Greenhouse Gases-Science and Technology
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2025
·
IF 2.8
Qihang Wen,Yifei Feng,Haoyuan Gu,Haitao Yan,Zixu Yang,Minghui Zhu,Jing Xu
The performance of bimetallic catalysts is closely related to their surface structure, and the surface reconstruction process can affect the distribution of active sites, electronic structure, and reactant adsorption behavior. Traditional research has mostly focused on optimizing synthesis processes, such as controlling the size and distribution of metal particles, whereas there is relatively little research on the effect of pretreatment conditions on the dynamic structure of catalysts. In this study, a 10Ni─1Cu catalyst was synthesized using the deposition–precipitation method, and the effects of different pretreatment conditions on its performance were investigated. The catalyst was first pretreated at 500°C in a 60%H 2 /40%N 2 atmosphere, followed by reduction under different pretreatment atmospheres (10%H 2 /90%N 2 or 15%CO 2 /60%H 2 /25%N 2 ) at the same temperature. At 400°C and a space velocity of 30 L h −1 g −1 , the methane production rate of the catalyst treated in the reaction atmosphere significantly increased from 12.4 to 15.8 µmol g −1 s −1 compared to the catalyst treated with hydrogen alone. Characterization techniques, such as TEM, x-ray photoelectron spectroscopy (XPS), and diffuse reflectance infrared Fourier transform spectroscopy (CO-DRIFTS), were employed to study the structural properties of the catalysts, focusing on the surface properties after reduction and the surface species during the reaction. This study demonstrates that catalysts pretreated in the reaction atmosphere enhance methane production rates by regulating the surface structure and forming Ni─Cu alloy structures with a lower Ni/Cu ratio, thereby optimizing the selectivity of hydrogenation products.
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ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Mei Ma,Jia-qi Bai,Huangfei Liu,Ben Liu,Zhangkai Qian,Suiqin Li,Jingshuai Chen,Mengdie Cai,Song Sun
The preparation of methyl-substituted amines by direct N-methylation of amines with CO2/H2 is an important reaction for CO2 utilization and organic synthesis. However, the design and construction of effective and stable non-noble-metal catalysts for this reaction remain challenging. Here, a cheap non-noble-Cu-based catalyst was prepared and applied in the direct N-methylation reaction of N-methylaniline with CO2 and H2. 5%Cu-ZnO(3.75%)/TiO2 showed 98.8% yield with an initial TOF of 7.7 h–1 after 24 h under 453 K, 1.5 MPa CO2, and 4.5 MPa H2, which was superior to 5%Cu/TiO2, 5%Cu/ZnO, and reported Cu-based catalysts. Furthermore, 5%Cu-ZnO(3.75%)/TiO2 can be reused at least four times and applied to the direct N-methylation of various amines with excellent selectivity. The various characterizations and experimental results showed that Cu0 was the active site, and 5%Cu-ZnO(3.75%)/TiO2 exhibited the largest surface Cu0 amount, thereby contributing to superior catalytic performance. The reaction mechanism of the direct N-methylation reaction of N-methylaniline with CO2 and H2 was proposed based on spectroscopic studies, kinetic studies, and control experiments. The reaction proceeded with the HCHO and N-methylformanilide intermediates, and the formation of HCHO from H2 and CO2 was the rate-determining step.
