PLASMA CHEMISTRY AND PLASMA PROCESSING
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2023
·Vol. 43
·期 6
·1963-1978
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IF 3.6
Lv Huan,Liu Xinyuan,Hao Yingzi,Yi Yanhui
The industrial utilization of methane to methanol is based on the indirect pathway with syngas as an intermediate product, but the reaction conditions are very harsh and the costs in equipment and operations are extremely high. Therefore, the direct oxidation of methane to methanol (DOMTM) under mild conditions is more desirable. In this paper, coupling of non-thermal plasma and Cu–zeolite (Cu–ZSM-5 and Cu–S-1) catalysts have been studied for DOMTM. The effect of Si/Al ratios (Cu–ZSM-5 and Cu–S-1 catalysts) on the reaction performance has been investigated. Cu–S-1 catalyst exhibited the best catalytic performance, i.e., 5.8% methane conversion and 50.6% methanol selectivity. The employed catalysts have been characterized by XRD, UV–Vis, XPS and FT-IR. The results show that Cu–ZSM-5 catalysts with high Si/Al ratio are conducive to the formation of isolated Cu 2+ species, and Cu–S-1 catalyst exhibits the most abundant isolated Cu 2+ species. Furthermore, Cu–S-1 catalyst shows the most abundant O ads species. The plentiful surface silicon defects on S-1 is the reason why Cu–S-1 catalyst shows the most abundant isolated Cu 2+ and O ads species, and these two species are interdependent to form a Si–O–Cu species, which may be the active site for DOMTM. Based on these findings, the possible catalytic mechanism was proposed.
研究领域:
化学工程
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催化化学
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高影响因子
ACS Nanoscience Au
·
2024
·
IF 4.8
Dan Luo,Zhiheng Xie,Shuangqun Chen,Tianyi Yang,Yalin Guo,Ying Liu,Zhouhao Zhu,Liyong Gan,Lingmei Liu,Jianfeng Huang
Electrochemical semihydrogenation (ESH) of alkynes to alkenes is an appealing technique for producing pharmaceutical precursors and polymer monomers, while also preventing catalyst poisoning by alkyne impurities. Cu is recognized as a cost-effective and highly selective catalyst for ESH, whereas its activity is somewhat limited. Here, from a mechanistic standpoint, we hypothesize that electron-deficient Cu can enhance ESH activity by promoting the rate-determining step of alkene desorption. We test this hypothesis by utilizing Cu–Ag hybrids as electrocatalysts, developed through a welding process of Ag nanoparticles with Cu nanowires. Our findings reveal that these rationally engineered Cu–Ag hybrids exhibit a notable enhancement (2–4 times greater) in alkyne conversion rates compared to isolated Ag NPs or Cu NWs, while maintaining over 99% selectivity for alkene products. Through a combination of operando and computational studies, we verify that the electron-depleted Cu sites, resulting from electron transfer between Ag nanoparticles and Cu nanowires, effectively weaken the adsorption of alkenes, thereby substantially boosting ESH activity. This work not only provides mechanistic insights into ESH but also stimulates compelling strategies involving hybridizing distinct metals to optimize ESH activity.
