Catalysts
·
2025
·Vol. 15
·期 11
·1091
·
IF 4
Qiang Zhang,Shiming Qiu,Yanfei Zheng,Yingying Huang
The development of highly active, thermally stable, and low-CO-selective catalysts is critical for practical methanol steam reforming (MSR) to produce high-purity hydrogen for fuel cell applications. In this work, a series of Mn–Cu/Al2Oxcatalysts with varying Mn/Cu/Al molar ratios were synthesized via co-precipitation and systematically investigated to establish the relationship between composition, structure, and catalytic performance. XRD analysis revealed the formation of spinel-type CuAl2O4and MnAl2O4phases, with Mn preferentially occupying octahedral B-sites to form MnAl2O4, thereby inducing lattice distortion and inhibiting grain growth. SEM and TEM–EDS mapping confirmed uniform elemental distribution and a porous nanoscale morphology, while H2-TPR results suggested that increasing the Mn/Cu ratio strengthens Mn–Cu interactions, shifts Cu2+reduction to higher temperatures, and enhances Cu dispersion (up to 26.11 m2/g). XPS analysis indicated that Mn doping enriches Mn3+species and facilitates oxygen vacancy formation, which promotes water–gas shift (WGS) activity and suppresses CO formation. Catalytic testing (240–300 °C) showed that Mn2Cu2Al4Oxachieved the highest methanol conversion while maintaining low CO selectivity; in contrast, reducing the Mn/Cu ratio increased CO selectivity, detrimental to hydrogen purification. Stability tests under continuous steam exposure for 24 h demonstrated minimal activity loss (~2%) and negligible increase in CO selectivity (<1%), confirming excellent hydrothermal stability. The results indicate that tailoring the Mn/Cu ratio optimizes the balance between redox properties and metallic Cu dispersion, offering a promising route to design low-CO, durable catalysts for on-site hydrogen generation via MSR.
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JOURNAL OF ORGANIC CHEMISTRY
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2020
·
IF 4.335
Shimin Xie,Lebin Su,Min Mo,Wang Zhou,Yongbo Zhou,Jianyu Dong
An alternative thioesterification reaction via copper-catalyzed oxidative coupling of readily available aroylhydrazides with disulfides is developed, in which oxidative expulsion of N2 overcomes the activation barrier between the carboxylic acid derivatives and the products. The reaction produces various thioesters in good to excellent yields with good functional group tolerance. In the reaction, stable and easily available aroylhydrazides are used as acyl sources and the relatively odorless disulfides are used as S sources. Mechanistic investigations demonstrate that the reaction of copper salt and oxidant (NH4)2S2O8 allows for achievement of tandem processes, including deprotonation, free-radical-mediated denitrogenation, and C–S bond formation.
研究领域:
有机化学
·
催化反应
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Nano Research
·
2023
·Vol. 16
·期 5
·6290-6297
·
IF 9.9
Cai Jiahao,Song Shizheng,Zhu Lijie,Lu Qipeng,Lu Zong,Wei Yanying,Wang Haihui
A kind of two-dimensional (2D) metal-organic framework (MOF) material, Cu-meso-tetrakis (4-carboxyphenyl) porphine (Cu-TCPP) nanosheets with wrinkled and flat morphologies are used as building blocks to assemble membranes by vacuum filtration (VF) and electrophoretic deposition (EPD) as energy-efficient nanofiltration (NF) membranes to remove dyes from water. Since the nanosheets with wrinkled structure can provide additional water transport channels, thereby increasing the water permeance, in the premise of a high rejection (> 97.0%) for the dye brilliant blue G (BBG) (1.60 nm × 1.90 nm), the water permeance of the membrane assembled by the wrinkled nanosheets (∼ 1170 nm) is about 4 times that of the membrane assembled by the flat nanosheets (∼ 530 nm), reaching 16.39 L·m −2 ·h −1 ·bar −1 . Additionally, the use of the relatively flat nanosheets and the membrane preparation method of electrophoretic deposition is more conducive to stack nanosheets orderly and reduce defects. Therefore, the water permeance of the membrane prepared by EPD (∼ 1170 nm) with flat nanosheets is about twice that of the membrane prepared by VF (∼ 530 nm), achieving 9.40 L·m −2 ·h −1 ·bar −1 with similar rejection (> 97.0%) of dye evans blue (EB) (3.10 nm × 1.20 nm). Furthermore, these membranes still exhibit good separation performance at high pressure of 0.6 MPa. Nanosheets with diverse structures and various membrane fabrication processes provide new directions for the separation performance optimization of 2D MOF materials for water purification.