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ChemistrySelect
·
2024
·Vol. 9
·期 8
·e202304917
·
IF 1.9
M. S. Tao Song,M. S. Yimin Wang,Zhen Yuan,Hai Liu,B. S. Xiaoli Zhang,B. S. Li Cui,B. S. Yuewen Chen,Tianxia Liu,Xiya Zhang
Graphical The porous carbon material derived from Cu-doped ZIF-8 is first utilized for the electrocatalytic reduction of CO 2 to CO, exhibiting a CO Faradaic efficiency of 89 % and a satisfactory stability for over 13 hours. The high content of pyridinic nitrogen, large surface area, average pore size, and the presence of Cu-N 4 particles are proven to facilitate CO 2 adsorption and enhance the catalytic performance. Electrochemical reduction of carbon dioxide presents a promising pathway to tackle global energy and environmental challenges. Porous carbon materials from metal-organic frameworks exhibit high specific surface area, abundant active sites, and adjustable pore structure, demonstrating excellent electrocatalytic performance. With their abundant resources and tunability, copper-based catalysts are well-suited for efficient carbon dioxide conversion. However, the selectivity and stability of copper-based catalysts is poor. This study presents the preparation of the first Cu-doped ZIF-8-derived carbon materials and investigates their effect on electrocatalytic carbon dioxide reduction. At the optimal potential of −0.7 V vs . RHE, the CO Faradaic Efficiency (FE) of the Cu 0.5 -N−C catalyst reaches 89 %. Furthermore, the electrochemical current density and CO FE of Cu 0.5 -N−C catalyst remain nearly unchanged within 13 hours in 0.1 mol L −1 KHCO 3 electrolyte. Compared to most of the reported copper-based catalysts, Cu 0.5 -N−C exhibits better stability. Characterization results show that Cu 0.5 -N−C has a larger Cu-N 4 , higher pyridinic N content, larger specific surface area, and average pore size, which help promote CO 2 adsorption and enhance catalyst stability. This work provides new insights and pathways for electrocatalytic carbon dioxide reduction, with enormous potential to contribute to the global energy transition and environmental protection.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2024
·
IF 8.2
Na Liu,Yinhui Li,Minggu Zhang,Naiju Che,Xianliang Song,Yanli Liu,Chengliang Li
As the substitutes of legacy long-chain per-/polyfluoroalkyl substances (PFASs), short-chain PFASs have been widely detected in the environment. Compared to long-chain PFASs, short-chain PFASs have smaller molecules and are more hydrophilic. Therefore, they are more likely to experience long-distance transport and pose lasting environmental impacts. In this study, Fe-doped (R-Fe) and Cu-doped biochars (R-Cu) were prepared using reed straw biochar (R). The results showed that the PFBA and PFPeA sorption capacities of R-Fe were 25.81 and 43.59 mg g −1 , 1.65 and 1.55 times higher than those of R, respectively. The PFBA and PFPeA sorption capacities of R-Cu were 19.34 and 33.69 mg g −1 , 1.24 and 1.20 times higher than those of R, respectively. In addition, R, R-Fe, and R-Cu exhibited higher PFBA and PFPeA sorption capacities than the biochars previously reported. The excellent PFAS sorption performances of the biochars were attributed to the highly porous structure of R, which provided rich adsorption sites. Ion-pair sorption, pore filling, electrostatic interaction between the Fe/Cu and cationic groups on biochar and the anionic groups of PFASs, and hydrophobic interaction between the hydrophobic surface of biochar and the fluorinated tails of PFASs were the underlying sorption mechanisms. The biochars presented high removal rates (>86 %) of multiple PFASs (∑PFAS: 350 μg L −1 ) from synthetic wastewaters, including legacy and emerging PFASs of different chain lengths and with different functional groups. The biochars reported in this study are promising candidate adsorbents for treating waters contaminated with short-chain PFASs.