研究领域:
化学工程
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电催化
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材料科学
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DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
·
IF 21.1
Hongman Sun,Yuanyuan Wen,Yaqian Li,Rong Fan,Yonglian Lu,Chao Feng,Hao Liu,Youhe Wang,Zhipeng Ma,Yu Zhang,Rose Amal,Zifeng Yan
Ag@Cu 2 O tandem catalysts is effective to improve the selectivity of hydrocarbons in CO 2 RR, where Ag core generates *CO intermediates, which migrate to Cu 2+ /Cu + interface, promoting proton transfer and C-C coupling forming *OCCHO. However, Cu + crucial for C-C coupling exhibits instability under reductive conditions. Herein, we used Ag@Cu 2 O tandem catalysts as a sacrificial template to synthesize Ag@Cu 2 O@Cu-BDC (BDC = 1,4-benzenedicarboxylic acid) tandem catalysts through an in-situ conversion strategy, which can not only introduce Cu 2+ , but also stabilize Cu + by forming a Cu-BDC MOF shell. In addition, by adjusting the amount of sacrificial template, the controllable regulation of Cu 2+ and Cu + content was successfully achieved, forming a Cu 2+ /Cu + valence state fluctuation buffer zone. It is found that this modulation not only significantly improve the selectivity towards hydrocarbons (CH 4 +C 2 H 4 ), but also enables the regulation of the reaction pathway, thereby allowing for fine-tuning of product selectivity. Notably, the Ag@Cu 2 O@Cu-BDC-5 tandem catalyst with a lower Cu 2+ /Cu + ratio demonstrated superior CH 4 selectivity (59.3 %), while the Ag@Cu 2 O@Cu-BDC-10 tandem catalyst with a higher Cu 2 ⁺/Cu + ratio achieved dominant C 2 H 4 production (43.0 %) under applied potential of −1.4 V vs. RHE for 20 h. This is attributed to Cu 2+ sites facilitated *CHO generation, while Cu + sites promoted C-C coupling as evidenced by the in-situ infrared and DFT calculations. Additionally, this study demonstrated the existence of a tandem catalysts that could increase the CO coverage on Cu sites, ensuring the full utilization of Cu + and Cu 2+ sites to further enhance product selectivity and reduce the overpotential for optimal product generation.
研究领域:
电化学
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催化
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材料科学
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二氧化碳还原
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能量转换
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表面化学
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纳米技术
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DOI
高影响因子
Nanomaterials
·
2020
·Vol. 10
·期 3
·509
·
IF 4.324
Shuzhen Zhou,Lihua Kang,Xuening Zhou,Zhu Xu,Mingyuan Zhu
Ethylene is an important chemical raw material and with the increasing consumption of petroleum resources, the production of ethylene through the calcium carbide acetylene route has important research significance. In this work, a series of bimetallic catalysts with different Cu/Ni molar ratios are prepared by co-impregnation method for the hydrogenation of calcium carbide acetylene to ethylene. The introduction of an appropriate amount of Cu effectively inhibits not only the formation of ethane and green oil, thus increasing the selectivity of ethylene, but also the formation of carbon deposits, which improves the stability of the catalyst. The ethylene selectivity of the Ni–Cu bimetallic catalyst increases from 45% to 63% compared with the Ni monometallic counterpart and the acetylene conversion still can reach 100% at the optimal conditions of 250 °C, 8000 mL·g−1·h−1and V(H2)/V(C2H2) = 3. X-ray diffraction and transmission electron microscopy confirmed that the metal particles were highly dispersed on the support, High-resolution transmission electron microscopy and H2-Temperature programmed reduction proved that there was an interaction between Ni and Cu, combined with X-ray photoelectron spectroscopy and density functional theory calculations results, Cu transferred electrons to Ni changed the Ni electron cloud density in NiCuxcatalysts, thus reducing the adsorption of acetylene and ethylene, which is favorable to ethylene selectivity.Keywords:Ni–Cu;calcium carbide acetylene;selective hydrogenation;ethylene