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Friction
·
2023
·
IF 6.8
Yang Xiao,Wang Yunbo,Cao Weihua,Jiang Ruizheng,Xie Guoxin,Cao Yuying,Qi Xiaowen
To utilize Cu-benzene-1,3,5-tricarboxylate (Cu-BTC) adsorbed lubricant oils in the self-lubricating field, the adsorption properties of Cu-BTC on different 1-olefins must be clarified. In this work, 1-hexene, 1-octene, 1-nonene, 1-decene, 1-undecene, and 1-dodecene were studied by the Monte Carlo method and experimentally. The adsorption limit of Cu-BTC for n-olefins was determined as 1-undecene by the adsorption isotherms. This suggested a limit for even straight-chain molecules to the adsorption of Cu-BTC. The maximum ratio of the olefin length of the largest pore diameter ( L / D ) of Cu-BTC was approximately 1.57. Furthermore, theoretical calculations (radial distribution function (RDF)) and experiments (infrared (IR) spectra) confirmed the interaction of n-olefin adsorbates and the Cu-BTC framework occurred between the -CH= of olefins and the Cu and O atoms of the Cu-BTC framework. This work adds to the understanding and investigation of the adsorption of liquid lubricants using Cu-BTC as a metal-organic framework (MOF).
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yabo Gao,Qing Zhu,Zhong Huang,Shaowei Zhang,Yongxin Wang,Gongye lv,Hang Li,Xin Zhang,Zhaoping Hou,Haijun Zhang
Nanoporous metals are considered as the ideal catalysts owing to their open pore structure and high surface area. In the present work, a series of nanoporous Cu-based metamaterial (nano-Cu/MM) catalysts with triply periodic minimal surface (TPMS) were developed by the selective laser melting (SLM) and chemical dealloying process. The TPMS structure endowed the porous metamaterial with an excellent mechanical property and an abundant pathway for mass transfer. The as-prepared nano-Cu/MM was applied as a Fenton-like catalyst in the advanced oxidation process, and the degradation rate of methylene blue (MB) was as high as 99 % in 10 min. In addition, the catalyst showed a good applicability, which could effectively degrade the complex dyes and tetracycline drugs. To meet the practical application, a TPMS-structured coaxial circular with nanoporous structure was designed and prepared by the same process, which could be simply assembled with an electric motor to achieve a continuous catalytic degradation, demonstrating its potential for the industrial applications.