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Surfaces and Interfaces
·
2025
·
IF 6.3
Zhao-Yun Wang,Xin Zhao,An-Ni Zheng,Lei Jin,Jia-Qiang Yang,Jun-Yang Liu,DongPing Zhan,Da-Quan Yu,Fang-Zu Yang,Shi-Gang Sun
Metallization of micro through silicon via (TSV) is vital in 3-dimensional integration of chips and high-density printed circuit boards. As the diameter decreases and aspect ratio increases, realizing a uniform copper seed layer inside TSV becomes increasingly challenging by using traditional techniques of high-cost physical vapor deposition (PVD) and chemical vapor deposition (CVD). Cu electroless deposition (Cu-ELD) is a promising technique for growing a conductive seed layer on the wall of TSV, and promotes the completion of metallization of micro TSV following by Cu electroplating. In the current study, an advanced method is developed to form Cu seed layer on micro TSV by Cu-ELD catalyzed through Ag nanoparticles. The Ag nanoparticles are synthesized using gallic acid as the reducing agent (denoted as GA-Ag NPs). Ultraviolet–visible absorption spectroscopy and transmission electron microscopy are applied to study the mechanism of conformal Cu-ELD catalyzed by GA-Ag NPs, and results demonstrate that all Ag ions are reduced to spherical Ag NPs of 9.7 nm in average size. Electrochemical tests and finite element simulation illustrate that the high catalytic activity of GA-Ag NPs facilitates Cu-ELD to achieve an effective conformal deposition in TSV. The obtained continuous and uniform Cu seed layer enables the void-free filling of TSV ultimately by Cu electroplating. An in situ XRD device is designed and built up for investigation of Cu-ELD process, which reveals that the Cu layer catalyzed by GA-Ag NPs during growth is stable and exhibits a mixed crystalline structure with texture coefficient ( TC ) values of Cu (220) and Cu (311) close to and higher than 25 %.
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Crystals
·
2025
·Vol. 15
·期 3
·205
·
IF 2.4
Xiaochun Zheng,Hao Zhang,Haoming Jiang,Lei Sun,Yuanze Sun,Qingcao Liu,Shoutian Ren,Yunpeng Zhuang,Xiaofeng Gong
Carbon dots (CDs) are efficient fluorescent probes for metal ion detection due to their high sensitivity, nontoxicity and stability, but their rich functional groups lead to simultaneous responses to multiple ions. So, how to realize highly selective detection for specific ions is still a challenging task. In this work, “bare CDs” were synthesized using the electrochemical stripping method, followed by grafting with hydroxyl and carboxyl groups following the hydrothermal method with boric acid. Transmission electron microscopy, an X-ray diffractometer, Fourier transform infrared spectroscopy, UV–visible spectrophotometers and a fluorescence spectrometer were used to characterize their morphology, surface functional groups and optical properties, respectively. The modified CDs exhibit a high sensitivity of 65% and selectivity towards Cu2+. Meanwhile, they also exhibited a short response time of less than 1 min and a good stability in terms of pH and ionic strength.
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Molecular Catalysis
·
2024
·
IF 3.9
Siyi Pu,Lu Sun,Chunyan Yang,Jie Chu,Ying Wang,Chungang Min,Xiaoqin Zou,Changfu Zhuang
The low-cost Cu-based catalysts have excellent selectivity in biomass hydrogenation, but it is challenging to improve their catalytic activity at low temperature. Herein, the trimetallic Cu x CoZn@NC (where x = 0.1, 0.3, 0.5 mmol is the molar mass of Cu) were prepared by in suit pyrolysis using trimesic acid with stronger coordination ability. When it was applied to the furfural (FF) selective hydrogenation process, the catalytic yield of the optimal Cu 0.3 CoZn@NC reached >99 % under mild condition of 90 °C, which was 29 times superior to that of the CoZn@NC without Cu doping. The results demonstrate that the doping of Cu reduces the activation energy of Cu