研究领域:
催化化学
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材料科学
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DOI
PubMed
高影响因子
CATALYSIS TODAY
·
2024
·
IF 5.2
Mingze Xu,Guangjie Wang,Haiyu Li,Tingsong Zhang,Jinhua Li,Yu Wang,Yue Peng,Wenzhe Si
The issue of water pollution has emerged as a formidable challenge, prompting a pressing need for solutions. The utilization of metal nanoparticles with surface plasmon resonance and semiconductor composite photocatalysts is regarded as a highly effective approach to solve this problem. g C 3 N 4 is an effective catalyst for the degradation of organic pollutants. Its photocatalytic performance could be enhanced by the use of the metal such as Au, Ag, and Cu. However, the Schottky barrier is generally believed to be the reason that Cu can enhances the photocatalytic performance of g C 3 N 4 . In fact, the plasmonic of Cu will also have an effect on the photocatalytic effect of g C 3 N 4 , like Au and Ag. In this study, it is first proposed that the photocatalytic performance of g C 3 N 4 can be enhanced by combining the plasmonic of Cu and the Schottky barrier. Cu g/C 3 N 4 nanocomposites with stable crystal structure, with Cu as the core and g C 3 N 4 as surface coating, were synthesized and characterized by transmission electron microscopy (TEM), X ray diffractometer (XRD) and ultraviolet visible spectroscopy (UV Vis) and X ray photoelectron spectroscopy (XPS). Then, it is optimized that the Cu/g C 3 N 4 composite material which were prepared with 200 nm Cu particles, GSH as the ligand bridge, and a Cu: g C 3 N 4 ratio of 5:1, have the best photocatalytic property, which is 16.7 times of the photocatalytic property of g C 3 N 4 . Besides, the transfer efficiency of hot electrons of 33% (from Cu to g C 3 N 4 ) under the influence of the Schottky barrier (0.58 eV) is calculated theoretically. On this basis, the mechanism of Cu nanoparticles enhancing the photocatalytic performance of g C 3 N 4 was also been proved through the calculation result and transient photocurrent spectroscopy (TPC), electrochemical impedance spectroscopy (EIS), and steady state transient fluorescence spectroscopy (PL) characterization. The excellent photocatalytic performance of the Cu/g C 3 N 4 composites is due to the simultaneous influence of Schottky barrier and LSPR of Cu.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
Nano-Micro Letters
·
2023
·Vol. 15
·期 1
·1-15
·
IF 26.6
Li Minhan,Zhang Fangzhou,Kuang Min,Ma Yuanyuan,Liao Ting,Sun Ziqi,Luo Wei,Jiang Wan,Yang Jianping
Electrochemical reduction of CO 2 into high-value hydrocarbons and alcohols by using Cu-based catalysts is a promising and attractive technology for CO 2 capture and utilization, resulting from their high catalytic activity and selectivity. The mobility and accessibility of active sites in Cu-based catalysts significantly hinder the development of efficient Cu-based catalysts for CO 2 electrochemical reduction reaction (CO 2 RR). Herein, a facile and effective strategy is developed to engineer accessible and structural stable Cu sites by incorporating single atomic Cu into the nitrogen cavities of the host graphitic carbon nitride (g-C 3 N 4 ) as the active sites for CO 2 -to-CH 4 conversion in CO 2 RR. By regulating the coordination and density of Cu sites in g-C 3 N 4 , an optimal catalyst corresponding to a one Cu atom in one nitrogen cavity reaches the highest CH 4 Faraday efficiency of 49.04% and produces the products with a high CH 4 /C 2 H 4 ratio over 9. This work provides the first experimental study on g-C 3 N 4 -supported single Cu atom catalyst for efficient CH 4 production from CO 2 RR and suggests a principle in designing highly stable and selective high-efficiency Cu-based catalysts for CO 2 RR by engineering Cu active sites in 2D materials with porous crystal structures.
