APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Yangzhi Xu,Zirui Gao,Yao Xu,Xuetao Qin,Xin Tang,Zhiwei Xie,Jinrong Zhang,Chuqiao Song,Siyu Yao,Wu Zhou,Ding Ma,Lili Lin
Hydrogenation of CO 2 into methanol at low-temperature on Cu-based catalysts is of great significance, but remains challenging to enhance activity. In this paper, we report an inverse catalyst constructed with nano-ZrZnO x supported on Cu particles with outstanding methanol synthesis performance at 220 ℃, two times higher than that of commercial Cu/ZnO/Al 2 O 3 catalysts under the same conditions. Detailed structure characterization and performance evaluation demonstrate that the ZrZnO x mixed oxide serves as the most active oxide-metal interface site for CO 2 hydrogenation. The ZrZnO x /Cu inverse catalyst increases the weak and medium CO 2 adsorption sites which are further demonstrated responsible to the methanol productivity. In situ DRIFTs studies reveal that the inverse interface accelerates the reduction of asymmetric formate intermediates and prevents the generation of CO. The combination of enhanced CO 2 activation capability and accelerated hydrogenation rate of intermediates over the ZrZnO x /Cu inverse catalyst probably contribute to the remarkable methanol synthesis performance from CO 2 .
研究领域:
催化化学
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能源化学
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材料科学
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产品关联
DOI
高影响因子
Catalysts
·
2025
·Vol. 15
·期 3
·250
·
IF 4
Jingjing Wang,Peixiang Shi,Jiahao Han,Yuhao Tian,Zhiqiang Yan,Pengcheng Luo,Hongyan Ban,Yanchun Li,Weijie Cai,Guanjing Lin,Zhiqiang Zhai,Congming Li
The hydrogenation of CO2to methanol over Cu-based catalysts is one of the attractive routes to reduce greenhouse gas emissions and generate high-value-added chemicals. Industrial CuZnAl catalysts possess some shortcomings, but various promoters can enhance the activity and durability of Cu-based catalysts for CO2hydrogenation. Herein, we systematically investigated the variations in the physicochemical properties of ternary CuZnM (M: Cr, Ce, Zr, Al) catalysts induced by different promoters, as well as their impact on CO2hydrogenation to methanol. The results demonstrate that the catalytic activity followed the order of CZCr > CZCe > CZZr > CZAl, with CZCr exhibiting the highest stability among them. Combined with XRD, SEM, TEM, H2-TPR, TPD, XPS, Raman findings and the experimental results, the smaller Cu particle size was conducive to increasing the CH3OH yield, and the lower Cu+/Cu0ratio exhibited better stability in CO2hydrogenation to methanol reaction. This approach offers theoretical insights and practical solutions for the industrial application of ternary Cu-based catalysts.
研究领域:
催化化学
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材料科学
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环境科学
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产品关联
DOI
高影响因子
FUEL
·
2024
·
IF 6.7
Wei Fu,Muhammad Kashif,Chen Cai,Jiayin Chen,Hao Zhou,Bingtao Zhao,Philippe M. Heynderickx,Yaxin Su
The hydrothermal technique was applied to prepare a new metal–organic framework, MIL-100(Fe), which was modified by ultrasonic impregnation with different wt % of copper. The results showed that the NO x conversion over 2.3Cu-MIL-100(Fe) was 100 % at 275 °C and maintained at ≥ 85 %, with N 2 selectivity ≥ 90 % in the temperature range of 275–400 °C and high SO 2 resistance. An increase in the Cu content up to 2.3 wt% showed the highest surface area (1206 m 2 /g) observed in N 2 adsorption–desorption. The results show that the introduction of Cu increased the oxygen vacancies on the catalyst surface. Electron transfer and a synergistic effect were observed between Cu and Fe. The shift of the reduction peaks to lower temperatures after the addition of Cu confirmed that Cu improved the reducibility of the catalysts. The 2.3Cu-MIL-100(Fe) exhibited the highest Lewis content (44.97 μmol/g), which functions as an active site for the selective catalytic reduction (SCR) reaction. By precisely controlling the acid-base properties of the catalyst, the specificity for the desired products can be increased in complicated reaction systems, especially in hydrocarbon-SCR technology.
研究领域:
材料科学
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环境科学
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催化化学
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Kailin He,Shunli Zeng
CuMn, CuMnCe, and CuCe metal oxide catalysts were prepared and applied in oxidizing CO and benzene as representative volatile organic compounds (VOCs). Various characterization methods and in situ diffuse reflectance infrared Fourier transform spectra (DRIFTS) were used to explore mutual effects between CO and benzene oxidation and the role of reactive oxygen species. CuMn shows the highest activity in independent and simultaneous oxidation of CO and benzene due to its spinel Cu 1.5 Mn 1.5 O 4 structure, which gives abundant Cu + sites, acidic sites, O α , and O β . Cu + sites and O α benefit CO oxidation, while acidic sites, O α , and O β contribute to benzene oxidation, producing intermediates decomposable at low temperatures. Mechanism study reveals that benzene inhibits CO oxidation by competing for O α at low temperatures to retard carbonate intermediates formation. CO enhances benzene oxidation by promoting benzene preliminary oxidation and intermediates deep degradation. On CuMn, the formation and degradation of maleate and acetate are facilitated, while maleate and formate degradation are promoted on CuMnCe and CuCe, respectively.
