Journal of Physical Chemistry C
·
2024
·
IF 3.3
Fumei Wang,Qi Cai,Xinhua He,Boxiong Shen,Leila Negahdar,Shuo Feng,Andrew M. Beale
Cu/SAPO-34 catalysts have been widely used for the reduction of NOx from diesel exhaust by ammonia-selective catalytic reduction (SCR). Sulfur poisoning remains a challenge for Cu/SAPO-34 catalysts in NH3–SCR, restricting its application. In this study, Cu/SAPO-34 samples containing a mixture of Cu species comprising isolated Cu2+ located in the 6MR, Cu(OH)+ in 8MR, CuO clusters/nanoparticles, and Cu+ species were prepared. The Cu speciation during SO2 and hydrothermal aging of Cu/SAPO-34 SCR catalysts was subsequently studied. While hydrothermal aging had little effect on catalytic activity, the sulfur-aged sample exhibited deterioration in NH3–SCR activity over the temperature range of 100–575 °C. The breakage and collapse of the zeotype framework and chemical deactivation of the Cu/SAPO-34 catalyst after exposure to SO2 and H2O took place. A combination of X-ray photoelectron spectroscopy (XPS) and TGA-DT-DSC revealed the presence of ammonium bisulfate, copper bisulfate/sulfate, aluminum sulfate, and sulfuric acid after SO2 and H2O copoisoning under SCR conditions. Furthermore, Cu(OH)+ tended to migrate to form isolated Cu2+ and Cu+, as well as agglomerate to form CuO particles. Density functional theory (DFT) calculations revealed that SO2 and O2 could readily be absorbed by CuO particles to form stable copper bisulfate/sulfate species with the following order of preference: CuO > Cu+ > Cu2+ > Cu(OH)+. In contrast, Cu(OH)+ was less prone to be poisoned by easily releasing SO3 than other Cu species sites.
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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 Energy Storage
·
2024
·
IF 8.9
Jianguo Duan,Xinshuai Yan,Kun Lei,Jianguo Cheng,Yaxiong Wang,Qingzong Su,Shimin Xu,Jianming Li,Qing Ma
The phase change materials (PCMs) are encapsulated into porous materials for collecting and storing heat energy has been widely used to overcome the intermittency of solar energy utilization. However, due to the inherent big pore structure and surface characteristics, metal porous materials are not ideal for PCM leakage-proof and slow photo-thermal response. To address these issues, A micro/nanostructured graphene-polyvinyl alcohol nanosheets/Cu(OH) 2 nanowire on a three-dimensional Cu foam (CF) to fill with PCM was designed and prepared. In the composite PCM, the polyvinyl alcohol/reduced graphene oxide (PRG) films coated on Cu(OH) 2 @Cu foam (CCF) provided a large number of active sites for the adsorption of modified paraffin wax (PWS). The prepared composite PCM has a stable structure and high thermal conductivity properties, meanwhile, the strong PRG films play a key role in enhancing leakage-proof and stability. The results show that the enthalpy value of PRG-CCF/PWS are 160.25 J·g −1 after 200 thermal cycles; which still maintains excellent cycle thermal reliability. In addition, under the simulated solar irradiation intensity is 120 mW·cm −2 , the heat storage rate and photo-thermal conversion efficiency of PRG-CCF/PWS are 1.37 J·s −1 and 90.25 %, respectively. It shows excellent photo-thermal response and uniform temperature distribution. This work provides an efficient, sustainable and affordable strategy for manufacturing high-performance composite PCM that can efficiently achieve solar energy utilization and energy management.
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ELECTROCHIMICA ACTA
·
2015
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IF 4.504
Ningyan Cheng,Yurui Xue,Qian Liu,Jingqi Tian,Lixue Zhang,Abdullah M. Asiri,Xuping Sun
In this paper, we develop a novel strategy toward the in-situ growth of core/shell nanorods array consisting of Cu(OH) 2 -CuO nanosheets as the shell and Cu as the core on Cu foil [Cu/(Cu(OH) 2 -CuO) NA/CF]. As an integrated 3D non-noble-metal oxygen evolution anode, the Cu/(Cu(OH) 2 -CuO) NA/CF shows high catalytic activity with an onset overpotential of 350 mV and a Tafel slope of 76 mV/dec. It needs an overpotential of 417 mV to drive current density of 10 mA/cm 2 and maintains its catalytic activity for at least 22 h. The attractive performances make it promising candidate as a future high-performance catalyst for applications.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Kunli Song,Shuqi Zhao,Zhenguo Li,Kaixiang Li,Yurong Xu,Yijun Zhang,Yonghong Cheng,Jian-Wen Shi
SSZ-13 has been commercialized as a catalyst in diesel engines for the selectivity catalytic reduction of nitrogen oxides (NO x ) with ammonia (NH 3 -SCR), but the catalyst is facing the problem of poisoning. Herein, two well-designed catalysts, Cu-SSZ-13 and cerium (Ce) doped Cu-SSZ-13 are synthesized, and their tolerance to zinc (Zn) and phosphorus (P) poisoning alone and together are explored in detail. The research found that Zn and P poisoning alone leads to the destruction of Cu-SSZ-13 structure, resulting in the decline of denitration (de-NO x ) performance following the mechanism dominated by Eley-Rideal (E-R). Surprisingly, it is found that zinc phosphate particles are formed at inactive sites on the surface of Cu-SSZ-13 in the presence of Zn and P together, which protects the active sites, enhances the adsorption of nitric oxide. As a result, the excellent de-NO x performance of Cu-SSZ-13 is well maintained following the dual mechanism of E-R and Langmuir-Hinshelwood (L-H). In addition, the introduction of Ce stabilizes the active sites, so as to improve the de-NO x performance and the poisoning tolerance of Cu-SSZ-13. This work deeply analyzes the reasons of Zn and P poisoning and the positive effect of Ce on Cu-SSZ-13, which provides ideas for improving the poisoning tolerance of Cu-SSZ-13 and promotes the further application.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Qia Zhang,JianXiong Zou,Jin Ai,XiaoTian Pan,DongHong Qiao,Seong Chan Jun,Vijaykumar V. Jadhav,Ling Kang,Chun Huang,Jian Zhang
The current collector serves as a crucial element in supercapacitors, acting as a medium between the electrode material and the substrate. Due to its excellent conductivity, a metal collector is typically favored. Enhancing the binding strength between the collector and the substrate as well as between the collector and the electrode material has emerged as a critical factor for enhancing the capacitance performance. In this study, a Ag film with a grass root-like structure was initially grown on a PI substrate through the surface modification and ion exchange (SMIE) process. This Ag interlocking structure contributes to strong binding between the PI substrate and Ag without compromising the mechanical properties of the Ag film. To further enhance the electrochemical properties at low scan rates, electroless-plated Cu was subsequently deposited on the Ag film to form the Cu/Ag current collector. Moreover, the Cu within the Cu/Ag current collector served as a precursor for the growth of FeOOH–Cu(OH)2 via a two-step in situ method. The resulting FeOOH–Cu(OH)2/Cu/Ag structure as a whole is binder-free. Supercapacitors employing symmetric FeOOH–Cu(OH)2/Cu/Ag structures were assembled, and their energy storage properties were investigated. The solution-based low-temperature process used in this study offers the potential for cost-effective and large-scale applications.
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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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