研究领域:
化学
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材料科学
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电化学
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环境科学
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产品关联
DOI
PubMed
高影响因子
LANGMUIR
·
2022
·
IF 4.331
Yibo Ao,Jinqing Ao,Ling Zhao,Liwei Hu,Fengsheng Qu,Biao Guo,Xue Liu
Cu(OH)2 nanomaterials are widely investigated for non-enzymatic glucose sensors due to their low-cost and excellent performance. Cu(OH)2 nanomaterials usually grow on substrates to form sensor electrodes. Reported works mainly focus on structure adjusting of the Cu(OH)2 nanostructures, while the optimization of substrates is still lacking. In the present work, directional porous Cu (DPC) was applied as the substrate for the growth of Cu(OH)2 nanograss (NG), and hierarchical structures of Cu(OH)2@DPC were prepared by alkaline oxidation. The morphology and microstructure evolution of the prepared hierarchical structures was investigated, and the non-enzymatic glucose sensing performance was evaluated. Cu(OH)2@DPC exhibits enhanced comprehensive non-enzymatic glucose sensing performance compared to the reported ones, which may benefit from both the effective adsorption of the Cu(OH)2 NG with a relatively high surface area and the high solute exchange of the DPC by a channel effect. This work provides new insights into the further improvement of the non-enzymatic glucose sensing performance of Cu(OH)2 nanostructures by optimizing the substrate structure.
研究领域:
材料科学
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传感器技术
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纳米技术
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DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Xiaoxue Zhao,Linlin Sun,Xian Jin,Mengyang Xu,Shikang Yin,Jinze Li,Xin Li,Dong Shen,Yan Yan,Pengwei Huo
Z-scheme heterojunction can effectively separate photo-generated carriers and enhance photocatalytic activity of CO 2 reduction. In this work, we report indirect Z-scheme heterojunction of UiO-66-NH 2 /Cu 2 O/Cu, which achieves highly CO 2 photocatalytic conversion to CO. Among these, UiO-66-NH 2 /Cu 2 O/Cu-0.39 (U/C/Cu-0.39) displays the best activity with a CO yield of 4.54 μmol·g −1 ·h −1 , which is 37.8 times higher than that for UiO-66-NH 2 and 50.4 times higher than that for Cu 2 O. Cu not only acts as the electron conductor of the indirect Z-scheme heterojunction to promote the charge carrier transmission, but also acts as the active site of CO 2 reduction. The increase of active sites and the CO 2 adsorption capacity results in the superior photocatalytic performances.
研究领域:
材料科学
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化学
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环境科学
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DOI
高影响因子
INORGANIC CHEMISTRY COMMUNICATIONS
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2019
·
IF 1.795
Qing-Qing Huang,Yang-Jie Lin,Rui Zheng,Wei-Hua Deng,Chiranjeevulu Kashi,P. Naresh Kumar,Guan-E Wang,Gang Xu
Metal-organic frameworks (MOFs) are a kind of functional porous materials with the potential applications in gas adsorption and separation, catalysis, energy storage, sensor, and electrical conductivity . However, the insulating nature of the mostly MOFs limits their application in the electronic field. A new three-dimensional (3D) metal-organic framework composed of Cu 2+ centres and polyacid linkers (TATAB 3− ) was synthesized by solvothermal method , which contains two types of Cu 24 cages. The crystal structure is cubic and each Cu is coordinated by five oxygen atoms which can be confirmed by the single crystal X-ray diffraction, infrared spectra and TGA analysis. The conductivity for this 3D MOF is increased by four orders of magnitude after doping with 7,7,8,8-tetracyanoquinodimethane (TCNQ) and realizes the transformation from an insulator to semiconductor.
研究领域:
材料科学
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电子工程
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DOI
高影响因子
INORGANIC CHEMISTRY
·
2022
·
IF 5.436
Chunpei Yu,Bonan Gu,Jiaxin Wang,Junhong Chen,Wenchao Zhang,Wei Shi,Gexing Yang,Xiaoting Lei,Junwu Zhu
The development of green primary explosives has become a “holy grail” of energetic materials research. Cu-based 5-nitrotetrazolate is considered one of the most promising candidates due to its excellent blasting power and environmentally benign nature. However, synthesizing Cu-based 5-nitrotetrazolate controllably and securely remains highly challenging. Herein, room-temperature anodization of metallic Cu and a Cu(I)–imidazole nanowire array on copper substrates in a sodium 5-nitrotetrazolate electrolyte leads to in situ electrosynthesis of Cu(I) 5-nitrotetrazolate (DBX-1, CuNT) and its analogue, Cu(II) 5-nitrotetrazolate [Cu(NT)2], respectively. Both obtained CuNT and Cu(NT)2 films demonstrate remarkable energy output and good laser-induced ignition performance. The thermal stability (Tp = 291 °C) and electrostatic safety (E50 = 2.54 mJ) of CuNT proved to be superior to those of Cu(NT)2 (Tp = 257 °C, and E50 = 0.57 mJ). Remarkably, this study provides an exciting new method for the rational design and development of Cu-based 5-nitrotetrazolate as a primary explosive for advanced initiating applications.
