FUEL
·
2024
·
IF 6.7
Baozhu Chen,Zefeng Zheng,Changsong Hu,Ziyu Zengcai,Zhonghai Liu,Minglei Lu,Qingwei Meng,Tiejun Wang
The development of a highly efficient non-noble catalyst for rapid releasing of hydrogen from methanol/water at low temperature is urgent, but challenge. In this paper, the high content of graphited N-doped carbon encapsulated reducing state copper catalyst was fabricated for low-temperature aqueous reforming of methanol. The Cu@NGC-600 catalyst gives excellent hydrogen production rate of 46.15 μmol·g cat -1 ·s -1 at 190 °C, which is 4 times higher than the commercial 20 % Pt/C catalyst and 3 times higher than other reported Cu-based catalysts (such as the Cu@NC-200 catalyst). Characterization and DFT calculation results revealed that rich doping of graphite N and the synergistic effect of Cu–N strengthened the electron transfer between copper and the NC matrix, decrease the reduction temperature of catalyst, which enabled the Cu to maintain a highly reduced state of Cu 0 /Cu + during APRM for low temperature (150–190 °C) hydrogen production.
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高影响因子
ChemistrySelect
·
2024
·Vol. 9
·期 18
·e202304772
·
IF 1.9
Chenghao Tang,Chaoyang Song
Graphical Copper encapsulated N-rich carbon material derived from porous organic polymer was found to be highly active heterogeneous catalyst for solvent-free coupling of acyl chlorides with alkynes. Copper promoted Sonogashira coupling has recently emerged as an attractive route for synthesizing α, β-Acetylenic ketones (ynones). In this study, a porous organic polymer based on [2,6-Bis(1,2,3-triazol-4-yl)pyridine] (BTP) was prepared through oxidative coupling. By incorporating copper salt and subsequent pyrolysis, copper encapsulated N-doped carbon materials were obtained. The resulting copper/carbon materials exhibited excellent catalytic performance for the coupling of acyl chlorides and alkynes due to their large surface area, abundant mesopores, and uniformly distributed metal nanoparticles. The reaction proceeded efficiently, yielding ynones with good to excellent yields at room temperature within a short reaction time (4 h) using only 0.4 mol % catalyst. Compared to previously reported copper nanocatalysts, the N-doped carbon materials supported copper catalyst demonstrated higher catalytic activity and operated at lower reaction temperatures. Additionally, the catalyst displayed reliable recyclability without any significant loss in catalytic activity.
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LUMINESCENCE
·
2024
·Vol. 39
·期 10
·e4916
·
IF 3.2
Chen Wang,Wenheng Li,Xiaohong Wang,Dongshan Xiang,Kun Zhai
In this paper, a highly sensitive method for sulfur ion (S 2− ) detection was developed based on a four-color fluorescence probe constructed from copper-containing metal–organic framework (CuBDC) and four dye-labeled single-strand DNA (ssDNA). In the absence of S 2− , dye-labeled ssDNA can be adsorbed on the surface of CuBDC, and the dyes are close to copper ion on the CuBDC surface, their fluorescence is quenched by copper ion, and their fluorescence signals are weak. In the presence of S 2− in the system, S 2− reacts with copper ion in CuBDC to form CuS, which has a more stable structure than complex CuBDC, resulting in the decomposition of CuBDC. In this case, dye-labeled ssDNA are detached from the CuBDC surface and dissolved in the solution, and the fluorescence of the dyes is restored. Under the optimized conditions, there is a good linear relationship between the total fluorescence intensity of four dyes and the concentration of S 2− in the range of 2 × 10 −9 to 5 × 10 −8 mol/L; the detection limit is 2.2 × 10 −10 mol/L. The method has a good selectivity and accuracy, and it can be applied to the analysis and detection of S 2− in actual water samples.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Shuangfu Gang,Yongxin Qian,Tianshun Xiong,You Li,Wang Li,Zheng Ma,Wenguang Zhang,Hui Long,Yingchao Wei,Xin Li,Qinghui Jiang,Yubo Luo,Junyou Yang
All-scale hierarchical defects induced by structural designing from unit cell to mesoscale play a significant role in oscillating and dissipating electromagnetic wave energy under external microwave radiation. To construct such all-scale hierarchical defects, hereby, high-entropy alloy nanoparticles coated by microscale carbon (HEA@C) with a core–shell structure were obtained by carbonizing Ni-Mn-Co-Cu-Al metal–organic. Thus, all-scale hierarchical defects were gained, including lattice distortion and nanotwins caused by the high entropy effect, vacancy and topological defects within carbon, and the heterojunction between high entropy nanoparticles and carbon. These all-scale hierarchical defects combined with the magnetic and conductive nature of HEA@C enable us to achieve a high electromagnetic wave absorption performance, with a reflection loss (RL min ) value of −52.36 dB and an effective absorption bandwidth (EAB) of 5.01 GHz. It implies that HEA@C should be an effective electromagnetic wave (EMW) absorber.