x CoZn@NC and increases the catalytic activity at low temperature relative to CoZn@NC. The characterizations and density functional theory (DFT) calculations show that the incorporation of suitable Cu content enhances the interaction between Cu and Co. The amount of surface-active Co 0 and the electron density are significantly enhanced, which effectively stimulates the dissociation of hydrogen. Moreover, the Lewis acid content is significantly increased to facilitate the adsorption and activation of FF. Meanwhile, the impact of Cu content variation on the performance of the multi-metal catalyst is discussed. This work is promising to establish a foundation for the accurate design of polymetallic catalysts through adjusting the Cu content to regulate the reaction activity and selectivity.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2024
·
IF 4.9
Ziwei Yan,Hui Zhang,Jinghao Chen,Qingqing Xu,Shuaipeng Feng,Qinfu Zhao,Siling Wang
Photothermal effect produced in photothermal therapy (PTT) can not only eradicate tumors but also allow the promotion of biological and chemical reactions in tumor tissues, leading to the potential of photothermal-enhanced anti-tumor therapy with desirable outcomes. Biodegradable polydopamine (PDA) nanoparticles exhibit remarkable photothermal conversion efficiency and stability, making them ideal photothermal agents (PTAs) to achieve photothermal-enhanced anti-tumor therapy. The high affinity of PDA to metal ions provides a broad application prospect for the development of multi-functional nanoplatforms to achieve cancer therapy with high efficacy and specificity. In this work, we fabricated Cu(II)-doped mesoporous PDA nanoparticles with polyethylene glycol (PEG) modified (CMP-P), which not only possessed higher photothermal conversion efficacy than mesoporous PDA nanoparticles , but also presented distinctive self-enhanced chemodynamic (CDT) performance. CMP-P mediated CDT was predicated on catalyzing the Fenton-like reaction to generate hydroxyl radicals (·OH). Impressively, CMP-P further triggered glutathione (GSH) depletion intracellular to prevent the consumption of ·OH, and the photothermal effect further improved ·OH generation. Meanwhile, CMP-P exhibited favorable degradability, the process of which was elaborated intuitively by transmission electron microscope (TEM). CMP-P was then employed for doxorubicin (DOX) loading, and enabled the enhanced DOX release in-situ under the stimulation of photothermal effect and tumor micro-environment (TME). The lower IC 50 value of DOX/CMP-P (1.68 μg/mL) than the signal therapy suggested the superior synergistic effect of DOX/CMP-P. Meanwhile, in vivo experiments also revealed the considerably improved anti-tumor efficacy of synergistic therapy mediated by DOX/CMP-P.
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Scientific Reports
·
2024
·Vol. 14
·期 1
·1-12
·
IF 3.8
Wang Hui-Hui,Yin He-Liang,Yin Wei-Wei,Song Yong-Li,Chen Hong
This study introduces a novel approach for synthesizing a Cu(II)-based coordination polymer (CP), {[Cu(L)(4,4´-OBA)]·H 2 O}n ( 1 ), using a mixed ligand method. The CP was successfully prepared by reacting Cu(NO 3 ) 2 ·3H 2 O with the ligand 3,6-bis(benzimidazol-1-yl)pyridazine in the presence of 4,4´-H 2 OBA, demonstrating an innovative synthesis strategy. Furthermore, a novel hydrogel composed of hyaluronic acid (HA) and carboxymethyl chitosan (CMCS) with a porous structure was developed for drug delivery purposes. This hydrogel facilitates the encapsulation of CP 1 , and enables the loading of paclitaxel onto the composite to form HA/CMCS-CP 1 @paclitaxel. In vitro cell experiments demonstrated the promising modulation of thyroid cancer biomarker genes S100A6 and ARID1A by HA/CMCS-CP 1 @paclitaxel. Finally, reinforcement learning simulations were employed to optimize novel metal–organic frameworks, underscoring the innovative contributions of this study.