研究领域:
含能材料
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炸药化学
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电化学
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材料科学
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DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Jicheng Wang,Yanhong Quan,Linjie Li,Shunan Yin,Xinxin Ding,Jun Ren
A series of Cu/SBA-15 catalysts with different Cu loadings are prepared by the ammonia evaporation method for the liquid-phase hydrogenation of furfural (FF) to furfuryl alcohol (FA). The results show that the supported Cu loading influences the structure and catalytic activity during FF hydrogenation. The 20Cu/SBA-15 catalyst shows the optimum performance with 99.3 % FF conversion, 99.0 % selectivity to FA, nearly pure FA product, and a turnover frequency reaching up to 81.7h −1 . The effect of Cu loading can be related to Cu dispersion and the interaction between the metal and support, which further promotes the surface Cu + /Cu 0 ratio. Additionally, the correlation of FF conversion with Cu + /Cu 0 ratio confirms that the excellent performance of 20Cu/SBA-15 is mainly derived from the synergy of Cu + and Cu 0 species, although the range of performance is not large. Finally, the optimal reaction conditions are screened using a reaction temperature of 150 °C, a reaction pressure of 4 MPa, a catalyst dosage of 0.1 g, and a reaction time of 60 min. The present study confirms that the Cu loading has a significant effect on the structure of Cu/SBA-15 and nearly pure objective FF product can be feasibly obtained with an appropriate Cu support in the synthesis of FA from FF hydrogenation.
研究领域:
催化化学
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材料科学
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Kaicheng Qian,Tong Wei,Xiaoqing Yan,Dongming Qi,Mingwu Tan,Renhong Li
Element doping is a viable strategy to regulate the metal–support interface for enhancing the catalytic performance of supported metal catalysts. Herein, Cu/ZnO:Cu-TH catalysts are prepared by immobilizing Cu nanoparticles (NPs) on ZnO nanorods featuring an adjustable oxygen vacancy, in which partial Cu atoms at the Cu–ZnO interface are incorporated into the ZnO lattice to form CuxZn1–xO species. Such Cu atom doping induces the creation of distinctive Cu–CuxZn1–xO interface sites and optimizes electron transfer from ZnO to Cu NPs, thereby achieving intermediate activation and ultimately endowing the catalyst with superior performance in reforming alkali-free formaldehyde (HCHO) into hydrogen at low temperatures. The Cu–CuxZn1–xO interface sites serve as pivotal centers for HCHO reforming, where the Cu sites and CuxZn1–xO sites selectively engage in the cleavage of C–H bonds in HCHO and O–H bonds in H2O, respectively. Meanwhile, the presence of oxygen vacancies bolsters the Cu–CuxZn1–xO sites in enhancing the adsorption of HCHO and H2O, further improving the activity. The Cu/ZnO:Cu-450H catalyst, distinguished by abundant Cu–CuxZn1–xO sites and a high concentration of oxygen vacancies, demonstrates optimal activity with TOF values of 16.9 and 72.4 h–1 under anaerobic and aerobic conditions, respectively, which are 8.9 and 29.0 times higher than those of the Cu/ZnO-450N catalyst, which lacks doped Cu atoms and oxygen vacancies.
研究领域:
催化化学
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材料科学
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产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）