研究领域:
催化化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2025
·
IF 9.5
Zhijian Chen,Zhenghui Ma,Wenlin Yang,Guoli Fan,Baoming Ren,Feng Li
Due to the high energy barrier of C-C coupling and the intense competition from by-products, achieving superior ethylene selectivity in electrochemical CO2 reduction reaction (eCO2RR) remains challenging. Herein, we reported a distinctive Cu-based electrocatalyst fabricated from a three-dimensional (3D) tentacle-like Cu2(OH)2CO3 precursor. After electrochemical activation, abundant surface structural hydroxyls chemically bonded to Cu+ species (Cu+-OH structures) formed on the resulting Cu-based electrocatalyst. Such structural hydroxyl-rich Cu-based catalyst exhibited excellent eCO2RR performance, with a Faradaic efficiency (FE) of 43.7% for ethylene (partial current density up to 130.6 mA·cm-2) and a FE of ~70% for C2+ products at -1.5 V vs RHE in a flow cell, far exceeding those over the hydroxyl-deficient Cu-based one. By combining operando spectroscopic analysis with density functional theory calculations, it was unveiled that inherent surface Cu+-OH structures over Cu-based electrocatalysts could result in the electron loss of neighboring active Cu0 sites, which was favorable for the creation of crucial *COH and *OCCOH intermediates and thus the formation of ethylene product. Consequently, dual reaction pathways for the eCO2RR based on both key *COH and *CHO intermediates coexisting on the Cu-based electrocatalyst with abundant Cu+-OH structures powerfully boosted electrochemical CO2 reduction to produce ethylene. This work presents an innovative strategy for the construction of Cu-based electrocatalyst rich in structural hydroxyls and highlights the crucial role of inherent Cu+-OH structures in switching the formation of intermediates to boost ethylene production in the eCO2RR.
研究领域:
材料科学
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催化化学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
Inorganic Chemistry Frontiers
·
2019
·Vol. 6
·期 7
·1799-1812
·
IF 5.934
Xiaosong Hu,Chaoyue Zhao,Qingxin Guan,Xin Hu,Wei Li,Jun Chen
The chemical transformation of CO2 not only mitigates CO2 released into the atmosphere but also produces fuels and chemicals with important additional value. The activation of stable CO2 molecules is the key difficulty for the efficient conversion of CO2. Herein, we designed a ternary catalyst containing Cu, ZnO, and CeOx and dispersed them in SBA-15 using incipient wetness impregnation. Interestingly, the catalytic performances were improved greatly when the related active components were dispersed inside and outside the pore channels of SBA-15 using the incipient wetness impregnation method. Methanol and CO were controllably produced on the interface of Cu and metal oxides (ZnO and CeOx) due to the synergistic effects between the three active components. The metal oxides play a more important role in CO2 conversion as well as the product selectivity compared to Cu. CeO2 is more efficient than ZnO in promoting the dispersion of Cu nanoparticles and methanol generation. The suitable pore channels of SBA-15 promote the mass transfer and heat transfer while the high specific surface area is favorable to the dispersion of active components, which will facilitate the production of methanol and CO. After continuous hydrogenation evaluation for 100 h, the catalytic performance of the catalyst was still very stable. This work provides a viable strategy to prepare a supported catalyst with highly dispersed active sites, and the catalyst exhibits an efficient catalytic effect on producing methanol and CO.