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NANO
·
2020
·
IF 1.566
Bo Tang,Li Ji,Yuanzhe Dai,Haiqun Chen,Zhenyu Zhang,Zhengwei Wang,Sen Li
MOF-based composite material is adopted to modify photoanode, and the obtained large BET area is found meaningful to the dye loading amount, which brings about a high short circuit current and incident photon to current conversion efficiency. Meanwhile, three-dimensional graphene networks (3DGNs) are employed to provide a fast transport channel for photo-induced electrons. The morphology is analyzed by SEM, TEM, XRD and Raman spectrum, and the photovoltaic performances are recorded to reveal the specific functions of MOF and 3DGNs. The synergy between MOF, 3DGNs and TiO 2 is achieved by adjusting their mass fraction. Moreover, the average size of MOF exerts a significant influence on the resulting properties resulting from the scattering ability to incident light. After corresponding optimizing, the short circuit current, open circuit voltaic, fill factor and energy conversion efficiency reach 20.5 mAcm − 2 , 680 mV, 0.619% and 8.63%.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Jia-Fang Xie,Jie-Jie Chen,Yu-Xi Huang,Xing Zhang,Wei-Kang Wang,Gui-Xiang Huang,Han-Qing Yu
In this work, a novel Cu-Pd heterostructure, derived from CuCl-PdO x hexagonal microplates, was prepared to tune selective single hydrocarbon production from electrochemical CO 2 reduction. The CuCl-PdO x hexagonal microplates were synthesized by a dual-potential electrodeposition technique, followed by electrochemical reduction to form Cu-Pd heterostructure. This Cu-Pd heterostructure exhibited a much higher CO 2 -to-CH 4 selectivity (32 % Faradaic efficiency, FE) compared to pure Cu or Pd. Moreover, Cu-Pd heterostructure showed excellent suppression on C 2 H 4 generation (below 1 % FE). The density functional theory calculations suggested that the hollow site of Pd region in the Cu-Pd heterostructure could stablize CO* intermediate and selectively lowered the energy demand for CH 4 formation rather than C 2 H 4 . This work provides new opportunities of designing Cu-based electrocatalysts for selective CO 2 reduction to single hydrocarbon.
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LANGMUIR
·
2024
·
IF 3.7
Yuling Shi,Qing Liu,Qianqian Pan,Danlong Yang,Yangeng Lan,Tao Wang
Nanoparticle composite microspheres are a versatile material with unique features and wide-ranging applications, including catalysis, biological medicine, and electronic devices. The adsorption behavior of nanoparticles on the surface of microspheres plays a crucial role in determining the further application potentials. The understanding of nanoparticle adsorption behavior on microsphere surfaces is essential for guiding future applications in nanoparticle composite microspheres. In this work, the adsorption behavior of unstable copper nanoparticles (Cu NPs) on polystyrene-based (PS-based) microspheres was investigated. The influence of PS-based microspheres’ surface properties and the oxidation degree of Cu NPs were determined. The adsorption mechanism of Cu NPs on PS-based microspheres was analyzed. Furthermore, the amounts and rates of adsorption were examined. It was found that the Cu NPs can be rapidly and firmly adsorbed on the surface of carboxyl-modified polystyrene microspheres. Additionally, precise control over the distribution of Cu NPs on the surface of PS-based microspheres can be achieved by manipulating the solvent’s polarity.
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PubMed
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-14
·
IF 14.7
Liu Shikai,Li Yuheng,Wang Di,Xi Shibo,Xu Haoming,Wang Yulin,Li Xinzhe,Zang Wenjie,Liu Weidong,Su Mengyao,Yan Katherine,Nielander Adam C.,Wong Andrew B.,Lu Jiong,Jaramillo Thomas F.,Wang Lei,Canepa Pieremanuele,He Qian
The reconstruction of Cu catalysts during electrochemical reduction of CO 2 is a widely known but poorly understood phenomenon. Herein, we examine the structural evolution of Cu nanocubes under CO 2 reduction reaction and its relevant reaction conditions using identical location transmission electron microscopy, cyclic voltammetry, in situ X-ray absorption fine structure spectroscopy and ab initio molecular dynamics simulation. Our results suggest that Cu catalysts reconstruct via a hitherto unexplored yet critical pathway - alkali cation-induced cathodic corrosion, when the electrode potential is more negative than an onset value ( e.g ., −0.4 V RHE when using 0.1 M KHCO 3 ). Having alkali cations in the electrolyte is critical for such a process. Consequently, Cu catalysts will inevitably undergo surface reconstructions during a typical process of CO 2 reduction reaction, resulting in dynamic catalyst morphologies. While having these reconstructions does not necessarily preclude stable electrocatalytic reactions, they will indeed prohibit long-term selectivity and activity enhancement by controlling the morphology of Cu pre-catalysts. Alternatively, by operating Cu catalysts at less negative potentials in the CO electrochemical reduction, we show that Cu nanocubes can provide a much more stable selectivity advantage over spherical Cu nanoparticles.