 RR catalysts.
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Journal of Materials Research and Technology-JMR&T
·
2024
·
IF 6.2
Xinyue Wang,Haixue Chen,Zhoudong Yang,Wenting Liu,Zejun Zeng,Guoqi Zhang,Jing Zhang,Jiajie Fan,Pan Liu
With the increased deployment of power modules in demanding conditions, sintering materials, especially composite sintering materials, have raised growing interest due to their cost-effectiveness and suitability. Therefore, this study explores the viability of Cu–Ag composite sintering material, focusing on solvent influence through microstructure and mechanical behavior analysis. Micron-sized particle-based Cu–Ag composite pastes were designed and compared using eight solvents (four epoxy-free and four epoxy-added) based on fluidity and thermal stability. The sintered joints' performance, assessed through shear strength analysis, showed comparable values to pure silver sintering for both epoxy-free and epoxy-added samples. Optimized samples from each solvent system underwent reliability analysis, demonstrating that Cu–Ag joints with epoxy resin exhibited significantly higher shear strength after high-temperature storage and thermal cycling tests. Micromorphology and elemental composition analysis revealed differences in aging mechanisms, primarily attributed to variations in porosity due to oxide formation and pore filling by epoxy resin under different solvent systems. Further nanoindentation characterization of micromechanical properties, including hardness, modulus, and creep properties, during high-temperature aging, established constitutive models for insights into reliability evolution. In conclusion, the optimized epoxy-added Cu–Ag sintered joints proposed in this study demonstrated exceptional reliability and acceptable micromechanical properties, presenting a promising option for high-temperature power packaging.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2017
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IF 9.446
Piyong Zhang,Ting Song,Tingting Wang,Heping Zeng
Cu nanoparticles (NPs) are low-cost plasmonic metals and have been used for photocatalytic hydrogen evolution due to their surface plasmon resonance (SPR) effect. An efficient photocatalyst consisting of plasmonic Cu NPs on reduced graphene oxide (rGO) nanosheets support (Cu/rGO) is successfully prepared by a facile in-situ photoreduction process to form multiple nanoscale junctions for enhancement of photocatalytic hydrogen evolution. Compared to individual Cu NPs, the coupling to rGO nanosheets produces a higher photocatalytic ability with the highest H 2 evolution rate of 59 mmol g −1 h −1 for sample C , which contains 1.0 wt% of rGO nanosheets. The rGO nanosheet possesses an extremely high conductivity and, can accept and transfer photogenerated electrons with no barrier. Therefore, recombination of photoinduced charges can be efficiently suppressed and the accepted electrons can be rapidly transferred to reactive sites for H 2 evolution across its two-dimensional plane. More importantly, a near-infrared photocatalytic activity for sample C was obtained under monochromatic light irradiation at 800 and 900 nm due to the broad spectrum response of plasmonic Cu NPs. Furthermore, a possible reaction mechanism is proposed for the photocatalytic activity improvement as well as the detailed charge transfer condition.
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ANALYTICAL CHEMISTRY
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2018
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IF 6.042
Xiangying Yu,Man-Chu Chau,Wai Kit Tang,Chi-Kit Siu,Zhong-Ping Yao
Naproxen is one of the most consumed nonsteroidal anti-inflammatory drugs and marketed as S-naproxen since R-naproxen is hepatotoxic. In this study, chiral recognition of naproxen has been investigated by tandem mass spectrometry (MS/MS). Among all diastereomeric complexes formed between naproxen and the examined chiral selectors, including cyclodextrins (α/β/γ-CD), modified phenylalanines (N-acetyl-phenylalanine, N-t-butoxycarbonyl-phenylalanine, N-9-fluorenylmethyloxycarbonyl-phenylalanine), amino acids (Trp, Phe, Tyr, His), glucose, tartaric acid, and vancomycin, a novel binuclear metal bound diastereomeric complexes [(M(II))2(S/R-naproxen)(l-His)2−3H]+ (M = Cu, Ni, or Co with Cu being the best) could allow effective identification of the absolute configuration of naproxen and determination of its enantiomeric excess (ee) through MS/MS analysis. The key candidate structure of [(Cu(II))2(S/R-naproxen)(l-His)2−3H]+ has been revealed by means of collision-induced dissociation, ion mobility mass spectrometry and density functional theory calculations, indicating an interesting and unusual self-assembled compact geometry with the two Cu(II) ions bridged closely together (Cu–Cu distance is 3.04 Å) by the carboxylate groups of the two histidines. It was shown that the difference in dissociation efficiency between the two diastereomers was attributed to the interaction between the NH2 bond of the amino group of one histidine and the naphthyl ring of naproxen. The present report is the first to observe and characterize the complex of (Cu(II))2(His)2 with aromatic acid, which could contribute to the chiral recognition of other chiral aromatic acids, design of catalysts based on binuclear copper bound complex, as well as the better understanding of metal ion complexation by His or His-containing ligands.
