CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Xianlong Lu,Lili Wang,Xueyang Zhao,Binbin Pan,Zhendong Li,Xiangfei Du,Shihan Zhang,Fan Dong,Bangwei Deng
Copper (Cu)-based catalysts show significant potential for producing high value-added C 2+ products in electrocatalytic CO 2 /CO reduction reactions (CO (2) RR). However, the structural reconfiguration during operation poses substantial challenges in identifying the intrinsic catalytic active site, especially under similar mass transport conditions. Herein, three typical and commercial Cu-based catalysts (Cu, CuO, and Cu 2 O) are chosen as representatives to elucidate the structure-activity relationship of CORR in the membrane electrode assembly electrolyzer. Notably, only the Cu catalyst demonstrates the most suppression of hydrogen evolution reaction, thus achieving the highest FE of 86.7% for C 2+ products at a current density of 500 mA cm –2 and maintaining a stable electrolysis over 110 h at a current of 200 mA cm –2 . The influence of chemical valence state of Cu, electrochemical surface area, and local pH were firstly investigated and ruled out for the significant FE differences. Finally, based on the structure analysis from high resolution transmission electron microscope, OH – adsorption, in situ infrared spectroscopy and density functional theory calculations, it is suggested that the asymmetric C-C coupling ( via *CHO and *CO) is the most probable reaction pathway for forming C 2+ products, with Cu (100)-dominant grain boundaries (GBs) being the most favorable active sites. These findings provide deeper insights into the synergistic relationship between crystal facets and GBs in electrocatalytic systems.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Chunyi Ye,Yang Yang,Shujing Chen,Chunhua Liu,Xiao-Qing Sun,Danni Liu,Jiujun Zhang,Jing-Li Luo,Xian-Zhu Fu
Hydrogen (H 2 ) is a promising green alternative fuel; however, the widespread adoption of H 2 production technologies is limited by high energy consumption and significant carbon emissions. Here, we have developed a bipolar H 2 production electrolyzer that purifies wastewater and produces H 2 with ultra-low energy consumption by combining the formaldehyde 1-electron oxidation reaction (FOR-1) at the anode and the hydrogen evolution reaction (HER) at the cathode. The electroless Cu electrode exhibits high selectivity and activity for the 1-electron pathway of formaldehyde oxidation (i.e., FOR-1), enabling the anodic conversion of formaldehyde into valuable H 2 and formate. This facilitates the treatment of toxic formaldehyde waste while doubling H 2 production efficiency of the electrolyzer. Unlike conventional water electrolysis, the formaldehyde-water electrolyzer demonstrates a cell voltage reduction of 1.49 V at 10 mA/cm 2 . At 100 mA/cm 2 , the energy consumption is reduced to only 25 % of that in conventional systems, even with the use of a nickel foam cathode. Moreover, formaldehyde in wastewater is fully degraded within 50 min, highlighting its practical application potential.
✓ 已验证
产品关联
DOI
高影响因子
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.
✓ 已验证
DOI
高影响因子
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.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ORGANIC CHEMISTRY
·
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
✓ 已验证
DOI
高影响因子
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.
✓ 已验证
产品关联
DOI
高影响因子
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%.
✓ 已验证
产品关联
DOI
高影响因子
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.
✓ 已验证
产品关联
DOI
高影响因子
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).
✓ 已验证
产品关联
DOI
高影响因子
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.
✓ 已验证
产品关联
DOI
高影响因子
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.
✓ 已验证
产品关联
DOI
高影响因子
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.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）