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Wei Zhou,Mazhar Ahmed Memon,Mengmeng Niu,Xinqiang Fan,Yanan Jiang,Xian Zhang,Yuan Liu
Copper (Cu) based catalysts are frequently used in CO 2 hydrogenation, particularly in reverse water-gas shift (rWGS) and CO 2 -to-methanol reaction. Cu 0 and Cu + are the key species affecting the catalyst performance and product distribution . Therefore, constructing and adjusting Cu 0 /Cu + active pairs is significant for the catalyst design . In this study, Cu 0 /Cu + active pairs are obtained by utilizing the properties of perovskite-type oxides (PTOs). A series of CaTi 1-x Cu x O 3 and Ca 0.8 La 0.2 Ti 1-x Cu x O 3 (x = 0.05, 0.10, 0.15, 0.30, 0.40 and 0.50) were synthesized via citric acid complexing method and part of the Cu species entered the PTOs lattice. After reduction, large Cu particles and highly-dispersed Cu clusters were obtained simultaneously. The dispersed Cu clusters have more interfaces with the PTOs and provide abundant Cu + while large Cu particles tend to aggregate and supply mainly Cu 0 . Cu 0 activates H 2 and CO 2 and plays a vital role in the rWGS reaction . Cu + is the active site for methanol synthesis and it can strongly absorb CO. The ratio of Cu 0 /Cu + varies with different Cu content and doping La can also adjust the chemical state of surface Cu. The performance test demonstrates that both excessively high and low Cu 0 /Cu + ratios are beneficial for CO generation, while a moderate ratio is suitable for methanol synthesis . These insights provide a method for regulating the chemical state of surface metal species and help the catalyst design for CO 2 hydrogenation.
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FIBERS AND POLYMERS
·
2017
·Vol. 18
·期 7
·1250-1254
·
IF 1.113
Chen Yingbo,Liu Huiqiang,Hu Xiaoyu,Cheng Bowen,Liu Dongqing,Zhang Yufeng,Nair Sankar
Membranes with high water permeation capability as well as high rejection to dye molecules are very important for dye separation. In this study, a metal organic framework structure (Cu-BTC) was fabricated in situ on a poly(vinyl difluoride) hollow fiber support for nanofiltration of dye solution. In order to protect the Cu-BTC layer, the surface was coated by crosslinking polyvinyl alcohol. The composite membranes showed no rejection to divalent salts and high rejection to Congo Red dye. It was noticed that several Cu-BTC layers could enhance dye rejection of the composite membranes. This novel composite membrane showed promising applications in the separation of dye molecules from aqueous solutions containing dissolved salts.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-9
·
IF 16.6
Feng Sihua,Duan Hengli,Tan Hao,Hu Fengchun,Liu Chaocheng,Wang Yao,Li Zhi,Cai Liang,Cao Yuyang,Wang Chao,Qi Zeming,Song Li,Liu Xuguang,Sun Zhihu,Yan Wensheng
The development of two-dimensional (2D) magnetic semiconductors with room-temperature ferromagnetism is a significant challenge in materials science and is important for the development of next-generation spintronic devices. Herein, we demonstrate that a 2D semiconducting antiferromagnetic Cu-MOF can be endowed with intrinsic room-temperature ferromagnetic coupling using a ligand cleavage strategy to regulate the inner magnetic interaction within the Cu dimers. Using the element-selective X-ray magnetic circular dichroism (XMCD) technique, we provide unambiguous evidence for intrinsic ferromagnetism. Exhaustive structural characterizations confirm that the change of magnetic coupling is caused by the increased distance between Cu atoms within a Cu dimer. Theoretical calculations reveal that the ferromagnetic coupling is enhanced with the increased Cu-Cu distance, which depresses the hybridization between 3 d orbitals of nearest Cu atoms. Our work provides an effective avenue to design and fabricate MOF-based semiconducting room-temperature ferromagnetic materials and promotes their practical applications in next-generation spintronic devices.
研究领域:
材料科学
·
凝聚态物理
·
自旋电子学
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