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高影响因子
Nanoscale
·
2024
·Vol. 16
·期 6
·3034-3042
·
IF 5.8
Haoyang Wu,Zhili Wang,Benqiang Tian,Yaping Li,Zheng Chang,Yun Kuang,Xiaoming Sun
Electrocatalytic CO2 reduction (ECR) to high value-added chemicals is an excellent method to attenuate the impact of greenhouse effect caused by CO2. At the same time, multicarbon products (C2+) get extensive attention in view of their relatively high energy density and market price. At present, Cu is an important metal electrocatalyst to convert CO2 into multicarbon products (e.g. ethylene, ethanol, and n-propanol); however, its poor selectivity impedes its practical application. It is well-known that the Cu(100) crystal facet can enhance the selectivity toward multicarbon products among different Cu crystal facets. Herein, the Cu nanoparticles were firstly prepared using the inductive effect of different gases (CO2, CO, Ar, N2, and air) during the Cu electrodeposition processes, in which the CO2-induced Cu catalyst (Cu-CO2) showed the largest normalized content of the Cu(100) crystal facet and the highest C2+ faradaic efficiency of 69% at a current density of 80 mA cm−2 in ECR. Subsequently, the different CO2 pressures during the Cu electrodepositions were studied to reveal the optimal CO2 pressure in the CO2-induced Cu synthesis for improved Cu(100) content as well as C2+ faradaic efficiency. Finally, density functional theory (DFT) calculations confirmed that CO2 molecules preferred to get adsorbed on the Cu(100) crystal facet, which resulted in not only the presence of dominant Cu(100) during the CO2-induced Cu synthesis but also the good electrocatalytic performance in ECR.
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高影响因子
International Journal of Minerals Metallurgy and Materials
·
2024
·
IF 5.6
Qiu Yuhua,Huang Yingping,Wang Yanlan,Liu Xiang,Huang Di
Advanced processes for peroxymonosulfate (PMS)-based oxidation are efficient in eliminating toxic and refractory organic pollutants
from sewage. The activation of electron-withdrawing HSO
− 5
releases reactive species, including sulfate radical (·SO
− 4
), hydroxyl radical (·OH), superoxide radical (·O
− 2
), and singlet oxygen ( 1 O 2 ), which can induce the degradation of organic contaminants. In this work, we synthesized a variety of M-OMS-2 nanorods (M = Co, Ni, Cu, Fe) by doping Co 2+ , Ni 2+ , Cu 2+ , or Fe 3+ into manganese oxide octahedral molecular sieve (OMS-2) to efficiently remove sulfamethoxazole (SMX) via PMS activation. The catalytic performance of M-OMS-2 in SMX elimination via PMS activation was assessed. The nanorods obtained in decreasing order of SMX removal rate were Cu-OMS-2 (96.40%), Co-OMS-2 (88.00%), Ni-OMS-2 (87.20%), Fe-OMS-2 (35.00%), and OMS-2 (33.50%). Then, the kinetics and structure–activity relationship of the M-OMS-2 nanorods during the elimination of SMX were investigated. The feasible mechanism underlying SMX degradation by the Cu-OMS-2/PMS system was further investigated with a quenching experiment, high-resolution mass spectroscopy, and electron paramagnetic resonance. Results showed that SMX degradation efficiency was enhanced in seawater and tap water, demonstrating the potential application of Cu-OMS-2/PMS system in sewage treatment.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Pan Guo,Weili Gu,Junyu Lu,Keying Zhang,Fei Liu,Hongzhi Liu,Nan Sheng,Chunyu Zhu
The deployment of phase change materials (PCMs) presents a viable strategy for enhancing solar energy conversion and storage, providing a continuous thermal energy generation process in line with carbon neutrality objectives. Through the modification of carbon felts (CF) with polydopamine (PDA) and subsequent controlled integration of Cu nanoparticles, this study achieved the development of flexible phase change composites (FPCCs) for enhanced solar thermal energy conversion and storage, incorporating thermally-driven shape memory and spatial adaptability. Notably, the CF/PDA/Cu/PW variant demonstrated a thermal conductivity of 1.43 W m −1 K −1 , marking a 680 % enhancement relative to pure paraffin wax (PW), with an energy storage density of 171.3 J/g. Moreover, these composites exhibited rapid responsiveness, near-complete thermal shape recovery, and maintained stable solar-to-thermal conversion efficiency and shape stability. These findings suggest the potential of these FPCCs for utilization in solar thermal energy systems, as well as in thermal management under spatial and shape constraints.