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MOLECULES
·
2024
·Vol. 29
·期 20
·4860
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IF 4.2
Fuyan Zhang,Miaomiao Ma,Shuang Li,Yuting Zhou,Jian Zeng,Meiqi Huang,Qi Sun,Tao Le
In the critical domain of wastewater treatment, the development of cost-effective, durable, and recyclable adsorbents with high adsorption capacities remains a significant challenge. This study introduces a novel magnetic bimetallic Metal–Organic Framework (MOF) adsorbent, MZIF-67-Co/Cu, doped with copper ions. The MZIF-67-Co/Cu adsorbent was successfully synthesized and structurally characterized, demonstrating remarkable selectivity for removing methyl orange (MO) from water. This high selectivity is attributed to the adsorbent’s high porosity and Lewis base properties at the coordinating metal ion center. The incorporation of Cu ions significantly enhances the porous architecture and increases the number of metal adsorption sites, leading to an impressive maximum MO adsorption capacity of 39.02 mg/g under optimized conditions (0.5 g/L adsorbent concentration, pH 3.0, 250 rpm agitation speed, adsorption time > 10 min). The adsorption kinetics closely follow the pseudo-second-order model, and the isotherm data fit well with the Langmuir model. The primary adsorption mechanisms involve electrostatic attraction and mesoporous interaction. This study highlights MZIF-67-Co/Cu as a highly efficient adsorbent with magnetic recovery capabilities, positioning it as a promising candidate for addressing critical issues in wastewater treatment.
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2024
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IF 6.9
Shupo Liu,Zixiang He,Xiaobin Liao,Xinyue Liu,Menglan Gao,Huayu Zhang,Jing Zou,Zhenming Zhou,Baoling Yuan,Zhimin Yang
Antibiotics and ammonia are generally co-existed in aquaculture tailwater; moreover, ammonia would also be produced from during ozonation, and should be simultaneously removed before discharge or reuse. In this study, catalyst Cu-Co/γ-Al 2 O 3 was screened from a variety of metal oxides and applied in catalytic ozonation of three kinds of antibiotics and NH + 4 -N. Factors that affected their removal, including catalyst dosages, O 3 concentration, initial pH as well as co-existing ions, were investigated. Moreover, the mechanisms were probed by exploring free radicals’ role as well as intermediates identification; and the characteristics of catalysts before and after use were evaluated using SEM, EDS, XRD, XPS, and BET. Results demonstrated that Cu-Co/γ-Al 2 O 3 could significantly stimulate the degradation of the selected antibiotics and NH + 4 -N during ozonation. The degradation efficiencies of ciprofloxacin (CIP), tetracycline (TC), sulfamethoxazole (SMX) and NH + 4 -N can reach up to 95.0 %, 100.0 %, 96.2 %, and 75.7 %, respectively. Plenty of oxygen vacancy (O vs ) and sufficient alkaline sites on the surface of catalyst facilitated the adsorption of pollutants. Furthermore, the transformation of metal ions Cu + /Cu 2+ and Co 2+ /Co 3+ enhanced the electron transfer capacity and favored the formation of reactive oxygen species (ROS) during catalytic ozonation reaction, and their roles in catalytic ozonation has also been verified. The radical quenching experiments demonstrated that ·OH was the main contributor for enhancing pollutants removal. The results of Gaussian calculation coincided with those intermediates detected by UPLC-Q-TOF-MS, the pollutants’ removal mechanisms by catalytic ozonation were proposed basing on them. The overall toxicities were compared for ozone only/catalytic ozonation by zebrafish embryo experiment. The results of this study would provide new a feasible way for treating antibiotics and NH + 4 -N simultaneously in aquaculture wastewater.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Liming Liu,Junjie Li,Sidra Subhan,Xin Yu,Zhonghe Liu,Rubiao Chen,Jiguang Deng,Hongbing Ji,Zhongxing Zhao,Zhenxia Zhao
A major challenge in utilizing metal–organic frameworks (MOFs) for volatile organic compound (VOC) capture was their inclination for strong adsorption, which consequently impeded desorption and elevated energy demand. To overcome this challenge, the construction of HKUST-1@Cu nanofibers (HK@Cu-NF) with thermal conductive adsorption sites was proposed to synchronous enhance toluene adsorption and desorption efficiency for VOCs capture. In this work, Cu-based HKUST-1 was designed to grow on Cu nanofibers, and formed uniform coverage MOF layer with tight connection via homologous Cu self-transformation growth strategy. The synthesized composite was proved to maintain high surface area (1473 m 2 /g) and generate abundant unsaturated Cu sites on its nanointerface based from the thermally conductive Cu nanofibers. This unique connection structure endowed these adsorption sites with high affinity towards toluene and high thermal conductivity as well, and finally formed thermal conductive adsorption sites. As a result, HK@Cu-NF composite (80 % loading of HKUST-1) exhibited 1.9 times higher of toluene adsorption capacity at P / P 0 = 0.002 and >3 times higher of thermal diffusivity than pure HKUST-1. Furthermore, it achieved enhancement in both adsorption and desorption efficiency for toluene, which reached 4.8 and 6.9 times of pure HKUST-1. Therefore, construction of thermal conductive adsorption sites successfully improved the adsorption efficiency and regeneration efficiency for VOCs capture, and realized the low energy VOCs desorption process.