研究领域:
化学工程
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催化科学
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产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2023
·
IF 5.5
Yaoyu Zhang,Yuxiong Wang,Yue Liu,Yuxing Wang,Ling Zhou,Huimin Xu,Zhongbiao Wu
A series of Cu-based catalysts with different types of supports (TiO 2 , Al 2 O 3 , S-1, HZSM-5 SiO 2 /Al 2 O 3 = 27 and 85) were investigated for selective catalytic combustion of acetonitrile (CH 3 CN). Among all catalysts, the Cu/TiO 2 and Cu/Al 2 O 3 catalysts had superior activity accompanied with the generation of massive NO x , while Cu/ZSM-5 catalysts exhibited excellent N 2 selectivity. The characterization results indicated that the surface acidity of catalysts played a decisive role in reaction behavior. For the Cu/TiO 2 and Cu/Al 2 O 3 catalysts mainly with Lewis acid sites, CH 3 CN underwent an initial hydrolysis step with surface hydroxy group to form acetamide anion (CH 3 CONH ad ), then occurred further hydrolysis reaction to form NH 3 at low temperatures, or turned to proceed oxidation reaction with numerous NO x generation at high temperatures. Whereas, the enriched Brønsted acid sites on the Cu/ZSM-5 catalysts brought abundant isolated Cu 2+ ions, which guaranteed the processing of iSCR reaction, thereby promoting the occurrence of hydrolysis and oxidation reaction pathways in parallel and benefiting the improvement of N 2 selectivity. These results elucidated the influence of supports with different acidic types in reaction pathway and provided precious reference for the development of high-performance NVOCs catalysts.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
·
IF 13.2
Wen-Jing Yi,Jingyi Yang,Yongzhen Gao,Xiaotian Zhou,Wenlei Zhang,Meng Zhang,Zhongyi Liu
Copper catalysts have garnered considerable interest as promising active metals for upgrading biomass resources, especially in selective furfural (FF) hydrogenation reaction. However, effectively enhancing the interactions between active metals and supports while providing abundant surface reaction sites remains enormous challenge to improve catalytic performance. Herein, we present a unique hydrotalcite-derived Cu-based catalyst featuring well-dispersed Cu 0 /Cu + nanodots towards selectively hydrogenated FF to furfuryl alcohol (FA). Impressively, the optimized CuMg 3 Al-R catalyst exhibits the exceptional hydrogenation performance, achieving almost 100 % FF conversion and 99.3 % FA selectivity. Comprehensive studies reveal that the small sized Cu species with well dispersion, the synergistic effect of Cu 0 and Cu + , combined with the selective adsorption and activation of C O groups jointly contribute to the enhanced catalytic performance. This work offers a promising strategy to rationally design well-dispersed Cu species for the selective hydrogenation of C O groups, which holds great significance for biomass-related hydrogenation reaction.
研究领域:
催化化学
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生物质能
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Honglin Li,Shoufu Cao,Hongman Sun,Yonglian Lu,Ying Zhang,Xiaoqing Lu,Jingbin Zeng,Zifeng Yan
Copper (Cu) has been proved as an efficient catalyst in carbon dioxide electrochemical reduction reaction (CO 2 RR) towards hydrocarbons, but still suffers from low selectivity and poor stability. Herein, Cu-based/CxNy catalysts were fabricated by facile pyrolysis of CuNCN in sealed quartz tubes. It is found that CuNCN pyrolyzed at 300 °C (CuNCN-300) exhibits a high C 2 H 4 Faradaic efficiency of 48.5% at 500 mA cm - 2 . However, increasing the pyrolysis temperature above 400 °C gives rise to CH 4 being the predominant product and CuNCN-500 achieves CH 4 Faradaic efficiencies of 66.3% at 300 mA cm - 2 . Combining experimental and DFT calculation results, Cu 3 N plays a crucial role in the formation of C 2 H 4 , while tri-s-triazine units in CuNCN-500 reduce the barrier of *CO hydrogenation to *CHO and retard C-C coupling on Cu surface. These findings mark the significance of precise tailoring of the synergistic effect between g-C 3 N 4 and different Cu species for achieving the desired selectivity during CO 2 RR.
研究领域:
材料科学
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电化学
·
理论计算
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2025
·
IF 4.8
Shuai Hu,Xiaoxuan Zhu,Yan Zhu,Chenliang Zhou,Gewen Yu,Yanming Wang,Cong Wang,Zhenfeng Wang,Jian Ding,Yuqing Wang,Xiaohui Guo
To enhance the activity and selectivity of Cu-based catalysts in the CO 2 hydrogenation reaction, this study systematically investigated the regulation effect of Nd-doping on the structure and surface properties of different oxide support (MgO, Al 2 O 3 , ZrO 2 , and CeO 2 ), and further explored its influence on the state of Cu species as well as the catalytic performance in CO 2 hydrogenation to methanol. The results show that the introduction of Nd 3 + can effectively induce lattice distortion of the support which promotes the generation of oxygen vacancies and the formation of surface basic sites, thereby enhancing the interfacial electronic interaction between Cu and support and improving the stability of Cu + active centers. Among them, the Cu catalyst supported on Nd-doped ZrO 2 exhibited the best catalytic performance such as the high CO 2 conversion and selectivity to methanol. Various characterization (XRD, SEM, in-situ XPS, H 2 -TPR, CO 2 -TPD, and H 2 -TPD) results confirmed the key role of Nd-doping in regulating the oxygen defects, electronic structure, and Cu species distribution over support. This study reveals the structural regulation mechanism of Nd in constructing efficient Cu-based catalysts for CO 2 hydrogenation from the perspective of support engineering, providing theoretical basis and practical guidance for the design of new high-performance catalytic materials.
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产品关联
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
·
材料科学
·
电化学
·
环境科学
✓ 已验证
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）