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高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2024
·
IF 8
Ting Li,Xianfa Zhang,Xiaoli Cheng,Yingming Xu,Shan Gao,Lihua Huo
It is necessary to achieve highly sensitive and low temperature detection of Cl 2 for the protection of the environment and human life and health. How to achieve sensitive detection of Cl 2 at low temperature remains a challenge. The construction of heterojunction is beneficial for promoting carrier transfer, increasing active sites, thus effectively improving sensing performance of materials. In this study, the flower sphere-like Cu 2 O/CuO composite with p-p heterojunction was obtained by using Cu-CPs as precursor followed with sintering treatment. The Cu 2 O/CuO sensor exhibits high response (S=405) to 10 ppm Cl 2 at low temperature (50 °C), the response/recovery time is 50 s/2420 s. At the same time, the Cu 2 O/CuO sensor has a low detection limit (50 ppb) and good long-term stability (60 days). The characterization results, e.g. electron paramagnetic resonance (EPR), O 2 /Cl 2 -temperature programmed desorption ( O 2 /Cl 2 -TPD), X-ray photoelectron spectroscopy (XPS) etc., reveal that oxygen vacancy effectively promotes the increase of surface adsorbed oxygen, the formation of p-p heterojunction not only modulates the electronic properties of Cu 2 O/CuO but also provides abundant adsorption sites for gas. The synergistic effect of the above factors makes Cu 2 O/CuO composite exhibit satisfactory Cl 2 sensing performance.
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高影响因子
ACS Applied Nano Materials
·
2024
·
IF 5.3
Qinglin Chen,Long Tian,Ming Ruan,Yi Liu,Cheng Peng,Weigang Cui,Wei Liang,Shaoyun Shan,Tianding Hu
Fenton-like reactions with Fe-based metal–organic framework (MOF) catalysts have been extensively explored in the field of environmental remediation. However, easy precipitation of Fe2+/Fe3+ and the production of sludge under basic conditions caused catalyst loss and greatly limited their large-scale application in industry. The development of an Fe-free Fenton-like reaction is of extreme importance and remains in its infant stage. Herein, a series of Fe-free dual MOF nanoparticles (HKUST-1/ZIF-67-X) were fabricated by in situ coating of ZIF-67 on HKUST-1 and were systematically analyzed by various characterization techniques, such as scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), Fourier transform infrared (FT-IR), X-ray photoelectron spectroscopy (XPS), and N2 adsorption–desorption isotherms. Subsequently, these materials were applied in catalyzing methylene blue (MB) degradation. The effects of several operation parameters, i.e., pH, H2O2 dosage, catalyst dosage, and reaction temperature, on MB degradation were investigated. It was unveiled that HKUST-1/ZIF-67-7% exhibited an outstanding catalytic activity without the production of any sludge, which could reach as high as 93.29% MB degradation efficiency within 40 min. This was attributed to the unique core–satellite histoarchitecture of HKUST-1/ZIF-67-7% and the synergistic effect between HKUST-1 and ZIF-67. The HKUST-1/ZIF-67-7% composite still achieved up to 80.17% MB degradation efficiency at the fifth catalysis cycle. Importantly, HKUST-1/ZIF-67-7% exhibited significant catalytic efficiency under a wide pH range (4.2–10.1) and top catalytic efficiency at the near neutral pH value. The low cost, environment benignancy, satisfactory degradation efficiency, wide pH application range, and excellent reusability emphasize its great application potential in Fenton-like degradation of pollutants. This contribution could provide a paradigm investigation for designing non-iron-based MOF catalysts to solve the increasingly pressing pollution issues.