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SENSORS AND ACTUATORS B-CHEMICAL
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2024
·
IF 8
Ke Wu,Lulu Guo,Wei Wang,Zhimin Yang,Haishun Liu
Humidity-temperature dual-functional sensors show great demand in healthcare and archaeology, requiring sensors with high sensitivity, high resolution and high stability. In this work, utilizing the post-coordination strategy, the uncoordinated N atoms in MOF-303 were used as the metal chelate sites to chelate CuCl 2 , and due to the accordion-like morphology, the obtained material shows potential in humidity sensing and temperature sensing. The CuCl 2 -MOF-303 based sensor shows whole range humidity sensing with response of 11.4 at 33 % RH and 56,700 at 95 % RH, 1 % RH of resolution and good long-term stability (>90 days), and excellent temperature sensing performance of high sensitivity (–3.3 %/°C), high linearity (R 2 >0.99) and high resolution (0.3 °C) in the temperature range of 35–38 °C. Furthermore, the application of sensor in healthcare, noncontact sensing and information transmission is verified. This study provides a preliminary exploration for the application of MOFs in humidity-temperature dual-functional sensors.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
·
IF 8.1
Keyao Wang,Yinghui Cui,Jiupai Ni,Chengsheng Ni
BaFe 0.8-x Cu x Zr 0.1 Y 0.1 O 3-δ (0 ≤ x ≤ 0.15) perovskite was investigated as the cathode material for low-temperature proton-conducting solid oxide fuel cells (H-SOFCs). Cu doping in BaFe 0.8 Zr 0.1 Y 0.1 O 3-δ (Cu0) improves the proton conductivity and surface exchange kinetics. The chemical bulk diffusion coefficient ( D chem ) and the chemical oxygen surface exchange coefficient ( K chem ) of BaFe 0.75 Cu 0.05 Y 0.1 Zr 0.1 O 3-δ (Cu5) and BaFe 0.7 Cu 0.1 Y 0.1 Zr 0.1 O 3-δ (Cu10) were both increased compared to Cu0. Thermogravimetric analysis (TGA) of Cu5 and Cu10 in air showed larger revsivle oxygen loss than that of Cu0. A significant improvement in current output was observed at 600 °C: cell with BaFe 0.65 Cu 0.15 Y 0.1 Zr 0.1 O 3-δ (Cu15), Cu10 and Cu5 cathode demonstrated current densities 100.7 %, 438.4 %, and 253.8 % higher, respectively, than the one with Cu0 at 0.6 V after more than 100 h of durability. This work demonstrated that the optimal Cu doping on ferrite cathode could improve the proton transport kinetics and is able to deliver a improved performance and stability for low-temperature (≤600 °C) H-SOFCs.
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Materials Today Communications
·
2024
·
IF 3.7
Xianze Meng,Qianru Zhang,Xuantong Lv,Jiabo Chen,Yingzi Peng,Pengxuan Dong,Qingqing Sun
The corrosion inhibition performance of three amino acids, namely L-Phenylalanine (Phe), L-Methionine (Met) and L-Histidine (His) on 7150 Al alloy in 0.1 M HCl + 1 M NaCl solution was investigated by using electrochemical impedance spectroscopy (EIS), cyclic polarization, DFT and MD simulations. Electrochemical results indicate that all the studied amino acid inhibitors are cathodic type, and the inhibition efficiency follows the following order under all studied temperatures (25, 35 and 45 ℃): His > Met > Phe. A strong correlation between corrosion inhibition efficiency and DFT parameters is not evident, but the adsorption sites (N and O of NH 2 -COOH-, S atom of Met and two N atoms in the imidazolyl ring of His) can be determined by Fukui indices and Mulliken charges of the local atoms. In addition, MD simulations indicate that corrosion inhibition efficiency increases with the decreasing of adsorption energy.
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