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2024
·
IF 11.2
Zhenxin Zhao,Zonglin Yi,Rong Niu,Jiajun Chen,Rajesh Pathak,Yongzhen Wang,Jeffrey W Elam,Xiaomin Wang
While neutral aqueous metal batteries, featuring cost-effectiveness and non-flammability, hold significant potential for large-scale energy storage, their practical application is hampered by the limited specific capacity of cathode materials (less than 500 mAh g −1 ). Herein, capacity-oriented CoS 2 and rate-optimized Co 9 S 8 cathodes are developed based on the aqueous copper ion system. The charge-storage mechanism is systematically investigated through a series of ex-situ tests and density functional theory calculations, focusing on the reversible transitions of Co 9 S 8 →Cu 7 S 4 →Cu 9 S 5 /Cu 1.8 S and CoS 2 →Cu 7 S 4 →Cu 2 S, which are associated with the redox reactions of Cu 2+ /Cu + ‖Co 2+ /Co and Cu 2+ /Cu + ‖S 2 2− /S 2− , respectively. The electrochemical results show that CoS 2 can exhibit a superior capacity of 619 mAh g −1 at 1 A g −1 after 400 cycles, while Co 9 S 8 maintains an outstanding rate performance of 497 mAh g −1 at 10 A g −1 (the retention rate is 95% compared to 521 mAh g −1 at 1 A g −1 ). As a proof of concept, an advanced CoS 2 //Zn hybrid aqueous battery demonstrates a working voltage of 1.20 V and a specific energy of 663 Wh kg cathode −1 . This work provides an alternative direction for developing sulfide cathodes in energetic aqueous metal batteries.
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Journal of Materials Chemistry A
·
2024
·
IF 10.7
Rui Li,Yingdan Ye,Yibin Zhang,Huaiyuan Zhao,Weichen Du,Zhaoyin Hou
Dehydrogenation of cyclohexanol to cyclohexanone is a vital step in manufacturing nylon; however, this endothermic reaction is unfavourable at low temperatures. In this work, a high-entropy oxide (Cu0.75Zn0.15Mg7.1Al1Sc1O11-HEO) was synthesized from a well-structured Cu0.75Zn0.15Mg7.1Al1Sc1(OH)20CO3 layered double hydroxide. Characterization results disclosed that Cu0.75Zn0.15Mg7.1Al1Sc1O11-HEO possesses a large specific surface area (157 m2 g−1), enhanced basicity and high Cu dispersion in the framework of HEO (74.0%). The reduced Cu0.75Zn0.15Mg7.1Al1Sc1O11-HEO catalyst was highly active and stable in the dehydrogenation of cyclohexanol compared with Cu-based catalysts prepared using binary, ternary, and quaternary mixed metal oxides. More interestingly, the conversion of cyclohexanol could be enhanced when acetone was used as the solvent and/or hydrogen acceptor. Thus, it was confirmed that the addition of acetone can enhance the yield of cyclohexanone and simultaneously result in the hydrogenation of acetone to isopropanol.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Yaqing Zhao,Kang Qin,Yaqing Zhou,Wei Liu,Zhixian Gao,Yuan Peng
Organophosphorus pesticides, commonly used in agricultural practices, remain as residues in food and the environment, presenting a significant risk to human health. The removal of these pesticides is essential to protect both human health and the environment. This study presents an in-situ synthesis technique that combines Cu-MOF (ZZU-282) with electrospinning technology to create a novel cross-linked MOF fiber membrane (cross-linked Cu-MOF-PAN FM, with PAN representing Polyacrylonitrile). The coexistence of micro/meso/macropores within the cross-linked Cu-MOF-PAN FM reduces mass transfer resistance and improves its pesticide removal capacity. The half-life for chlorpyrifos removal by the cross-linked Cu-MOF-PAN FM is about 18 s. The Langmuir model estimates the theoretical maximum removal capacity for chlorpyrifos at 208.3 mg g –1 . Additionally, the removal performance of organophosphorus pesticides is tested in simulated water samples, with results showing that over 70 % of six mixed organophosphorus pesticides are removed within 10 min using the proposed FM. The cross-linked Cu-MOF-PAN FM demonstrates superior efficiency in both rapid and sustained removal of organophosphorus pesticides from water, offering promising potential for environmental applications and pollutant removal. Moreover, the cross-linking process enhances the membrane’s resistance to organic solvents. This in-situ growth and cross-linking method offers a promising approach for fabricating MOF fiber membrane composites.
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