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高影响因子
BIOMATERIALS
·
2024
·
IF 12.8
Yiqun Zhang,Ni Zhang,Jianghao Xing,Yiwei Sun,Xu Jin,Cailiang Shen,Liang Cheng,Yuanyin Wang,Xianwen Wang
Chemodynamic therapy (CDT) involving the use of metal nanozymes presents new opportunities for the treatment of deep-seated tumors. However, the lower ROS catalytic rate and dependence on high H 2 O 2 concentrations affect therapeutic efficacy. To address this issue, a hydrogel was constructed for the treatment of osteosarcoma by combining Cu–Fe 3 O 4 nanozymes (NCs) and artemisinin (AS) coencapsulated in situ with sodium alginate (ALG) and calcium ions. This hydrogel can release nanoparticles and AS within tumor tissue for an extended period of time, utilizing the multienzyme activity of NCs to achieve ROS accumulation. The carbon radicals (•C) generated from the interaction of Fe 2+ /Cu 2+ with AS amplify oxidative stress, leading to tumor cell damage. Simultaneously, the NCs activate ferroptosis via the GPX4 pathway by depleting GSH and activate cuproptosis via the DLAT pathway by causing intracellular copper overload, enhancing therapeutic efficacy. In vitro experiments confirmed that the NCs-AS-ALG hydrogel has an excellent tumor cell killing effect, while in vivo experimental results demonstrated that it can effectively eliminate tumors with excellent biocompatibility , providing a new approach for osteosarcoma treatment.
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高影响因子
Surfaces and Interfaces
·
2024
·
IF 5.7
Cijun Shuai,Gao Pan,Qi Zhong,Shuping Peng
Bacterial infections considerably limit the success of scaffold transplantation. CuO 2 may generate hydroxyl radicals through a self-cascade catalytic process, which is effective for sterilization. However, reducing CuO 2 -derived Cu + ions to Cu° can lead to a decline in catalytic activity. To overcome these limitations, we anchored CuO 2 onto MoS 2 to establish stable Cu-S-Mo interfacial sites. The CuO 2 /MoS 2 nanozyme was fabricated using a low-temperature co-precipitation technique and introduced into poly- l -lactic acid scaffolds using selective laser sintering. The Cu-S-Mo interfacial sites showed a triad of functions that synergistically enhanced catalytic performance. These sites stabilized the Cu atoms, augmented catalytic activity by facilitating efficient electron transfer through the Mo 4+ /Mo 6+ redox couple, and improved the conduction of heat derived from the photothermal response of MoS 2 to the Cu catalyst. The synergistic action of chemodynamic and photothermal therapy, mediated by the Cu-S-Mo sites, resulted in remarkable antibacterial efficacy, with 92.3 % and 93.5 % inhibition rates against Staphylococcus aureus and Escherichia coli , respectively. Experimental evidence and simulations demonstrated that Cu-S-Mo structure stabilized the Cu atoms and improved electron transfer via interatomic charge transfer. These results highlight the potential of the CuO 2 @MoS 2 /PLLA scaffold in eliminating bacterial infections.
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高影响因子
Journal of Materials Chemistry A
·
2024
·
IF 10.7
Katam Srinivas,Zhuo Chen,Anran Chen,He Huang,Chengtao Yang,Fei Wang,Ming-qiang Zhu,Yuanfu Chen
Replacing platinum-based electrocatalysts with iron single-atom catalysts (Fe–N4–C) for the oxygen reduction reaction (ORR) remains challenging due to the symmetric electronic structure of atomically dispersed Fe–N4 sites and sluggish kinetics. To address this issue, we introduce Cu–Nx sites and graphene-encapsulated core–shell Fe–Cu nanoalloy (FeCu@G) particles into the Fe–Nx site surroundings through the self-assembly and pyrolysis of a metal–organic framework (MOF). This strategy leverages synergistic interactions with the associated species to modify the uniform electronic structure of Fe single-atom sites, thereby enhancing oxygen-adsorption/desorption kinetics. Density functional theory (DFT) calculations reveal that the incorporation of Cu–Nx sites and FeCu@G nanoalloy particles significantly alters the electronic structure of Fe–Nx sites, leading to improved ORR activity. Consequently, the optimized FeCu-DSAs@CNT, comprising dual single-atom sites (DSAs: Fe–Nx and Cu–Nx) and FeCu@G nanoalloy within MOF-derived nitrogen-doped carbon nanotubes (CNTs), exhibits a significantly improved half-wave potential (E1/2 = 0.91 V) and feasible ORR kinetics (Tafel slope = 48.15 mV dec−1), surpassing the Pt/C benchmark (E1/2 = 0.847 V and Tafel slope = 56.76 mV dec−1). Notably, FeCu-DSAs@CNT shows a 58 mV more positive E1/2 compared to monometallic Fe–SAs@CNT, attributed to synergistic interactions with Cu species. Moreover, it demonstrates excellent power density, specific capacity, and cycling stability in a lab-made zinc–air battery, outpacing the Pt/C-battery. This study addresses gaps in understanding Fe–Nx site interactions with associated species, providing valuable insights for the advancement of Fe–Nx–C electrocatalysts.
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